Composition of the raw paper sludge
\\n\\n
Dr. Pletser’s experience includes 30 years of working with the European Space Agency as a Senior Physicist/Engineer and coordinating their parabolic flight campaigns, and he is the Guinness World Record holder for the most number of aircraft flown (12) in parabolas, personally logging more than 7,300 parabolas.
\\n\\nSeeing the 5,000th book published makes us at the same time proud, happy, humble, and grateful. This is a great opportunity to stop and celebrate what we have done so far, but is also an opportunity to engage even more, grow, and succeed. It wouldn't be possible to get here without the synergy of team members’ hard work and authors and editors who devote time and their expertise into Open Access book publishing with us.
\\n\\nOver these years, we have gone from pioneering the scientific Open Access book publishing field to being the world’s largest Open Access book publisher. Nonetheless, our vision has remained the same: to meet the challenges of making relevant knowledge available to the worldwide community under the Open Access model.
\\n\\nWe are excited about the present, and we look forward to sharing many more successes in the future.
\\n\\nThank you all for being part of the journey. 5,000 times thank you!
\\n\\nNow with 5,000 titles available Open Access, which one will you read next?
\\n\\nRead, share and download for free: https://www.intechopen.com/books
\\n\\n\\n\\n
\\n"}]',published:!0,mainMedia:null},components:[{type:"htmlEditorComponent",content:'
Preparation of Space Experiments edited by international leading expert Dr. Vladimir Pletser, Director of Space Training Operations at Blue Abyss is the 5,000th Open Access book published by IntechOpen and our milestone publication!
\n\n"This book presents some of the current trends in space microgravity research. The eleven chapters introduce various facets of space research in physical sciences, human physiology and technology developed using the microgravity environment not only to improve our fundamental understanding in these domains but also to adapt this new knowledge for application on earth." says the editor. Listen what else Dr. Pletser has to say...
\n\n\n\nDr. Pletser’s experience includes 30 years of working with the European Space Agency as a Senior Physicist/Engineer and coordinating their parabolic flight campaigns, and he is the Guinness World Record holder for the most number of aircraft flown (12) in parabolas, personally logging more than 7,300 parabolas.
\n\nSeeing the 5,000th book published makes us at the same time proud, happy, humble, and grateful. This is a great opportunity to stop and celebrate what we have done so far, but is also an opportunity to engage even more, grow, and succeed. It wouldn't be possible to get here without the synergy of team members’ hard work and authors and editors who devote time and their expertise into Open Access book publishing with us.
\n\nOver these years, we have gone from pioneering the scientific Open Access book publishing field to being the world’s largest Open Access book publisher. Nonetheless, our vision has remained the same: to meet the challenges of making relevant knowledge available to the worldwide community under the Open Access model.
\n\nWe are excited about the present, and we look forward to sharing many more successes in the future.
\n\nThank you all for being part of the journey. 5,000 times thank you!
\n\nNow with 5,000 titles available Open Access, which one will you read next?
\n\nRead, share and download for free: https://www.intechopen.com/books
\n\n\n\n
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The pulp and paper industry, in Europe, generates 11 million tons of solid waste each year (Monte et al., 2009). Paper waste covers a diverse range of non-hazardous waste streams, prominent among which are different types of sludge, boiler ash, combustion furnace ash and organic and inorganic rejects. Manufacturing processes to produce new paper from the deinking of recycled paper account for 70% of these waste products.
\n\t\t\tFollowing its reception, sorting and storage, the recycled paper is transformed into an aqueous suspension of fibers, while inappropriate materials are eliminated in different cleaning processes. Following this initial treatment, the resultant paper sludge is subjected to deinking in a froth flotation process, which produces waste known as de-inked sludge. This waste sludge is fundamentally composed of water, fiber, ink and a mineral load. In addition, various paper manufacturing processes have water treatment plants that generate sludges with high humidity contents.
\n\t\t\tThe deinked paper sludge and the sludge from the water treatment process have a high humidity content (≈ 50%), and are roughly composed of organic material with their origin in paper fibers (≈ 25%) and mineral loads such as calcium carbonate, kaolin, talc and titanium oxide (≈ 25%). A similar composition highlights the wealth of energetic and mineral resources saturating the paper sludge. Thus, the most advanced techniques for the use of paper sludge are intended to take full advantage of the saturated biomass and the recovery of the mineral constituents in the inorganic fraction.
\n\t\t\tThe most common options for the processing of paper industry sludge range from their exploitation for agricultural purposes, composting, or use as a primary material in the manufacture of ceramics and cement (Moo-Young & Zimmie, 1997; Ahmadi & Al-Khaja, 2001; Lima & Dal Molin, 2005; Conesa et al., 2008), to energy recovery in biomass boilers or fluidized bed systems. Thus, the Dutch CDEM process (International Patent, 2006) represents a pioneering recovery system, where the paper sludge is treated at temperatures of around 730ºC, in a fluidized bed combustion system, so as to activate the latent pozzolanic properties of its mineral content. The CDEM process was industrialized after the pioneering work of research groups led by Prof. Pera (Pera & Amrouz, 1998), which demonstrated that controlled calcination of the deinked sludge produces a highly reactive pozzolanic material, within a temperature range of between 700 and 750ºC.
\n\t\t\tOn the basis of the scientific knowledge presented earlier, a team of Spanish researchers led by Dr. Frías, has been conducting in-depth research over the past decade into the scientific, technological and environmental aspects of obtaining active admixtures from the calcination of paper sludge and its behavior in cement and mortar.
\n\t\tThe characteristic composition of this industrial waste is a mixture of organic material (non-recovered cellulose) and inorganic materials (principally, kaolinite and limestone), normally used as loadings in the manufacture of paper.
\n\t\t\t\tAn example of the chemical and mineralogical composition of this type of waste is presented in Table 1. The characterization of this dry material is provided by the Spanish paper manufacturer Holmen Paper Madrid, S.L, which uses 100% recycled paper as the raw material. X-Ray Fluorescence (XRF) confirms that the principal oxides are CaO, SiO2 and Al2O3, the sum of which exceeds 43% of the total mass. The high Loss on Ignition (LOI) in these waste products, at around 54%, should be underlined, due to the presence of organic material, kaolinite dehydroxylation and the decarbonation process of calcite. These values, for guidance only, vary in accordance with the type of paper, its origin, the percentage of recycled paper used as primary material, the loadings, and the type of process etc. With respect to its mineralogical composition, it is worth highlighting the presence of cellulose residue (about 32%, determined according to the results of XRF and XRD), as well as the presence of calcite and kaolinite content in a ratio of 3.3 (Frías et al., 2010). This value is above those in other research works that report ratios of under 2, even for samples from the same paper manufacturing process (Pera & Amrouz, 1998; Frías et al., 2008a). The variation in the composition of this industrial waste is therefore confirmed.
\n\t\t\t\t\n\t\t\t\t\t\t\t\tChemical composition by XRF (%)\n\t\t\t\t\t\t\t | \n\t\t\t\t\t\t||||||||||
CaO | \n\t\t\t\t\t\t\tSiO2\n\t\t\t\t\t\t\t | \n\t\t\t\t\t\t\tAl2O3\n\t\t\t\t\t\t\t | \n\t\t\t\t\t\t\tMgO | \n\t\t\t\t\t\t\tFe2O3\n\t\t\t\t\t\t\t | \n\t\t\t\t\t\t\tSO3\n\t\t\t\t\t\t\t | \n\t\t\t\t\t\t\tTiO2\n\t\t\t\t\t\t\t | \n\t\t\t\t\t\t\tNa2O | \n\t\t\t\t\t\t\tK2O | \n\t\t\t\t\t\t\tP2O3\n\t\t\t\t\t\t\t | \n\t\t\t\t\t\t\tLOI | \n\t\t\t\t\t\t
25.43 | \n\t\t\t\t\t\t\t10.79 | \n\t\t\t\t\t\t\t6.82 | \n\t\t\t\t\t\t\t0.86 | \n\t\t\t\t\t\t\t0.46 | \n\t\t\t\t\t\t\t0.33 | \n\t\t\t\t\t\t\t0.28 | \n\t\t\t\t\t\t\t0.13 | \n\t\t\t\t\t\t\t0.24 | \n\t\t\t\t\t\t\t0.13 | \n\t\t\t\t\t\t\t54.34 | \n\t\t\t\t\t\t
\n\t\t\t\t\t\t\t\tMineralogical composition (%)\n\t\t\t\t\t\t\t | \n\t\t\t\t\t\t||||||||||
Organic material | \n\t\t\t\t\t\t\tBy XRD | \n\t\t\t\t\t\t|||||||||
Calcite | \n\t\t\t\t\t\t\tKaolinite | \n\t\t\t\t\t\t\tPhyllosilicates (talc, mica) and quartz | \n\t\t\t\t\t\t||||||||
32.34 | \n\t\t\t\t\t\t\t45.27 | \n\t\t\t\t\t\t\t13.67 | \n\t\t\t\t\t\t\t8.72 | \n\t\t\t\t\t\t
Composition of the raw paper sludge
In the same way as with other clayey materials, this waste has to be subjected to a process of thermal activation to provide it with pozzolanic properties. As it is not a pure natural kaolinite, research into its thermal activation has centered on the range of temperatures between 500 and 800ºC, with retention times in the furnace of between 2 and 5 hours (Frías et al., 2008b; Rodríguez et al., 2009). All of this has the purpose of establishing optimal conditions that will guarantee total elimination of the organic material, an appropriate transformation of the kaolinite into MK, as well as a minimum content of free lime, which relates to aspects of volumetric instability.
\n\t\t\tKnowledge of the chemical, physical, mineralogical and pozzolanic properties that determine the behavior of Portland cements prepared with activated wastes in the form of active additions represents a key point for the evaluation of their viability.
\n\t\t\t\tLaser diffraction granulometry confirms the presence of particle sizes of less than 90 micrometers. The distribution density curves show 2 maximums located at 40 and 4 micrometers. The BET surface area varies between 7 and 8 m2/g, for original activated sludge, a much higher value than that found for a cement type I 42.5 R (<1 m2/g), reaching values of around 12-13 m2/g for activated paper sludge that is ground down to particle sizes of less than 45 micrometers (Ferreiro, 2010).
\n\t\t\t\t\tThe different coloration between the raw paper sludge and the activated product is also worth mentioning (Fig.1). Whereas the former presents a grayish coloring due to the deinking process, the latter shows a white color.
\n\t\t\t\t\tAppearance of the sludges before (left) and after calcination (right)
Determination of the colorimetric variables (Fig. 2) show values for the coordinate of luminosity (L*)(or whiteness index) of between 75% and 94%. It may be seen that the luminosity value increases with the conditions of activation (higher temperature and a longer retention time). The increase in luminosity is directly related to different processes that take place in that temperature interval (presence of organic residues, inks, degree of
\n\t\t\t\t\tLuminosity values (%) versus activation conditions
transformation of the kaolinite into metakaolinite and degree of calcite decarbonation). This parameter is of greater importance when using these activated products as pozzolans in the manufacture of commercial cements, especially in white cements, the minimum required value of which is 85% (RC-08).
\n\t\t\t\tIn a similar way to the processes described for basic paper sludges, the products yielded by thermal activation are formed principally of silica (20-30%), lime (34-45%), alumina (13-20%) and magnesia (2-3.5%). The remaining oxides are present in amounts of less than 1%. The chemical values increase with the intensity of the activation conditions, as a consequence of the reduction in loss on calcination. These results are in accordance with those obtained by Bai (Bai et al., 2003), but differ from those indicated by Toya (Toya et al. 2006).
\n\t\t\t\tThe mineralogical composition of the activated sludge from the most labile (500ºC for 2 hours) to the most drastic (800ºC for 2 hours) conditions reflects the changes undergone in the different minerals due to heating. The paper sludge calcined at 500ºC for 2 hours is composed of talc, kaolinite, illite, dolomite, calcite and quartz. As the temperature increases (550ºC/2 hours), the kaolinite is transformed into metakaolinite. This compound is detected by SEM, as it is not a crystalline material (Fig. 3). The talc and quartz remain unaltered in the range of temperatures under study. In contrast, the dolomite is transformed at 550ºC/2 hours and the calcite disappears at 800ºC/2 hours, as a result of the decarbonation of those minerals. The illite undergoes a transformation process at 800ºC/2 hours. The appearance of portlandite is notable at 650ºC/5 hours or more as a consequence of the exposure of the paper sludge to environmental humidity, while the formation of dicalcium silicate (bredigite) is detected at 800ºC or more.
\n\t\t\t\t\tStability fields of the different materials identified in the interval 500ºC/2h and 800ºC/2h
Morphologically, the formation of aggregates takes place with the increase in heat through the coldest to the warmest stages, which entails an increase in the specific surface of the materials and means that they become absorbent. Fig. 4 (left) shows the situation of the crystals at 500ºC/2 hours, whereas Fig. 4 right illustrates the great number of aggregates present in the activated paper sludge, corresponding above all to metakaolinite and portlandite, at 800ºC, after 2 hours.
\n\t\t\t\tThe fundamental property for a material or an industrial waste product to be used as an active admixture in the manufacture of commercial blended cements is its pozzolanic nature. A rapid method of supplying information in the short term is through the use of an accelerated chemical method in the pozzolan/lime system (Frías et al., 2008c).
\n\t\t\t\t\tLeft) Large crystals of kaolinite, talc and calcite. Right) Aggregates of metakaolinite and portlandite
The results obtained for the different types of paper sludge, which are activated at temperatures of between 500 and 800ºC after two furnace retention times of 2 and 5 hours (Fig. 5), reveal good pozzolanic activity in all cases. No appreciable differences have been found between periods of 2 and 5 hours. With regard to the activation temperature, it is clearly observed that lime consumption drops at temperatures of 700ºC. This phenomenon may be attributed, on the one hand, to morphological changes in the metakaolinite in the form of more compact aggregates and less specific surface area and; on the other hand, to the initiation of the decarbonation process of the calcite that is present in the waste, liberating free CaO in dissolution, which overlaps with the pozzolanic reaction itself.
\n\t\t\t\t\tA comparative study of these results with pozzolans, normally included in the standards currently in force, shows that the activity of this activated waste is similar to that obtained for pure metakaolin (MK), and very close to silica fume (SF) (Frías et al., 2008d).
\n\t\t\t\t\tAs a consequence of the above, together with the mineralogical and morphological observations, it is recommended that the activation of this type of paper sludge should be at temperatures of between 650 and 700ºC for 2 hours, so as to ensure high pozzolanic activity, to reduce energy costs and to minimize the generation of CO2 associated with the calcite decarbonation process. Higher temperatures generate high contents of quicklime, whereas lower temperatures reveal the presence of kaolinite that is not transformed into metakaolinite.
\n\t\t\t\t\tAt present, in view of the current global crisis, the preparation of commercial cements with more than one pozzolan (Types II/M, IV and V) acquires great importance from the economic and energetic point of view. For this reason, the pozzolanic behavior of this activated waste is analyzed when mixed with fly ash (1:1 by weight), as this is one of the most widely-used pozzolans in the world (Sanjuan, 2007).
\n\t\t\t\t\tEvolution of fixed lime (%) versus reaction time
\n\t\t\t\t\t\tFig. 6 summarizes the evolution of pozzolanic activity for the activated sludge-fly ash systems Ca(OH)2, for the first 90 days of the reaction. The figure shows an analysis of two waste paper sludges activated in different ways: a laboratory scale production (LPS) obtained under optimal conditions and secondly, an industrial scale production (IPS) at temperatures of over 700ºC, which is commercialized and patented (Patent, 1996).
\n\t\t\t\t\tEvolution of fixed lime in pozzolanic activated sludge mixtures /FA
The results show that the pozzolan mixtures under analysis behave in different ways. As the fly ash is the same in both cases, these differences in pozzolanic activity are directly related to the activation conditions of the paper sludge. This fact may be explained as the consequence of the sludge activation temperature that is higher at an industrial scale than it is at a laboratory scale. Moreover, other parameters may be involved such as the morphology of metakaolinite, the different origins of the paper sludge and the kaolinite/calcite ratio.
\n\t\t\t\t\tAfter a reaction time of 28 days, the pozzolanic behavior of both mixtures was very similar and evened out at reaction times of over 90 days, due to the slower speed of the pozzolanic reaction of the fly ash (Sánchez de Rojas et al., 1993 and 1996). It is worth highlighting that in the ISP/FA mixture, a significant jump in lime consumption takes place between day 7 and day 28 of the reaction time. This fact may be due to the fly ash acting as an activator of the pozzolanic reaction between the activated sludge and the surrounding lime, as additional quicklime is available from the industrial sludge.
\n\t\t\t\tIn general, the kinetics of pozzolanic reactions depends on various chemical, physical and mineralogical factors. In a study of the influence of the activation conditions on the hydrated phases, percentages of 10 and 20% cement were replaced in this study, which gave similar results. For example, the mineralogical behavior is described here over the reaction time in prismatic specimens (1x1x6 cm) of paste cement prepared with the addition of 10% paper sludge calcined at 700ºC/2h.
\n\t\t\t\t\tXRD and SEM/EDX techniques were used to perform the kinetic study of the reaction, so as to semi-quantify the formation of hydrated phases and the development of their morphologies with the reaction time. The XRD results are provided in Table 2, where the appearance of allite, portlandite, calcite, calcium aluminate hydrates (C4AH13), and LDH compounds (or compounds of double oxides, at times referred to as hydrotalcite-type compounds) were detected; the last three materials being the most stable over longer periods.
\n\t\t\t\t\tCement with 10% activated sludge | \n\t\t\t\t\t\t\t\t1 day | \n\t\t\t\t\t\t\t\t7 days | \n\t\t\t\t\t\t\t\t28 days | \n\t\t\t\t\t\t\t\t180 days | \n\t\t\t\t\t\t\t\t360 days | \n\t\t\t\t\t\t\t
Allite (%) | \n\t\t\t\t\t\t\t\t21 | \n\t\t\t\t\t\t\t\t10 | \n\t\t\t\t\t\t\t\t9 | \n\t\t\t\t\t\t\t\t4 | \n\t\t\t\t\t\t\t\t1 | \n\t\t\t\t\t\t\t
Portlandite (%) | \n\t\t\t\t\t\t\t\t38 | \n\t\t\t\t\t\t\t\t37 | \n\t\t\t\t\t\t\t\t41 | \n\t\t\t\t\t\t\t\t32 | \n\t\t\t\t\t\t\t\t27 | \n\t\t\t\t\t\t\t
C4AH13 (%) | \n\t\t\t\t\t\t\t\t6 | \n\t\t\t\t\t\t\t\t13 | \n\t\t\t\t\t\t\t\t5 | \n\t\t\t\t\t\t\t\t7 | \n\t\t\t\t\t\t\t\t8 | \n\t\t\t\t\t\t\t
LDH compounds (%) | \n\t\t\t\t\t\t\t\t2 | \n\t\t\t\t\t\t\t\t1 | \n\t\t\t\t\t\t\t\t19 | \n\t\t\t\t\t\t\t\t15 | \n\t\t\t\t\t\t\t\t9 | \n\t\t\t\t\t\t\t
Calcite (%) | \n\t\t\t\t\t\t\t\t33 | \n\t\t\t\t\t\t\t\t40 | \n\t\t\t\t\t\t\t\t27 | \n\t\t\t\t\t\t\t\t41 | \n\t\t\t\t\t\t\t\t55 | \n\t\t\t\t\t\t\t
Semiquantitative mineralogical composition by XRD of cement pastes with the addition of 10% activated sludge
Morphologically, layers of allite surrounded by CSH gels are much more easily identified by SEM/EDX (Fig. 7a), although they go undetected by XRD, given their amorphous nature. The CSH aggregates are arranged in bundles of short fibers, together with the LDH compounds (Fig. 7b) and the same situation reoccurs throughout the test period. Chemical composition by EDX analysis after curing for one year is shown in Table 3.
\n\t\t\t\t\ta) Aggregates of gels and allite layers; b) CSH gels and LDH compounds
Oxides (%) | \n\t\t\t\t\t\t\t\tC-S-H Gel | \n\t\t\t\t\t\t\t\tAllite | \n\t\t\t\t\t\t\t\tPortlandite | \n\t\t\t\t\t\t\t\tLDH Compounds | \n\t\t\t\t\t\t\t
Al2O3\n\t\t\t\t\t\t\t\t | \n\t\t\t\t\t\t\t\t6.27±0.38 | \n\t\t\t\t\t\t\t\t2.87±0.36 | \n\t\t\t\t\t\t\t\t- | \n\t\t\t\t\t\t\t\t7.70±0.58 | \n\t\t\t\t\t\t\t
SiO2\n\t\t\t\t\t\t\t\t | \n\t\t\t\t\t\t\t\t29.45±1.52 | \n\t\t\t\t\t\t\t\t29.87±1.46 | \n\t\t\t\t\t\t\t\t- | \n\t\t\t\t\t\t\t\t22.66±1.04 | \n\t\t\t\t\t\t\t
CaO | \n\t\t\t\t\t\t\t\t64.28±0.95 | \n\t\t\t\t\t\t\t\t67.26±0.74 | \n\t\t\t\t\t\t\t\t100 | \n\t\t\t\t\t\t\t\t69.64±1.36 | \n\t\t\t\t\t\t\t
CaO/SiO2\n\t\t\t\t\t\t\t\t | \n\t\t\t\t\t\t\t\t2.18 | \n\t\t\t\t\t\t\t\t2.25 | \n\t\t\t\t\t\t\t\t- | \n\t\t\t\t\t\t\t\t3.07 | \n\t\t\t\t\t\t\t
CaO/Al2O3\n\t\t\t\t\t\t\t\t | \n\t\t\t\t\t\t\t\t10.25 | \n\t\t\t\t\t\t\t\t23.44 | \n\t\t\t\t\t\t\t\t- | \n\t\t\t\t\t\t\t\t9.04 | \n\t\t\t\t\t\t\t
SiO2/Al2O3\n\t\t\t\t\t\t\t\t | \n\t\t\t\t\t\t\t\t4.70 | \n\t\t\t\t\t\t\t\t10.41 | \n\t\t\t\t\t\t\t\t- | \n\t\t\t\t\t\t\t\t2.94 | \n\t\t\t\t\t\t\t
EDX chemical analysis in the cement with the addition of 10% calcined sludge.
In the case of paper sludge, the pioneering studies (Pera et al., 1998 and 2003) established that the formation of their hydrated phases depended on the relative quantities of metakaolinite and calcium carbonate present in the calcined sludge. Any variant that is introduced into the system will have a direct influence on the kinetic reaction. This is the case of the pozzolan mixtures where the influence of the calcined sludge in the reaction will be conditional upon the competitiveness of the other reaction with the surrounding lime. The absence of scientific works in this area means that these aspects are not extensively applied to the technical properties of cement matrices, principally with regard to their durability.
\n\t\t\t\t\tThe study of these scientific aspects is based on ternary cements, prepared with the substitution of different percentages of Portland cement (6%, 21%, 35% and 50%), which gave similar results. The description therefore centered on the samples in which 21% of the Portland cement was replaced by a mixture of pozzolans, activated sludge and fly ash at a ratio of 1:1 by weight. The result of this system was the same for the OPC/activated sludge system, except for the presence of mullite from the fly ash and type II CSH gels, according to the Taylor classification (Taylor, 1997), with Ca/Si ratios of between 1.5 and 2.5 (Fig. 8).
\n\t\t\t\t\tLeft) Formation of gels and layers on amorphous forms. Right) Bundles of CSH gel (II) fibers.
The fresh state of any base cement material may be defined as the period between the initial cement hydration process and its setting. During this period the mixtures show a plastic behavior. A study of a base cement mixture during its plastic state and its properties are of special interest, in order to ensure appropriate preparation and transport and the on-site laying of mortars and concretes. Once the cement has set, the material shows a certain capacity to withstand mechanical stress.
\n\t\t\t\t\tThe binary mixtures were studied on the basis of the reference cement pastes and mortars prepared with proportions (0%, 10% and 20% of the Portland cement (CEM I 52,5N) replaced by paper sludge activated at 700ºC for 2 hours. The mortars were prepared at a water/binder ratio of 0.5 and at a binder/sand ratio equal to 1/3. Table 4 presents the main characteristics of the blended cements in their fresh state.
\n\t\t\t\t\tPercentage in weight of CEM I 52.5N Portland cement substituted by calcined paper sludge | \n\t\t\t\t\t\t\t\tRatio of water consistency/ binder | \n\t\t\t\t\t\t\t\tInitial setting time (minutes) | \n\t\t\t\t\t\t\t\tFinal setting time (minutes) | \n\t\t\t\t\t\t\t\tExpansion by Le Chatelier needles (mm) | \n\t\t\t\t\t\t\t
100/0 | \n\t\t\t\t\t\t\t\t0.29 | \n\t\t\t\t\t\t\t\t145 | \n\t\t\t\t\t\t\t\t255 | \n\t\t\t\t\t\t\t\t< 0.5 | \n\t\t\t\t\t\t\t
90/10 | \n\t\t\t\t\t\t\t\t0.32 | \n\t\t\t\t\t\t\t\t120 | \n\t\t\t\t\t\t\t\t170 | \n\t\t\t\t\t\t\t\t< 0.5 | \n\t\t\t\t\t\t\t
80/20 | \n\t\t\t\t\t\t\t\t0.37 | \n\t\t\t\t\t\t\t\t60 | \n\t\t\t\t\t\t\t\t130 | \n\t\t\t\t\t\t\t\t< 0.5 | \n\t\t\t\t\t\t\t
Fresh state properties of binary blended cements prepared with paper sludge calcined at 700ºC
The incorporation of thermally activated paper sludge under optimal conditions produces a parabolic increase in water demand for normal consistency. The greater specific surface of the thermally activated paper sludges, together with the distribution of finer sized particles, complicates the fluidity of the paste. Greater quantities of water are required with these additions to wet the cement surface.
\n\t\t\t\t\tThese paper wastes accelerate setting times, especially when they replace percentages of over 10% of Portland cement (Vegas et al., 2006; Frías et al., 2008e). This phenomenon may be attributed to the joint presence of metakaolinite and calcium carbonate. Ambroise and colleagues (Ambroise et al., 1994) demonstrated that MK produces an accelerator effect on the hydration of C3S when the ratio C3S:MK is below 1.40; or in other words, when up to 30% of clinker is replaced by MK.
\n\t\t\t\t\tThe expansion results reveal that the inclusion of activated paper sludge does not influence the variation in the volume of cement pastes. In fact, the values of the test are well below the limit of 10 mm established in the UNE-EN 197-1 for common cements.
\n\t\t\t\t\t\n\t\t\t\t\t\tFig. 9 illustrates the evolution of relative compressive strength determined for standardized mortars with partial additions of 0%, 10% and 20% of thermally activated paper sludge. Up until 14 days of curing, an increase is observed in the relative compressive strength, as the incorporation of calcined paper sludge is increased. The acceleration of cement hydration and the pozzolanic reaction constitute the principal effects that explain the evolution of these strengths. The relative maximum is achieved after 7 days of curing. Likewise, replacement of 20% of the cement by calcined sludge provides greater relative compressive strength during the first fortnight of curing. This discussion coincides with the findings of other authors (Wild et al., 1996) when studying this mechanical property in cement mortars or concretes prepared with pure metakaoline. The lower the content of metakaolinite in the added sludge (10%), the further the values of relative compressive strength will fall for curing periods of over 14 days. The pioneering studies of Pera (Pera & Ambroise, 2003) demonstrated that the most influential parameter in pozzolanic activity at 28 days is the quantity of metakaolinite present in the sludges, regardless of other parameters, such as specific surface area, numbers of particles under 10 micrometers or the average diameter of the distribution of particle sizes.
\n\t\t\t\t\tRelative compressive strength of blended cements with paper sludge calcined at 700ºC
\n\t\t\t\t\t\tTable 5 presents other physico-mechanical properties of binary blended cements with paper sludge calcined at 700ºC.
\n\t\t\t\t\tPercentage in weight of CEM I 52.5N Portland Cement replaced by calcined paper sludge | \n\t\t\t\t\t\t\t\tModulus of longitudinal deformation (GPa) | \n\t\t\t\t\t\t\t\tTotal retraction at 28 days (%) | \n\t\t\t\t\t\t\t\tCreep deformation after one year of constant load (%) | \n\t\t\t\t\t\t\t
100/0 | \n\t\t\t\t\t\t\t\t34.8 | \n\t\t\t\t\t\t\t\t0.04 | \n\t\t\t\t\t\t\t\t0.114 | \n\t\t\t\t\t\t\t
90/10 | \n\t\t\t\t\t\t\t\t33.0 | \n\t\t\t\t\t\t\t\t0.09 | \n\t\t\t\t\t\t\t\t0.120 | \n\t\t\t\t\t\t\t
80/20 | \n\t\t\t\t\t\t\t\t34.9 | \n\t\t\t\t\t\t\t\t0.12 | \n\t\t\t\t\t\t\t\t0.093 | \n\t\t\t\t\t\t\t
Modulus of longitudinal deformation, retraction and creep of binary cement mixtures prepared with paper sludge calcined at 700ºC
In general terms, it may be concluded that the inclusion of paper sludge calcined at 700ºC, up to a percentage of 20%, hardly modifies the value of the elastic modulus at 28 days of curing. There are few bibliographic references that cover the influence of pozzolanic additions on this mechanical parameter. Qian (Qian & Li., 2001) establishes that the partial replacement of cement by metakaolin, in percentages of up to 15%, produces an increase in the concrete’s elastic modulus. These mineral additions show a certain refinement in the porous network of the base cement material; above all, for amounts replaced of 20%. This greater densification means that the fines contribute to a greater extent to the modulus of deformation.
\n\t\t\t\t\tDrying shrinkage increases with the percentage inclusion of paper sludge calcined at 700ºC. After 28 days of drying, cement shrinkage with 20% thermally activated paper sludge triples that shown in the reference cement sample. Greater contraction shown by those mortars that incorporate thermally activated paper sludge may be explained on the basis of phenomenon such as:
\n\t\t\t\t\tNucleation of hydration products on the particles of this mineral additions, accelerating the hydration of cement, and therefore, increasing the drying of the product.
Pozzolanic reaction between the metakaolinite and the calcium hydroxide, either from the calcined sludge, or from hydration of the cement clinker. This reaction requires greater water consumption, accelerating drying of the mixture.
Increase in capillary pressure, as a consequence of a greater refinement of the distribution of pore size. The greatest relative refinement is observed at 14 days of curing.
The inclusion of 20% thermally activated paper sludge reduces creep deformation by approximately 20% of the deformation observed in the reference mortar sample, after one year subject to a pressure state of 40% of the respective compressive strengths. In a similar way to the explanations of other mechanical characteristics, this reduction may be attributed to a denser pore structure, a stronger cement matrix, and greater adherence between the cement paste and the fines (Brooks & Megat, 2001). As a more refined porous network is created, the movement of free water is prevented, which is responsible for the initial creep. Likewise, the pozzolanic activity contributes to the consumption of water, and therefore, to reductions in early creep.
\n\t\t\t\tThe characteristics of the ternary mixtures were determined in standardized pastes and mortars prepared with Portland cement (CEM I 52.5N), thermally activated paper sludge calcined at 700ºC and fly ash. Table 6 presents the percentage mixture of each agglomerate.
\n\t\t\t\t\tPercentages in weight OPC replaced by calcined paper sludge | \n\t\t\t\t\t\t\t\tCEM I 52.5N (% in weight) | \n\t\t\t\t\t\t\t\tPaper sludge calcined at 700ºC (% in weight) | \n\t\t\t\t\t\t\t\tFly ash (% in weight) | \n\t\t\t\t\t\t\t
100/0 | \n\t\t\t\t\t\t\t\t100 | \n\t\t\t\t\t\t\t\t0 | \n\t\t\t\t\t\t\t\t0 | \n\t\t\t\t\t\t\t
94/6 | \n\t\t\t\t\t\t\t\t94 | \n\t\t\t\t\t\t\t\t3 | \n\t\t\t\t\t\t\t\t3 | \n\t\t\t\t\t\t\t
79/21 | \n\t\t\t\t\t\t\t\t79 | \n\t\t\t\t\t\t\t\t10.5 | \n\t\t\t\t\t\t\t\t10.5 | \n\t\t\t\t\t\t\t
65/35 | \n\t\t\t\t\t\t\t\t65 | \n\t\t\t\t\t\t\t\t17.5 | \n\t\t\t\t\t\t\t\t17.5 | \n\t\t\t\t\t\t\t
50/50 | \n\t\t\t\t\t\t\t\t50 | \n\t\t\t\t\t\t\t\t25 | \n\t\t\t\t\t\t\t\t25 | \n\t\t\t\t\t\t\t
Proportions of ternary cement mixtures with activated paper sludge
\n\t\t\t\t\t\tTable 7 presents the principal characteristics of the ternary cement mixtures under study in their fresh state.
\n\t\t\t\t\tPercentage in weight of OPC replaced by calcined paper sludge and fly ash | \n\t\t\t\t\t\t\t\tRatio water consistency /binder | \n\t\t\t\t\t\t\t\tInitial setting time (minutes) | \n\t\t\t\t\t\t\t\tFinal setting time (minutes) | \n\t\t\t\t\t\t\t\tExpansion Le Chatelier needles (mm) | \n\t\t\t\t\t\t\t
100/0 | \n\t\t\t\t\t\t\t\t0.28 | \n\t\t\t\t\t\t\t\t155 | \n\t\t\t\t\t\t\t\t270 | \n\t\t\t\t\t\t\t\t0.7 | \n\t\t\t\t\t\t\t
94/6 | \n\t\t\t\t\t\t\t\t0.29 | \n\t\t\t\t\t\t\t\t140 | \n\t\t\t\t\t\t\t\t225 | \n\t\t\t\t\t\t\t\t0.3 | \n\t\t\t\t\t\t\t
79/21 | \n\t\t\t\t\t\t\t\t0.31 | \n\t\t\t\t\t\t\t\t105 | \n\t\t\t\t\t\t\t\t165 | \n\t\t\t\t\t\t\t\t0.5 | \n\t\t\t\t\t\t\t
65/35 | \n\t\t\t\t\t\t\t\t0.34 | \n\t\t\t\t\t\t\t\t90 | \n\t\t\t\t\t\t\t\t165 | \n\t\t\t\t\t\t\t\t0.4 | \n\t\t\t\t\t\t\t
50/50 | \n\t\t\t\t\t\t\t\t0.41 | \n\t\t\t\t\t\t\t\t35 | \n\t\t\t\t\t\t\t\t70 | \n\t\t\t\t\t\t\t\t0.2 | \n\t\t\t\t\t\t\t
Fresh state properties of ternary cement mixtures prepared with paper sludge calcined at 700ºC and fly ash
In a similar way to the description of the study of binary mixtures, the thermally activated paper sludge calcined at 700ºC appears to control water demand for water consistency, although this result is less apparent in binary mixtures due to the presence of fly ash. This latter mineral addition requires less water content as a consequence of its spherical morphology, thereby minimizing the surface/volume ratio of the particle (Li & Wu, 2005). Likewise, the joint presence of paper sludge calcined at 700ºC and fly ash accelerates the setting times, though there is no evidence of a significant effect on the expansion of cement pastes.
\n\t\t\t\t\t\n\t\t\t\t\t\tFig. 10 illustrates the evolution of relative compressive strength determined from standardized cement mortars with partial additions of 0%, 6%, 21%, 35% and 50% of the mineral additions under study. The ternary cements 79/21, 65/35 and 50/50, with a thermally activated paper sludge content of over 10% in weight, display lower mechanical strength than the reference cement sample, although the decrease in their strength is lower than the total percentage of cement that is replaced. At 90 days, a recovery of mechanical resistance is observed in the ternary cements as a consequence of the activity developed by the fly ash.
\n\t\t\t\t\tRelative compressive strength in relation to ternary cement mixtures with paper sludge calcined at 700ºC and fly ash
Durability is understood as a capacity that maintains a structure or element safely in service for at least a specific period of time, which is referred to as its useful life, in the environment where it will be sited, even when the surrounding conditions (physical, chemical and biological) are unfavorable. In short, the condition demanded from the construction materials and components is that they should perform the function for which they were intended, throughout a certain period of time.
\n\t\t\t\t\tThis section discusses the behavior of binary mixtures prepared with thermally activated paper sludge when exposed to weathering action. The durability of the ternary mixtures is at present under study, for which reason it can not be included in this chapter. Among the various degradation mechanisms, two types of aggressive attack are covered: one of a physical nature where extreme temperatures and water intervene, the second of a chemical type in the presence of sulfates.
\n\t\t\t\t\tBinary cement mortars that include 10% and 20% thermally activated paper sludge present, respectively, two and three times more strength faced with freezing/thawing actions than the standard reference mortar (Fig. 11). As the exposure cycles progress, the increase in total porosity is less for those cements that incorporate thermally activated paper sludge. The higher the percentage substitution of cement by calcined paper sludge, the denser the mortar microstructure throughout a higher number of freezing/thawing cycles. Moreover, the greater the replacement percentage of thermally activated paper sludge, the slower the loss of compressive strength in the mortars exposed to freezing/thawing cycles (\n\t\t\t\t\t\t\t\tVegas et al., 2009\n\t\t\t\t\t\t\t).
\n\t\t\t\t\t\tEvolution of the dynamic modulus of binary cement mixtures with paper sludge activated at 700ºC subjected to freezing/thawing cycles
It is well known that sulfates constitute one of the most aggressive agents against cement based materials, and cause different deterioration mechanisms as a consequence of the direct reaction between sulfate ions and the alumina phases in the cement, giving rise to ettringite, a highly expansive compound. The cements prepared with pozzolans of a siliceous-aluminous nature (fly ash and metakaolinite) can be more susceptible to sulfate attacks, owing to the incorporation of the reactive alumina of the pozzolan (Taylor, 1997; Siddique, 2008). The bibliographic data found on the behavior of normal Portland cements prepared with calcined paper sludge highlights the lower strength in the face of sulfate attacks (external and internal source) with respect to the reference cement sample. Thus, in accordance with the research into cement/calcined sludge/gypsum mortars by \n\t\t\t\t\t\t\t\tVegas (Vegas, 2009\n\t\t\t\t\t\t\t) that is in agreement with the American standard (ASTM C 452-95), the following considerations are proposed:
\n\t\t\t\t\t\tThe reference cement (CEM I 52.5N) may be categorized by a high resistance to sulfates, given that ΔL28 days ≤ 0.054% and ΔL14 days ≤ 0.040%.
Binary mixtures with percentages of thermally activated paper sludge above 10% may be classified as having low resistance to sulfates presenting a ΔL28days ≥ 0.073%.
Observing the increase in length at 7 days, and in accordance with the physical requirements of the ASTM C 845-04 standard, binary cements with 10% and 20% in volume of activated paper sludge may be classified as hydraulic cements, given that the values ΔL7days are greater than 0.04% and less than 0.10%.
The paper industry that uses 100% recycled paper as a primary material generates waste paper sludge which, by its nature, constitutes an inestimable source of kaolin, with the subsequent environmental benefits.
\n\t\t\tControlled calcination of waste (500-800ºC) supplies an alternative approach to obtain recycled metakaolin, a highly pozzolanic material for the manufacture of commercial cements.
\n\t\t\tThe products obtained in this way present a high pozzolanic behavior, comparable to a natural metakaolin, which is very close to silica fume; temperatures of between 650-700ºC and 2 hours of retention time in the furnace are established as the most efficient laboratory conditions to obtain these pozzolans. It is likewise worth highlighting their high pozzolanic compatibility with fly ash.
\n\t\t\tThe cement pastes prepared with 10% sludge calcined at 700ºC/2h generate LDH compounds and CSH gels as stable products. The incorporation of a second pozzolan (fly ash) into the blended cement system does not modify the reaction kinetics, for which reason it is worth highlighting the compatibility between both pozzolans.
\n\t\t\tIn the manufacture of binary cements, and in a similar way to the regulations for silica fume, it is recommended that the percentage should be limited to around 10% clinker for paper sludge calcined at 700ºC. A compromise has to be reached between the positive effect on the mechanical properties and the determining factors associated with the reduction in setting times, loss of workability and excessive total drying shrinkage.
\n\t\t\tIn the manufacture of ternary cements that contain sludge calcined at 700ºC and fly ash, the percentage of clinker replaced by the addition of these minerals should not exceed 21%, in order to guarantee the maximum pozzolanic effect (synergy between the two industrial by-products), while ensuring that the workability of the mixture is not adversely affected.
\n\t\t\tThe results of this research have clearly shown the scientific and technical viability of including thermally activated waste paper sludges as active admixtures in the manufacture of binary and ternary cements.
\n\t\tThe authors would like to thank the different Spanish ministries for having funded this research (Projects ref: MAT2003-06479-CO3, CTM2006-12551-CO3 and MAT2009-10874-CO3)
\n\t\tSemiconductor materials are defined as materials in solid form whose conductivity has a value between conductors and insulators. Semiconductor materials play an important role in the advances in the modern electronics industry in the twenty-first century and in the industrial applications of many electronic devices. These materials include many materials such as silicon, gallium arsenide, germanium, cadmium sulfide, and cadmium telluride, which are widely used today. From the first silicon integrated circuits produced in semiconductor technology, high-tech microprocessors, solar cells, and many other electronic devices have developed rapidly to the present day [1].
Especially with the development of nanotechnology and polymer science, interest in the research and production of both efficient and lower-cost semiconductor thin film materials is increasing day by day. The use of nano-structured thin films for the efficient use of solar cells in the production of n-type semiconductor materials is one of the most important sources of energy and new-generation energy. In short, semiconductor devices for nanotechnology and polymer science have taken the advancement of research in semiconductors to a new step, aiming to improve the chemical and physical properties of these materials. To understand the nature of these crucial engineering materials, the difference and theory between conductors, insulators, and semiconductors must be fully understood. In addition, basic concepts such as band theory, doping processes, and p-n connection theory of solids are theoretical bases that will give a general idea of understanding semiconductors.
It is important to assimilate the band theory that explains the nature of semiconductors in terms of energy levels between the valence and the conduction bands in order to gain knowledge about semiconductor materials. The main difference between metallic materials and semiconductors is that the current is provided by electron flow in metallic conductors, whereas in semiconductors this flow occurs not only by the electron flow but also by the flow of positively charged holes.
Electrical conductivity is directly related to the band structure of a material. If we look at the basis of the theory, atomic energy levels of each atom are equal when two different atoms are sufficiently distant from each other. However, as these atoms approach each other, differences in the original energy levels of the atoms are observed, and as a result of these differences, an interaction occurs that creates molecular bands between the atoms. Therefore, it is for this reason that materials with different band structures show different conductivity properties. In conductors, the energy difference between partially filled energy levels and empty levels is very low. Therefore, when a potential is applied to metals, electron mobility between the filled and empty levels, which takes place by using very low energy, is easily realized, and the flow of electrons is provided. Therefore, it would not be the right approach to talk about an obstacle between the levels defined as valence band and conduction band in metals. As known, an electron must have an empty energy level to move, otherwise electrons cannot move in solid material. Based on this approach, it can be clearly understood why electrical current is not observed in insulating structures. In insulators, the valence band is the highest band fully filled by electrons, and the conduction band is the lowest empty band, with a forbidden band gap of about 5–10 eV between these two bands [2]. This broadband between the valence band and the conduction band prevents the transmission of electrons to the conduction band, and no electrical current is generated in the insulating materials. Similar to the band structure of the insulators, semiconductors have a valence band occupied by electrons and a conduction band ready to be filled with electrons. In semiconductors, just like insulating materials, there is a band gap between these two bands. The main difference between the band gap in these two groups excluding conductors is that the band gap value is much smaller in semiconductors (1.1 eV for silicon) than in the insulator [3]. Since the thermal energy in semiconductors creates the driving force for the movement of electrons, the conductivity of these materials is directly related to the temperature. The conductivity of a semiconductor material as a result of a decrease in resistivity can be associated with increased kinetic energy with temperature. Figure 1 schematically shows the energy band gaps in conductors, semiconductors, and insulators.
Energy band gaps in materials.
In semiconductors, the valence band that is below the forbidden band gap is almost completely full. On the other hand, there is a nearly empty conduction band over the prohibited band gap. When a semiconductor material is excited, if the energy of the photon is greater than the band gap, the electrons will easily pass to the conduction band, and electrical current will occur. According to the theory, as a result of the transition of an electron to the conduction band, the excited electron leaves a hole in place that can flow through the material and act as a positively charged particle. Here, carrier production and recombination can be defined as two basic factors in the creation of charge-carrying electrons and positively charged holes [4].
In general, depending on the level of doping, semiconductors can be classified into two main groups such as intrinsic semiconductors and extrinsic semiconductors. The intrinsic semiconductors are pure semiconductors and no addition is made. In this type of semiconductor, conductivity is provided by the thermal stimulation of electrons. At the same time, the number of excited electrons and positively charged holes is equal. The behavior here appears as a result of the carrier production and recombination steps [5].
On the other hand, extrinsic semiconductors have low conductivity values, and an important process called doping is applied to overcome the problems encountered in applications and to increase the conductivity [6]. This process can be explained simply by adding small amounts of impurities in the concentrations of charge-carrying electrons and positively charged holes, thereby increasing the conductivity level. The aim is to change the electronic structure by impurity addition into the structure without changing the crystal structure. For example, arsenic with five valence electrons to an atom and germanium with four valence electrons will cause the arsenic atom to covalently bond with the germanium atom. The extra fifth electron of the arsenic atom will have the electrical conductivity as it will have the freedom to move from one atom to another [4]. Such semiconductors, which the dopant element donates an electron, are called n-type semiconductors. In addition to producing free electrons in n-type doping, an equal number of positive charges are also produced in pairs with free electrons. As a result, the doped semiconductor material remains electrically neutral. However, these positive charges should not be understood as positively charged holes. These charges occur in the absence of free electrons, but do not contribute to a current flow. Another contribution of free electrons to pure semiconductors is that the donor electron is much closer to the conduction band than an electron in the valence band of the original atom. In another saying, the energy level of the donor electron is at another level that is much narrower than the energy level for valence electrons and facilitates the flow of current in the n-type semiconductor.
In another type of extrinsic semiconductor, if a pure semiconductor with trivalent electrons (e.g., germanium) is replaced by gallium, this type of semiconductor is called p-type semiconductors. Three of the four covalent bonds are occupied in the structure; the bond remains empty and acts as a relatively moving hole in the opposite direction of a moving electron, which is not a real move. The main phenomenon is defined as a relative movement caused by the movement of electrons from one bond to another and leaving a hole after. Similar to the energy band structure of n-type semiconductors, which differs from pure semiconductors, p-type semiconductors also have a higher acceptor energy level than the valence band.
Materials are produced with developing semiconductor technology; it has been used for more than 50 years in the production of a wide variety of devices such as diodes, transistors, sensors, microprocessors, and solar cells. On the other hand, thin film nano- or microstructures are frequently used in applications developed in semiconductor technology. The most common area that benefits semiconductor thin film technology refers to photovoltaic applications. Simply, this application is the technology field for using solar cells to produce solar energy. The importance of photovoltaics comes from the fact that photovoltaics are not only important in terrestrial applications to gain renewable and clean energy but also enable the benefits of solar energy which can be used as a major source of electrical power for space systems [7]. Besides, all the concerns based on environment, renewability, and sustainability have increased attention for using alternative, new energy sources, where photovoltaics are seen as the new trend.
In general, semiconductor thin films are produced in one or more thin layers. Common applications of such structures include many electronic materials such as transistors, sensors, and photovoltaic devices. The structural, chemical, and physical properties of semiconductor thin films are directly related to the production technique, and their thickness ranges from a few nanometers to hundreds of micrometers [8].
Especially in recent years, semiconductor thin films can be obtained compared to the use of bulk materials, making it a promising ideal candidate in the electronic material industry due to its wide variety of properties. First of all, a wide range of chemical, electrochemical, and physical deposition techniques (see Section 5) enables the low-cost production of semiconductor material on large areas of the desired geometry and structure. In addition, single- or multi-crystalline structures with complex geometry and even microstructures of nanocrystalline thin films can be easily obtained by changing the method, temperature, substrate, and other production parameters depending on the method. Industrial applications of electronic materials come to life with different junction types between different semiconductor materials to improve the electrical properties of thin films.
Thin film solar cells, which we have already mentioned and attracted great interest from researchers, consist of materials of different structure and properties in the form of several thin layers deposited on various substrates. To draw a general schematic, the common structure of a solar cell consists of a hard or flexible substrate, a transparent conductive oxide (TCO) layer, a window layer made of n-type semiconductor, p-type semiconductor layer, and a metal contact and absorbent layer. In order to make the structure more understandable, the schematic of a solar panel is examined in Figure 2 [9].
Schematic of a laminated solar panel.
Additionally, the flowchart of solar energy diagram using the panels is given below sequentially:
Solar panels convert sunlight to DC current.
Inverter converts DC electricity to AC.
Electricity then gets used by home applications.
Extra electricity gets credited into the grid.
In a solar panel, each of the components given in Figure 2 has different physical and chemical properties. The performance of the solar cell depends on the properties of the previously mentioned layer components and the compatibility between them. The layers described should be mechanically and chemically stable as well as compatible with each other based on their properties. The high processing temperature, which is a requirement of most processes, results in the need of a hard substrate such as glass, because flexible substrates (can be polymeric, etc.) do not have high temperature stability. On the other hand, it is reported that the choice of the substrate has a direct effect on the efficiency of the cells and the grain structure of the films grown on this substrate [10, 11, 12].
When it comes to the transparent conductive oxides, which are among the trend research subjects of recent years (see Section 6), it provides an integration between the substrate and the window layer with good electrical conductivity and high optical permeability in the visible region. In order to reduce the total resistance of the system, high transparency is required for good conductivity feature and higher degree of light passing through the absorbent layer. The window layer, on the other hand, has the function of directing the maximum amount of incoming light to the junction point and the absorbent layer in a hetero combination with an absorbent layer. Moreover, the compatibility of the window layer with the absorbent layer and the lattice structure is of great importance for device performance.
The coating process is the basis for the production of devices based on thin film technology. In improving device performance, high-quality thin films produced by using rapid, economical, and effective techniques are required. The semiconductor industry, which is almost entirely based on solid thin films, has demonstrated the importance of coating technology and has contributed to its rapid development, especially in recent years. In this context, there are various methods for creating thin films on nano-micro scale. Basically, deposition techniques can be divided into two groups as chemical and physical methods [13].
Subgroups of chemical and physical deposition methods can be defined as (i) chemical vapor deposition (CVD), including chemical bath deposition, electroplating, molecular beam epitaxy, and thermal oxidation, and (ii) physical vapor deposition (PVD), including evaporation and spraying. It is possible to mention that CVD and PVD have an important place in new-generation thin film technologies.
Of these techniques, CVD is used to create high-purity and effective solid thin films [14, 15]. In this process, the substrate is placed inside a reactor where it is exposed to volatile gasses, and a solid layer is formed on the substrate surface by chemical reactions between the gas used and the substrate. CVD method can produce high-purity single- or polycrystalline or even amorphous thin films. Another feature of CVD is that both pure and complex materials can be synthesized at the desired purity at low temperatures. The chemical and physical properties of the forms to be created can be easily adjusted by properly adjusting the reaction and precipitation parameters such as temperature, pressure, gas flow rate, and gas concentration.
As another technique, PVD can be defined as thin film production by condensing the evaporated materials released from a source (target material) on the substrate surface. Sub-methods of this technique are spraying and evaporation, respectively.
Spraying method is based on the principle of removing surface atoms from a target and depositing them on the substrate. Among the advantages of the spraying method, thin films with the desired composition closest to the composition of the target material can be easily obtained. Besides, the method provides better adhesion to the surface, and evaporation of materials with a high melting point is possible.
Evaporation is another common PVD method in thin film production. In this technique, the evaporated particles are condensed on the substrate to form a solid thin film, while the source material (mostly metallic) is evaporated in a vacuum tube. The great advantage of evaporation compared to sputtering is that the process is relatively faster.
Due to the wide range of applications mentioned in Section 4 and the unique optical and electrical properties that can be combined, TCO materials are used in transparent and flexible device applications such as flat panel displays, plasma screen panels, organic light-emitting diodes, solar cells, and gas sensors. As the most common TCOs, indium, tin, cadmium, and group III and VII doped zinc oxide can be mentioned. It consists of semiconductor metal oxides with a wide band gap. These materials show high conductivity, transparency, and reproducibility, and the possibility of producing very flat films and tin-doped indium oxide (ITO) is the most employed TCO. Due to the cost and difficulty of finding indium in TCO, cost-effective and alternative materials with the same properties are needed. In addition to high conductivity TCO, the development of materials other than ITO has increased in few years. ITO’s cost and potential supply limit are among the reasons for research in this field. Current candidate materials for high conductivity TCOs include CdO, SnO, In2O3, and ZnO with these binary combinations along with alternative additives. ZnO as the current candidate is considered to be the primary candidate of binary oxide TCO materials, with its high conductivity and low cost. However, it is very sensitive to oxygen, and process control is more difficult; the development of ZnO with alternative impurity continues.
ZnO:Al (AZO) produced with pulsed laser deposition (PLD) shows at least equivalent resistivity with ITO. However, PLD is not considered to be a suitable deposition method for large area applications. Metallic and ceramic targets are used to develop robust process control and to scale wide area bases in the production magnetron sputtered (MS) ZnO:Al (AZO) films. AZO and ZnO:Ga (GZO) are both commercially applicable in thin film solar cells and can be used as translucent electrodes [16].
In ZnO film growth, several techniques with their own advantages and disadvantages are used such as evaporation, radio-frequency magnetron sputtering (RF-MS), direct current magnetron sputtering (DC-MS), ion beam sputter, spray pyrolysis, sol–gel process, PLD, and CVD. Transparent n-type ZnO semiconductors can easily be fabricated by B, Al, In, and F doping. According to the results of several research in which RF-MS, DC-MS, and MOCVD are used, ZnO:Al with relatively low resistivity values is found to be 1.4 × 10−4, 3.4 × 10−4, and 3.0 × 10−4 Ωcm, respectively. These resistivity values are quiet close to the electrical properties of ITO. The optoelectronic properties of these thin film TCOs may change after thermal annealing in an inert gas or reactive gas atmosphere [17].
Lastly, if we consider PVD as one of the trending methods in the past few years and even a more innovative sub-method, the magnetron sputtering technique, the applicability problems brought by the researcher who has practical experience in this field and the applicability of the method to large surfaces as an assessment of the literature-scale results are known. In such semiconductor materials, homogeneity is another problem to be solved and mostly at high-temperature processes after coating (additional heat treatments). This makes the aforementioned method disadvantageous. In addition, while many traditional methods used in semiconductor technologies are generally suitable for coating applications on metal or ceramic substrate, the phase transformation and/or defect removal with additional heat treatments makes these techniques unsuitable for developing polymer-based semiconductor applications for high-technology semiconductor field.
From this point of view, the search for alternative methods that will meet the advancing technology and meet technological requirements not only for metal and ceramic substrates but also polymer-based ones encouraged researchers to work on new techniques and methods. “Ceramic powder aerosol deposition method,” which is pointed, is not only requiring additional high-temperature heat treatment or sintering steps but also homogeneous and continuous applicability to large areas. It has become a trend that draws the attention of researchers on semiconductor material technologies annually. As a result of all these advantages, the aerosol deposition method has been deemed worthy of examination both in terms of its technical details and applicability, and because it is a virgin technology that is still open to development in the field, it may meet the need in new-generation semiconductor technologies.
Aerosol deposition technique, in terms of homogeneous, continuous, and applicability to large area TCO, is a convenient method for industrial production of materials that has not been studied much before. As it is known, new-generation ceramic integration technologies require device performance improvement for various applications such as size reduction and/or micro-mechanical systems, image technologies, fuel cells, and optical devices. Common industrial applications of these devices are high-speed coatings and productions that bring low processing temperatures and thin lithographic processes in ceramic coatings. “Ceramic powder aerosol deposition method” has many advantages to meet many of the requirements mentioned above when compared to other conventional film/coating applications.
While ceramic material productions generally require sintering over 1000°C, this makes it impossible to integrate metal, glass, and even polymers with relatively low melting point with functional ceramics. On the other hand, high-temperature film applications trigger high-temperature crack formations and substrate-coating incompatibilities and discontinuities, as well as long processing times. Especially in film-type applications, the substrate-coating incompatibilities and surface discontinuities will adversely affect the optical, electrical, and mechanical properties of the device for the application and also decrease its performance. Similar results were observed in our previous research studies in the form of surface cracks and unexpected decrease in electrical properties as a result of ZnO-based coatings obtained by magnetron scattering method, which requires additional heat treatment up to 700°C.
The main output of the aerosol deposition method in the development of a new technique and industrial product with high-speed coating efficiency, low processing temperature, and even at room temperature reduces costs and production time and adversely affects properties.
The basic principle of the technique is based on the conversion of some of the kinetic energy of the previously prepared and suitable form of fine ceramic particles with the substrate at high speeds, into both interparticle and interparticle-binding energy. In this context, while the aerosol deposition method offers many advantages compared to traditional thin/thick film methods and thermal spray coating techniques, it has not been fully understood as a new method, revealing the open points for the research. A schematic of this method is given in Figure 3.
Room temperature aerosol deposition system.
Simply, aerosol deposition method is based on the principle of ultra-pressure ceramic particles coming together with the surface of the substrate and solidification with effective pressure and shock loading. First, ceramic particles are mixed with a gas in the system chamber to form an aerosol. This aerosol is then sprayed through a nozzle onto various targets to create a film layer with the aid of pressure. During the process, some of the kinetic energy of the particles is converted into thermal energy, which partially increases the temperature in the interaction zone. In this way, the bonding between the substrate and the particles and also the particles with each other is provided and results in a high-density continuous coating layer.
In general terms, aerosol deposition technique is as follows:
Appearing as a suitable method for all types of substrates.
As a horizon for the electronics industry.
Not only for energy conversion applications but also for various semiconductor technology applications.
Does not require additional heat treatment.
Most importantly, as it is a low-temperature process, in terms of being a feasible method without changing or destroying the substrate form.
It is thought that this new technology will make important contributions to the relevant field and bring a new perspective and direct scientific research in process-structure–property-performance relation.
Due to the cost and difficulty of finding indium in TCO, cost-effective and alternative materials with the same properties are needed. In addition to high conductivity TCO, the development of materials other than ITO has increased in few years. ITO’s cost and potential supply limit are among the reasons for research in this field.
Besides, not only for the metallic and/or ceramic substrates but also for the substrates with low melting point or polymers need to be focused on new semiconductor fabrication technologies. At this point, room temperature aerosol deposition method seems to be an alternative technique and may bring a new perspective in high-technology semiconductor applications.
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