Formation of phosphorites during Upper Cenozoic phosphogenesis [26].
\r\n\t
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He holds 27 patents and has developed electrical equipment for machine tools, spooling machines, high power ultrasound processes and other, with the homologation of 18 prototypes and 12 zero manufacturing series.",coeditorOneBiosketch:null,coeditorTwoBiosketch:null,coeditorThreeBiosketch:null,coeditorFourBiosketch:null,coeditorFiveBiosketch:null,editors:[{id:"1063",title:"Prof.",name:"Constantin",middleName:null,surname:"Volosencu",slug:"constantin-volosencu",fullName:"Constantin Volosencu",profilePictureURL:"https://mts.intechopen.com/storage/users/1063/images/system/1063.jpeg",biography:"Constantin Volosencu is a professor at the Polytechnic University of Timişoara, Department of Automation. He is the editor of 9 books, author of 10 books, 5 book chapters, and over 180 scientific papers published in journals and conference proceedings. He is also a holder of 27 patents, and a manager of research grants. 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by",editors:[{id:"37194",title:"Dr.",name:"Theophanides",surname:"Theophile",slug:"theophanides-theophile",fullName:"Theophanides Theophile"}],productType:{id:"1",chapterContentType:"chapter",authoredCaption:"Edited by"}},{type:"book",id:"3161",title:"Frontiers in Guided Wave Optics and Optoelectronics",subtitle:null,isOpenForSubmission:!1,hash:"deb44e9c99f82bbce1083abea743146c",slug:"frontiers-in-guided-wave-optics-and-optoelectronics",bookSignature:"Bishnu Pal",coverURL:"https://cdn.intechopen.com/books/images_new/3161.jpg",editedByType:"Edited by",editors:[{id:"4782",title:"Prof.",name:"Bishnu",surname:"Pal",slug:"bishnu-pal",fullName:"Bishnu Pal"}],productType:{id:"1",chapterContentType:"chapter",authoredCaption:"Edited by"}}]},chapter:{item:{type:"chapter",id:"49984",title:"Phosphate Rocks",doi:"10.5772/62214",slug:"phosphate-rocks",body:'\nApatite [Ca5(PO4,CO3)3(OH,F,Cl)] is the most abundant phosphate mineral, which accounts for more than 95% of all phosphorus in the Earth’s crust and is found as an accessory mineral in most rock types[1] -\n on the Earth’s surface, primarily because it is stable in a wide variety of geological conditions and over a range of different geological processes [1],[2],[3],[4],[5],[6],[7],[8]. According to the list of symbols for rock- and ore-forming minerals, the abbreviated symbol used for apatite is Ap [9].
\nHowever, exploitable deposits of apatite are mainly found in igneous rocks and also in sedimentary and metamorphic rocks. The former comprises the stratiform phosphorite deposits in shelf-type shale-carbonate sequences, which contain high phosphorus ores of microcrystalline CO2-rich fluorapatite (francolite) and cryptocrystalline collophane. The igneous deposits comprise fluorapatite ores, which mostly accommodate carbonatites and other types of alkaline intrusions. The magmatic ores are generally of lower grade but give higher-quality beneficiation products with low contents of unwanted contaminants (Cd, Pb, As, U, Th, Mg and Al) [11],[12].
\nThe average distribution of trace elements in phosphate rock [17].
The beneficiation products of apatite ores as a commodity are traded as phosphate rock. It is the only significant global resource of phosphorus used dominantly in the manufacturing of nitrogen-phosphorus-potassium (NPK) fertilizers for food-crop nutrition and in the production of animal feed supplements. Only 10 – 15% of the world’s production of phosphate rock has other applications (e.g. pharmaceuticals, ceramics, textiles and explosives) and represents an important alternative source of rare-earth elements (REE) [12],[13]. The REE contents in apatites are useful in paleoceanographic studies to identify the seawater masses and circulation patterns or to quantify the redox state of the ocean [14].
\nThe composition of phosphate rocks varies from one deposit to another. Therefore, phosphate rocks from different sources may be expected to behave differently in beneficiation and acidulation processes. Phosphate rocks are primarily composed of the apatite group in association with a wide assortment of accessory minerals, mainly fluorides, carbonates, clays, quartz, silicates and metal oxides [13],[15],[16].
\nSi, Ca, Fe and Al are the most common companion elements in phosphate rocks, with the median abundances of 53.3 wt.%, 30.0 wt.%, 13.6 wt.% and 8.0 wt.%, respectively, compared with P2O5. In some low-grade phosphate rock mines, the content of Fe and Al is even higher than that of P2O5, and it is usual that the P2O5 content in phosphate rock is less than the Si and Ca content. In addition, some elements that are very rare in the Earth’s crust are found to be relatively abundant (Fig. 1) in phosphate rocks [17].
\nWhen rock contains phosphate components between 5 and 50% (by volume), then it is phosphatic, and the name of the main lithology is used as a suffix (phosphatic limestone, phosphatic claystone, etc.). In addition, the dominant textural form of the phosphate components in a phosphorite can be used in defining the rock name (e.g. peloidal[1] -) (phosphorite, coprolitic phosphorite, etc.) [10],[18].
\nThere are two main kinds of phosphate rocks deposits in the world [10],[20],[21],[22],[17],[23]:
Sedimentary phosphate rocks: marine phosphate deposit, metamorphic deposit, biogenic deposit (bird and bat guano accumulation) and phosphate deposit as the result of weathering. The sedimentary deposits contain the varieties of carbonate-fluorapatite that are collectively called as francolite (Section 2.6). The most common non-phosphatic accessory minerals associated with sedimentary phosphate rocks are quartz, clay and carbonates (calcite and dolomite). Phosphate rocks of high concentration of phosphates (10 – 15% of P2O5) are called phosphorites.
Igneous phosphate rocks: apatite is a common accessory mineral occurring in practically all types of igneous rocks (acid, basic or ultrabasic).
Depending on their origin (igneous or sedimentary), phosphate rocks have widely varying mineralogical, textural and chemical characteristics [23]. The locations of the major phosphate rocks deposit and producers are shown in Fig. 2\n [20],[24].
\nSedimentary phosphate deposits are exploited to produce about 80% of the total world production of phosphate rocks. Igneous phosphate deposits are often associated with carbonatites[1] - and/or alkalic (silica-deficient) intrusions. Igneous phosphate rock concentrates are produced from the deposits mainly exploited in Russia, the Republic of South Africa, Brazil, Finland and Zimbabwe. Igneous phosphate ores are often low in grade (less than 5% P2O5) but can be upgraded to high-grade products (from about 35% to over 40% P2O5) [22],[23].
\nThe distribution of the world’s phosphate resources [20].
The atom ratio of P:N = 1:15(16) in the oceans is not greatly different from that found in living organisms. The availability of soluble phosphate from weathering of apatite-containing rocks may initially has been the rate-determining factor in early live development. In most ecological systems, the phosphate content is the limiting factor for growth. Nearly all igneous rocks contain some phosphate, even if it is only ~0.1% (0.2% P2O5 on average in lithosphere), with nearly all of it in the form of apatite. Sedimentary rocks generally contain rather less (~0.1% P2O5 on average). Sedimentary phosphorite is believed to originate from widely dispersed apatite mainly in igneous rocks [25].
\nMost marine sediments and rocks contain less than 0.3% of P2O5. However, periodically through geological time, phosphorites (with the content of P2O5 of 5% or greater) formed on the seafloor in response to specialized oceanic conditions and accumulated in sufficient concentrations to produce major deposits of regional extent[1] - [26].
\nMarine phosphate formation and deposition represent the periods of low rates of sedimentation in combination with large supplies of nutrients. Phosphorus is then concentrated by various mechanisms, possibly bacterial (refer to discussion of Fig. 7), at either the sediment-water interface or within interstitial pore waters. This process leads to primary formation and growth of phosphate grains, which remain where they were formed or are transported as clastic particles within the environment of formation. During subsequent periods of time, some primary phosphate grains may be physically reworked into another sediment unit in response to either changing or different environmental processes [26].
\nStratigraphic distribution of phosphorites based on 1982 production data (a) and distribution of major Proterozoic-Cambrian phosphorites (b) [28].
The stratigraphic distribution[1] - [29] of phosphorites [28] is shown in Fig. 3(a). The major discoveries in Proterozoic and Cambrian rocks were not made until late 1930s, initially in the USSR (Kazakhstan), Poland, Korea, China and northern Vietnam. Early discoveries were made in the course of regional geological mapping and exploration for metal deposits, but later deposits were found mainly using more direct exploration techniques. It is possible that the greatest global phosphogenic episode in geological history took place in Late Proterozoic and Cambrian. While pelletal phosphorites are common in most Cambrian deposits, the Proterozoic age phosphorites contain mudstone (Fig. 3(b), microphosphorite) and stromatolitic phosphorite[1] - [28],[30].
\nSome phosphates were formed during all major sea-level transgressions during 67 million years of Cenozoic history; however, some periods were more important than others with respect to producing large volumes of phosphorites and preserving them in the geologic column. During the Paleocene and Eocene, several major episodes of phosphogenesis occurred within the major episodes of phosphogenesis in the major east-west ocean, which included Tethys [31],[1] - producing extensive amounts of phosphorites throughout the Middle East, Mediterranean and northern South American regions. By the Neogene, this circum-global ocean had been destroyed by the plate tectonic processes, and the north-south Pacific and Atlantic oceans dominated global circulation patterns. Upper Cenozoic phosphogenesis (Table 1) occurred along the north-south ocean-ways, which now contain modern continental margins. On the basis of the extent of known phosphate deposits, the Miocene was by far the most important episode of phosphate formation in Upper Cenozoic [26].
\nGeological period | \nAge | \nDuration | \n|||
---|---|---|---|---|---|
Phanerozoic (541 ma to present) Cenozoic (66 ma to present) | \nQuaternary 258 ma to present | \nHolocene 0.0117 ma to present | \n<3 ma | \n10 ta | \n|
Pleistocene\n 2.58 – 0.0117 ma | \n|||||
Neogene\n 23.03 – 2.58 ma | \nPliocene\n 5.333 – 2.58 ma | \n5 – 4 ma | \n1 ma | \n||
Miocene\n 23.03 – 5.333 ma | \n19 – 13 ma | \n6 ma | \n|||
\n | \n | Paleogene 66 – 23.03 ma | \nOligocene 33.9 – 23.03 ma | \n29 – 25 ma | \n4 ma | \n
Formation of phosphorites during Upper Cenozoic phosphogenesis [26].
ma – million years ago, ta – thousand years
Phosphorites and phosphatic sediments are known on the floor of the Pacific, Indian and Atlantic oceans. They occur in a number of inshore areas (the shelves and upper part of the continental slopes) and in pelagic zones, chiefly on seamounts. Most of the shelf phosphorites are localized in four very large oceanic phosphorite provinces [32],[26],[33]:
East Atlantic: Portugal, northwest Africa throughout South Africa and Agulhas Bank;
West Atlantic: North Carolina throughout Florida, Cuba, Venezuela and Argentina;
East Pacific: California throughout Baja California, Mexico and Peru throughout Chile;
West Pacific: Sakalin Island, Sea of Japan, Indonesia, Chathman Rise east of New Zealand and East Australian shelf.
Sedimentary rocks with the content of 18 – 20 wt.% of P2O5 are termed as phosphorites. The main phosphate mineral in phosphorites is carbonate-fluorapatite (CAF, francolite): Ca10−a−b−cNaaMgb(PO4)6−x(CO3)x−y−z(CO3,F)y(SO4)zF2, where x = y + a + 2c and c denotes the number of Ca vacancies, present as grain or mud. Most phosphorites are of marine origin [34],[35],[36]. Phosphorites on the sea floor occur in two types of environments on [37]:
Continental margins in association with terrigenous;
Submerged mountains in association with calcareous and volcanogenic rocks.
Phosphorites consist mainly of phosphate cement enveloping small grains of phosphatic and non-phosphatic materials. Phosphate in the cavities of foraminifera is purer than that enveloping the grains [37].
\nThe largest phosphorite-bearing regions are situated along the west coasts of Africa and America, at the east coast of the USA, off New Zealand and in the central part of the northern Pacific. The phosphatic matter of phosphorites consists of carbonate-fluorapatite and is intermixed with variable amounts of terrigenous, biogenic and diagenetic non-phosphatic components, which are the cause of a wide range of fluctuations in their chemical compositions. The age of sea-floor phosphorites varies from Cretaceous to Recent. Recent phosphorites are localized in the south west of Africa and at Peru-Chile shelves, which are the areas influenced by strong upwelling of nutrient-rich waters (Fig. 4(a)), resulting in high biological productivity, intensive biogenic sedimentation and diagenetic redistribution of geochemically active, mobile, organic-derived phosphorus in sediments. This phosphorus is accreted in the form of initially soft and friable nodules undergoing gradual lithification [27],[37].
\nThe surface currents in an idealized ocean, showing the areas of ascending nutrient-rich water (a) and the distribution of upwelling water and related phenomena in modern oceans (b) [27].
Pronounced climatic, biological and geologic effects accompany upwelling, especially where it is produced by the divergence in coastal areas (Fig. 4(b)). The presence of cold waters along the coasts produces the coastal fogs and humid-air deserts, such as those of northern Chile and southwest Africa. The nutrient-rich waters that lie alongside these deserts are the lushest gardens of the sea, as the upwelling cold waters there support tremendous quantities of organisms. Most of large accumulations of guano (Section 7.2.2) are formed by the seafowl colonies feeding in these waters, and it is the extremely dry climate created by upwelling that makes the preservation of guano possible [27].
\nSedimentary deposits usually contain varieties of carbonate-fluorapatite called francolite (described in Section 2.6). Francolite is defined as apatite that contains significant amount of CO2 with less than 1% of fluorine. Apatite associated with igneous source rocks may be of primary magmatic, hydrothermal or secondary origin. Primary apatite from igneous sources may be of fluorapatite, hydroxylapatite or chlorapatite varieties. Pure apatites from igneous deposits contain slightly over 42% of P2O5 [23].
\nSince a wide range of very different particles and processes of formation complicates the simple classification of phosphorites, there is not any unified phosphorite classification[1] - [18],[36],[38]. The proposed classification schemes for phosphorites describe their constituent particles, such as pelletal phosphorite. Nonetheless, the descriptor pelletal indicates nothing more than rounded phosphate particles of any origin. A widely recognized distinction in phosphorites is based on the grain size and holds specifically among phosphorites where the phosphate particles are of sand- or coarse silt-size and those that are of clay- and fine silt-size [28]. The phosphorites can be classified as follows [37]:
Non-conglomeratic (also termed as nodular) phosphorites: consist of phosphatized limestones and gluconate-quartz sandstones. Two varieties of nodular phosphorites can be recognized:
Ferruginized with glazed surface. The cement of ferruginized phosphorites is much richer in finely dispersed goethite than that of non-ferruginized phosphorites. Furthermore, ferruginized phosphorites do not contain the fragments of macrofauna.
Non-ferruginized with rough surface. In non-ferruginized phosphorites, the cement is micrite-collophane and its color varies form yellow (collophane, described in Section 2.6) to gray (micrite[1] - [19]). The chambers of foraminifera are filled with phosphate-carbonate cement, less often with glauconite or goethite (FeO(OH) [33]).
Some nodules of phosphatized limestone are coated with a discontinuous layer of secondary phosphate with the thickness up to 1 cm.
Conglomeratic phosphorites consist of pebbles of phosphatized limestone (up to 50% of the rock) held together by the cement similar in composition to the phosphatized glauconite-quartz sandstones described above. In many samples of this type, two or three conglomerate layers are clearly visible, differing in size of pebbles and in content of glauconite. The bedding planes separating the layers with denser or less dense packing of grains are also distinguished in the cement. The surface of these planes is glazed and brown due to higher content of iron hydroxides and organic matter. Upon impact, the rock breaks along the planes. In addition, irregular microerosion surfaces are observed in the conglomeratic phosphorites, which run across the grains of glauconite, shells and bedding planes [33].
The investigation of the microstructure of phosphorites by electron microscopy enables to recognize the following varieties [33]:
Gel-like, phosphatized diatomaceous oozes, analogous (except phosphate content) to the enclosing diatomaceous oozes.
Microgranular, forming solid masses and globules from 1 to 3 mm in diameter. The rough surface of phosphate is caused by the fact that it consists of granules less than 0.1 mm in size.
Fibrous, constituting inner parts of globules.
Ultramicrocrystalline phosphate, forming a “jacket” on the surface of globules of amorphous phosphate. The size of crystal of apatite is 0.1 – 0.3 μm.
Microcrystalline phosphate, consisting of crystal of 1 – 3 μm in size. Euhedral crystals are often formed in the cavities within the carbonate grains.
Multiphase microgranular cement consisting of carbonate, phosphate, quartz and layered silicates.
With regard to their texture and petrographic character, phosphorites can be classified according to the predominant size of the phosphorite component into four types [40]:
Microgranular (oolitic microgranular) phosphorites, conditionally including aphanite: 0.01 – 0.1 mm;
Granular phosphorites: 0.1 – 1 mm;
Nodular phosphorites: 1 – 5 mm;
Shelly phosphorites: 5 – 100 mm.
Although the types are named on the structural basis, the phosphate grains do not always have the dimensions given above. At the same time, the classified types fairly differ in many features, such as the association with various geological formations, the phosphate mineralogy and the stratigraphic sequence, thus being of lithologic character [40].
\nMost attempts to classify the phosphorite rocks adopt and modify the classification scheme for carbonates [36]. In 1962,
The classification scheme of carbonate rocks modified for phosphorites [28].
The macroscopic classification scheme for phosphate sediments suggested by
F-phosphates are friable, light-colored micronodules and peloids of carbonate-fluorapatite (CFAP); they were formed by the precipitation of CFAP in laminated diatom muds deposited within the oxygen-minimum zone.
Phosphatic sands, termed as P-phosphates, consist of phosphatic peloids, coated grains and fish debris, often having an admixture of fine siliciclastic grains. These sands occur in thin layers and burrowed beds up to 2 m thick.
Dark and dense phosphates, herein called D-phosphates, are the most abundant. They occur as nodules, gravels and hard grounds. These phosphates were formed through complicated cycles of CFAP precipitation during early diagenesis, erosion and exhumation and reburial and rephosphatization processes associated with changing energy conditions, which may reflect the effects of changes in the sea level.
CFAP cements in P- and D-phosphates are often replaced microbial structures, but our data do not reveal whether this microbial involvement was passive or active. F-phosphates are most common in deeper water, outer-shelf/upper-slope sites, whereas D- and P-phosphates tend to predominate at shallower shelf sites more subjected to episodic high-energy conditions, especially during the low stands of sea level. This concept reveals the paleoenvironmental and time relationships of various phosphate sediments [39],[43].
\nThe classification scheme of phosphorites proposed by Riggs (a) and Garrison and Kastner [\n43\n].\n
Phosphorites can be formed in nature authigenically or diagenically. In authigenesis, phosphorite forms as a result of the reaction of soluble phosphate with calcium ions forming corresponding insoluble phosphate compound. The role of microbes in these processes may be one or more of the following [44]:
Making reactive phosphate available;
Making reactive calcium available;
Generating or maintaining the pH and redox conditions, which favor the precipitation of phosphate.
The schematic presentation of formation of phosphorite in marine environment [44].
The models of authigenic phosphorite genesis (Fig. 7) assume the occurrence of mineralization of organic phosphorus in biologically productive waters, such as at ocean margins, that is, at shallow depths on continental slopes, shelf areas or plateaus [44].
\nHere, detrital accumulations may be mineralized at the sediment-water interface and in interstitial pore waters, liberating phosphate, some of which may then interact chemically with calcium in seawater to form phosphorite grains. These grains may be subsequently redistributed within the sediments units. The dissolution of fish debris (bones) is also considered an important source of phosphate in authigenic phosphorite genesis. The upwelling probably also plays an important role in many cases of authigenic formation of phosphorite. During non-upwelling period in winter, the phosphate-sequestering bacteria of oxidative genera Pseudomonas and Acinetobacter become dominant in the water column. Fermentative Vibrios and Enterobacteriaceae are dominant during upwelling in summer. It was suggested that Pseudomonas and Acinetobacter, which sequester phosphate as polyphosphate under aerobic conditions and hydrolyze polyphosphate under anaerobic conditions to obtain the energy of maintenance and to sequester volatile fatty acid from polyhydroxybutyrate formation, contribute to the phosphorite formation. Locally elevated, excreted orthophosphate becomes available for the precipitation as phosphorite by reacting with seawater calcium [44].
\nAuthigenic phosphorite formation at some eastern continental margins, where upwelling, if occurred at all, was a weak and intermittent process that may have been formed more directly as a result of intracellular bacterial phosphate accumulation, which became transformed into carbonate-fluorapatite upon the death of cells accumulated in sediments in areas where the sedimentation rate was very low [44].
\nThe model of diagenetic formation of phosphorite generally assumes the exchange of phosphate for carbonate in accretions that have the form of calcite and aragonite. The role of bacteria in this process is to mobilize phosphate by mineralizing detrital organic matter. The demonstration of this process in marine and freshwater environment under laboratory conditions leads to the hypothesis that the diagenesis of calcite to form apatite explains the origin of some deposits in the North Atlantic. The phosphorite deposits of Baja California and in the core of eastern Pacific Ocean seem to have formed as a result of partial diagenesis [44].
\nApatites of igneous origin include hydrothermal veins and disseminated replacements, marginal differentiations near the boundaries of intrusions and pegmatites, but the largest deposits are intrusive masses or sheets associated with carbonatite, nepheline-syenite and other alkalic rocks [27]. Igneous rocks are classified on the basis of their [21],[45]:
Color index: means the volume percentage of dark-colored mineral and divides the rocks to leucocratic (color index varies from 0 to 30%), mesocratic (from 30 to 60%) and melanocratic (from 60 to 100%).
Texture: coarse-grained rocks, which crystallize at depth, are termed as plutonic rocks (as the rate of crystallization is slow, such rocks are holocrystalline[1] -). Fine-grained rocks containing minerals embedded in glassy matrix[1] - (often devitrified) are named as volcanic or effusive rocks. The crystallization of volcanic rocks takes place on the surface and is associated with rapid cooling and loss of volatile constituents of the lava. Their texture is therefore vesicular [46][1] - (vesicle-rich) and hypocrystalline.[1] -\n
Rocks that crystallize partly at depth and partly near the surface are called hypabyssal\n[1] - (subvolcanic). The term porphyry is also related to hypabyssal rocks, which are characterized by one or more than one minerals present as phenocrysts in fine-grained groundmass.
Chemistry and mineralogy: the rocks comprising more than 90 vol.% of ferromagnesian minerals, such as olivine, pyroxene, amphibole and biotite, are called ultramafic (ultrabasic) rocks. The rocks composed from essentially one or more ferromagnesian minerals are termed as mafic\n[1] - (basic) rocks. In mafelsic rocks, the mafic and felsic minerals are present in approximately equal amounts. Felsic rocks\n[1] - contain predominantly light-colored minerals, such as quartz, feldspar, feldspathoid and muscovite.
An acidic rock contains > 60% SiO2, whereas a basic rock is characterized by silica content ranging from 44 to 52% of SiO2. Many of ultramafic rocks are ultrabasic with the content of silica < 44%, but such ultramafic rocks as pyroxenites and amphibolites are not ultrabasic, but they are rather basic [21].
Igneous rocks are formed by the solidification of silicate melt from high temperatures. Since the sequence of crystallization follows the liquidus-solidus phase relationships, the minerals of low content will normally crystallize the least, but diorite and granodiorite melts may have enough phosphorus present for the FAP phase field to intersect the liquidus and to allow early formation of fluorapatite. Later-crystallizing phases should form in the interstices between early-crystallizing phases of alkali-rich igneous rocks and should form an immiscible phosphate-rich liquid phase, which leads to large late-stage segregations of FAP, some of which are associated with magnetite [47].
\nWhere the content of phosphorus is very low, phosphorus may remain in the fluid phase, and apatite will form during the time at which the rock re-reacts with this fluid. This reaction is termed as pneumatolitic, and formed crystals will be small and often euhedral (with crystal facets). They may be included inside preexisting mineral grains. This situation is often encountered in granites and other related siliceous igneous rocks. The concentration of apatite minerals in igneous rocks is rarely sufficient to yield the source for mining the deposits for the phosphorus content [47].
\nThe biogenic (endogenous) mineral deposits form in surface environments as the transformation of primary organic aggregates or as a result of biochemical processes. Since the organism produces many of the same substances that form inorganically in rocks, the biogenic minerals are not minerals in the conventional sense1. Biogenic minerals originate from living organisms or with their assistance (Table 2). These compounds are crystallized within living organisms as a result of cell activity and are surrounded by organic matter. Classical examples are the bones of vertebrates. The bones and teeth consist of fine fibers or platy crystals (Section 10.9.2) of a mineral closely related to carbonate-hydroxylapatite (Section 4.6). These crystals are suspended in organic collagen. The crystals of apatite, which often do not exceed 10 nm in length, comprise up to 70% of weight of dried bone. The proteins make up the remaining 30% [48].
\nComposition | \nPlant or animal examples | \n|
---|---|---|
Silica (opal, chalcedony, quartz) | \nRadiolaria, siliceous sponges, diatomic algae | \n|
Carbonate | \nCalcite | \nArcheocyatha, foraminifera, stromatoporoids, carbonate sponges, echinoderms, brachiopods, belemnites, ostracods, coccolithophora, cyanophycerae, purple algae, some mollusk shells, eggshells or birds and reptiles | \n
Calcite crystals | \nEyes of trilobites and brittle star | \n|
Aragonite | \nCorals, shells of mollusks and cephalopods | \n|
Aragonite transforming to calcite | \nCorals, bryozoa, gastropods, pelecypods | \n|
Phosphate | \nApatite | \nBones, teeth, scales of vertebrates, brachiopods | \n
Barite, gypsum | \nEar stones of animals | \n|
Struvite | \nKidney and gall stones | \n|
Oxalates | \nWhewellite, weddellite | \nKidney and gall stones | \n
Phosphate-bearing carbonates | \nBrachiopods | \n|
Magnetite | \nIn brain tissue of birds and insects (carrier pigeons, bees, etc.), bacteria (Magnetospirillum magnetotacticum). Magnetite is used for navigation and orientation. | \n|
Fe-hydroxides | \nShells of diatoms, pediculates of Protozoa | \n
Mineralogical composition of solid plant and animal tissues [48].
In addition to the occurrence within the bones and teeth of vertebrates, mineral-organic aggregates are also found in mollusk shells, solid tissues of foraminifera corals, trilobites and other arthropods, echinoderms, some algae, etc. Some other biogenic processes involve bacteria. Large deposits of native sulfur, manganese oxides and hydroxides and iron are attributed to bacterial activity. Bacterial activity is also involved in the weathering processes of sulfide oxidation and transformation of kaolinite into bauxites [48].
\nBiogenic apatite is one of the most promising authigenic phases in this respect, as it is present in most siliciclastic deposits and is strongly enriched in a large suite of trace elements. Biogenic (fish teeth and bones) and diagenetic apatites are essential repositories of sedimentary phosphorus. They occasionally form huge deposits, as in West Africa, which are actively mined to provide agricultural fertilizers. Some of these deposits, found in particular in the Late Precambrian of China, after chemical precipitates seem to be associated with the episodes of global glaciation. In low-temperature waters, phosphates form numerous complexes. The concentration of phosphorus in sea and river water is limited by very low solubility of apatite. Phosphate radicals often attach to the surface of iron oxyhydroxide colloids when they precipitate in estuaries [49].
\nThe genetic classification proposed by
Silicate-apatite (ijolite[1] -): ijolite is a medium- to coarse-grained equigranular rock composed of nephelite and aegirite-augite, or other pyroxene, in nearly equal proportions. There are varieties richer in nephelite, approaching the composition of urtite.[1] - Nephelite is an equant anhedrons, pyroxene forms euhedral crystals with zonal structure and margin of more sodic pyroxenes than that in the center, which is commonly titaniferous. Some varieties contain titaniferous melanite and iivaarite. Apatite is a prominent constituent and titanate is generally present in small amounts.
Silicate-magnetite-apatite (phoscorite): phoscorites[1] - are spatially and temporally associated with carbonatites, often forming multiphase phoscorite-carbonatite series [56]. The term “phoscorite” was originally used to describe the magnetite-olivine-apatite rock with a carbonate core by
Carbonate-apatite (carbonatite): the crystalline products of low-volume and high-temperature carbonate melts that have been evolving from the upper mantle (Fig. 8) for at least the past 2 Ga. Many are associated with crustal complexes of alkali-rich silicate rocks from which they may have evolved by liquid immiscibility.
The location of upper mantle on the cross-section of the Earth, core and mantle drawn to scale [44] (a). Ternary equilibrium phase diagram of the apatite bearing ijolite-urtite rock (b) approximated by the system NaAlSiO4-CaMgSi2O6-Ca5(PO4)3F [6]: olivine (Ol), melilite (Me), silicophosphate (Sph), apatite (Ap) and immiscibility field (L1+L2).
The endogenous apatite deposits can be classified[1] - into the following types [60],[61]:
Crystallized and concentrated in the late magmatic stage, which can be further divided to (a) apatite-magnetite deposits (e.g. Kiruna deposit in Sweden) and (b) nepheline-apatite (e.g. Khibiny in Kola Peninsula in Russia).
Skarns (e.g. Ontario and Quebec in Canada).
Carbonatites (e.g. Sukulu in Uganda and Dorowa in Zimbabwe).
Hypothermal veins with phlogopite (e.g. Kaceres in Spain).
Mesothermal type (e.g. Toledo in Spain).
Metamorphosed sedimentary phosphates (e.g. Southern Peribaikalia, the Aldan massif in Russia (regional-metamorphosed subtype) and Karatau in Russia (contact-metamorphosis subtype)).
Sedimentary phosphates, which yield 85% of the world production, form in the sea by biochemical processes, in either:
Geosynclinal sea: e.g. in the Late Cretaceous and in Paleogene on the shelf of the Tethys geosyncline with the deposits in Morocco (Khouribga and Youssoufia), Algeria (Djebel Onk, El Kouit), Tunis (Gafsa), of the Permian geosyncline of the Rocky Mountains, with the deposits in the Phosphoria Formation in Idaho, Wyoming, Utah and Montana (USA), of the Caledonian geosyncline Karatau (Russia), large deposits are in the Upper Cretaceous in Kazakhstan, in the neighborhood of Aktyubinsk.
Epicontinental sea: e.g. in the Cenomanian of the south Russian digression and in the Jurassic of the Moscow region, at the margin of the African Shield in the Eocene complex near Hahotoe (Togo) and Taiba (Senegal), in the upper Cretaceous of Egypt [60].
The Earth’s crust contains about 0.27% of P2O5. About 200 minerals are known, which contain 1% or more P2O5. Minable concentrations of phosphate, containing from 5 to 35% of P2O5, are formed in all phases of the phosphate cycle (Section 7.3.1). The primary deposits include igneous apatites, sedimentary phosphorites and guano. The secondary deposits form from each of these as the result of weathering. Apatite is the principal primary mineral, but a number of others (Section 7.5) are common in the deposits formed during weathering of phosphate rocks and guano, e.g. brushite (CaHPO4·2H2O), monetite (CaHPO4), whitlockite (β-Ca3(PO4)2), crandallite (CaAl3(PO4)2(OH)5·H2O), wavellite (Al3(OH)3(PO4)2·5H2O), taranakite (K2Al6(PO4)6(OH)2·18H2O), millisite (Na,K)CaAl6(PO4)4(OH)9·3H2O), variscite (AlPO4·2H2O) and strengite (FePO4·2H2O) [27].
\nIn general, phosphate rock reserves are non-metallic ores[1] - that can be economically produced at the present time using existing technology. Phosphate rock resources include reserves and any other materials of interest that are not reserves. A reserve base is a portion of the resource from which future reserves may be developed. The classification applying to phosphate rocks include [23].\n\n
Resource is defined as a concentration of naturally occurring phosphate material in such a form or amount for which the economic extraction of a product is currently or potentially feasible. The resources are divided into many categories depending on the amount of pertinent information available to define the amount of material potentially available and if it is economic, marginally economic or sub-economic to exploit these resources.
Reserve base is the part of an identified resource that meets the minimum criteria related to current mining and production practices including grade, quality, thickness and depth.
Reserves are the part of the reserve base that can be economically extracted or produced at the time of the determination. They may be termed as marginal, inferred or inferred marginal reserves. This does not signify that the extraction facilities are in place or functional.
The grades of apatite deposits from the economic point of view are introduced in Table 3\n. The locations of the world’s phosphate deposits are shown in Fig. 9\n and the average content of P2O5 is listed in Table 4\n.
The most known Miocene phosphate deposits (Table 1) are in North Carolina, Florida, Venezuela, California, Baja California and Peru. In several cases, these emerged deposits are only the up dip limit of a larger Miocene section that extends seaward beyond the coastal plain and constitute large portions of the upper sediment regime that built the modern continental shelves [26].
\n\nGrade | \nP2O5 [wt.%] | \nBLP [%] | \nLocation | \n|
---|---|---|---|---|
1 | \nEconomic | \n20 | \n40.70 | \nFlorida and Moroccan sedimentary phosphorites, Kola and Palabora crystalline igneous apatites | \n
2 | \nSub-economic | \n5 – 20 | \n10.93 – 40.70 | \nWestern USA phosphoria, Russia nepheline-apatites | \n
3 | \nNon-economic | \n1 – 5 | \n2.19 – 10.93 | \nLow-grade ores, phosphatic limestones | \n
4 | \nNon-phosphatic | \n0.1 – 1.0 | \n0.22 – 2.19 | \nWidely distributed apatite in almost all igneous rocks | \n
Grades of apatite deposits [25].
The overview of the world’s phosphate deposits (a) [20] and the location of the major phosphate rock-producing areas of some known deposits (b) [26],[63].
Locally, these Miocene sediments are exposed on the seafloor; however, generally, they are buried below thin covers of Plio-Pleistocene and Holocene surface sediments. Thus, there is high potential for discovering new phosphate deposits within the Miocene sediments on the world’s continental shelves, because [26]:
Phosphate genesis is known to occur throughout the shelf in upper slope environments.
Thicker and more extensive sequences of Miocene sediments occur on the shelves than on adjacent coastal plains.
The shallow subsurface Neogene geology of most of the world’s shelves is poorly known.
Source | \n% | \nSource | \n% | \nSource | \n% | \n
---|---|---|---|---|---|
Fluorapatite | \n42 | \nTunisia (sedimentary) | \n28 | \nBasic slag | \n10 – 20 | \n
Kola (igneous) | \n40 | \nWest USA (phosphoria) | \n18 – 30 | \nBone meal | \n20 | \n
Nauru (phosphorite) | \n39 | \nQueensland | \n16 – 30 | \nGuano | \n12 – 15 | \n
Florida (sedimentary) | \n35 | \nVenezuela | \n20 | \nCalifornia (seabed) | \n30 | \n
Kazakhstan | \n23 | \nChina (Yunnan) | \n32 – 36 | \nAustralia (Queensland) | \n24 | \n
Morocco (sedimentary) | \n35 | \nKola (nepheline) | \n12 – 20 | \n— | \n— | \n
Grades of apatite deposits [25].
Two important sediment relationships were developed concerning reworked phosphate in surficial sediments on the North Carolina continental shelf [26],[63]:
The distribution of phosphate in surface sediments closely reflects the distribution within underlying Miocene sediments units.
The process of reworking significantly dilutes the concentration of phosphate in the surficial sediments.
The history of the discovery of the world’s phosphate resources [22].
These relationships were also recognized on the shelves of northwest and southwest Africa and could represent important exploration tools for richer Tertiary[1] - phosphorites occurring within the shallow subsurface on many continental shelves in the world [26].
\nThe deposits of apatite of igneous origin occur as intrusive masses or sheets, as hydrothermal veins or disseminated replacements, as marginal differentiations along or near the boundaries of intrusions or as pegmatites. Intrusive masses are the largest of these deposits. They are commonly associated with alkalic igneous rock complexes, many of which such as those in Africa, Brazil and Sweden are associated with the rift valley structures. Carbonatite, ijolite, nepheline-syenite and pyroxenite are common members of the rock assemblage. Many of these complexes have a ring like structure, with carbonatite as the central core [27].
\nPhosphate deposits have been discovered within the past 100 years at the rate far greater than the rate of consumption (Fig. 10). Since new phosphate deposits are expected to be discovered in the future, the oil exploration programs have probed most of the coastal sedimentary basins of the world during the past 20 – 30 years, and any large-scale discoveries of phosphate rock would probably have occurred in conjunction with these activities [22].
\nOther important commercial sources of phosphorus (Table 4) include [25]:
Guano [25],[27],[64],[65],[66]: natural deposit (accumulation) formed from decaying bones and excreta from fish-eating birds.[1] - Fresh seafowl droppings contain about 22% N and 4% P2O5. Bat guanos are the most abundant in the cave areas of temperate and tropical regions. Although many bat guano deposits were found and mined, most of them are measured in hundreds or thousands of tons, and only sporadic production is obtained from them now. Seafowl deposits are mainly confined to islands and coastal regions at low latitudes. The largest lie along the west coasts of lower California, South America and Africa and on islands near the equatorial currents.
It was known that bird dung was utilized by the Carthaginians as early as 200 BC in order to improve crop yields. The content of P2O5 in guano can vary in dependence on the age of the deposit,[1] - the local climate and the bird kind. Guano deposits are found in Chile, Peru, Mexico, Seychelles, Philippines, the Arabian Gulf and elsewhere, but they account for less than 2% of the world’s phosphate production.
Guano is used almost exclusively as fertilizers. The Nauru and Christmas Island phosphorite deposits may be guano in origin, but they are of very limited extent. It is believed that rainwater can carry soluble phosphate from guano and trickle over rocks, where phosphate interacts to form phosphatic layers, e.g. phosphatized coral rock. Bird guano, mainly from Peru, achieved the greatest importance in about the middle of the 19th century, shortly before the phosphate rock industry began to establish itself.
Basic slag [25]: is a minor source of phosphorus. This waste is the product from blast furnaces operating on iron ores with significant content of phosphorus. Basic slag contains tetracalcium phosphate (Ca3(PO4)2·CaO) and silicocarnotite (Ca3(PO4)2·Ca2SiO4), which are applied directly as fertilizers. Recorded world production is mainly from France, Germany and Luxembourg.
Meat and bone meal (MBM) or bone ash [25],[68]: as an animal byproduct, MBM contains not only substantial amounts of phosphorus in soluble organic form but also calcium and microelements. Ground (bone meal) or calcined and ground (bone ash) bones were recognized as a source of phosphorus at an early date.
Other important commercial sources of phosphorus are casein and lecithin. Casein is obtained from bovine milk. Lecithin was extracted from soy bean oil [25].
\nWeathering (Section 7.3.2) leads to the formation of enriched residual and replacing deposits from phosphatic deposits not otherwise minable. The Tennessee “brown rock” phosphate deposits consist of nowadays residuum developed through the decomposition of phosphatic limestones of Ordovician age. The “river pebble” deposits prominent in early history of phosphate mining in Florida and South Carolina are mostly placers formed by alluvial concentration of phosphatic pebbles eroded from the phosphatic formations of adjacent terrain [27].
\nThe Tennessee “white rock” and Florida “hard rock” deposits were formed by the redeposition of phosphate derived from the decomposition of apatite under more advanced weathering. The same decomposition-phosphatization process accounts for the formation of calcium aluminum phosphate and aluminum phosphate in the “leached zone” of the Bone Valley field and deeply weathered Cretaceous and Eocene deposits of west Africa [27].
\nAs was described above, the number of different elements can substitute into the structure of apatite,[1] - and this mineral can contain a number of trace elements by the substitution in both anion and cation sites. This means that apatite can be used as an indicator of planetary halogen compositions. The quantitative ion microprobe measurements of apatite from lunar basalts showed that portions of the lunar mantle and/or crust are richer in volatile species than previously thought [4].
\nApatite was also used to determine the characteristics of metamorphic fluids within the mantle. For example,
Apatite A: is inferred to result from the metasomatism by CO2- and H2O-rich fluids derived from a primitive mantle source region;
Apatite B: compositions are consistent with the crystallization from magmas within the carbonate-silicate compositional spectrum.
This classification is based on halogen content, presence or absence of structural CO2, Sr and trace elements (especially U, Th and light rare-earth) and association with either metasomatized mantle wall-rock peridotites (Apatite A) or high-pressure magmatic crystallization products (Apatite B) [4],[69],[70].
\nIn addition, apatite can be used as a probe to determine the petrogenetic evolution of granites, and significant amounts of research were devoted to the use of apatite in granitic rocks to distinguish between S- and I-type granites [4],[71].
\nThe chemical composition of apatite is also a useful guideline for the petrogenetic and metallogenic history of magmas for the following reasons [4]:
Apatite Eu and Ce anomalies provide the evidence of the redox state of the magmas that formed the host granitic rocks, with Eu enrichment and Ce depletion being indicative of oxidized magma and Eu depletion and Ce enrichment being indicative of reduced magma.
Apatite 87Sr/86Sr ratios reflect the Sr isotopic composition of the host granitic rocks.
Apatite F and Cl concentrations can reflect the enrichment or depletion of halogens within the host granitoids, with apatite associated with slab dehydration containing more Cl and less F, whereas apatites related to magmas formed by partial melting of the crust contain less Cl and more F.
In recent sedimentary systems, the major phosphorus deposition occurs within upwelling zones at continental margins. Upwelling of deep ocean waters rich in phosphorus triggers high biological production in the photic zone and eventually high concentration of phosphorus in organic-rich sediments, as in recent Namibian and Peruan shelves [72],[73], [74],[75].
\nIn the Earth’s crust, phosphorus takes the second place after carbon, and in comparison with all known elements, it takes about 12th place in natural abundance [25]. The phosphorus cycle is quite different from the nitrogen and sulfur cycles in which phosphorus is present in only one oxidation state and it forms no gases stable in biosphere or atmosphere. Also, in contrast to nitrogen and sulfur, substantial proportions of phosphorus in soil appear in inorganic form [76],[77].
\nAbout 10 Mt of phosphorus are released by weathering of apatite annually. In soil, monobasic (H2PO4\n−) and dibasic (HPO4\n2−) phosphates are generally available to plants. Phosphates are precipitated by calcium in alkaline soils and most of phosphate is adsorbed on aluminum and iron oxides in acidic soils. Phosphates are most readily available in slightly acidic to neutral soil. Much of such phosphorus in surface soils appears in organic matter. This phosphorus is used repeatedly by recycling in plants and organisms that decompose the plant detritus. Little amount of phosphorus is lost by leaching through soils, but the erosion losses of soil particles and the plant detritus carried off to aquatic systems may be substantial [76].
\nMajor natural cycle of phosphorus (a) and the contribution of the man to the cycle (b) [78].
The availability of phosphorus is a major factor limiting the biomass production in both terrestrial and aquatic ecosystems. Mycorrhizas are efficient scavengers of phosphorus for plants growing in soils with limited availability of this element. The phosphorus fertilization in agricultural lands can have detrimental effect, as it increases phosphate amounts in the runoff soil resulting in the accumulation of phosphate in aquatic plants and algal growth. If the decomposers of plants and algae use practically all oxygen from water, the habitat becomes unsuitable for fish and other aquatic animals. The process of abundant nutrient-induced biomass production in lakes and rivers and its decay to deplete the water oxygen is called the eutrophication [25],[76],[78].
\nDespite the advantage for which phosphorus is used, it is doubtful that man has significant contribution to the Earth’s cycle of phosphorus (Fig. 11). The 2·109 tons of mined phosphate rock is less than 0.15% of known reserves of phosphorus ore and less than 1·10−5% of the Earth’s cycle of phosphorus [78].
\nAt least 100 millions years before humankind exerted any influence on the cycles of phosphorus, the pattern had already been established (Fig. 12). Phosphorus was continuously leached from igneous rocks as the rocks were weathered to sedimentary deposits and this released phosphorus flowed to the seas, which had long since become saturated with phosphorus. Each new addition causes a similar quantity of phosphorus to precipitate as sediment. If the precipitate formed when an island sea had invaded a land area, the new sediment became landlocked. The new landlocked sedimentary deposits are more easily leached than igneous rocks from which they are derived. When the seas recede sufficiently to expose the new sediments to the greater solvent action of fresh water, the sediments begin to weather and the cycle is complete. Best estimates of the cycle time of phosphorus in the oceans today are in the range of 50,000 years. This is a short period compared to 3·109 years, which were required for the saturation of oceans for the first time [78].
\nThe establishment of the Earth’s cycle pattern of phosphorus [78].
Natural and artificial cycles of phosphorus [25].
Recently, man has only a slightly stronger influence on the total amount of the Earth’s phosphorus than his prehistoric ancestors. If man made a significant alteration in the cycles of phosphorus, it had an impact on the cycles of fresh surface waters. The detergent phosphates have been blamed for degrading freshwater lakes and there is no doubt that several lakes have been overabundant with phosphates and sewage. Sewage treatment will alleviate most of the problems associated with point-source loading of lakes [78].
\nThe overall natural and artificial cycles involving phosphorus are introduced in Fig. 13\n.
\n\nWeathering and leaching processes from millions of years ago led to the transfer of phosphate to rivers and oceans where it was concentrated in shells, bones and marine organism that were deposited on the sea floor. Subsequent uplift and other geological movements led to these accumulations becoming dry land deposits [25],[78].
\nGenerally, weathering of apatite occurs synergistically through biotic and abiotic processes and leads to the release of mineral phosphate. Inorganic phosphate cannot be assimilated by plants, but it can be converted to the bioavailable form orthophosphate (HPO4\n2−, H2PO4\n−) by some species of phosphate-solubilizing fungi and bacteria. The main mechanism underlying the microbial phosphate solubilization is the secretion of organic acids that, by changing the soil pH and acting as chelators, may induce the dissolution of phosphorus from minerals and its release into the pore water of soils [79],[80]. The dissolution of apatite is described in Section 3.4.
\nApatite represents an important source of inorganic P for natural ecosystems and may favor the establishment of microbial communities able to exploit it [79]. The microorganisms can cause the fixation or immobilization of phosphate, either by promoting the formation of inorganic precipitates or by the assimilation of phosphate into organic cell constituents on intracellular polyphosphate granules. Insoluble forms of inorganic phosphorus, e.g. calcium, aluminum and iron phosphates, may be solubilized through the microbial action. The mechanisms by which the microbes accomplish this solubilization vary [44]:
The first mechanism may be the production of inorganic or organic acids that attack the insoluble phosphates.
The second mechanism may be the production of chelators such as gluconate and 2-ketogluconate, citrate, oxalate and lactate. All these chelators can complex the cation portion of insoluble phosphate salts and thus force their dissociation.
The third mechanism of phosphate solubilization may be the reduction of iron in ferric phosphate, e.g. strengite (Fe3+PO4·2H2O [81]), to ferrous iron by enzymes and metabolic products of nitrate reducers such as Pseudomonas fluorescens and Alcaligenes spp. in sediments.
The fourth mechanism is the production of hydrogen sulfide (H2S), which can react with iron phosphate and precipitate it as iron sulfide, thereby mobilizing phosphate, as in the reaction [44]:
The phosphate-solubilizing ability is a feature of many free-living and plant-symbiotic bacterial taxa, such as [79]:
Pseudomonas [82]: the genus Pseudomonas sensu stricto comprises many species characterized by their metabolic diversity and by a wide range of niches that they can colonize.
Rhizobium [83]: specific group of bacteria that have the capability of symbiotic nitrogen fixation.
Burkholderia [84]: aerobic, non-spore-forming bacteria. Burkholderia is very versatile and occupies a wide range of ecological niches.
Microbial rock weathering is common in all climate zones and usually acts very slowly [80].
\nThe fission-track (FT) dating is a radiometric dating method[1] - based on the analysis of radiation damage trails (fission tracks) in uranium-bearing, non-conductive minerals and glasses. It is routinely applied to the minerals apatite, zircon and titanite. Fission tracks are produced continuously through geological time as a result of spontaneous fission track of 238U atoms[1] - that undergo spontaneous fission.[1] - The atom splits into two parts that move rapidly in opposite directions, creating a long thin region of damage. The submicroscopic features with an initial width of approximately 10 nm and the length of up to 20 μm can be revealed by chemical etching.[1] - Crucially, fission tracks are semi-stable features that can self-repair (shorten and eventually disappear) by the process known as annealing at a rate that is a function of both time and temperature. The extent of any track shortening (exposure to elevated temperatures) in a sample can be quantified by examining the distribution of fission-track lengths [6],[85],[86],[87],[88].
\nThis unique sensitivity of the apatite fission-track system is now of considerable economic importance due to the coincidence between the temperature range over which annealing occurs and that over which liquid hydrocarbons are generated. Other applications include the determination of timing of emplacement and the thermal history of ore deposits. There is abundant literature on both fission-track dating and its use in evaluating the tectonic and thermal history of rocks [6],[89],[90],[91].
\nApatite is the most frequently used material for fission-track dating [92]. Apatite fission-track (AFT) analysis serves as a thermochronological tool to investigate the low-temperature thermal history of rocks below ~120°C [93],[94]. The estimates of closure temperatures for fission-track retention in apatite are usually in the range from 75 to 120°C at cooling rates between 1 and 100°C/m.y. [6].
\nThermochronology may be described as the quantitative study of the thermal histories of rocks using temperature-sensitive radiometric dating methods such as 40Ar/39Ar and K-Ar, fission track and (U-Th)/He. Among these different methods, apatite fission track and apatite (U-Th-Sm)/He (AHe) are now, perhaps, the most widely used thermochronometers, as they are the most sensitive to low temperatures (typically between 40 and 125°C for the durations of heating and cooling in the extent of 106 years). They are ideal for investigating the tectonic and climate-driven surficial interactions that take place within the top few (<5 km) kilometers of the Earth’s crust. These processes govern the landscape evolution, influence the climate and generate the natural resources essential to the well-being of mankind [85],[95].
\nOn Earth, magmatic volatiles (i.e. H2O, F, Cl, C-species and S-species) play an important role in the physicochemical processes that control thermal stabilities of minerals and melts, in magma eruptive processes and in the transportation of economically important metals. On the Moon, magmatic volatiles in igneous systems are poorly understood, and the magmatic volatile inventory of lunar interior, aside from being very low, is not well constrained. Although the Moon is a volatile-depleted planetary body, there is evidence indicating that magmatic volatiles have played a role in igneous processes on the Moon. Specifically, magmatic volatiles were implicated as the propellants that drove fire-fountain eruptions, which produced the pyroclastic glass deposits encountered at the Apollo 15 and 17 sites [96]. That is supported by recent discoveries of water-rich apatite from lunar mare basalts [97],[98].
\nApatite was found in a large number of samples of igneous lunar rocks, although it typically occurred in only trace amounts and is typically reported as coexisting with REE-merrillite [(Mg,Fe)2REE2Ca16P14O56], and those two minerals make up the primary mineralogical budget for P on the Moon [96]. Merrillite, also known as the mineral whitlockite (or more precious and dehydrogenated whitlockite) [99], is one of the main phosphate minerals, along with apatite, which occur in lunar rocks, in Martian meteorites and in many other groups of meteorites. Significant structural differences between terrestrial whitlockite and lunar (and meteoritic) varieties require the use of “merrillite” name for the H-free extraterrestrial material, and the systematic enrichment of REE in lunar merrillite requires the use of “REE-merrillite”. Lunar merrillite, ideally (Mg,Fe2+,Mn2+)2[Ca18−x(Y,REE)x] (Na2−x)(P,Si)14O56, contains high concentrations of Y + REE [100],[101].
\nThe structure of lunar merrillite (a) [102] and terrestrial whitlockite (b).
Lunar merrillite (Fig. 14(a), trigonal, the space group
A number of sources potentially contributed to the overall inventory of lunar water, including primary indigenous water acquired during lunar accretion, late addition of water through asteroidal and cometary impacts and solar wind implanting H into lunar soils. The average D/H ratios of apatite in norite (Apollo sample 78235) and in the granite clast (14303) are consistent with the estimates for the H isotopic composition of recent bulk-Earth and terrestrial mantle. By contrast, the average H isotopic composition of apatites in norite 77215 is lower. The content of water in norite parental melts provides strong evidence that the magmas involved in secondary crust production on the Moon were hydrated, in agreement with recent findings of water in lunar ferroan anorthosites. Water they contain, locked in the crystalline structure of apatite, is characterized by an H isotopic composition similar to that on Earth and in some carbonaceous chondrites [103].
\nApatite preserves a record of halogen and water fugacities that existed during the waning stages of crystallization of planetary magmas, when they became saturated in phosphates. The thermodynamic formalism based on apatite-merrillite equilibria that makes it possible to compare the relative values of halogen and water fugacities in Martian, lunar and terrestrial basalts, accounting for possible differences in pressure, temperature and oxygen fugacities among the planets, was described by
They showed that planetary bodies have distinctive ratios among volatile fugacities at apatite saturation and that these fugacities are, in some cases, related in a consistent way to volatile fugacities in the mantle magma sources. Their analysis shows that the Martian mantle parental to basaltic SNC meteorites was dry and poor in both fluorine and chlorine compared to the terrestrial mantle. Limited data available from Mars show no secular variations in mantle halogen and water fugacities from ~4 Ga to ~180 Ma. Water and halogens found in recent Martian surface rocks have thus resided in the planet’s surficial systems since at least 4 Ga and may have been degassed from the planet’s interior during the primordial crust-forming event. In comparison to the Earth and Mars, the Moon, and possibly the eucrite parent body too, appear to be strongly depleted not only in H2O but also in Cl2 relative to H2O. The chlorine depletion is the strongest in mare basalts, perhaps reflecting an eruptive process characteristic with large-scale lunar magmatism [104].
\nMars does not recycle crustal materials via the plate tectonics. For this reason, the magmatic water reservoir of the Martian mantle has not been affected by the surface processes, and the deuterium/hydrogen (D/H) ratio of this water should represent the original primordial Martian value. Following this logic, hydrous primary igneous minerals on the Martian surface should also carry this primordial D/H ratio, assuming no assimilation of Martian atmospheric water during the crystallization and no major hydrogen fractionation during the melt degassing. Hydrous primary igneous minerals, such as apatite and amphibole, are present in Martian meteorites here on Earth. Provided these minerals have not been affected by terrestrial weathering, Martian atmospheric water or shock processes after the crystallization, they should contain a good approximation of the primordial Martian D/H ratio. As Nakhla was seen to fall on the Egyptian desert in 1911, the terrestrial contamination is minimized in this meteorite. The nakhlites are also among the least shocked Martian meteorites. Therefore, apatite within Nakhla could contain primordial Martian hydrogen isotope ratios. The similar D/H ratios indicate that the Earth and Mars, and possibly the other terrestrial planets, accreted water from the same source [105].
\nVesta, as the second most massive asteroid, has long been perceived as anhydrous. Recent studies suggesting the presence of hydrated minerals and past subsurface water have challenged this long-standing perception. The volatile components indicate the presence of apatite in eucrites. Eucritic apatite is fluorine rich with minor chlorine and hydroxyl (calculated by difference) [106],[107],[108].
\nThe biochemist and sci-fi author
The search for phosphate rock deposits became a global effort in the 20th century as the demand for phosphate rocks increased. The development of deposits further intensified in the 1950s and 1960s. The world production reached its peak in 1987 – 1988 and then again in 2008 with over 160 million metric tons (mmt) of the product. Phosphate rock mining has evolved over time, and worldwide, it relies on high volume and advanced technology using mainly open-pit mining methods and advanced transportation systems to move hundreds of millions of tons of overburden to produce hundreds of millions of tons of ore, which are beneficiated to produce approximately 160 mmt of phosphate rock concentrate per year. The concentrate of suitable grade and chemical quality is then used to produce phosphoric acid, the basis of many fertilizer and non-fertilizer products [23]. The world phosphate production rate since 1850 according to
The estimates of the world’s phosphate reserves and availability of exploitable deposits vary greatly and the assessments of how long it will take until these reserves are exhausted vary also considerably. Furthermore, it is commonly recognized that the high-quality reserves are being depleted expeditiously and that the prevailing management of phosphate, a finite non-renewable source, is not fully in accordance with the principles of sustainability. The depletion of current economically exploitable reserves is estimated to be completed in some 60 to 130 years. Using the median reserve estimates and under reasonable predictions, it appears that phosphate reserves would last for at least 100+ years [20].
\nWorld phosphate production rate [20].
Preliminary estimates of phosphate rock reserves range from 15,000 mmt to over 1,000,000 mmt, while the estimates of phosphate rock resources range from about 91,000 mmt to over 1,000,000 mmt. Using available literature, the reserves of various countries were assessed in the terms of reserves of concentrate. The IFDC[1] - estimate of worldwide reserve is approximately 60,000 mmt of concentrate. Based on the data gathered, collated and analyzed for the IFDC report, there is no indication that a “peak phosphorus” event will occur in 20 – 25 years. Based on the data reviewed, and assuming current rates of production, phosphate rock concentrate reserves to produce fertilizers will be available for the next 300 – 400 years [23].
\nPhosphate rock prices will increase when the demand approaches the limits of supply. When the phosphate rock prices increase, some resources will become reserves, marginal mining projects will become viable and the production will be stimulated. In the future, fuel and fuel-related transportation costs may become even more important components in the world phosphate rock production scenario. The political disruption is always an unknown factor, and it can profoundly influence the supply and demand for fertilizer raw materials on a worldwide basis [22].
\nApart from those in the supergroup of apatite minerals, the well-known phosphate minerals include [25]:
Autunite [110],[111]: is orthorhombic mineral (space group
The examples of forms and the structure of mineral atunite [110] viewed along the b-axis.
The mineral was named by The examples of forms and the structure of mineral meta-atunite [112] viewed along the b-axis.Fig. 17.
Crandallite [113]: CaAl3(OH)6[PO3(O1/2(OH)1/2]2, has hexagonal structure (a = 7.005 Å and c = 16.192 Å), which is analogous with alunite. The structure of mineral (Fig. 18) consists of corner-sharing Al octahedra, which are linked into trigonal and hexagonal rings to form the sheets perpendicular to the c-axis. Ca ions, surrounded by 12 oxygen and hydroxyl ions, lie in large cavities between the sheets. Each phosphate tetrahedron shares three corners with three Al octahedra from a trigonal ring in the sheet. The unshared corner is turned away from the trigonal hole towards the adjacent sheet to which it is hydrogen bonded. The mineral “deltaite” was found to be identical to crandallite, within the accuracy of the structural results. The structure of mineral crandallite [113] viewed along the c-axis.Fig. 18.
Lazulite [114],[115]: monoclinic mineral of the composition of MgAl2(PO4)2(OH)2, which crystallizes in the P2
The form and the structure of lazulite [114] viewed along the c-axis.
Millisite [116]: tetragonal mineral of the composition of NaCaAl6(PO4)4(OH)9·3H2O (the space group P4
Monazite [117],[118]: is natural light rare-earth element phosphate that generally contains large amounts of uranium and thorium. The monazite-type compounds (AXO4, Fig. 21) form an extended family that is described in this review in the terms of field of stability versus composition. They crystallize in a monoclinic lattice with the space group P2
The structure of monazite-(Ce): a = 6.7902 Å, b = 7.0203 Å, c = 6.4674 Å and β = 103.38° (a) and monazite-(Sm) (b): a = 6.6818 Å, b = 6.8877 Å, c = 6.3653 Å and β = 103.386° (b) [118] viewed along the b-axis.
Monazite (Fig. 20) and xenotime dimorphs[1] - [119] are the most ubiquitous rare-earth (REE) minerals. Monazite incorporates preferentially larger, light rare-earth elements (LREEs, here, La-Gd), whereas xenotime tends to incorporate smaller, heavy rare-earth elements (HREEs, here, Tb-Lu, and Y).\n
The classification diagram of AXO4-type compounds. The monazite stability domain is colored by gray [117].
The structure of tobernite and isostructural zeunerite [120] viewed along the c-axis.
Tobernite [120],[121]: tetragonal torbernite (
These minerals contain the autunite-type sheet, of the composition of [(UO2)(PO4)]−, which involves the sharing of equatorial vertices of uranyl square bipyramids with phosphate tetrahedra. In each of these structures, Cu2+ cations are located between the sheets in Jahn-Teller[1] - [122] distorted (4 + 2) octahedra, with short bonds to four H2O groups in a square-planar arrangement and two longer distances to oxygen atoms of uranyl ions. A symmetrically independent H2O group is held in each structure only by H-bonding, and in torbernite (and in zeunerite), it forms the square-planar sets of interstitial H2O groups both above and below the planes of Cu2+ cations. In metatorbernite (and in metazeunerite), the square-planar sets of interstitial H2O groups are either above or below the planes of Cu2+ cations. The bond-length-constrained refinement provides the crystal-chemically reasonable descriptions of H-bonding in those four structures [120].
Turquoise [123],[124]: CuAl6(PO4)4(OH)8·4H2O is a copper analogue of triclinic mineral fausite ZnAl6(PO4)4(OH)8·4H2O (the space group P1 with the cell parameters a = 7.410 Å, b = 7.633 Å, c = 9.904 Å, α = 68.4°, β = 69.65° and γ = 65.05°). The structure (Fig. 23) consists of distorted MO6 polyhedra (M= Zn, Cu), AIO6 octahedra and PO4 tetrahedra. By the edge- and corner-sharing of these polyhedra, a fairly dense three-dimensional framework is formed, which is further strengthened by a system of hydrogen bonds. The metal atoms in the unique MO6 (M = Zn or Cu) polyhedron show a distorted [2 + 2 + 2] coordination, the distortion being more pronounced in turquoise. About 10% of the M site is vacant in both minerals. In turquoise, a previously undetected structural site with very low occupancy of (possibly) Cu is present at the position (1/2,0,1/2). The structure of turquoise viewed along the b-axis [124].Fig. 23.
Vivianite [125],[126],[127]: is monoclinic mineral of the composition of Fe3(PO4)3·8H2O, which crystallizes in the space group of The structure of vivanite viewed along the b-axis [125].Fig. 24.
Wavellite [129]: the mineral of the composition of Al3(PO4)2(OH)3·4.5-5H2O (the space group Pcmn, a = 9.62 Å, b = 17.36 Å and c = 6.99 Å). The two aluminum atoms in the structure are octahedrally coordinated (Fig. 25): one is bonded to two O atoms, two –OH groups and two H2O molecules and the other to three O, two (–OH) and one H2O. Phosphorus is in tetrahedral coordination with oxygen. Al octahedra, linked through (OH) corners, form chains parallel to the c-axis, and P tetrahedra are attached to this chain by sharing O atoms of subsequent octahedra. An extra H2O molecule occupies the large cavity between the chains, and as indicated by a high temperature factor, it has a statistical distribution within this cavity. The structure of wavellite viewed along the b-axis (a) and stereoscopic view of the wavellite structure (b) [129].Fig. 25.
Xenotime [118]: monazite (Fig. 26) is isostructural with zircon (
The structure of xenotime-(Y): a = 6.8947 Å, b = 6.8947 Å and c = 6.0276 Å (a) and xenotime-(Dy) (b) a = 6.9052 Å, b = 6.9053 Å and c = 6.0384 Å (b) [118] viewed along the b-axis.
Isostructural arsenate analogues of many phosphate minerals are known, and in some cases, vanadates too. Some orthophosphates capable of forming complete ranges of solid solutions with the corresponding orthoarsenates are [25]:
Variscite group: MXO4·2H2O, where M = Fe, Al and X = P or As;
Fairfieldite group: Ca2M(XO4)2·2H2O, where M = Mn, Fe, Mg, Ni, Zn, Co and X = P, As;
Vivianite group: M3(XO4)2·8H2O, where M = Fe, Mn, Mg, Zn, Co, Ni and X = P, As;
Monazite group: MXO4, where M = Ce, La, Nd, Th, Bi and X = P, As;
Rhabdophane group: MXO4·H2O, where M = Ce, La, Nd, Th and X = P, As;
Xenotime group: MXO4, where M = Y, Ce, Bi and X = P, V;
Autunite group: M[(UO2)2(XO4)]·nH2O, where M = Ca, Ce, Ba, K, NH4\n+, Sr, Pb, Mg, Na, Zn and X = P, As, V;
Crandallite group: MM’3(XO4)2(OH)6·H2O, where M = Ca, Sr, Ba, M’= Al, Fe and X = P, As.
Phosphate minerals, like silicate minerals, are found with a great variety of cations. Unlike the latter group that contains numerous types of condensed silicate anions, almost all phosphate minerals are orthophosphates that contain PO4\n3− anion. Non-phosphorus anions, such as O2−, OH−, F−, Cl−, SO4\n2−, SiO4\n4− and AsO4\n3−, may also be present in these stoichiometric (or as occluded) materials [25].
\nUterine fibroids are high prevalent benign tumors that originate from muscle cells of the uterus with remained incompletely understood incidence, progression disease and natural history [1]. The above mentioned tumors may appear single or multiple but usually remain asymptomatic [1, 2]. Fibroids appear in various areas of uterus, different sizes and exist not a general accepted classification system for fibroid evaluation [3, 4]. They represent a tremendous public health problem with multiple difficulties and financial cost on society [1, 2, 3, 4].
Treatment strategies to prevent the fibroid limit growth and non-surgical treatment are needed [5, 6, 7, 8]. Minimally invasive methods like uterine artery embolization (UAE) as treatment option of fibroids by retaining the uterus among the women during middle or late reproductive years is the summarized goal of this literature review with detailed 12 years results report of Department Obstetrics and Gynecology in cooperation with Interventional Radiology Unit of Radiology Department, Democritus University of Thrace in Greece. The aim of this retrospective study was to investigate the contribution of UAE and the occurrence of transient, or permanent amenorrhea as well as reappearance of regular menstruation, inflammation, pain in premenopausal women up to one year of postoperative follow-up UAE.
The fibroids occur in a phenotype in wide of genetic diseases, clinically not as single disease entity and their progression varies and based on the various types of disease in different national groups [9, 10]. The incidence of asymptomatic but sonographically fibroids detected as remarkably high and the incidence depending on women age and race. Their prevalence is 9% in white women, three to nine times higher prevalence in African American, diagnosed in 3.3% of 25 to 32 year olds, 7.8% of the 33 to 40 year olds and increased 20-fold to 6.20 per 1000 women years by ages 45to 50 [9, 10, 11, 12, 13, 14]. Familial aggregation studies confirm heritability of fibroids 2.5 times more at risk in first degree relatives, increasing to 5.7 for women with an affected first degree relative of less than 45 years old. The grow and recur rate of fibroids after abdominal myomectomy reported as 5 year risk 62% with 9% risk an additional major surgical procedure. Relapses of 27% over a period of 10 years are reported with increasing frequency rate approaching to premenopausal period [9, 14, 15].
The recurrence risk is lower in women with single fibroid with small size and in those women who noticed a subsequent successful pregnancy. Oral contraceptives administration decreased the occurrence of fibroids depending to the duration of oral contraceptives use [16, 17, 18]. Moreover, early menarche and high body mass index (approximately 18% for each 19 kg increase) are some other factors that lead to the development of fibroids [9, 14, 15, 19]. Clinically fibroids occur at least three distinct phenotypes like: single, multiple varying size and in association with adenomyosis or alone [9]. Fibroids interfere not only with implantation but also with successful labor and if there are not existing, is for a woman more likely to be pregnant. Pregnancy prevents the development of fibroids, because is associated with fibroid inflated effect [9, 14, 16, 17, 18]. The risk of fibroids decrease with parity up to fivefold [9, 14]. Although subfertility may be caused by fibroids, however the detected fibroids during pregnancy not influence the age of delivery of the first child, but change the age of last term labor. The presence of fibroids in the majority are not associated to any symptoms but is poorly explain their contribution to symptoms menstrual disorders heavy menstrual flow or longer duration of menses, pelvic pain and infertility. Based on the published literature is demonstrated a relationship between diastolic pressure and fibroids [9, 16, 17, 18, 19, 20]. High diastolic blood pressures led to atherogenesis, cause injury and damage of muscle cells like a similar mechanism as in vascular muscle system, release cytokine in uterus muscle, which led to promotion of fibroid growth [9, 16, 17, 18, 19, 20]. Approximately 10 mm Hg increasing of blood pressure led to 8–10% increased fibroid risk. Myometrial injury based either on ischemia, hypertension or atheromatic type mechanisms are associated positively also to pelvic inflammatory disease [9, 16, 17, 18, 19, 20]. The risk of fibroids is low, if the estrogen levels are low and this could be explain the low risk associated with smoking, alcohol and caffeine consumption.
Some fibroids reflected genetic syndromes feature fibroids development such Reed’s, Bannayan Zonana, Cowden syndrome, herediatary leiomatosis and renal cell cancer (HLRCC). Reed’s syndrome is well known as familial leiomyomatosis cutis and uteri (MIM150800) is an autosomal dominant trait with reduced penetrance associated with cutaneous fibroids. Bannayan Zonana (MIM153480), Cowden (MIM158350) syndromes are autosomal dominant hamartomatous polyposis disorders included lipomas, interstinal hamartomatous polyps and various nonneoplastic manifestations [21, 22, 23, 24].
Intracellular mutation such as chromosomal translocations and deletions are reported. None of the mentioned patterns of inheritance have been clearly proved in fibroids as a solitary phenotype.
In addition, different genetic subtypes can be found in different fibroids of the same patient. Many fibroids in a uterus may be of different cytological origin. The heterogeneity from growth and development of fibroids based on enzyme glucose-6-phosphate dehydrogenase (G6PD) isoenzyme analysis and using androgen receptor (AR) gene assays reveal that fibroids are monoclonal lesions arise independently from the same uterus and may associated to various chromosomal abnormalities which results in a distinct fibroid is a monocyte in the origin of the monoclonal independent lesion [25, 26, 27, 28].
In uterus referred high rate of estrogen receptors, which comprised spiral linear muscle fibers separated from the natural surrounding uterine muscle tissue by a pseudocapsule of connective tissue.. Many distinct factors contribute to tumor progression [25, 26, 27, 28].
Approximately 40% of fibroids are karyotypically abnormal which compared to normal fibroids are generally more cellular and have a greater mitotic index lower DNA content. The most prevalent types of chromosomal aberrations are as following: t(12,14), (q14-q15,q23-q24), rearrangement of 6p21, del(7)(q22q32), 1p36, 10q22, 13q21–22 nad of x chromosome partial deletion 3q, trisomy 12. [29, 30, 31, 32]. Fibroids with abnormal karyotypes are associated to anatomically positions 12% of submucosal, 29% of subserosal and 35% of intramural. Based on low frequency of karyotypic rearrangement is the explanation that submucosal fibroids are highly symptomatic and led to menorrhagia. Further research in the genetics of fibroids is needed to investigate the heritability based on their clonal mosaic nature to correlate genotypic and clinically characteristics. [29, 30, 31, 32, 33, 34].
In UAE practice for therapy of symptomatic types adenomyosis either of pure (diffuse, focal) or mix form (coexistence with fibroids) in 70% and 30% of cases respectively depending on size and number of fibroids (adenomyosis dominance, fibroid dominance) is reported a ratio 7:2:1 between the treated women [35].
Adenomyosis is characterized by the development of ectopic endometrial glands and a stroma in the myometrium, at a depth > 2.5 mm from the endometrial-myometrial separation surface and moreover by hypertrophy or hyperplasia of the smooth muscles of the myometrium [36, 37, 38, 39]. An older description is given by Rokintasky 1860 adenoid cystosarcoma of the uterus and for the first time by Frankl 1925 the term of adenomyosis of the uterus. [36, 37, 38, 39]. Clinical diagnosis of adenomyosis is only hypothetical, histological examination poses diagnosis of the disease after hysterectomy. [36, 37, 38, 39]. It is diffuse (adenomyosis) or focal (adenomyoma), asymmetrically affects the uterine wall of premenopausal women (usually the posterior) and often coexists with myomas [36, 37, 38, 39]. The disease is common (5% - 70% in the surgical series, using strict criteria 10% - 18%), progressing and manifested with non-specific symptoms, which are similar to the symptoms caused by myomas (bleeding - anemia, pain, dysmenorrhea, dyspareunia, pelvic load (bulk symptoms) - sensitive uterus or a combination of the above), so it is difficult to diagnose only by clinical criteria [36, 37, 38, 39]. An incidence of 10% -30% is described, in hysterectomy preparations it was found in a percentage of 10% - 18%. 80% of women with adenomyosis have another uterine condition like pelvic endometriosis and endometrial polyps (2% - 20%) endometrial hyperplasia, adenocarcinoma [36, 37, 38, 39]. In 35% of women with adenomyosis do not show any symptoms and the diagnosis of the disease is random [38, 39, 40, 41]. The pathogenesis of adenomyosis remains unknown. Etiology: According to various studies the endometrial glands of the disease express more in immunochemical examinations the ratio of HCG/LH receptors found in endometrial cancers and trophoblastic disease, compared to natural [36, 37, 38, 39]. Other theories of pathogenesis include elevated estrogen levels, endometrial injuries in surgeries such as scraping, fibromyectomy, cesarean section, and residual of Muller Duct. Adenomyosis occurs mainly in multiparas with an incidence of 5–70%. Symptoms of adenomyosis (menorrhagia (50%), dysmenorrhea (30%), uterine bleeding (20%), dyspareunia (sporadic additional symptom) [38, 39, 40, 41]. The clinical diagnosis of adenomyosis is only hypothetical and only histological diagnosis makes the diagnosis of the disease after hysterectomy. Preoperative transvaginal ultrasonography (TVUS) and magnetic resonance (MRI) are useful diagnostic examinations Main diagnostic TVUS criteria are as following: asymmetrical uterine enlargement, subendometrial halo thickening, indistinct endometrial myometrial border, myometrium is thickened ventrally and associated to heterogeneous echotexture. MRI is another recommend imaging examination preprocedural of UAE with higher specificity compared to TVUS approximately (86–96%)and excellent to recognize fibroids,adenomyomas if the myometrial thickness is increased or the myometrium occur anatomical area changes In focal adenomyosis occurs low signal intensity within the myometrium, while in diffuse adenomyosis appear the junctional zone diffuse thickening also with low signal intensity in T2 weighted MRI The treatment options are: Drug treatment (usually ineffective), Presence of estrogen receptors in fibroids promote the increase in fibroid size. Progesteroids such as medroxyprogesterone acetate, norethindrone in GnRH-suppressed patients may increase in size. Stimulation of fibroid enlargement is a complex process involving the interaction of estrogen-progestogens in combination with local growth factors [38, 39, 40, 41]. Antiprogesteroids such as mifepristone RU-486 reduce fibroid size. Invasive treatment of fibroids: myomectomy (open - intra-abdominal, laparoscopic, hysteroscopic), hysterectomy, myolysis - catalysis cryocatalysis, thermal catalysis by microwave or radio frequency (RF-ablation), ultrasound focus catalysis (FUS) and laser photocatalysis] and uterine artery percutaneous embolization (UAE) [38, 39, 40, 41, 42].
The majority of 60–70% are asymptomatic. The clinical recognized significantly underestimates the true occurrence due to the fact that the routine ultrasound screening in not obligatory indicated [43, 44, 45, 46].
Approximately 62% of women with symptomatic fibroids visit the gynecologists due to multiple symptoms depending on their anatomical location, (subserosal, intramural, submucosal or intracavity) size number and associated degenerative morphological changes [43, 44, 45, 46]. The referred symptoms are as following: abnormal vaginal bleeding (most common), anemia, pelvic mass, frequent urination, possible incontinence constipation tenesmus rectal pressure, pelvic pain and infertility[43, 44, 45, 46]. Pregnancy related fibroid behavior: growth which is reported controversy concerning to increasing or remain the same the uterus size, degeneration, pain, spontaneous abortions, obstetric complication (premature labor in 15%, intrauterine restriction in 10% and malpresentation in 20%) .[43, 44, 45, 46]. The pregnancy in coesting of fibroids depending on their anatomical location and the distance to placental site. Other rare associations are as following: Ascites development due the transudation of fluid after torsion and obstruction of vessels in floating fibroids, Polycythemia secondary detected, familial syndromes with renal cell carcinoma, intravenous leiomatosis and benign matastasizing uterine fibroids [43, 44, 45, 46].
The most common symptom in the majority of cases in clinical practice is the abnormal vaginal bleeding. This symptom in association with myomas occurs either as menorrhagia or hypermenorrhea, while metrorrrhagia is not typical for fibroids and need more investigation to rule out malignancies. The exact mechanism of abnormal bleeding from fibroids is not yet well known. Fibroids alter the nature of uterine muscle contractions and prevent the uterus from controlling the degree and intensity of bleeding during menstruation. The submucosal fibroids due to total or partial protrusion in uterus cavity led most likely to menorrhagia while the intramural myomas have obstructive effect on uterine vessels and subsequent led to endometrial vessels ectasia with profuse menstrual bleeding [43, 44, 45, 46].
Hypermenorrhea occur most likely in endometritis in association to submucous myomas. The palpation of myomas based on enlarged irregular uterine contour can be useful to clinically diagnosis of fibroids and the findings described as uterus size like in pregnancy [43, 44, 45, 46, 47, 48]. If the uterus size is more than 12–20 week can be palpated on abdominal examination. In cases of increased size of uterus arise pelvic pressure on adjacent organs like urinary tract, rectosigmoid with frequent urination, ureteral obstruction tenesmus due to incarceration of enlarged uterus in Douglas pouch and dysmenorrhea [43, 44, 45, 46, 47, 48].
The incidence of malignant mutation in sarcomas is reported to be 0.1–0.29% of diagnosed fibroids [43, 49, 50]. Leiomyosarcoma is an independent malignant tumor in the absolutely majority and arises de novo, however recently published studies reveal that in very rare cases is possible in fibroids with chromosome deletions to develop in leiomyosarcoma most common in the 5th–6th decade of life. Γλωσσική επιμέλεια.
It is characterized by extensive abnormal bleeding and a rapid increase in uterine size in postmenopausal patients [43, 49, 50]. The main microscopic features which are significant predictors of leiomyosarcoma clinical course included: coagualtive tumor cell necrosis, degenerating hyperchromatic, pleomorphic nuclei, cytologic atypia, mitotic index MI (MI denotes definite mitotic figures (mf) per 10 high power field (hpf) MI ≥ 5mf/10hpf, differentiation. In case of fibroids, the MI < 5mf/10hpf no atypia and necrosis and in the subgroup of leiomyosarcoma or smooth muscle of uncertain malignant potential (STUMP) [43, 49, 50]. In STUMP tumors the main diagnostic criterion associated to prognosticate biologic behavior is the MI < 5mf/10hpf but is presence of moderate to severe atypia without necrosis [43, 49, 50]. The least subgroup of tumors is accompanied by lymph nodes in the lung or other sites with histopathological occurrence similar to the original tumor approximately 15 years after hysterectomy. Immunostaining for expression of cell cycle regulatory proteins like Ki-67,cyclins E,A,cdks (cdk2,cdc2), p16, progesterone receptors, p53 Her-2/neu based on significant elevated levels in leiomyosarcomas can be useful in discriminating and identifying STUMP tumors, leiomyosarcoma and fibroids [43, 49, 50].
The uterine fibroids is the most common uterine pathology with a prevalence more than 25% of all reproductive years and approximately 1.6 million women in United States diagnosed with uterus myomatosus. Asymptomatic fibroids could be found incidentally on pelvic imaging and management therapeutical strategy depending on their causing clinical symptoms [51]. If cases which are asymptomatic need not any treatment and after menopause due to their regression expectant management is the recommended therapy option. In symptomatic fibroids based on the most common symptoms, heavy menstrual bleeding and painful menstruation is very useful. Fibroid classification system based on the fact that the above mentioned symptoms caused by fibroids which distort the uterine cavity [49].
Fibroid classification system is referred as following:
Type 0 completely intracavity fibroids.
Type1 ≥ 50% in the cavity intramural.
Type 2 < 50% in the cavity intramural.
Type 3 intramural but approach endometrium.
Type 4 intramural.
Type 5 subserosal but at least 50% intramural.
Type 6 subserosal but less than 50% intramural.
Type 7 subserosal pedunculated.
Type 8 cervical [51].
According to Donnez [52, 53] staging, submucosal fibroids are classified as following:
Grade I Fibroids with the largest diameter in the endometrial cavity.
Grade II Fibromyomas with the largest diameter in the myometrium.
Grade III Appearance of multiple fibroids>2.
Medical therapies based on therapeutical manipulating the fibroid hormonal environment. Steroid hormones, especially estrogen and progesterone are associated to fibroids behavior, proved by clinical molecular biological pharmacological models and play an important role to their medical treatment. The combination of estrogen progestin or progestin alone is the first line medical therapy for uterine fibroids.
GnRH (gonadotropin releasing hormone)-agonists led to down regulation of GnRH receptors at level of pituitary after initially increase the release of gonadotropins flare effect of heavy vaginal bleeding, reduce the FSH (follicle stimulating hormone) LH (luteinizing hormone) and ovarian steroid hormone and produce a hypoestrogenic menopause state [52, 53, 54, 55, 56]. Subsequent results amenorrhea and reduction of the size of fibroids pronounced within three months after beginning of treatment [54, 55, 56, 57, 58]. The reduction can reach 40–50% of the tumor in 3 months but is reversible after stopping treatment. This effect is more pronounced in submucosal fibroids due to a higher number of estrogen and progesterone receptors.
GnRH antagonists often used to treat myomas before surgical procedure, block pituitary receptors and led immediately to declination of FSH, LH levels and fibroid, uterus volume reduction within 3 weeks of therapy beginning. Their directly promptly block gonadotropin effect has rapid clinical character and is associated to initial flare effect. They are currently indicated only for ovulation induction [54, 55, 56, 57, 58].
The presence of aromatase in fibroids and additional to ovarian estrogen activity, interleukin 1βc AMP analoque, prostaglandin E2 led to estrogen production in fibroids cells [54, 55, 56, 57, 58]. Fibroids express aromatase higher levels compared to surrounding intact myometrium. In these cells occur significant conversion of androstendione to estrone and subsequent to estradiol which has full biologic activity and act positively to significant stimulation of proliferation of fibroids cells [54, 55, 56, 57, 58].
Aromatase inhibitors inhibit ovarian and peripheral estrogen production due to cellular proliferation inhibition, androstendione inhibition and reduce estradiol levels after 24 hours of treatment. SERMs (selective estrogen receptor modulator) are nonsteroidal agents who bind estrogen receptor and based on target tissue show estrogen agonist or antagonist effect [51, 59, 60]. While the SERM Tamoxifen has agonist effect in endometrium, Raloxifen exhibit no agonist activity and decrease the fibroid size. Antiprogesterone agents act at the level of progesterone receptors (PR-A PR-B), which are abundant in the fibroid. It is reported that progesterone induce proliferation, up regulate growth factors, antiapoptotic proteins like EGF in fibroid cells [51, 59, 60]. Mifepristone is the most studied antagonist of progesterone and due to high progesterone affinity led to amenorrhea, reduction of fibroid size and improvement the clinical symptoms [51, 59, 60]. The administration of ulipristal acetate, who is a selective progesterone receptor modulator, has proved successful effects on therapy of fibroids with clinical symptoms reduction of their size and endometrium cystic glandular changes. Danazol (19a nortestosterone derivate) inhibits pituarity gonadotropin secretion, led to ovarian steroid production and suppression of endometrial growth after 6 months treatment [51, 59, 60]. The use of progestin containing intrauterine contraceptive device (LNG -IUDs) as local therapy for menorrhagia and symptomatic uterine fibroids has been studied and confirmed a significant reduction in bleeding and fibroid size. However uterus myomatosus with a distorted uterine cavity or a submucosal fibroid is a contarindication for LNG –IUD [51, 59, 60].
Although the traditional treatment for uterine fibroids remains the hysterectomy either abdominal or vaginal classical, total laparoscopic assisted vaginal hysterectomy, robotic assisted laparoscopic hysterectomy as the predominant surgical procedure, however is preferred only in women who have completed their family planning [61, 62, 63, 64, 65].
In late reproductive age and premenopausal period available therapeutic options to preserve the uterus allow possible an attempt at conception and are surgical or conservative options. Over the past decade, the hysterectomy rate has decreased while alternative therapy options for symptomatic fibroids have been increased. The surgical procedures include myomectomy, abdominal myomectomy, laparoscopic myomectomy, laparoscopic thermal ablation, percutaneous ablative methods, hysteroscopic myomectomy, myolysis, laparoscopic morcellation and finally uterine artery ligation and occlusion performed either as surgical ligation during laparoscopy [61, 62, 63, 64, 65]. (παρακάτω θα μπορούσε να μπεί παράγραφος για τους κινδύνους της σε περίπτωση STUMP tu).
In cases of laparoscopic morcellation is of great importance to exclude based on evaluations criteria like presence of coagulations necrosis, no significant atypia and mitotic index ≤10 STUMP tu due to unknown malignant potential behavior. Minimally invasive therapies non-surgical procedures are as following: Magnetic resonance guided focused ultrasound ablation (MRgFUS) and UAE. MRgFUS based on ultrasound energy through the abdominal layers without requirement of incisions under real time MRI monitoring to reduce fibroid size [66]. Γλωσσική επιμέλεια UAE blocks selective the uterine artery blood flow led to shrink of fibroids [67]. The goal of this review was to report our 12 years of experience from the impact of UAE on ovarian reserve (OR) (which refer to number and quality of the follicles left in the ovaries) of normal menstruating premenopausal women and to estimate the degree of pain and inflammation caused by UAE in our patients based on AMH levels and inflammatory parameters (CRP, temperature, white blood cells) respectively.
UAE to treatment of fibroids as alternative to surgical procedure was reported for first time by Ravina in 1995 [67]. This is not only treatment option for fibroids but used successfully also in refractory postpartum bleeding, or after gynecologic surgery, abnormal malignancy suspicious vaginal bleeding or in cases with uterine arteriovenous malformation. Although several reports confirm satisfactory results of treatment of symptomatic fibroids without necessity of surgical procedure based on the optimal cooperation between gynecologist and interventional radiologist, however the absolutely majority is retrospective and exist no prospective randomized trials to prove the effectiveness of this procedure compared to other therapy options [67, 68, 69, 70]. The UAEs were performed in the Department of Radiology by an experienced interventional radiologist.
All study participants were normal menstruating premenopausal women aged between of 38–50 years old (42.6 ± 7 years on average), had attended the department of obstetrics and gynecology of our University hospital complaining of serious symptoms of uterine fibroids (menorrhea, anemia, pelvic pain, bulky symptoms, pressure effects) underwent UAE for uterus fibromyomas and/or adenomyosis (pure or mix type). The enrolled premenopausal women diagnosed with and normal ovarian reserve as defined by AMH and FSH measurements (serum FSH concentration > 10 IU/L (on day 3 of menstrual cycle), serum AMH (2–8 pg./l). In all patients were available cervical pap smear test and previously performed fractional curettage. Exclusions criteria: Women with pelvic infection, pregnant (or willing to be pregnant) women, cases suspicious of any pelvic malignancy, postmenopausal women, women with resistant clotting disorders or severe allergy to contrast media, ovulatory problems, previous ovarian surgery, PCOS (polycystic ovarian syndrome) or coagulopathy, immunocompromised, previous pelvic irradiation or women who had been offered hormonal therapy for fibroids with GnRh agonists, were excluded. All patients underwent MR Imaging on a 1.5 Tesla (Multiva, Koninklijke Philips N.V.) or an 1 Tesla equipment (GE Healthcare, Milwaukee, USA) up to 60 days before UAE, using phased-array pelvic coils (Figure 1a-f). MR imaging included at least sagittal, coronal and transverse T2-weighted images, T2*-weighted images, T2-weighted fat saturated images, Diffusion-weighted images, T1-weighted images, and sagittal, coronal and transverse fat saturated T1-weighted images pre and post contrast. AMH, FSH, TSH, LH, fT 4 E, PROG, PROL, TESTOST and DHEAS were measured on day 3 of the menstrual cycle before UAE. C reactive protein (CRP) and white blood cell count lab exams were carried out prior to and after UAE. Two patients that had undergone fibromyectomy and with fibromyoma recurrence were included. Preoperative imaging management enhances the ability to diagnosis and to identify pathology induced anatomic changes and is crucial in optimizing information to treatment.
Description of UAE procedure course.
Transvaginal ultrasonography (TVUS) has an efficacy of 65–99% and consists the gold standard for imaging of the woman’s pelvis. MRI is crucial in the diagnosis. Differential diagnosis with MRI has a sensitivity of 88% - 93% and a specificity of 66% - 91%. MRI examination is important to rule out malignancy in the uterus, eg sarcoma and to identify nondegenerated fibroids. Degenarated fibroids occur as hyalinized fibroids, cystic changes as hypertense, myxoid degeneration as high signal intensity, necrotizing has components of necrotizing or coagulative necrosis.
All patients had signed a written consent before the UAE. The UAE procedures were performed in the hybrid angiography suite of Radiology Department using a biplane angiography system (Philips Allura Xper Cath/angio system, Koninklijke Philips N.V.).
Bilateral UAE was performed, under local anesthesia, i.v. antibiotic prophylaxis, and sedation when required. In all cases a bladder catheter has been placed. The procedure included a single percutaneous puncture of the right common femoral artery, selective crossover contralateral and unilateral advance of a 4-French flush angiographic catheter (Simmons 1 or Cobra 1) to both uterine arteries. When the catheter bypassed the arteries for the vagina and cervix, administration of the embolic particles started. In the most of the cases a 2.7-Frence or 2.8-Frence microcatheter (Progreat, Terumo Europe, Leuven, Belgium) has then been positioned away from the cervicovaginal branches (Figure 2a-f).
MRI imaging of fibroid course pre- and post embolization.
Special radiation protection care was taken, using fluoroscopic guidance of the catheterizations, fluoroscopy time reduction to the minimal possible and, mostly, fluoroscopic imaging of contrast angiography opacifications.
Fibroid ischemia was achieved by using of spherical, tightly calibrated, biocompatible, non-resorbable, hydrogel coated microspheres, 700 μm and 900 μm in diameter (Embozene, CeloNova BioSciences Inc./Boston Scientific, San Antonio, USA). The angiographic embolization endpoint was defined as complete stasis of contrast agent in the ascending segment of the uterine artery during selective digital subtraction angiography at the end of the embolization procedure. Adenomyosis patients were embolized with the use of 500 μm and/or 700 μm Embozene microspheres. Criterion for the particle administration stop in adenomyosis cases was the fluoroscopic finding of “almost complete stasis”.
Regarding pain treatment, post-intervention 50 mg of pethidine was intramuscular administered, and after 4 hours the dosage was repeated by intramuscular injection in the first 24 hours. 100 mg tramadol was taken every 6 hours and anti-inflammatory tablets were taken every 12 hours for a week. Pain assessment results were determined based on a visual analogue scale (0 min-10max). After daily stay at the hospital, patients were discharged and administered broad spectrum antibiotics for one week. Clinical, laboratory and imaging follow up examinations by trans–vaginal ultrasonography and MRI scans of the patients were performed at the 1rst, 3rd, 6th and 12th month after the procedure (Figure 1e-f).
Main outcome measures were menstruation, hormonal status and presence of menopausal symptoms. Hormonal status and ovarian reserve were evaluated by means of AMH and FSH serum levels on 1st, 3rd, 6th and 12th month after UAE. Subsequently, FSH and LH levels began to decrease and reached the base line values on the 12th month after UAE (Figure 3) [71]. The AMH levels showed a decrease on the 1st month, reaching the minimum values on the 3rd month and retaining the base line values on the 3rd month in contrary to the other examined hormones. No Case of amenorrhea was noted in women ≤45 years old, while 0.6% of women >45 years old experienced amenorrhea only the first 3 months after UAE (Figure 4) [71] According to our findings, a leukocytosis value of up to 16,000 Κ/μl and an increase in CRP level of up to 8 mg/dl, are not alarming [70]. In our study were included only premenopausal women and especially women who completed their family planning. However, reported two unplanned pregnancy cases, which they have decided to terminate the pregnancy. We have no noticed no case for emergency hysterectomy. In Table 1 are summarized the complications in our participants and according to international literature with the maximally respectively referred complications rate. The first column of the table refers to our results in the time from 2008 to 2020 while in the second column are shown the respective values of the examinated parameters in average concerning to international literature [72, 73, 74, 75, 76].
Hormonal changes (FSH,LH) during the follow up period (Tsikouras et al. [71]).
Hormonal changes (AMH) during the follow up period (Tsikouras et al. [71]).
Our results Range (min-max) | International literature results Range (min-max) | |
---|---|---|
Transient amenorrhea | ||
< 45 years old | 0.2–0.5% | 1–2% |
> 45 years old | 1.5% | 2–4% |
Permanent amenorrhea | 0 | |
< 45 years old | 0 | 2–3% |
> 45 years old | 0 | 5–6% |
Fibroma protrusion | 0.3% | |
Aseptic endometritis | 0.1–0.2% | 2% |
Septic endometritis | 0 | 1.2% |
Uterine necrosis | 0 | <1% |
Unsuccessful UAE | 0 | <1% |
UAE complications: our results and various published reports.
The course of myoma size according to a follow up for a period of 1 year post UAE was mean reduction 75% of fibroid volume compared to fibroid size before beginning of treatment. The percentage of technical success of the performed UAEs was estimated at 100% and the MRI examinations revealed that the uterine volume continues to shrink over follow up time. In no case was noticed continuity of worsening preprocedure symptoms, permanent amenorrhea, necessity of subsequent hysterectomy or minimal shrinkage of fibroid size after 6 months postprocedural. The positive results expressed as clinical included: Reduce of bleeding and pressure symptoms and as imaging reduction in uterine size and fibroids. According to our findings after UAE the fibroids shrank by 60–70% and the size of the uterus by 50–60%. In particular, mild symptoms of metabolic syndrome in four cases were observed. Over time, shrinkage increases. The reduction in symptoms is expected to be close to 98%.
Specifically, menstruation improved in 95–100% of cases, while symptoms (flatulence, pelvic pressure and frequency) are reduced to 91–100% depending on how the result is calculated. High satisfaction rates for women. The recurrence of fibroids reaches 4%, but is thought to be due to an increase in the size of old incomplete embolized myomas and adenomyosis. The main cause of failure was not the initial size of the fibroids, but their failure shrank below 30% of the original size. In three cases it was mandatory to repeat the procedure of UAE due to the anatomical location of the fibroids, intra-ligamentally.
UAE is a minimally invasive procedure which improves symptoms by interrupting the blood flow uterine vessel branches to fibroids after bilateral (from right and left) hyper-selective catheterization of the myometric feeder arteries and embossing of pistons induceing irreversible ischemic damage and degeneration/shrinkage in the fibroids. [65, 75, 76, 77, 78, 79, 80] According to bibliography, therapy success rate during menorrhagia, was is 80–100% and at? pressure phenomena 60–100%. A decrease in fibroid size by 40–70% was noted in the first 6 months, followed by 50–80% in the months that ensued [67, 77, 78, 79, 80, 81, 82]. There are various reports regarding uterus size course [67, 77, 78, 79, 80, 81, 82]. Some authors mention uterus size as criteria, whilst others use both fibroids and uterus size as successful therapy assessment criteria. Inflammation appearance rate is 1–2% based on tissue reactions due to post interventional ischemia is an interaction between cells and cytokine and should be diagnosed at an early stage so that sepsis, hysterectomy and death can be avoided [81, 82, 83, 84]. There have been reports of 100.000 successful UAEs in total so far [84, 85, 86, 87].
Patients should be notified in detail and contact their doctor. Fundamental is the co-operation between gynecologist and interventional radiologist before, during and after UAE. In general, complications include either catheterization or the effects of uterine ischemia that can cause fibrotic necrosis, pain and septic imaging. The ovaries may be affected. The reported deaths following UAE are extremely rare (approximately 1: 1600) and are mainly related to pulmonary embolism, which may be due to the effect of necrotic tissue on activation of the coagulation mechanism and on inflammation. The complications of catheterization are rare (<1%), such as hematoma, allergy to contrast media and pseudo-aneurysm or vascular separation [75, 76, 87, 88, 89, 90]. Elimination of uterine fibroids occurs in 5% of cases and can cause inflammation requiring scanning or hysterectomy. The necrotic tissue, if not removed in time, can become infected and the condition becomes severe. Cases with submucosal fibroids should be treated hysteroscopically [75, 76, 87, 88, 89, 90]. Ischemia may cause endometritis, pelvic inflammation and pyometra with poor outcome if hysterectomy does not occur. According to the literature, menorrhagia is successfully treated in 91–100% of cases, while symptoms such as flatulence, pressure on organs of the pelvis and loss of urine are reduced to 92–100% [67, 75, 76, 87, 88, 89, 90]. Uterine size does not appear to be a determinant, as remission of symptoms is also common in patients with a uterus greater than 24 weeks gestation. These results are also confirmed by studies of the last four years, which show that patients are 98–1000% satisfied [67, 75, 76, 87, 88, 89, 90]. UAEs also have a beneficial effect in cases of adenomyosis, although there is not much experience. In a series of 28 patients with genuine adenomyosis an improvement of 95.3% was recorded [67, 75, 76, 87, 88, 89, 90]. Although there are no long-term data, follow-up of up to 72 months shows postembolization syndrome include: pain and cramps (eliminated in the first hours after procedure with good/systemic analgesic treatment), nausea and fever (controlled with appropriate medications), aseptic or (rarely) septic inflammation (in a few patients, total 4 in our study controlled with anti-inflammatory/antibiotics) for 3–6 months) or (rare) menopause after UAE (small number of patients, almost always aged>45 years) [67, 75, 76, 87, 88, 89, 90]. In these cases were diagnosed large fibroids and the reported complications affect range according to published literature 2–15% needed readmission for monitoring of symptoms. The necessity of hysterectomy after UAE approximately reported in 1% of cases. In our study participants reintervention was necessary only in 4 cases due the anatomical fibroid positions. According to international literature reintervention’s rate is by 9% at 1 year and 28% at 5 years [67, 75, 76, 87, 88, 89, 90]. Pregnancies in the majority after the UAE reported and delivered at term without serious complications, however the cesarean section rate is high approximately 33–50% [67, 75, 76, 87, 88, 89, 90, 91]. Based on current medical knowledge concerning genetics and molecular biology of uterine fibroids will be the basis of development microarray analysis to investigate genes, which involved in fibroid formation and provide more specific and effective minimally preventive fibroid therapies to early intervention and improve the life impact of women.
UAE is a safe and effective treatment option for uterine fibroids with international recognition, however further multicentric studies required to provide clinical data and participate in randomized control trial to compare with the known surgical procedures.
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