50 organic pollutants most commonly detected in groundwater [11]
\\n\\n
More than half of the publishers listed alongside IntechOpen (18 out of 30) are Social Science and Humanities publishers. IntechOpen is an exception to this as a leader in not only Open Access content but Open Access content across all scientific disciplines, including Physical Sciences, Engineering and Technology, Health Sciences, Life Science, and Social Sciences and Humanities.
\\n\\nOur breakdown of titles published demonstrates this with 47% PET, 31% HS, 18% LS, and 4% SSH books published.
\\n\\n“Even though ItechOpen has shown the potential of sci-tech books using an OA approach,” other publishers “have shown little interest in OA books.”
\\n\\nAdditionally, each book published by IntechOpen contains original content and research findings.
\\n\\nWe are honored to be among such prestigious publishers and we hope to continue to spearhead that growth in our quest to promote Open Access as a true pioneer in OA book publishing.
\\n\\n\\n\\n
\\n"}]',published:!0,mainMedia:null},components:[{type:"htmlEditorComponent",content:'
Simba Information has released its Open Access Book Publishing 2020 - 2024 report and has again identified IntechOpen as the world’s largest Open Access book publisher by title count.
\n\nSimba Information is a leading provider for market intelligence and forecasts in the media and publishing industry. The report, published every year, provides an overview and financial outlook for the global professional e-book publishing market.
\n\nIntechOpen, De Gruyter, and Frontiers are the largest OA book publishers by title count, with IntechOpen coming in at first place with 5,101 OA books published, a good 1,782 titles ahead of the nearest competitor.
\n\nSince the first Open Access Book Publishing report published in 2016, IntechOpen has held the top stop each year.
\n\n\n\nMore than half of the publishers listed alongside IntechOpen (18 out of 30) are Social Science and Humanities publishers. IntechOpen is an exception to this as a leader in not only Open Access content but Open Access content across all scientific disciplines, including Physical Sciences, Engineering and Technology, Health Sciences, Life Science, and Social Sciences and Humanities.
\n\nOur breakdown of titles published demonstrates this with 47% PET, 31% HS, 18% LS, and 4% SSH books published.
\n\n“Even though ItechOpen has shown the potential of sci-tech books using an OA approach,” other publishers “have shown little interest in OA books.”
\n\nAdditionally, each book published by IntechOpen contains original content and research findings.
\n\nWe are honored to be among such prestigious publishers and we hope to continue to spearhead that growth in our quest to promote Open Access as a true pioneer in OA book publishing.
\n\n\n\n
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He also works as a Honorary Senior Research Fellow at Birmingham University, UK, Lecturer at the Postgraduate European Institute, and has worked as Senior Manager in Accenture (2013-2014). He obtained his European PhD with a maximum distinction. He is a holder of the Runner Prize for Management Science and Engineering Management Nominated Prize (2020), Advancement Prize (2018), First International Business Ideas Competition 2017 Award (2017), Runner (2015), Advancement (2013) and Silver (2012) by the International Society of Management Science and Engineering Management (ICMSEM), and Best Paper Award in the international journal of Renewable Energy (Impact Factor 3.5) (2015). 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Kostogryzov"}],productType:{id:"1",chapterContentType:"chapter",authoredCaption:"Edited by"}}]},chapter:{item:{type:"chapter",id:"42294",title:"The Investigation and Assessment on Groundwater Organic Pollution",doi:"10.5772/53549",slug:"the-investigation-and-assessment-on-groundwater-organic-pollution",body:'
Groundwater is an important part of the water resource. It plays an irreplaceable role in supporting the national economy and social development. In China, more than 1/3 of the total water resources are utilized. As surveys shown, over 400 cities of all exploit groundwater. More seriously, many of them use groundwater as the only source of water supply.
A series of problems emerge gradually with the utilization of groundwater. Just as river waters have been over-used and polluted in many parts of the world, so have groundwater. The organic solvents and dioxins pollution of Love Canal occurred in 1978 is one of the most widely known examples, which contributes high rates of cancer and an alarming number of birth defects. Similar things occur frequently in recent decades. Governance of groundwater is so urgent a major matter of peace and prosperity. After years of researches, the nature and pollution mechanism of the contaminants in the groundwater have already got comprehended.
General scope of the organic contamination in groundwater is reviewed in this chapter. We will detail account the types of groundwater organic contamination, the pollution source of groundwater. and the fate and transport of chemicals in groundwater. Also a detailed description of the investigation and assessment method in this chapter. At last, we give some comments and suggestion on the groundwater investigation and assessment.
The figure 1 described some source of groundwater contamination, and the transport of chemicals in groundwater. We can see the landfills, leaking sewers, oil storage tanks, pesticides and fertilizer, and septic tank in the picture, all of these could be the pollution source of groundwater. We also can know the groundwater transport and flow in the unsaturated zone and saturated zone.
Diagram of the Groundwater Pollution [1].
Many studies have been conducted since 1970 to characterize concentrations of organic compounds in groundwater. In 1977, 16 drinking water wells have been closed in Gray town of Maine state because of there were at least 8 synthetic organics that were detected in drinking water wells. And in 1986, there were at least 33 organics that were detected in drinking water wells in USA [2]. It has been reported trace organic pollutants to be detected in all of 50 states. The U.S. Geological Survey(USGS) collected and assorted the test data the 1926 drinking water wells in the nation\'s rural areas from 1986 to 1999. And at least one VOCs were detected from 232 wells and the positive rate was 12%, with the highest positive rate were Chloroform, tetrachloroethylene and so on [3].
Similar conditions are to be found in other countries. In the 80s of last century, based on an inventory of the presence of halogenated substances in raw water of 232 groundwater pumping stations in The Netherlands a compilation of more than 100 organic substances identified in contaminated groundwater, the detection rate of trichloroethylene up to 67% [4]. The organic pollutants could be detected in groundwater in Britain. Flordward studied on 209 water supply wells in Britain shown that the main pollutant in the groundwater are the trichloroethylene and tetrachloroethylene. Beginning in 1974, Environment Agency of Japan conducted a nationwide comprehensive survey of chemical environmental safety. The trichloroethylene in groundwater was reported for the first time. The European Union is the largest pesticide consumer in the world, more than 600 pesticides were applied. Six of the top 10 were European countries in the pesticide application. Atrazine exists in groundwater all over the Europe, and the content always beyond the European Union drinking water standard(0.1μg/l) 10-100 times.
The research on organic pollutions of China is at starting stage, but there has serious organic contamination events in some areas. Based on a study of water pollution in sewage system in the Gaobeidian Prefecture of Beijing, 1988, organic substances identified in shallow wells and deep wells in South-east agriculture districts in Beijing. And 32 organic substances identified in deep wells, and 52 in shallow wells. Most of that are carcinogens (e.g. Chloroform and benzene) [5]. Analysis of the years groundwater monitoring data, and it is shown that the quality of groundwater is gradually worse.
A study on groundwater organic pollution in region of Beijing, Tianjin and Tangshan conducted by Institute of Chemistry of Chinese Academy of Sciences shows that the type of organic pollutants up to 133 [6]. The researchers Chen Honghan, He Jiangtao and others [7] have summed up the characteristics of organic contamination of shallow groundwater in a study area of the Taihu Lake basin. The results show that the detection probabilities of compounds in groundwater are higher but the concentrations of the compounds are lower. The concentrations of all the components of BTEX and halocarbons are lower than the standards set by the U.S. Environmental Protection Agency (EPA) for drinking water except for benzene in a few sampling sites.
Different types of groundwater contamination sources can pose different threats to human health and different problems in health risk assessment (table 1).
Volatile organic compounds (VOCs) are organic compounds with chemical and physical properties that allow the compounds to move freely between water and air. VOCs have been used extensively in industry, commerce, and households in the United States since the 1940’s. Many products contain VOCs including fuels, solvents, paints, glues, adhesives, deodorizers, refrigerants, and fumigants. In general, these compounds have low molecular weights, high vapor pressures, and low-to-medium water solubilities [8]. Many of these compounds show evidence of animal or human carcinogenicity, mutagenicity, or teratogenicity. And these compounds are quite persistent in groundwater, because of their relatively low biological and chemical reactivity. This persistence is assisted by low temperatures, absence of light and contact with the atmosphere, and comparatively low microbial concentrations typical of groundwater environments. By comparison with other organic compounds, VOCs may be transported for relatively long distances in groundwater, as a result of their relatively weak sorption affinity and their resistance to degradation. Because of human-health concerns, many VOCs have been the focus of national regulations, monitoring, and research during the past 10 to 20 years.
Pesticides consist of a large group of chemicals that are used in agriculture and residential settings to control plant and animal infestation. Pesticides are commonly applied on farms, fruit orchards, golf courses, and residential lawns and gardens. There are several different types of pesticides: Herbicides, Insecticides, Nematocides, Fungicides. Some pesticides do not break down easily in water and can remain in the groundwater for a long period of time. Likewise, the insecticide DDT, though banned for nearly twenty years, can still be found at trace levels in some groundwater. After prolonged exposure to high doses, some pesticides can cause cancer; some can also result in birth defects and damage to the nervous system. The use of pesticides and herbicides is one of the main ways of organic pollution of groundwater. Many water wells and irrigation wells have been closed for the byproducts from pesticides and herbicides be detected in shallow water in Colorado.
\n\t\t\t\tOrdering\n\t\t\t | \n\t\t\t\n\t\t\t\tComponent\n\t\t\t | \n\t\t\t\n\t\t\t\tCASRN\n\t\t\t | \n\t\t\t\n\t\t\t\tTypes\n\t\t\t | \n\t\t
1 | \n\t\t\tTrichloromethane | \n\t\t\t67-66-3 | \n\t\t\tVOCs | \n\t\t
2 | \n\t\t\tTetrachloroethylene | \n\t\t\t127-18-4 | \n\t\t\tVOCs | \n\t\t
3 | \n\t\t\t1,1,1-Trichloroethane | \n\t\t\t71-55-6 | \n\t\t\tVOCs | \n\t\t
4 | \n\t\t\tTrichloroethylene | \n\t\t\t79-01-6 | \n\t\t\tVOCs | \n\t\t
5 | \n\t\t\t1,1-Dichloroethene | \n\t\t\t75-35-4 | \n\t\t\tVOCs | \n\t\t
6 | \n\t\t\tMethyl tert-butyl ether | \n\t\t\t1634-04-4 | \n\t\t\tVOCs | \n\t\t
6* | \n\t\t\tcis-1,2-Dichloroethylene | \n\t\t\t156-59-2 | \n\t\t\tVOCs | \n\t\t
8 | \n\t\t\t1, 2, 4-Trimethylbenzene | \n\t\t\t95-63-6 | \n\t\t\tVOCs | \n\t\t
9 | \n\t\t\tToluene | \n\t\t\t108-88-3 | \n\t\t\tVOCs | \n\t\t
10 | \n\t\t\tPrometon | \n\t\t\t1610-18-0 | \n\t\t\tPesticides | \n\t\t
11 | \n\t\t\t1,1-Dichloroethane | \n\t\t\t75-34-3 | \n\t\t\tVOCs | \n\t\t
12 | \n\t\t\tBromacil | \n\t\t\t314-40-9 | \n\t\t\tPesticides | \n\t\t
13 | \n\t\t\tTebuthiuron | \n\t\t\t34014-18-1 | \n\t\t\tPesticides | \n\t\t
14 | \n\t\t\t1, 3-Dichlorobenzene | \n\t\t\t541-73-1 | \n\t\t\tVOCs | \n\t\t
15 | \n\t\t\t1,2-Dichloropropane | \n\t\t\t78-87-5 | \n\t\t\tVOCs | \n\t\t
16 | \n\t\t\tCarbon disulfide | \n\t\t\t75-15-0 | \n\t\t\tVOCs | \n\t\t
17 | \n\t\t\tDeethylatrazine | \n\t\t\t6190-65-4 | \n\t\t\tPesticides | \n\t\t
17* | \n\t\t\t1,4-Dichlorobenzene | \n\t\t\t106-46-7 | \n\t\t\tVOCs | \n\t\t
19 | \n\t\t\tSulfamethoxazole | \n\t\t\t723-46-6 | \n\t\t\tMedicine | \n\t\t
20* | \n\t\t\t1,2-Dichlorobenzene | \n\t\t\t95-50-1 | \n\t\t\tVOCs | \n\t\t
20 | \n\t\t\t2-Hydroxyatrazine | \n\t\t\t2163-68-0 | \n\t\t\tPesticides | \n\t\t
22* | \n\t\t\tTrichlorofluoromethane | \n\t\t\t75-69-4 | \n\t\t\tVOCs | \n\t\t
22 | \n\t\t\tBentazon | \n\t\t\t25057-89-0 | \n\t\t\tPesticides | \n\t\t
24 | \n\t\t\tAtrazine | \n\t\t\t1912-24-9 | \n\t\t\tPesticides | \n\t\t
25 | \n\t\t\tPicloram | \n\t\t\t1918-2-1 | \n\t\t\tPesticides | \n\t\t
26 | \n\t\t\tDiuron | \n\t\t\t330-54-1 | \n\t\t\tPesticides | \n\t\t
27* | \n\t\t\tBenzene | \n\t\t\t71-43-2 | \n\t\t\tVOCs | \n\t\t
27* | \n\t\t\tTetrachloromethane | \n\t\t\t56-23-5 | \n\t\t\tVOCs | \n\t\t
29 | \n\t\t\tChlorobenzene | \n\t\t\t108-90-7 | \n\t\t\tVOCs | \n\t\t
30* | \n\t\t\t2-Butanone | \n\t\t\t78-93-3 | \n\t\t\tVOCs | \n\t\t
30 | \n\t\t\tAcetone | \n\t\t\t67-64-1 | \n\t\t\tVOCs | \n\t\t
32* | \n\t\t\tm- + p-Xylene | \n\t\t\t106-42-3 | \n\t\t\tVOCs | \n\t\t
32* | \n\t\t\ttrans-1,2-Dichloro- ethylen | \n\t\t\t156-60-5 | \n\t\t\tVOCs | \n\t\t
32* | \n\t\t\t1,2-Dibromoethane | \n\t\t\t106-93-4 | \n\t\t\tVOCs | \n\t\t
35 | \n\t\t\tEthylbenzene | \n\t\t\t100-41-4 | \n\t\t\tVOCs | \n\t\t
36 | \n\t\t\tcaffeine | \n\t\t\t58-08-2 | \n\t\t\tMedicine | \n\t\t
37 | \n\t\t\tIsopropylbenzene | \n\t\t\t98-82-8 | \n\t\t\tVOCs | \n\t\t
38 | \n\t\t\to-Xylene | \n\t\t\t95-47-6 | \n\t\t\tVOCs | \n\t\t
38* | \n\t\t\t1,1,2-Trichloroethane | \n\t\t\t79-00-5 | \n\t\t\tVOCs | \n\t\t
38* | \n\t\t\tBromodichloromethane | \n\t\t\t75-27-4 | \n\t\t\tVOCs | \n\t\t
38* | \n\t\t\t1,1,1,2-Tetrachloroethane | \n\t\t\t630-20-6 | \n\t\t\tVOCs | \n\t\t
38* | \n\t\t\tn-Propylbenzene | \n\t\t\t103-65-1 | \n\t\t\tVOCs | \n\t\t
43 | \n\t\t\tChloromethane | \n\t\t\t74-87-3 | \n\t\t\tVOCs | \n\t\t
44 | \n\t\t\t1,1,2-Trichloro-1,2,2-trifluoroethane | \n\t\t\t76-13-1 | \n\t\t\tVOCs | \n\t\t
45 | \n\t\t\tDichlorodifluoromethane | \n\t\t\t75-71-8 | \n\t\t\tVOCs | \n\t\t
46 | \n\t\t\tMetolachlor | \n\t\t\t51218-45-2 | \n\t\t\tPesticides | \n\t\t
46* | \n\t\t\tSimazine | \n\t\t\t122-34-9 | \n\t\t\tPesticides | \n\t\t
48 | \n\t\t\tBromoform | \n\t\t\t75-25-2 | \n\t\t\tVOCs | \n\t\t
48* | \n\t\t\tImidacloprid | \n\t\t\t138261-41-3 | \n\t\t\tPesticides | \n\t\t
48* | \n\t\t\t1,3,5-Trimethylbenzene | \n\t\t\t108-67-8 | \n\t\t\tVOCs | \n\t\t
50 organic pollutants most commonly detected in groundwater [11]
*show the same detection with the front component. CASRN is the register number of chemical substances formulate by Chemical Abstracts Service, m means meta-position, p means para-position.
Tens of thousands of manmade chemicals are used in today\'s society with all having the potential to enter our water resources. There are a variety of pathways by which these organic contaminants can make their way into the aquatic environment [9]. If the groundwater is the drinking water sources, there will be potentially dangerous on human health. Pharmaceuticals and other organic contaminants are a set of compounds that are receiving an increasing amount of public and scientific attention. Water samples were collected from a network of 47 groundwater sites across 18 states in 2000 [10]. All samples collected were analyzed for 65 organic contaminants representing a wide variety of uses and origins. Thus, sites sampled were not necessarily used as a source of drinking water but provide a variety of geohydrologic environments with potential sources of organic contaminants. organic contaminants were detected in 81% of the sites sampled, with 35 of the 65 organic contaminants being found at least once. The most frequently detected compounds include N,N-diethyltoluamide (35%, insect repellant), bisphenol A (30%, plasticizer), tri(2-chloroethyl) phosphate (30%, fire retardant), sulfamethoxazole (23%, veterinary and human antibiotic), and 4-octylphenol monoethoxylate (19%, detergent metabolite).
Organic contamination includes all of natural and synthetic that could cause adverse effect on human health or ecology environment.
Naturally formed waters such as ocean water and connate brines can be sources of groundwater contamination under certain circumstances. Changes in pumping rates can cause fresh-water aquifers to be contaminated by intrusion of seawater. Similarly, changes in the groundwater flow field or leakage through imperfectly sealed wells can cause contamination of groundwater supply by naturally occurring brines or other poor-quality waters. Generally, trace amount of natural organic compounds existence in groundwater in most of regions. The major is humic acid, especially in forest and grassland. Although itself could not impair the groundwater quality, it could be enhance the heavy metal and other organic matters activities in groundwater.
As the human population grows, groundwater pollution from human activity also increases. There are a number of possible sources that could lead to groundwater contamination. Such as crude oil leakage in oil production, organic waste discharge, spills and leaks from underground storage tank and so on.
The treatment and disposal of sewage present health risks in both developed and undeveloped countries. In undeveloped countries, sewage may be directly applied to the land surface. In more developed areas, sewage is generally transported to municipal treatment plants or disposed of in septic tanks and cesspools. Groundwater contamination can result in all these cases. Sewage provides a source of pathogens, nitrates, and a variety of organic chemicals to groundwater. Land application of sewage can provide a direct contaminant source via infiltration. Treatment plants can act as contaminant sources in several ways. Leaks may occur in sewer lines and infiltration may occur from the ponds and lagoons within the treatment plants. In addition, the sewage sludge that is a product of sewage treatment processes is often disposed on land in conjunction with agricultural activity. Depending on the characteristics of the sludge, the soil characteristics, and the application process, such land application can act as a large non-point source of groundwater contamination. Land disposal of treated waste water can pose comparable risks. Depending on hydrogeologic conditions, septic tanks and cesspools may allow untreated sewage to enter the groundwater flow system. In addition, use of solvents to clean out the systems can cause groundwater contamination by synthetic organic compounds. The material cleaned out from septic tanks must eventually be disposed of, often by land application.
Industrial Wastewaters are applied to land in ponds or lagoons that are either designed to percolate the liquid into the soil or to store and/or evaporate the liquid above ground. In either case, such facilities act as potential groundwater contamination sources. Facilities designed to intentionally infiltrate into the ground include cooling ponds for power generation and for other industrial processes. The liquids in such facilities may contain potentially hazardous materials. Storage and evaporation ponds are often lined to prevent infiltration, but are likely to act as groundwater contamination sources under some circumstances, depending on surface runoff characteristics, the integrity and permeable of the liner(s), and the groundwater flow system. Poorly designed evaporation ponds may, in many cases, function as infiltration ponds.
In the United States, the big city and small town are commonly found in contaminated groundwater. An test on 39 groundwater supply in small towns conducted by the U.S. EPA, it reported that 11 VOCs could be detected in treated or untreated groundwater [12].
Land disposal of solid waste is the groundwater contamination source of most current concern to the general public in many developed countries and of most current regulatory interest.
Solid waste can be disposed in landfills, facilities engineered to safely contain the waste. While landfills may often prevent exposure of solid waste at the land surface, many landfills provide a direct connection with groundwater. In the past, landfill siting was based on the availability of inexpensive, undeveloped land requiring little modification for waste disposal, rather than on hydrogeologic suitability. Disposed materials often are very susceptible to leaching into groundwater.
Landfills may be grouped according to the type of materials they contain. Municipal landfills accept only non-hazardous materials, but are still likely to contain materials which pose potential health risks. Industrial landfills may contain either "hazardous" or "non-hazardous" materials. Until recently, little was known about how they were operated or what they contained. Open dumps and abandoned disposal sites generally have no engineering design. Their connection with the groundwater system and the type of materials present is often unknown. It is often in abandoned disposal sites that large volumes of highly toxic materials are found. The most hazardous solid waste disposal generally results from industrial and manufacturing activities as well as some governmental energy and defense activities. Populations of both developed and developing countries, where there is current or historical industrial activity, face potential health risks from solid waste disposal. It is reported that there will be the highest content and most types of organic contaminants in groundwater which is near the landfills. If there has 1 kilometers distance it still exist in the groundwater [13].
In recent years, there has been increasing awareness of the large number of potentially leaking underground storage gasoline tanks. For much of the twentieth century, underground storage tanks were constructed of unprotected carbon steel. Corrosion causes leaks in such tanks over some period of time, ranging from a few years to tens of years. Although the leakage from individual tanks is often small, it is often enough to contaminate a large volume of groundwater. In addition, the large number of buried tanks-several million in the United States-makes them a potentially significant groundwater contamination source. Above ground storage tanks pose less of a threat than underground tanks. Leak detection and maintenance is easier and the connection with the groundwater system is less direct. However leaks from such tanks may still act as groundwater contamination sources.
Numerous agricultural activities can result in non-point sources of groundwater contamination. Fertilizers, pesticides, and herbicides are applied as part of common agricultural practice throughout the world. These applications can act as sources of contamination to groundwater supplies serving large populations. Whether or not fertilizers, pesticides, and herbicides become sources of groundwater contamination depends on changing hydrogeologic conditions, application methods, and biochemical processes in the soil. In developing countries, animal and/or human waste is used for fertilizer. This is an example of the land application of sewage discussed earlier. There are the same concerns with pathogens and nitrates. The manufactured inorganic fertilizers widely used in developed countries, and finding increasing usage in all countries, also pose the threat of nitrate contamination of groundwater systems. Pesticide and herbicide application provides a source of numerous toxic organic chemicals to groundwater supplies.
Even without the introduction of fertilizers, pesticides, and herbicides, irrigation activities can lead to groundwater contamination. Naturally occurring minerals in the soil can be leached at higher rates leading to hazardous concentration levels in the groundwater. Evaporation of irrigation water can cause evaporative concentration of certain chemicals in the root zone. Flushing of these chemicals can then lead to hazardous concentration levels in groundwater.
Agricultural activities related to animals also can be groundwater contamination sources. These include the feeding of animals and the storage and disposal of their waste. Animal wastes and feedlot runoff are commonly collected in some sort of pit or tank creating the contamination threat described earlier for sewage disposal.
More than 300 pesticides were applied in Asia. The Japan is a country with the largest amount of pesticide on unit area cultivated land. Indonesia, Korea, India and China are the major consumers. But, there did not have pesticides routine monitoring in the developing countries in Asia [14].
Groundwater is but one component of the hydrologie cycle. Groundwater quality is very much influenced by surface-water conditions and vice versa. Contamination of any surface water bodies that recharge the groundwater system is a source of groundwater contamination. This includes "natural" recharge sources such as lakes and rivers as well as "man-made" recharge sources such as artificial recharge ponds/injection wells and infiltration of urban runoff. More generally, it is important to consider the interaction of all environmental sources and pathways of pollution. Environmental contaminant sources cannot be divided into separate, isolated compartments. For example, atmospheric pollution can lead to deposition of hazardous fallout to surface waters and to soils, and eventually lead to groundwater contamination.
Volatilization occurs in whether the vadose zone or saturated zone when the dissolved contaminants and non-aqueous phase contaminants exposed to gas. The factors affecting volatilization include solubility of the compound, molecular weight and water-saturated state of the geological media. The evaporation rate must be measured fundamentally in order to determine pollutions transporting into the atmosphere, changes of the pollution load in the vadose zone and groundwater. The process that the contaminants of deep soil volatilize to the atmosphere can be assumed as one-dimensional diffusion, which can be described with Fick\'s second law. Volatilization of the water-soluble organic matter, such as benzene dissolved in water is generally described by Henry\'s Law [15].
Adsorption in Soil and sediment makes an important influence on the behavior of organic pollutants. The mobility and biological toxicity reduced as organics are detained in the soil and sediment. Generally, adsorption is affected by sediments and soil properties, such as organic percentage, the type and quantity of clay minerals, cation exchange, pH and the physical and chemical properties of the contaminants. During the adsorption, the organic contaminants in the water adsorbed on the surface of the soil particles by the simultaneous distribution role of both water and solid, the driving force is mainly based on principle of "like dissolves like" and electrostatic adsorption of the polar group, and the following formulas is established [15]:
The equation (1) is existed when the adsorption systems reach equilibrium. Where, Csa is the amount of organic pollutants adsorbed per unit weight of soil particles; Cwa is concentration of organic pollutants; Ka is the total sorption coefficient.
The adsorption of organic contaminants in soil or sediment usually described by Ka (soil absorption coefficient) or Koc (organic carbon absorption coefficient). The former refers to the ratio of the concentration of organic matter in the soil or sediment and its aqueous phase concentration. As well, the latter factor represents the ratio of the concentration of organic matter adsorbed by organic carbon in the soil or sediment and its aqueous phase concentration.
Microorganisms may play an important role in contamination transformations within groundwater and on the soil. They can act as catalysts for many types of reactions. When modeling biochemical reactions in groundwater, additional processes must be considered. These include the changes in the availability of substrate for the microorganisms to utilize and reactions on the particles that the microorganisms are attached to. When microbial reactions are significant, there is a possibility of clogging of pores due to precipitation reactions or to biomass accumulation [16].
Microorganisms not only influence chemical reactions, but may be contaminants themselves. There is much current uncertainty about the fate and survival time of viruses, bacteria, and larger enteric organisms in groundwater [17-18]. Distribution of microorganisms will vary greatly with depth. Potential outbreaks of waterborne diseases due to biologic pollutants are of particular concern where there is land disposal of human waste (often via septic tanks) and animal waste. The potential for transmittal of waterborne diseases in groundwater is particularly high in areas of rapid velocities such as karst regions.
Biodegradation mainly depends on two factors [19], the intrinsic characteristics of the pollutants (the structure of organics, physical and chemical properties) and microorganism (the activity of microbial populations), and the environmental factors controlling the reaction rate (temperature, pH, humidity, dissolved oxygen). As the U.S. Environmental Protection Agency researched [20], soil microbial degradation of organic pollutants can be expressed as a one-order response equation:
Where, C is the mass fraction of soil organic matter[mg/g]; X is the number of active microbial in the organic matter of soil degradation[106 /g]; t is degradation time[d]; K is the one-order biodegradation rate constant [g/(d 106)]; kr is substrate removal constant[d-1].
From the above equation,
Substituted into with half-life formula,
The half-life of degradation of residual contamination is determined.
In many cases, the receptor medium for release of a contaminant will be the unsaturated zone. In contrast to the saturated zone, pores in the unsaturated zone are not completely saturated with liquid. This fundamentally affects the processes governing flow and chemical transport. A number of processes will affect the contaminant within the unsaturated zone before it enters the saturated groundwater system and potentially is tapped by supply wells. The uncertainties in characterizing releases just described lead to uncertainties in defining the source terms and initial and boundary conditions for modeling unsaturated transport. Analogously, uncertainties in characterizing unsaturated transport processes lead to uncertainties in defining the source terms and initial and boundary conditions for modeling saturated transport.
For the most part, computer simulation of contaminant transport has focused on movement in the saturated zone. Assumptions are made regarding the time required for movement through the unsaturated zone. Often some sort of lag between source release and entry of chemicals into the saturated flow system is introduced into source terms. It is important to be aware of the unsaturated processes that are actually occurring, the uncertainty associated with these processes, and the role of monitoring in reducing these uncertainties.
Once a chemical has been released into the ground and has either moved through the unsaturated zone or directly entered the saturated zone, saturated transport processes will determine if, how fast, and at what concentration a chemical reaches a supply well. A great deal of research has been carried out on understanding and modeling these processes. There is increasing recognition that chemical transport must be viewed as a stochastic process.
The same elements of uncertainty are present for saturated transport as for unsaturated transport. The important differences are that in saturated transport, water content equals porosity, hydraulic conductivity is no longer a function of water content or head, gravity rather than suction head is the driving force, and the scale of concern may be much larger
The current situation investigation main contents are as following:
Pollution source investigation: In groundwater polluted areas, investigate the non-point-source, line-source and point-source, and the type, pollution intensity, spatial distribution of natural source.
Investigation of unsaturated zone vulnerability: Investigate the unsaturated zone of thickness, lithological composition, composition, water permeability, the capability of degradation contaminations and so on.
Investigation of the pollution condition at the groundwater: Make sure the category, quantity or concentration of the pollutants, ascertain the pollution range, variation trend and the factors relation. All of these need samples collection in filed and laboratory test.
With the developed, groundwater pollution attracted wide attention. In view of existing situation, we launched the survey of pollution sources, including the following aspects: industrial pollution sources, domestic pollution sources, agricultural pollution sources and surface polluted waters.
According to industrial pollution sources, we must investigate the situation as: the company name, position, sewage, waste residue (tailings) emissions, discharge, scale, pathways and outfall location, types of pollutants, quantity, composition and hazards, and the abandoned site of major polluting enterprises, abandoned wells, oil and survey of solvents and other underground storage facilities.
The survey include the distribution of dumps, scale, waste disposal methods and effects, the generation of dump leaching filtrate and components, geological structure of storage site; amount of sewage generated, treatment and disposal of the way, main pollutants and their concentration and hazards
Agricultural pollution sources investigation mainly include land use history and current situation, the varieties, numbers, operations, time of farmland application of chemical fertilizers and pesticides, range of sewage irrigation, main pollutants and concentration, the number of sewage irrigation and sewage irrigation amount. The scale of farms and so on.
The surface polluted waters mainly about rivers, lakes, ponds, reservoirs and drains. We survey the distribution of polluted waters, the scales, the utilizations and water quality.
The coastal areas have to survey the situation of seawater invasion and saline water distribution.
The four steps of NAS was proposed by National Academy of Sciences, United States(NAS), was an assessment method on human health risk that led by the accident, air, water, soil and other medium. The method mainly in the following aspects: the hazard identification (qualitative evaluation the degree of hazards of the chemical substances on the human health and ecological); dose-response assessment (quantitative assessment the toxicity of chemical substances, established a relationship between the dose of chemical substances and the human health hazard); exposure assessment (quantitative or qualitative estimate or calculate the exposure, exposure frequency, exposure duration and exposure mode); exposure attribute (using the data to estimate the strength of the health hazards in the different conditions or the probability of the certain health effects). This method can qualitative analysis or quantitative analysis of groundwater contamination, or combine them, the results could be quantify and analysis, and provide more detailed information to the decision-makers.
In 1989, U.S. Environmental Protection Agency (EPA) promulgated the “risk assessment guidance for superfund: Human health evaluation manual”, there was a similar assessment method to NAS method [22]. The steps following as data collection, exposure assessment, toxicity assessment, risk characterization. Contrast the two methods, NAS is more common methods, the use range wider, suitable for a variety of health risk assessment; the EPA method is more specific, it emphasis on the various parameters of the collection of contaminated sites, for the evaluation of contaminated sites, it more operational.
The MMSOILS model is multi-media model which describe the groundwater, surface water, soil and air in the migration of chemicals, exposure and food chain accumulation [23]. Contaminate sites is multi-phase, multi-media complex. The model including the migration and transformation of pollutants module and human exposure module. Migration and transformation module include: (1)atmospheric transport pathway; (2)soil erosion; (3)groundwater migration pathway; (4)surface water pathway; (5)food chain bioaccumulation. Human exposure are: (1)adopt from drinking water, animals and plants and soil; (2)atmospheric volatiles and particulate inhalation; (3)soil, surface water and groundwater contact with skin. The model could be simulate a comprehensive migration pathway and widely used in foreign countries, and the parameters could be analysis the uncertainty.
The DRASTIC method is a national standards system that developed by US EPA to evaluation aquifer vulnerability. It including: Depth to Water(D); Net Recharge(R); Aquifer media(A); Soil Media(S); Topography(T); Impact of the Unsaturated Zone Media(I); Conductivity of Aquifer Hydraulic(C). Assignment of each element from 1 to 10, and them proportional to the degree of vulnerability of groundwater. At the same time, each element is assigned a weight, the weight should be reflect the sensitivity of groundwater. The model can objectively assess the groundwater vulnerability of different areas, and its assumption that all regions of the aquifer has a uniform trend. But all the geological, hydrogeological and other conditions are different, and the model calculations defect, the DRASTIC method has some limitations.
An important step in health risk assessment is the quantification of actual human exposure. Exposure can be expressed as either the total quantity of a substance that comes in contact with the human system or the rate at which a quantity of material comes in contact with the human system (mass per time or mass per time per unit body weight. The exposure assessment evaluates the type and magnitude of exposures to chemicals of potential concern at a site. The exposure assessment considers the source from which a chemical is released to the environment, the pathways by which chemicals are transported through the environmental medium, and the routes by which individuals are exposed. Parameters necessary to quantitatively evaluate dermal exposures, such as permeability coefficients, soil absorption factors, body surface area exposed, and soil adherence factors are developed in the exposure assessment. Exposure to chemicals in water can occur via direct ingestion, inhalation of vapors, or dermal absorption. Ingestion includes drinking of fluids as well as using water for rinsing and cooking of foods. Dermal absorption includes swimming and bathing.
Determination of average exposure levels for a particular population is quite difficult. This is due to difficulties in acquiring sufficient water-quality data, in identifying the exposed individuals, and in quantifying the concentrations in the different exposure pathways. For a given groundwater contamination problem, the U.S. Environmental Protection Agency stresses the importance of identifying both the currently affected population as well as possible changes in future land use. Subpopulations that may be especially sensitive to exposure should also be identified [24].
When attempting to estimate exposure to larger population entire countries, for example other concerns arise. Cothern [25] computed the average population exposure to volatile organic compounds in the United States, based on data from several thousand ground- and surface-water supplies. National exposure was estimated as a straight extrapolation of the concentration intervals from the original data. Best- and worst-case assumptions were applied for handling the "below detectable" category. Crouch et al. [26] applied an alternative approach to estimate population exposure levels. Rather than estimating a distribution for exposure, they made the worst-case assumption that individuals are exposed to water at the maximum measured concentration for their water supply.
According to the Risk Assessment Guidance for Superfund Volume I: Human Health Evaluation Manual (Part E, Supplemental Guidance for Dermal Risk Assessment) (U.S. EPA) [27], we calculation the dermal absorbed dose (DAD) and ingestion absorbed dose (IAD) [28].
Where:
DAD=Dermally Absorbed Dose (mg/kg-day),
DAevent=Absorbed dose per event (mg/cm2-event),
SA=Skin surface area available for contact (cm2),
EV=Event frequency (events/day),
EF=Exposure frequency (days/year),
ED=Exposure duration (years),
BW=Body weight (kg),
AT=Averaging time (days).
Where:
IAD= Ingestion absorbed dose (mg/kg-day),
ρ= Pollutant concentration in groundwater (mg/L),
U=Drinking amount per days (L/d),
EF=Exposure frequency (days/year),
ED=Exposure duration (years),
BW=Body weight (kg),
AT=Averaging time (days).
The DAD and IAD can be represent with continuous ingestion dose (CDI).
Based on the carcinogenesis of contamination, the risk could be classified into cancer risk and noncancer hazard.
Noncancer hazard: Generally, the reaction of the body to non-carcinogenic substance has a dose threshold.
Lower than the threshold, they could not affect our health adversely. The non-carcinogenic risk to represent with hazard index (HI). It is defined as a ratio that continuous ingestion dose with reference dose [28].
Where: CDI= continuous ingestion dose (mg/kg-days), RfD= reference dose (mg/kg-days).
Cancer risk: There does not have dose threshold for the carcinogenic. Once it exist in environments, it will affect human health adversely. Cancer risk will be represent with risk. It is defined as a product of continuous ingestion dose with carcinogenesis slope factor.
(If the low dose exposure risk>0.01)
Where: SF= carcinogenesis slope factor (mg-1•kg•d)
When calculating the risk of a variety of substances in a variety of ways, figure out all non-cancer risk and cancer risk respectively, then add all risks together. Regardless of synergistic effect and antagonistic effect.
Groundwater treatment technologies are mainly as follows: pump and treat, air sparging, in-situ groundwater bioremediation and in-situ reactive walls.
Pump and treat is the most common form of groundwater remediation. It is often associated with treatment technologies such as Air Stripping and Liquid-phase Granular Activated Charcoal.
Pump and treat involves pumping out contaminated groundwater with the use of a submersible or vacuum pump, and allowing the extracted groundwater to be purified by slowly proceeding through a series of vessels that contain materials designed to adsorb the contaminants from the groundwater. For petroleum-contaminated sites this material is usually activated carbon in granular form. Chemical reagents such as flocculants followed by sand filters may also be used to decrease the contamination of groundwater. Air stripping is a method that can be effective for volatile pollutants such as BTEX compounds found in gasoline.
For most biodegradable materials like BTEX, MTBE and most hydrocarbons, bioreactors can be used to clean the contaminated water to non-detectable levels. With fluidized bed bioreactors it is possible to achieve very low discharge concentrations which will meet or exceed discharge standards for most pollutants.
Depending on geology and soil type, pump and treat may be a good method to quickly reduce high concentrations of pollutants. It is more difficult to reach sufficiently low concentrations to satisfy remediation standards, due to the equilibrium of absorption (chemistry)/desorption processes in the soil.
At the figure 2, we can know how does pump and treat technology work. This system usually consists of one or more wells equipped with pumps. When the pumps are turned on, they pull the polluted groundwater into the wells and up to the surface. At the surface, the water goes into a holding tank and then on to a treatment system, where it is cleaned [29].
Pump and Treat Technology [29]
Air sparging is an in situ groundwater remediation technology that involves the injection of a gas (usually air/oxygen) under pressure into a well installed into the saturated zone. Air sparging technology extends the applicability of soil vapor extraction to saturated soils and groundwater through physical removal of volatilized groundwater contaminants and enhanced biodegradation in the saturated and unsaturated zones. Oxygen injected below the water table volatilizes contaminants that are dissolved in groundwater, existing as a separate aqueous phase, and/or sobbed onto saturated soil particles. The volatilized contaminants migrate upward in the vadose zone, where they are removed, and generally using soil vapor extraction techniques. This process of moving dissolved and non-aqueous volatile organic compounds (VOCs), originally located below the water table, into the unsaturated zone has been likened to an in situ, saturated zone, air stripping system. In addition to this air stripping process, air sparging also promotes biodegradation by increasing oxygen concentrations in the subsurface, stimulating aerobic biodegradation in the saturated and unsaturated zones(figure 3).
Air Sparging [31]
In-situ groundwater bioremediation is a technology that encourages growth and reproduction of indigenous microorganisms to enhance biodegradation of organic constituents in the saturated zone. In-situ groundwater bioremediation can effectively degrade organic constituents which are dissolved in groundwater and adsorbed onto the aquifer matrix.
In-situ groundwater bioremediation can be effective for the full range of petroleum hydrocarbons. While there are some notable exceptions (e.g., MTBE) the short-chain, low-molecular-weight, more water soluble constituents are degraded more rapidly and to lower residual levels than are long-chain, high-molecular-weight, less soluble constituents. Recoverable free product should be removed from the subsurface prior to operation of the in-situ groundwater bioremediation system. This will mitigate the major source of contaminants as well as reduce the potential for smearing or spreading high concentrations of contaminants.
In-situ bioremediation of groundwater can be combined with other saturated zone remedial technologies (e.g., air sparging) and unsaturated zone remedial operations (e.g., soil vapor extraction, bioventing).
Bioremediation generally requires a mechanism for stimulating and maintaining the activity of these microorganisms. This mechanism is usually a delivery system for providing one or more of the following: An electron acceptor (oxygen, nitrate); nutrients (nitrogen, phosphorus); and an energy source (carbon). Generally, electron acceptors and nutrients are the two most critical components of any delivery system.
In a typical in-situ bioremediation system, groundwater is extracted using one or more wells and, if necessary, treated to remove residual dissolved constituents. The treated groundwater is then mixed with an electron acceptor and nutrients, and other constituents if required, and re-injected upgradient of or within the contaminant source. Infiltration galleries or injection wells may be used to re-inject treated water. In an ideal configuration, a "closed-loop" system would be established. All water extracted would be re-injected without treatment and all remediation would occur in situ. This ideal system would continually recirculate the water until cleanup levels had been achieved. If your state does not allow re-injection of extracted groundwater, it may be feasible to mix the electron acceptor and nutrients with fresh water instead. Extracted water that is not re-injected must be discharged, typically to surface water or to publicly owned treatment works (POTW).
In-situ reactive walls are an emerging technology that have been evaluated, developed, and implemented only within the last few years. This technology is gaining widespread attention due to the increasing recognition of the limitations of pump and treat systems, and the ability to implement various treatment processes that have historically only been used in above-ground systems in an in situ environment. This technology is also known in the remediation industry as “funnel and gate systems” or “treatment walls”.
The concept of in-situ reactive walls involves the installation of impermeable barriers downgrading of the contaminated groundwater plume and hydraulic manipulation of impacted groundwater to be directed through porous reactive gates installed within the impermeable barrier. Treatment processes designed specifically to treat the target contaminants can be implemented in these reactive or treatment gates. Treated groundwater follows its natural course after exiting the treatment gates. The flow through the treatment gates is driven by natural groundwater gradients, and hence these systems are often referred to as passive treatment walls. If a groundwater plume is relatively narrow, a permeable reactive trench can be installed across the full width of the plume, and thus preclude the necessity for installation of impermeable barriers.
In-situ reactive walls eliminate or at least minimize the need for mechanical systems, thereby reducing the long-term operation and maintenance costs that so often drive up the life cycle costs of many remediation projects. In addition, groundwater monitoring and system compliance issues can be streamlined for even greater cost savings.
Bioventing, also a modification of vapor extraction technology, is briefly contrasted with air sparging. With bioventing, extraction or injection of air into the vadose zone increases subsurface oxygen concentration, promoting bioremediation of unsaturated soil contaminants. This technique is applicable to all biodegradable contaminants, but has been applied most frequently and reportedly most successfully to sites with petroleum hydrocarbon contamination
The past 40 years, groundwater subjected to pollution, it cannot be ignored that there has a serious threat to human health and ecological security problems. The research on groundwater pollution risk assessment will help understand the relationship between the soil conditions and groundwater pollution, identify the high-risk regions of groundwater pollution, provide a powerful tools for the land use and groundwater resource management, and help the policy maker and managers to develop effective management strategies and protection measures on groundwater. So we can offer some suggestions as following:
Continue to strengthen the research on the fate and transport in hydrogeological conditions. Hydrogeological conditions of the contaminated sites have a vital role in organic pollution of groundwater. We should pay attention to the impact that the thickness of the unsaturated zone, the aquifer lithology of unsaturated zone and groundwater, the groundwater runoff conditions on the organic pollution investigation and contaminated aquifer restoration. Unsaturated zone is the only avenue for the organic pollutant into the groundwater system. In the protection of groundwater quality, we should take impact of the physical, chemical, and biological characteristics of the unsaturated zone soil on the transport and degradation of organic pollutants into consideration.
In the future research, the natural attenuation of typical organic contamination in groundwater should be reinforce research, especially the organic degradation mechanism of microbes.
In recent years, the environmental hormone pollution research and prevention has begun to attract the attention of the world. Environmental hormone research has become the forefront and hot topic of environmental science research. But the mechanism of environmental hormone is not clearly, we should take more attention on these.
The research on groundwater pollution risk assessment to be carried out on the typical regions. To provide practical experience on established an reasonable and feasible groundwater pollution risk assessment system.
Exerting governmental function adequately and improving the laws, regulations and norms on groundwater quality monitor and assessment. Strengthening the cross-disciplinary exchanges and studies and establishing the groundwater pollution monitor network and the chemical toxicological database.
With entering a new era of environmental protection, the research of groundwater pollution risk assessment is bound to make new contributions to human survival and to protect and improve the natural environment, and to advance the theory research of environmental science.
This study is granted by the Specific Research on Public Service of Environmental Protection in China (No. 201009009). The authors appreciate the tutor and classmates for help.
Stability constant of the formation of metal complexes is used to measure interaction strength of reagents. From this process, metal ion and ligand interaction formed the two types of metal complexes; one is supramolecular complexes known as host-guest complexes [1] and the other is anion-containing complexes. In the solution it provides and calculates the required information about the concentration of metal complexes.
Solubility, light, absorption conductance, partitioning behavior, conductance, and chemical reactivity are the complex characteristics which are different from their components. It is determined by various numerical and graphical methods which calculate the equilibrium constants. This is based on or related to a quantity, and this is called the complex formation function.
During the displacement process at the time of metal complex formation, some ions disappear and form a bonding between metal ions and ligands. It may be considered due to displacement of a proton from a ligand species or ions or molecules causing a drop in the pH values of the solution [2]. Irving and Rossotti developed a technique for the calculation of stability constant, and it is called potentiometric technique.
To determine the stability constant, Bjerrum has used a very simple method, and that is metal salt solubility method. For the studies of a larger different variety of polycarboxylic acid-, oxime-, phenol-containing metal complexes, Martel and Calvin used the potentiometric technique for calculating the stability constant. Those ligands [3, 4] which are uncharged are also examined, and their stability constant calculations are determined by the limitations inherent in the ligand solubility method. The limitations of the metal salt solubility method and the result of solubility methods are compared with this. M-L, MLM, and (M3) L are some types of examples of metal-ligand bonding. One thing is common, and that is these entire types metal complexes all have one ligand.
The solubility method can only usefully be applied to studies of such complexes, and it is best applied for ML; in such types of system, only ML is formed. Jacqueline Gonzalez and his co-worker propose to explore the coordination chemistry of calcium complexes. Jacqueline and et al. followed this technique for evaluate the as partial model of the manganese-calcium cluster and spectrophotometric studies of metal complexes, i.e., they were carried calcium(II)-1,4-butanediamine in acetonitrile and calcium(II)-1,2-ethylendiamine, calcium(II)-1,3-propanediamine by them.
Spectrophotometric programming of HypSpec and received data allows the determination of the formation of solubility constants. The logarithmic values, log β110 = 5.25 for calcium(II)-1,3-propanediamine, log β110 = 4.072 for calcium(II)-1,4-butanediamine, and log β110 = 4.69 for calcium(II)-1,2-ethylendiamine, are obtained for the formation constants [5]. The structure of Cimetidine and histamine H2-receptor is a chelating agent. Syed Ahmad Tirmizi has examined Ni(II) cimetidine complex spectrophotometrically and found an absorption peak maximum of 622 nm with respect to different temperatures.
Syed Ahmad Tirmizi have been used to taken 1:2 ratio of metal and cimetidine compound for the formation of metal complex and this satisfied by molar ratio data. The data, 1.40–2.4 × 108, was calculated using the continuous variation method and stability constant at room temperature, and by using the mole ratio method, this value at 40°C was 1.24–2.4 × 108. In the formation of lead(II) metal complexes with 1-(aminomethyl) cyclohexene, Thanavelan et al. found the formation of their binary and ternary complexes. Glycine,
Using the stability constant method, these ternary complexes were found out, and using the parameters such as Δ log K and log X, these ternary complex data were compared with binary complex. The potentiometric technique at room temperature (25°C) was used in the investigation of some binary complex formations by Abdelatty Mohamed Radalla. These binary complexes are formed with 3D transition metal ions like Cu2+, Ni2+, Co2+, and Zn2+ and gallic acid’s importance as a ligand and 0.10 mol dm−3 of NaNO3. Such types of aliphatic dicarboxylic acids are very important biologically. Many acid-base characters and the nature of using metal complexes have been investigated and discussed time to time by researchers [7].
The above acids (gallic and aliphatic dicarboxylic acid) were taken to determine the acidity constants. For the purpose of determining the stability constant, binary and ternary complexes were carried in the aqueous medium using the experimental conditions as stated above. The potentiometric pH-metric titration curves are inferred for the binary complexes and ternary complexes at different ratios, and formation of ternary metal complex formation was in a stepwise manner that provided an easy way to calculate stability constants for the formation of metal complexes.
The values of Δ log K, percentage of relative stabilization (% R. S.), and log X were evaluated and discussed. Now it provides the outline about the various complex species for the formation of different solvents, and using the concentration distribution, these complexes were evaluated and discussed. The conductivity measurements have ascertained for the mode of ternary chelating complexes.
A study by Kathrina and Pekar suggests that pH plays an important role in the formation of metal complexes. When epigallocatechin gallate and gallic acid combine with copper(II) to form metal complexes, the pH changes its speculation. We have been able to determine its pH in frozen and fluid state with the help of multifrequency EPR spectroscopy [8]. With the help of this spectroscopy, it is able to detect that each polyphenol exhibits the formation of three different mononuclear species. If the pH ranges 4–8 for di- or polymeric complex of Cu(II), then it conjectures such metal complexes. It is only at alkaline pH values.
The line width in fluid solutions by molecular motion exhibits an incomplete average of the parameters of anisotropy spin Hamilton. If the complexes are different, then their rotational correlation times for this also vary. The analysis of the LyCEP anisotropy of the fluid solution spectra is performed using the parameters determined by the simulation of the rigid boundary spectra. Its result suggests that pH increases its value by affecting its molecular mass. It is a polyphenol ligand complex with copper, showing the coordination of an increasing number of its molecules or increasing participation of polyphenol dimers used as ligands in the copper coordination region.
The study by Vishenkova and his co-worker [8] provides the investigation of electrochemical properties of triphenylmethane dyes using a voltammetric method with constant-current potential sweep. Malachite green (MG) and basic fuchsin (BF) have been chosen as representatives of the triphenylmethane dyes [9]. The electrochemical behavior of MG and BF on the surface of a mercury film electrode depending on pH, the nature of background electrolyte, and scan rate of potential sweep has been investigated.
Using a voltammetric method with a constant-current potential sweep examines the electrical properties of triphenylmethane dye. In order to find out the solution of MG and BF, certain registration conditions have been prescribed for it, which have proved to be quite useful. The reduction peak for the currents of MG and BF has demonstrated that it increases linearly with respect to their concentration as 9.0 × 10−5–7.0 × 10−3 mol/dm3 for MG and 6.0 × 10−5–8.0 × 10−3 mol/dm3 for BF and correlation coefficients of these values are 0.9987 for MG and 0.9961 for BF [10].
5.0 × 10−5 and 2.0 × 10−5 mol/dm3 are the values used as the detection limit of MG and BF, respectively. Stability constants are a very useful technique whose size is huge. Due to its usefulness, it has acquired an umbrella right in the fields of chemistry, biology, and medicine. No science subject is untouched by this. Stability constants of metal complexes are widely used in the various areas like pharmaceuticals as well as biological processes, separation techniques, analytical processes, etc. In the presented chapter, we have tried to explain this in detail by focusing our attention on the applications and solutions of stability of metal complexes in solution.
Stability or formation or binding constant is the type of equilibrium constant used for the formation of metal complexes in the solution. Acutely, stability constant is applicable to measure the strength of interactions between the ligands and metal ions that are involved in complex formation in the solution [11]. A generally these 1-4 equations are expressed as the following ways:
Thus
K1, K2, K3, … Kn are the equilibrium constants and these are also called stepwise stability constants. The formation of the metal-ligand-n complex may also be expressed as equilibrium constants by the following steps:
The parameters K and β are related together, and these are expressed in the following example:
Now the numerator and denominator are multiplied together with the use of [metal-ligand] [metal-ligand2], and after the rearranging we get the following equation:
Now we expressed it as the following:
From the above relation, it is clear that the overall stability constant βn is equal to the product of the successive (i.e., stepwise) stability constants, K1, K2, K3,…Kn. This in other words means that the value of stability constants for a given complex is actually made up of a number of stepwise stability constants. The term stability is used without qualification to mean that the complex exists under a suitable condition and that it is possible to store the complex for an appreciable amount of time. The term stability is commonly used because coordination compounds are stable in one reagent but dissociate or dissolve in the presence of another regent. It is also possible that the term stability can be referred as an action of heat or light or compound. The stability of complex [13] is expressed qualitatively in terms of thermodynamic stability and kinetic stability.
In a chemical reaction, chemical equilibrium is a state in which the concentration of reactants and products does not change over time. Often this condition occurs when the speed of forward reaction becomes the same as the speed of reverse reaction. It is worth noting that the velocities of the forward and backward reaction are not zero at this stage but are equal.
If hydrogen and iodine are kept together in molecular proportions in a closed process vessel at high temperature (500°C), the following action begins:
In this activity, hydrogen iodide is formed by combining hydrogen and iodine, and the amount of hydrogen iodide increases with time. In contrast to this action, if the pure hydrogen iodide gas is heated to 500°C in the reaction, the compound is dissolved by reverse action, which causes hydrogen iodide to dissolve into hydrogen and iodine, and the ratio of these products increases over time. This is expressed in the following reaction:
For the formation of metal chelates, the thermodynamic technique provides a very significant information. Thermodynamics is a very useful technique in distinguishing between enthalpic effects and entropic effects. The bond strengths are totally effected by enthalpic effect, and this does not make any difference in the whole solution in order/disorder. Based on thermodynamics the chelate effect below can be best explained. The change of standard Gibbs free energy for equilibrium constant is response:
Where:
R = gas constant
T = absolute temperature
At 25°C,
ΔG = (− 5.708 kJ mol−1) · log β.
The enthalpy term creates free energy, i.e.,
For metal complexes, thermodynamic stability and kinetic stability are two interpretations of the stability constant in the solution. If reaction moves from reactants to products, it refers to a change in its energy as shown in the above equation. But for the reactivity, kinetic stability is responsible for this system, and this refers to ligand species [14].
Stable and unstable are thermodynamic terms, while labile and inert are kinetic terms. As a rule of thumb, those complexes which react completely within about 1 minute at 25°C are considered labile, and those complexes which take longer time than this to react are considered inert. [Ni(CN)4]2− is thermodynamically stable but kinetically inert because it rapidly exchanges ligands.
The metal complexes [Co(NH3)6]3+ and such types of other complexes are kinetically inert, but these are thermodynamically unstable. We may expect the complex to decompose in the presence of acid immediately because the complex is thermodynamically unstable. The rate is of the order of 1025 for the decomposition in acidic solution. Hence, it is thermodynamically unstable. However, nothing happens to the complex when it is kept in acidic solution for several days. While considering the stability of a complex, always the condition must be specified. Under what condition, the complex which is stable or unstable must be specified such as acidic and also basic condition, temperature, reactant, etc.
A complex may be stable with respect to a particular condition but with respect to another. In brief, a stable complex need not be inert and similarly, and an unstable complex need not be labile. It is the measure of extent of formation or transformation of complex under a given set of conditions at equilibrium [15].
Thermodynamic stability has an important role in determining the bond strength between metal ligands. Some complexes are stable, but as soon as they are introduced into aqueous solution, it is seen that these complexes have an effect on stability and fall apart. For an example, we take the [Co (SCN)4]2+ complex. The ion bond of this complex is very weak and breaks down quickly to form other compounds. But when [Fe(CN)6]3− is dissolved in water, it does not test Fe3+ by any sensitive reagent, which shows that this complex is more stable in aqueous solution. So it is indicated that thermodynamic stability deals with metal-ligand bond energy, stability constant, and other thermodynamic parameters.
This example also suggests that thermodynamic stability refers to the stability and instability of complexes. The measurement of the extent to which one type of species is converted to another species can be determined by thermodynamic stability until equilibrium is achieved. For example, tetracyanonickelate is a thermodynamically stable and kinetic labile complex. But the example of hexa-amine cobalt(III) cation is just the opposite:
Thermodynamics is used to express the difference between stability and inertia. For the stable complex, large positive free energies have been obtained from ΔG0 reaction. The ΔH0, standard enthalpy change for this reaction, is related to the equilibrium constant, βn, by the well thermodynamic equation:
For similar complexes of various ions of the same charge of a particular transition series and particular ligand, ΔS0 values would not differ substantially, and hence a change in ΔH0 value would be related to change in βn values. So the order of values of ΔH0 is also the order of the βn value.
Kinetic stability is referred to the rate of reaction between the metal ions and ligand proceeds at equilibrium or used for the formation of metal complexes. To take a decision for kinetic stability of any complexes, time is a factor which plays an important role for this. It deals between the rate of reaction and what is the mechanism of this metal complex reaction.
As we discuss above in thermodynamic stability, kinetic stability is referred for the complexes at which complex is inert or labile. The term “inert” was used by Tube for the thermally stable complex and for reactive complexes the term ‘labile’ used [16]. The naturally occurring chlorophyll is the example of polydentate ligand. This complex is extremely inert due to exchange of Mg2+ ion in the aqueous media.
The nature of central atom of metal complexes, dimension, its degree of oxidation, electronic structure of these complexes, and so many other properties of complexes are affected by the stability constant. Some of the following factors described are as follows.
In the coordination chemistry, metal complexes are formed by the interaction between metal ions and ligands. For these type of compounds, metal ions are the coordination center, and the ligand or complexing agents are oriented surrounding it. These metal ions mostly are the transition elements. For the determination of stability constant, some important characteristics of these metal complexes may be as given below.
Ligands are oriented around the central metal ions in the metal complexes. The sizes of these metal ions determine the number of ligand species that will be attached or ordinated (dative covalent) in the bond formation. If the sizes of these metal ions are increased, the stability of coordination compound defiantly decreased. Zn(II) metal ions are the central atoms in their complexes, and due to their lower size (0.74A°) as compared to Cd(II) size (0.97A°), metal ions are formed more stable.
Hence, Al3+ ion has the greatest nuclear charge, but its size is the smallest, and the ion N3− has the smallest nuclear charge, and its size is the largest [17]. Inert atoms like neon do not participate in the formation of the covalent or ionic compound, and these atoms are not included in isoelectronic series; hence, it is not easy to measure the radius of this type of atoms.
The properties of stability depend on the size of the metal ion used in the complexes and the total charge thereon. If the size of these metal ions is small and the total charge is high, then their complexes will be more stable. That is, their ratio will depend on the charge/radius. This can be demonstrated through the following reaction:
An ionic charge is the electric charge of an ion which is formed by the gain (negative charge) or loss (positive charge) of one or more electrons from an atom or group of atoms. If we talk about the stability of the coordination compounds, we find that the total charge of their central metal ions affects their stability, so when we change their charge, their stability in a range of constant can be determined by propagating of error [18]. If the charge of the central metal ion is high and the size is small, the stability of the compound is high:
In general, the most stable coordination bonds can cause smaller and highly charged rations to form more stable coordination compounds.
When an electron pair attracts a central ion toward itself, a strong stability complex is formed, and this is due to electron donation from ligand → metal ion. This donation process is increasing the bond stability of metal complexes exerted the polarizing effect on certain metal ions. Li+, Na+, Mg2+, Ca2+, Al3+, etc. are such type of metal cation which is not able to attract so strongly from a highly electronegative containing stable complexes, and these atoms are O, N, F, Au, Hg, Ag, Pd, Pt, and Pb. Such type of ligands that contains P, S, As, Br and I atom are formed stable complex because these accepts electron from M → π-bonding. Hg2+, Pb2+, Cd2+, and Bi3+ metal ions are also electronegative ions which form insoluble salts of metal sulfide which are insoluble in aqueous medium.
Volatile ligands may be lost at higher temperature. This is exemplified by the loss of water by hydrates and ammonia:
The transformation of certain coordination compounds from one to another is shown as follows:
A ligand is an ion or small molecule that binds to a metal atom (in chemistry) or to a biomolecule (in biochemistry) to form a complex, such as the iron-cyanide coordination complex Prussian blue or the iron-containing blood-protein hemoglobin. The ligands are arranged in spectrochemical series which are based on the order of their field strength. It is not possible to form the entire series by studying complexes with a single metal ion; the series has been developed by overlapping different sequences obtained from spectroscopic studies [19]. The order of common ligands according to their increasing ligand field strength is
The above spectrochemical series help us to for determination of strength of ligands. The left last ligand is as weaker ligand. These weaker ligand cannot forcible binding the 3d electron and resultant outer octahedral complexes formed. It is as-
Increasing the oxidation number the value of Δ increased.
Δ increases from top to bottom.
However, when we consider the metal ion, the following two useful trends are observed:
Δ increases with increasing oxidation number.
Δ increases down a group. For the determination of stability constant, the nature of the ligand plays an important role.
The following factors described the nature of ligands.
The size and charge are two factors that affect the production of metal complexes. The less charges and small sizes of ligands are more favorable for less stable bond formation with metal and ligand. But if this condition just opposite the product of metal and ligand will be a more stable compound. So, less nuclear charge and more size= less stable complex whereas if more nuclear charge and small in size= less stable complex. We take fluoride as an example because due to their smaller size than other halide and their highest electro negativity than the other halides formed more stable complexes. So, fluoride ion complexes are more stable than the other halides:
As compared to S2− ion, O22− ions formed more stable complexes.
It is suggested by Calvin and Wilson that the metal complexes will be more stable if the basic character or strength of ligands is higher. It means that the donating power of ligands to central metal ions is high [20].
It means that the donating power of ligands to central metal ions is high. In the case of complex formation of aliphatic diamines and aromatic diamines, the stable complex is formed by aliphatic diamines, while an unstable coordination complex is formed with aromatic diamines. So, from the above discussion, we find that the stability will be grater if the e-donation power is greater.
Thus it is clear that greater basic power of electron-donating species will form always a stable complex. NH3, CN−, and F− behaved as ligands and formed stable complexes; on the other hand, these are more basic in nature.
We know that if the concentration of coordination group is higher, these coordination compounds will exist in the water as solution. It is noted that greater coordinating tendency show the water molecules than the coordinating group which is originally present. SCN− (thiocynate) ions are present in higher concentration; with the Co2+ metal ion, it formed a blue-colored complex which is stable in state, but on dilution of water medium, a pink color is generated in place of blue, or blue color complex is destroyed by [Co(H2O)6]2+, and now if we added further SCN−, the pink color will not appear:
Now it is clear that H2O and SCN− are in competition for the formation of Co(II) metal-containing complex compound. In the case of tetra-amine cupric sulfate metal complex, ammonia acts as a donor atom or ligand. If the concentration of NH3 is lower in the reaction, copper hydroxide is formed but at higher concentration formed tetra-amine cupric sulfate as in the following reaction:
For a metal ion, chelating ligand is enhanced and affinity it and this is known as chelate effect and compared it with non-chelating and monodentate ligand or the multidentate ligand is acts as chelating agent. Ethylenediamine is a simple chelating agent (Figure 1).
Structure of ethylenediamine.
Due to the bidentate nature of ethylenediamine, it forms two bonds with metal ion or central atom. Water forms a complex with Ni(II) metal ion, but due to its monodentate nature, it is not a chelating ligand (Figures 2 and 3).
Structure of chelating configuration of ethylenediamine ligand.
Structure of chelate with three ethylenediamine ligands.
The dentate cheater of ligand provides bonding strength to the metal ion or central atom, and as the number of dentate increased, the tightness also increased. This phenomenon is known as chelating effect, whereas the formation of metal complexes with these chelating ligands is called chelation:
or
Some factors are of much importance for chelation as follows.
The sizes of the chelating ring are increased as well as the stability of metal complex decreased. According to Schwarzenbach, connecting bridges form the chelating rings. The elongated ring predominates when long bridges connect to the ligand to form a long ring. It is usually observed that an increased a chelate ring size leads to a decrease in complex stability.
He interpreted this statement. The entropy of complex will be change if the size of chelating ring is increased, i.e., second donor atom is allowed by the chelating ring. As the size of chelating ring increased, the stability should be increased with entropy effect. Four-membered ring compounds are unstable, whereas five-membered are more stable. So the chelating ring increased its size and the stability of the formed metal complexes.
The number of chelating rings also decides the stability of complexes. Non-chelating metal compounds are less stable than chelating compounds. These numbers increase the thermodynamic volume, and this is also known as an entropy term. In recent years ligands capable of occupying as many as six coordination positions on a single metal ion have been described. The studies on the formation constants of coordination compounds with these ligands have been reported. The numbers of ligand or chelating agents are affecting the stability of metal complexes so as these numbers go up and down, the stability will also vary with it.
For the Ni(II) complexes with ethylenediamine as chelating agent, its log K1 value is 7.9 and if chelating agents are trine and penten, then the log K1 values are 7.9 and 19.3, respectively. If the metal ion change Zn is used in place of Ni (II), then the values of log K1 for ethylenediamine, trine, and penten are 6.0, 12.1, and 16.2, respectively. The log βMY values of metal ions are given in Table 1.
Metal ion | log βMY (25°C, I = 0.1 M) |
---|---|
Ca2+ | 11.2 |
Cu2+ | 19.8 |
Fe3+ | 24.9 |
Metal ion vs. log βMY values.
Ni(NH3)62+ is an octahedral metal complex, and at 25 °C its log β6 value is 8.3, but Ni(ethylenediamine)32+ complex is also octahedral in geometry, with 18.4 as the value of log β6. The calculated stability value of Ni(ethylenediamine)32+ 1010 times is more stable because three rings are formed as chelating rings by ethylenediamine as compared to no such ring is formed. Ethylenediaminetetraacetate (EDTA) is a hexadentate ligand that usually formed stable metal complexes due to its chelating power.
A special effect in molecules is when the atoms occupy space. This is called steric effect. Energy is needed to bring these atoms closer to each other. These electrons run away from near atoms. There can be many ways of generating it. We know the repulsion between valence electrons as the steric effect which increases the energy of the current system [21]. Favorable or unfavorable any response is created.
For example, if the static effect is greater than that of a product in a metal complex formation process, then the static increase would favor this reaction. But if the case is opposite, the skepticism will be toward retardation.
This effect will mainly depend on the conformational states, and the minimum steric interaction theory can also be considered. The effect of secondary steric is seen on receptor binding produced by an alternative such as:
Reduced access to a critical group.
Stick barrier.
Electronic resonance substitution bond by repulsion.
Population of a conformer changes due to active shielding effect.
The macrocyclic effect is exactly like the image of the chelate effect. It means the principle of both is the same. But the macrocyclic effect suggests cyclic deformation of the ligand. Macrocyclic ligands are more tainted than chelating agents. Rather, their compounds are more stable due to their cyclically constrained constriction. It requires some entropy in the body to react with the metal ion. For example, for a tetradentate cyclic ligand, we can use heme-B which forms a metal complex using Fe+2 ions in biological systems (Figure 4).
Structure of hemoglobin is the biological complex compound which contains Fe(II) metal ion.
The n-dentate chelating agents play an important role for the formation of more stable metal complexes as compared to n-unidentate ligands. But the n-dentate macrocyclic ligand gives more stable environment in the metal complexes as compared to open-chain ligands. This change is very favorable for entropy (ΔS) and enthalpy (ΔH) change.
There are so many parameters to determination of formation constants or stability constant in solution for all types of chelating agents. These numerous parameters or techniques are refractive index, conductance, temperature, distribution coefficients, refractive index, nuclear magnetic resonance volume changes, and optical activity.
Solubility products are helpful and used for the insoluble salt that metal ions formed and complexes which are also formed by metal ions and are more soluble. The formation constant is observed in presence of donor atoms by measuring increased solubility.
To determine the solubility constant, it involves the distribution of the ligands or any complex species; metal ions are present in two immiscible solvents like water and carbon tetrachloride, benzene, etc.
In this method metal ions or ligands are present in solution and on exchanger. A solid polymers containing with positive and negative ions are ion exchange resins. These are insoluble in nature. This technique is helpful to determine the metal ions in resin phase, liquid phase, or even in radioactive metal. This method is also helpful to determine the polarizing effect of metal ions on the stability of ligands like Cu(II) and Zn(II) with amino acid complex formation.
At the equilibrium free metal and ions are present in the solution, and using the different electrometric techniques as described determines its stability constant.
This method is based upon the titration method or follows its principle. A stranded acid-base solution used as titrate and which is titrated, it may be strong base or strong acid follows as potentiometrically. The concentration of solution using 103− M does not decomposed during the reaction process, and this method is useful for protonated and nonprotonated ligands.
This is the graphic method used to determine the stability constant in producing metal complex formation by plotting a polarograph between the absences of substances and the presence of substances. During the complex formation, the presence of metal ions produced a shift in the half-wave potential in the solution.
If a complex is relatively slow to form and also decomposes at measurable rate, it is possible, in favorable situations, to determine the equilibrium constant.
This involves the study of the equilibrium constant of slow complex formation reactions. The use of tracer technique is extremely useful for determining the concentrations of dissociation products of the coordination compound.
This method is based on the study of the effect of an equilibrium concentration of some ions on the function at a definite organ of a living organism. The equilibrium concentration of the ion studied may be determined by the action of this organ in systems with complex formation.
The solution of 25 ml is adopted by preparing at the 1.0 × 10−5 M ligand or 1.0 × 10−5 M concentration and 1.0 × 10−5 M for the metal ion:
The solutions containing the metal ions were considered both at a pH sufficiently high to give almost complete complexation and at a pH value selected in order to obtain an equilibrium system of ligand and complexes.
In order to avoid modification of the spectral behavior of the ligand due to pH variations, it has been verified that the range of pH considered in all cases does not affect absorbance values. Use the collected pH values adopted for the determinations as well as selected wavelengths. The ionic strengths calculated from the composition of solutions allowed activity coefficient corrections. Absorbance values were determined at wavelengths in the range 430–700 nm, every 2 nm.
For a successive metal complex formation, use this method. If ligand is protonate and the produced complex has maximum number of donate atoms of ligands, a selective light is absorbed by this complex, while for determination of stability constant, it is just known about the composition of formed species.
Bjerrum (1941) used the method stepwise addition of the ligands to coordination sphere for the formation of complex. So, complex metal–ligand-n forms as the following steps [22]. The equilibrium constants, K1, K2, K3, … Kn are called stepwise stability constants. The formation of the complex metal-ligandn may also be expressed by the following steps and equilibrium constants.
Where:
M = central metal cation
L = monodentate ligand
N = maximum coordination number for the metal ion M for the ligand
If a complex ion is slow to reach equilibrium, it is often possible to apply the method of isotopic dilution to determine the equilibrium concentration of one or more of the species. Most often radioactive isotopes are used.
This method was extensively used by Werner and others to study metal complexes. In the case of a series of complexes of Co(III) and Pt(IV), Werner assigned the correct formulae on the basis of their molar conductance values measured in freshly prepared dilute solutions. In some cases, the conductance of the solution increased with time due to a chemical change, e.g.,
It is concluded that the information presented is very important to determine the stability constant of the ligand metal complexes. Some methods like spectrophotometric method, Bjerrum’s method, distribution method, ion exchange method, electrometric techniques, and potentiometric method have a huge contribution in quantitative analysis by easily finding the stability constants of metal complexes in aqueous solutions.
All the authors thank the Library of University of Delhi for reference books, journals, etc. which helped us a lot in reviewing the chapter.
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