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1.
The influence of carbon particle type in fly ashes on mercury adsorption   总被引:2,自引:0,他引:2  
Recent research has shown that certain fly ash materials produced in coal combustion for power generation have an affinity for the mercury compounds present in flue gases. However, the exact nature of Hg-fly ash interactions is still unknown and the different variables that influence mercury adsorption need to be identified. In this work the microscopic components of fly ashes derived from the combustion of different types of feed blends of different coal rank and mercury adsorption were investigated. The aim of this research was to establish relationships between Hg retention and the type of unburned carbons present in various fly ashes. The fly ashes and fly ash fractions studied were used as sorbent beds for high mercury concentrations, conditions in which mercury retention is highly favored. From the results obtained it was confirmed that the role of the unburned carbon components in mercury capture may depend, among other factors, on the type of unburned carbon. Fly ashes capture different species of mercury depending on their nature and the type of anisotropic particles.  相似文献   

2.
Mercury in coal and its emissions from coal-fired boilers is a topic of primary environmental concern in the United States and Europe. The predominant forms of mercury in coal-fired flue gas are elemental (Hg0) and oxidized (Hg2+, primarily as HgCl2). Because Hg2+ is more condensable and far more water soluble than Hg0, the wide variability in mercury speciation in coal-fired flue gases undermines the total mercury removal efficiency of most mercury emission control technologies. It is important therefore to have an understanding of the behaviour of mercury during coal combustion and the mechanisms of mercury oxidation along the flue gas path. In this study, a temperature programmed decomposition technique was applied in order to acquire an understanding of the mode of decomposition of mercury species during coal combustion. A series of mercury model compounds were used for qualitative calibration. The temperature appearance range of the main mercury species can be arranged in increasing order as HgCl2 < HgS < HgO < HgSO4. Different fly ashes with certified and reference values for mercury concentration were used to evaluate the method. This study has shown that the thermal decomposition test is a newly developed efficient method for identifying and quantifying mercury species from coal combustion products.  相似文献   

3.
Mercedes Diaz-Somoano 《Fuel》2005,84(6):717-721
In this work, the retention capacity of solid sorbents for cadmium species present in coal gasification flue gases at high temperature was investigated. The influence of HCl(g) on the gas atmosphere was also evaluated. The study was carried out in a laboratory scale reactor, using synthetic gas mixtures with the sorbent as fixed bed. The sorbents tested were kaolin, limestone, alumina and fly ashes. The results obtained were compared with data from the works of other authors, who used similar solid sorbents in typical coal combustion flue gases. Whereas in the combustion atmospheres described in the literature, kaolin, limestone and alumina showed high retention capacities for cadmium compounds (0.5-40 mg g−1), in the coal gasification atmospheres studied in the present work, the amount of cadmium captured by these solid sorbents was negligible. Fly ashes were found to be the most efficient for retaining cadmium in gasification atmospheres, their maximum retention capacity in the conditions studied being approx 0.75 mg g−1.  相似文献   

4.
The relevance of Al-Si glass in a number of fly ash applications, such as use as a pozzolanic material, zeolite synthesis, and geopolymer production, necessitated research towards investigation of methods for an easy and consistent determination of the glass content in this coal (co)-combustion by-products. A glass standard-addition X-ray powder diffraction (XRD)-based method is proposed in this study as an alternative to the non straightforward procedure of conventional methods for determining the amorphous components, mainly by difference of the total mass and the addition of quantified crystalline species. A >99% Al-Si glass slag sample was selected as a standard for glass. A number of glass standard/fly ash mixtures were performed on Fluidized Bed Combustion (FBC) and pulverized coal combustion (PCC) fly ashes and subsequently analyzed by XRD. The method provides results closer to quantitative proportions of the Al-Si amorphous material of this (co)-combustion by-product, with a range of values <3% when compared with those obtained by the conventional Reference Intensity Method (RIM) method, demonstrating suitability and consistence of the procedure. Furthermore, by the proposed method, the requirement of previous determination of the mineral phases of conventional techniques is avoided. Coupled with the easy calculations, this allowed a fast determination of the glass content of (co)-combustion fly ash. The mineralogy of FBC and PCC fly ash was also investigated using the RIM method. The occurrence and proportions of the crystalline components in fly ash are in line with the combustion technology and their inherent operational parameters, especially the (co)-combustion temperature. The FBC fly ash shows the highest content of relic phases from feed coal (quartz, illite, calcite, and feldspars) and lower contents of amorphous components. The PCC fly ash are characterized by the highest proportions of mullite and Al-Si glass and low contents of quartz an other relict phases. The occurrence and distribution of anhydrite and Fe-oxide species appears to be related to the content of Ca and Fe in the feed fuels, showing slightly higher contents in FBC than in PCC fly ash.  相似文献   

5.
The aim of this study was to assess the effect of iron species present in fly ashes produced from coal combustion on mercury retention and oxidation. To achieve this objective the work was divided into two parts. In the first part the relationship between the mercury and iron content in fly ashes of different origin and characteristics was evaluated. In the second, a series of fractions enriched in iron oxides were separated from the fly ashes to determine the effect of increasing iron content on mercury retention and oxidation. Special attention was paid to the influence of iron on mercury behavior in enriched carbon particles in fly ashes. From the results obtained it can be inferred that, in the range of fly ashes studied, iron species do not affect the retention of mercury and do not play any role in heterogeneous mercury oxidation.  相似文献   

6.
Two types of fly ash from fluidized bed (FBC) and pulverized coal combustors (PCC) were treated with calcium hydroxide (Ca(OH)2) to produce reactive SO2 sorbents. Treatment was performed using 28.6 mass% Ca(OH)2/fly ash mixtures slurried at 350 K for 8 h. Sulfation experiments were carried out in a thermogravimetric analyzer (TGA) at SO2 concentration ranging from 0.11 to 0.67 vol% and 10(53–1153 K temperature range. At conditions close to those prevailing in an atmospheric FBC (1123 K, 3000 ppmv ami 20 vol% excess air), about 92% and complete conversion of CaO to CaSO4 within 1 h reaction could be achieved with treated PCC and FBC fly ashes, respectively. Based on pore structural measurements for both sorbents, treatment enhanced the specific surface area (by about 8 times) as well as pore volume (by about 5 times). The shape of the N2-adsorption/desorption isotherms, specific pore area, and pore volume distribution curves remained unchanged. Study of the intrinsic kinetics of the reaction between treated fly ash and S02 indicated a first order reaction with respect to SO2 concentration up to 0.31 vol% SO2 (3.36 × 10?8 mol/cm3). Activation energies of 82.3 and 89.0 kJ/mol were calculated for treated PCC and FBC fly ashes, respsctively.  相似文献   

7.
M. Antonia López-Antón 《Fuel》2007,86(14):2064-2070
Mercury and selenium are present as trace elements in coal and may be emitted to the environment in gas phase during coal conversion processes or be partially retained on the fly ashes. The present work explores the possibility that selenium may contribute to mercury capture in fly ashes in two different situations: firstly the power station itself, in order to evaluate the influence of typical working conditions, and secondly in a fixed bed of fly ashes enriched with Se, in order to study the capture of mercury in more severe conditions. It was found that the presence of selenium in fly ashes may improve their capacity to capture mercury. However, in the four fly ashes of different origin studied, selenium is not the most important component for mercury retention. In fact, the presence of selenium in fly ash samples enriched in unburned carbon does not have any significant effect on mercury retention.  相似文献   

8.
《Fuel》2006,85(10-11):1418-1427
Fly ashes were collected from the electrostatic precipitator (ESPs) and/or the baghouse of seven coal-fired power plants. The fly ashes were sampled from power plants that use pulverized subbituminous and bituminous feed coals. Fly ash from bituminous coals and limestone feed coals from fluidized-bed power plant were also sampled. The fly ashes were examined for their mineralogies and elemental compositions. The fly ashes from pulverized low sulfur coals are ferrocalsialic, those from high sulfur coals are ferrosialic and the fly ashes from the fluidized bed coals are ferrocalcic. The concentrations of As, Cd, Hg, Mo, Ni, and Pb in fly ash are related to the S content of the coal. Generally, those feed coals with a high S content contain higher concentrations of these elements. The concentrations of these elements are also greater for baghouse fly ash compared to ESP fly ash for the same station. The S content of fly ash from high S coal is 0.1% for pulverized ESP fly ash and 7% for baghouse fly ash from the fluidized bed, indicating that most of the S is captured by fly ash in the fluidized bed. The baghouse fly ash from the fluidized bed has the highest content of Cd, Hg, Mo, Pb, and Se, indicating that CaO, for the most part, captures them. Arsenic is captured by calcium-bearing minerals and hematite, and forms a stable complex of calcium or a transition metal of iron hydroxy arsenate hydrate [(M2+)2Fe3(AsO4)3(OH)4·10H2O] in the fly ash. Most elements in fly ash have enrichment indices of greater than 0.7 indicating that they are more enriched in the fly ash than in the feed coal, except for Hg in all ESP ashes. Mercury is an exception; it is more enriched in baghouse fly ash compared to ESP. Fly ash collected from a station equipped with hot side ESP has a lower concentration of Hg compared to stations equipped with cold side ESP using feed coals of similar rank and mercury content. Fly ash particles from fluidized bed coal are angular and subangular with cores of quartz and calcite. The quartz core is encased in layer(s) of calcium-rich aluminosilicates, and/or calcium/iron oxides. The calcite core is usually encased in an anhydrite shell.  相似文献   

9.
The emission of mercury by coal-fired power plants has become a recent concern on the part of the electric utility industry. Knowledge of mercury kinetic mechanisms is imperative for the research of predicting mercury transformation and finding its effective control methods in coal combustion flue gas. Near the end of the flue gas path, mercury exists as a combination of elemental vapor and HgCl2 vapor. HgCl2 is more likely to be removed from the flue gas. Thus, the degree of oxidation is considered to be a critical factor that tends to reduce emission. In the present work, the microcosmic kinetic mechanisms of reactions between mercury and oxidizing species were investigated by ab initio calculations of quantum chemistry. The geometry optimizations of reactants, transition states, intermediates and products were made by the quantum chemistry MP2 method at SDD basis function level. All molecule energies were calculated at QCISD(T)/SDD level and corrected with zero point energy. The activation energies and heat of reactions were calculated. The reaction rate constants were calculated from transition state theory (TST). The performance of the ab initio calculations of quantum chemistry was assessed through comparisons with the literature data. The comparisons showed that the ab initio calculations of quantum chemistry were in agreement with the literature data. The results showed that quantum chemistry was an effective means for investigating kinetic mechanism of mercury interaction with combustion-generated flue gas.  相似文献   

10.
Sébastien Rio 《Fuel》2003,82(2):153-159
Coal combustion in power plant produces fly ash. Fly ash may be used in water treatment to remove mercury (Hg2+) from water or to immobilize mercury mobile forms in silts and soils. Experiments were carried out on two kinds of fly ashes produced by two circulating fluidized bed plants with different chemical composition: silico-aluminous fly ashes and sulfo-calcic fly ashes. For the two kinds of fly ashes, adsorption equilibrium were reached in 3 days. Furthermore, removal of mercury was increased with increasing pH. Sulfo-calcic fly ashes allow us to remove mercury more efficiently and more steady. The chemical analysis of fly ash surface was carried out by electron spectroscopy. The results show that mercury is bound to ash surface thanks to several chemical reactions between mercury and various oxides (silicon, aluminium and calcium silicate) of the surface of the ashes.  相似文献   

11.
Fariborz Goodarzi  James C. Hower   《Fuel》2008,87(10-11):1949-1957
Fly ashes produced from Canadian power plants using pulverized coal and fluidized bed combustors were examined for their carbon content to determine their ability to capture mercury. The feed coal used in these power plants were lignite, subbituminous, high and medium volatile bituminous, their blends, and also blends of coal with petroleum coke (Petcoke). The carbon and mercury content of the coals and fly ashes were determined using the ASTM standard method and by the cold vapour atomic absorption spectrometry method. The carbon content of the fly ash was concentrated by strong acid digestion using HCl and HF. The quantitative and qualitative analyses of the carbon concentrate were made by using a reflected light microscope. The results show that the carbon content of fly ash appears to be partially related to depositional environment during coalification and to the rank of the coal. The Hg captured by the fly ash depends on the rank and blend of the feed coals and the type of carbon in the fly ash. The isotropic vitrinitic char is mostly responsible for the capture of most Hg in fly ash. The inadvertent increase in carbon content due to the blending of coal with petroleum coke did not increase the amount Hg captured by the fly ash. The fly ash collected by the hot side electrostatic precipitator has a low Hg content and no relation between the Hg and carbon content of the ash was observed. These results indicate that the quantity of carbon in the fly ash alone does not determine the amount Hg captured. The types of carbon present (isotropic and anisotropic vitrinitic, isotropic inertinitic and anisotropic Petcoke), the halogen content, the types of fly ash control devices, and the temperatures of the fly ash control devices all play major roles in the capture of Hg.  相似文献   

12.
《Fuel》2006,85(10-11):1550-1558
Mercury, arsenic and selenium are trace elements well-known for their high volatility in underground coal gasification (UCG) which can lead to environmental and technical problems during gas utilization. In this paper, the volatilization of mercury, arsenic and selenium from coal in a seam during the process of UCG were investigated, based on comparison of their volatility during the transformation of coal to char and the conversion of char to ash. Three types of coal were involved in this study. The results indicate that the volatility of mercury, arsenic and selenium during UCG in the seam follows the sequence of Hg>Se>As. Mercury and selenium show volatility higher than 90% from coal to ash. The volatility of arsenic is lower than 60% as confirmed by arsenic enrichment in UCG ash. Arsenic volatilization during UCG is also enhanced by increasing temperature, which is different from the result during the combustion of crushed coal. Coal type has obvious effect on element volatilization. The higher the coal reactivity, the easier is the evaporation of the elements from coal in the seam. At the same time, thermodynamic equilibrium calculations using MTDATA program were performed to predict the possible species in UCG gas. With regard to UCG gas at the production well, mercury presents as Hg(g), H2Se(g) is the main gaseous species of selenium, whereas arsenic occurs in condensed phase as As2S3 and As. The effect of the pressure on the equilibrium composition of the gas results in major changes of the proportions of the species. High pressure leads to the formation and enhancement of the reduced species and increases the condensation temperature of the volatile elements.  相似文献   

13.
Distributions of mercury speciation of Hg0, Hg2+ and Hg P in flue gas and fly ash were sampled by using the Ontario Hydro Method in a 220 MW pulverized coal-fired boiler power plant in China. The mercury speciation was varied greatly when flue gas going through the electrostatic precipitator (ESP). The mercury adsorbed on fly ashes was found strongly dependent on unburnt carbon content in fly ash and slightly on the particle sizes, which implies that the physical and chemical features of some elemental substances enriched to fly ash surface also have a non-ignored effect on the mercury adsorption. The concentration of chlorine in coal, oxyge nand NO x in flue gas has a positive correlation with the formation of the oxidized mercury, but the sulfur in coal has a positive influence on the formation of elemental mercury. This work was presented at the 6 th Korea-China Workshop on Clean Energy Technology held at Busan, Korea, July 4–7, 2006.  相似文献   

14.
《Fuel》2006,85(7-8):1087-1093
The behaviour of some selected trace metals (Hg, Cd, As, Pb, Sb, Cr, Co, Cu, Mn, Ni and V) during co-combustion processes of bio-waste materials (sewage sludge, waste wood, refused derived fuel) and coal has been predicted by thermodynamic equilibrium calculations using the HSC-Chemistry 4.0 software. The influence of temperature, flue gas composition, trace element concentration and minor fly ash components on equilibrium composition was evaluated. For most of the elements, an increase in the HCl concentration favours the formation of gaseous species while increasing concentration of SO2 in the gas composition enhances the formation of condensed species. Trace element interactions with minor fly ash components were predicted. From results obtained in this study it may be concluded that, from a thermodynamical point of view, the addition of a secondary fuel in combustion processes does not produce an increase in trace element emissions to the environment. Generally, trace elements are captured in ashes avoiding that these elements reach the stack.  相似文献   

15.
Bench-scale investigations indicate that NO, NO2, hematite (α-Fe2O3), maghemite (γ-Fe2O3), and HCl promote the conversion of gaseous elemental mercury (Hg0) to gaseous oxidized mercury (Hg2+) and/or particle-associated mercury (Hg[p]) in simulated coal combustion flue gases. In this investigation, the effects of NOx, α-Fe2O3, γ-Fe2O3, and HCl on Hg transformations were evaluated by injecting them into actual coal combustion flue gases produced from burning subbituminous Absaloka and lignitic Falkirk coals in a 7-kW down-fired cylindrical furnace. A bituminous Blacksville coal known to produce an Hg2+-rich combustion flue gas was also burned in the system. The American Society for Testing and Materials Method D6784-02 (Ontario Hydro method) or an online Hg analyzer equipped to measure Hg0 and total gaseous mercury (Hg[tot]) was used to monitor Hg speciation at the baghouse inlet (160–195 °C) and outlet (110–140 °C) locations of the system. As expected, the baseline Blacksville flue gas was composed predominantly of Hg2+ (Hg2+/Hg[tot]=0.77), whereas Absaloka and Falkirk flue gases contained primarily Hg0 (Hg0/Hg[tot]=0.84 and 0.78, respectively). Injections of NO2 (80–190 ppmv) at 440–880 °C and α-Fe2O3 (15 and 6 wt.%) at 450 °C into Absaloka and Falkirk coal combustion flue gases did not significantly affect Hg speciation. The lack of Hg0 to Hg2+ conversion suggests that components of Absaloka and Falkirk combustion flue gases and/or fly ashes inhibit heterogeneous Hg0–NOx–α-Fe2O3 reactions or that the flue gas quench rate in the 7-kW system is much different in relation to bench-scale flue gas simulators.An abundance of Hg2+, HCl, and γ-Fe2O3 in Blacksville flue gas and the inertness of injected α-Fe2O3 with respect to heterogeneous Hg0 oxidation in Absaloka and Falkirk flue gases suggested that γ-Fe2O3 catalyzes Hg2+ formation and that HCl is an important Hg0 reactant. The filtration of Absaloka and Falkirk combustion flue gases at 150 °C through fabric filters with ≈60 g/m2 γ-Fe2O3 indicated that about 30% of the Hg0 in Absaloka and Falkirk flue gases was converted to Hg2+ and/or Hg(p). HCl injection (100 ppmv) into the Absaloka combustion flue gas converted most of the Hg0 to Hg2+, whereas HCl injection into the Falkirk flue gas converted most of the Hg0 and Hg2+ to Hg(p). Additions of γ-Fe2O3 and HCl did not have a synergistic effect on Hg0 oxidation. The filtration of Absaloka and Falkirk flue gases through much greater fabric filter loadings of 475 g/m2 γ-Fe2O3 essentially doubled the baghouse Hg[tot] removal efficiency to about 50%. Results from this investigation demonstrate the importance of evaluating potential Hg0 reactants and oxidation catalysts in actual coal combustion flue gases.  相似文献   

16.
Chemical-Looping Combustion (CLC) is an emerging technology for CO2 capture because separation of this gas from the other flue gas components is inherent to the process and thus no energy is expended for the separation. For its use with coal as fuel in power plants, a process integrated by coal gasification and CLC would have important advantages for CO2 capture. This paper presents the combustion results obtained with a Cu-based oxygen carrier in a continuous operation CLC plant (500 Wth) using syngas as fuel. For comparison purposes pure H2 and CO were also used. Tests were performed at two temperatures (1073 and 1153 K), different solid circulation rates and power inputs. Full syngas combustion was reached at 1073 K working at f higher than 1.5. The syngas composition had small effect on the combustion efficiency. This result seems to indicate that the water gas shift reaction acts as an intermediate step in the global combustion reaction of the syngas. The results obtained after 40 h of operation showed that the copper-based oxygen carrier prepared by impregnation could be used in a CLC plant for syngas combustion without operational problems such as carbon deposition, attrition, or agglomeration.  相似文献   

17.
F. Goodarzi  J. Reyes 《Fuel》2008,87(6):915-924
Feed coals and fly ashes from two coal-fired power plants burning Alberta subbituminous coal were analyzed for C, Cl, Hg, and S and calorific values (for feed coal only), every week for a period of 33 weeks. The feed coals used in this study were deposited in brackish water and are compared to the coals deposited in a freshwater environment. The Hg and char (unburnt carbon) content of the fly ash was monitored to determine the variation of Hg and its possible relationship to the char types in the fly ash. The feed coals have Hg content of 0.026-0.089 mg/kg and their fly ash contains 0.02-0.243 mg/kg of Hg. The C content of the fly ashes ranges from 0.15% to 0.51%. The carbon/char was separated from the fly ash using HF and HCl. Reactive vitrinitic (formed from woody part of plants) and less reactive inertinitic (natural char) chars were separated by density separations of various specific gravities using ZnBr2.The char is mostly reactive vitrinitic (67-80 vol.%). Both stations have similar range of C content for their respective fly ashes. However, station 2 shows a much wider range of Hg in fly ash compared to station 1. In general, the fly ash from coal deposited under brackish water environment (stations 1 and 2) appears to have same or higher Hg content for lower C content compared to the fly ash from coal deposited under fresh water environment.The calculated emitted Hg for the period of 33 weeks for station 1 is estimated to be 64-90% of the total input of Hg with an average of 74%. The calculated emitted Hg shows a more complex pattern for station 2 and falls into two groups; with group (a) showing higher enrichment index for both Hg and S. The calculated emitted Hg for this group is 43-74% with an average of 57%, indicative of more Hg being captured by fly ash, possibly due to interaction between Hg and S. In the second group (b) the emitted Hg is calculated to be 74-95% with an average of 85%. The relative enrichment of both Hg and S in group (b) is low compared to group (a), indicative of possible slight paleo-weathering of the feed coal.The present study indicates that geological parameters such as paleo weathering and also depositional environment of the feed coal may influence the Hg content of fly ash.  相似文献   

18.
The volatilization of fly ash has been examined by a number of techniques including TGA—DTA, Knudsen cell mass spectrometry, volatilization of neutron-activated fly ash, and X-ray fluorescence analysis of sized fly ash, low-temperature ash, and the parent coal. At low temperatures, H2O, CO2, SO2, and a number of organic compounds are the primary volatile species as determined by mass spectrometry. Analysis of the volatiles collected from activated fly ash heated to temperatures up to 1400 °C shows that Hg, Se, As, Br, and I are nearly completely volatilized. The analysis of the bulk and size fractions of fly ash, and parent coal, is consistent with this and provides evidence for volatilization of 15 elements during coal combustion. Comparison of coal and fly ash compositions also shows that significant amounts of Se are still present in the gas phase at the precipitators and more than 50 wt % of the Se is contained in the stack emissions. The results are consistent with present models for fly ash formation and trace element enrichment.  相似文献   

19.
循环流化床中烟气飞灰汞迁移规律   总被引:2,自引:0,他引:2       下载免费PDF全文
黄勋  程乐鸣  蔡毅  侯文慧  周劲松 《化工学报》2014,65(4):1387-1395
在小型热态循环流化床试验台上进行褐煤、烟煤、无烟煤燃烧试验,研究3种典型煤的烟气气态汞和飞灰颗粒汞迁移规律。试验结果表明:褐煤、烟煤、无烟煤在燃烧过程中,炉膛温度、空截面风速、给煤量以及煤颗粒大小变化时,汞元素在烟气和飞灰之间的迁移规律相似;降低炉膛密相区温度和增大炉膛空截面风速可促进烟气气态总汞HgT(g)迁移到飞灰颗粒汞Hg(p)中,同时也促进烟气气态零价汞Hg0(g)向烟气气态二价汞Hg2+(g)和Hg(p)转化;增加给煤量,烟气气态总汞HgT(g)和烟气气态零价汞Hg0(g)减少,飞灰颗粒汞Hg(p)含量增加,并且影响Hg0(g)的转化;选择合适的煤颗粒粒度可以促进Hg0(g)的转化以及HgT(g)向Hg(p)迁移。随燃烧工况的变化,3种煤HgT(g)、Hg(p)和Hg0(g)含量变化趋势相似,但含量相差较大,Hg0(g)占HgT(g)的比例y值也不同,其中无烟煤的y值高于烟煤和褐煤的y值。  相似文献   

20.
Iron Mössbauer spectroscopy and X-ray diffraction methods were applied to the study of a selection of ashes produced in a Lurgi gasification plant and fly ash from a pulverized coal combustion. The ashes contained hematite, magnetite, and goethite. Sixty percent or more of the iron in these ashes was in the oxide form, with the remainder present in mullite and other silicate phases. Iron was divalent in the latter, and present as both Fe+2 and Fe+3 in mullite. Ratios of Fe+2 and Fe+3 varied from 0.3 to 0.7. By comparison, a water-quenched molten bottom ash was free of iron oxides and contained only amorphous silicate phases with virtually all iron in the divalent state.  相似文献   

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