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21.
Kinetic study of the dehydroxylation of chrysotile asbestos with temperature by in situ XRPD 总被引:6,自引:0,他引:6
The kinetics of the dehydroxylation of chrysotile was followed in situ at high temperature using real-time conventional and
synchrotron powder diffraction (XRPD). This is the first time kinetics parameters have been calculated for the dehydroxylation
of chrysotile. The value of the order of the reaction mechanism calculated using the Avrami model indicates that the rate-limiting
step of the reaction is a one-dimensional diffusion with an instantaneous nucleation or a deceleratory rate of nucleation
of the reaction product. Hence, the rate-limiting step is the one-dimensional diffusion of the water molecules formed in the
interlayer region by direct condensation of two hydrogen atoms and an oxygen atom. The calculated apparent activation energy
of the reaction in the temperature range 620–750 °C is 184 kJ mol−1. The diffusion path is along the axis of the fibrils forming the fibers. The amorphous or short-range ordered dehydroxylate
of chrysotile is extremely unstable because forsterite readily nucleates in the Mg-rich regions. Moreover, it is less stable
than the dehydroxylate of kaolinite, the so-called metakaolinite, which forms mullite at about 950 °C. This difference is
interpreted in terms of the different nature of the two ions Mg2+ and Al3+ and their function as glass modifier and glass-forming ion, respectively.
Received: 10 April 2002 / Accepted: 7 January 2003
Acknowledgements This work is part of a COFIN project (04 Scienze della Terra, NR 17, 2000) supported by MURST. Dr Dapiaggi is kindly acknowledged
for help during the data collection at the Dipartimento di Scienze della Terra, University of Milan. 相似文献
22.
The rate of the reversible homogeneous disproportionation of polysulfides was studied by following the optical absorbance of polysulfide solutions in a continuous plug flow reactor equipped with an on-line photometric detector. In order to avoid heterogeneous slow reactions involving sulfur colloids or precipitate, the reaction was initiated by an abrupt pH change from an undersaturated solution containing predominantly tetrasulfide species to a pH where pentasulfide is the dominant species. The disproportionation was found to follow first order reversible reaction dynamics. At environmentally relevant conditions the characteristic time of the disproportionation reaction is of the order of 10 s. This characteristic time implies that necessary conditions for speciation of the different polysulfide species by chromatography or another separation and subsequent quantification scheme should be of the order of 1 s. 相似文献
23.
南黄海盆地油气资源潜力一直是中国海上油气勘探关心的问题,但仍未取得突破性进展。生烃动力学研究对烃源岩生烃潜力评价至关重要,而该区古近系烃源岩的生烃动力学的研究十分薄弱。为此,在对南黄海盆地南部凹陷烃源岩常规地球化学分析统计基础上,着重选择南二凹低成熟样品开展PY-GC,SRA 和MSSV 等实验分析及动力学模拟。结果表明:南二凹阜四段烃源岩已进入生烃阶段,其产出的石油类型为石蜡-环烷-芳香基低蜡型,活化能分布范围为43~60 kcal/mol,其活化能主峰为51 kcal/mol,占72%,指前因子A=9.66×1012,生烃窗温度为128~158℃。该套烃源岩生烃历程中所生成的烃类在渐新世末期(23~30 Ma)以气液两相共存的形式存在,其余时期均以单一液相存在于该地层,至今转化率仍处于50%~60%。研究获得的南黄海盆地南二凹古近系泥岩的生烃动力学特征对于估算该盆地油气资源潜力极为重要,可为该区下一步油气勘探开发决策提供参考依据。 相似文献
24.
Oxygen Isotope Exchange Kinetics Between Coexisting Minerals and Water in the Aral Granite Pluton of the Altay Mountains, Northern Xinjiang 总被引:2,自引:0,他引:2
Liu Wei Research Center of Mineral Resources Exploration Chinese Academy of Sciences Chinese Academy of Sciences BeijingHe Baichu Changsha Institute of Geotectonics Chinese Academy of Sciences Changsh Hunanand Chen ZhenshengYichang Institute of Geology Mineral Resources Chinese Academy of GeologicalSciences Yichang Hubei 《《地质学报》英文版》1996,70(4)
Coexisting quartz, feldspar and biotite vary widely in their δ18O values and display a remarkable 18O/16O disequilibrium relation; especially, a quartz-feldspar reversal (△ 18OQUartz_feldspar< 0) exsists in the Aral granite pluton of the Altay Mountains, northern Xinjiang. The 18O / 16O exchange reaction definitely occurred between granite and water. Initial δ18O values of the granite and exotic fluid are evaluated by the mass balance consideration. The conventional method of discrimination between various magma derivations simply with δ18O values of either whole rock or separate minerals is misleading and unreliable. Experiments carried out by the authors show that the 18O / 16O exchange reaction is not accompanied by what geologists describe as petrological and mineralogical alteration effect. This decoupling relation implies that exchange reaction occurs at a relatively high temperature during subsolidus-postmagmatic cooling of magmas. The exchange mechanism is mainly diffusion-controlled. It is 相似文献
25.
对我国南方中新生代地洼盆地中的砂岩铜矿床进行了化学动力学与热力学的理论与实验研究。矿源岩中以辉铜矿和黄铜矿最有利于溶解和迁移,NaCl对Cu的溶解和含矿流体的形成起了催化作用。溶液中Cu以络合物的形式迁移,其中以一价铜氯络合物为主;温度的降低和溶液中性化导致了络合物的失稳、分解和铜矿物的沉淀。铜矿物的化学动力学和热力学制约了砂岩铜矿中以辉铜矿为主及矿床分带的形成。 相似文献
26.
27.
Rate constants for the gas-phase reactions of OH radicals, NO3 radicals and O3 with the C7-carbonyl compounds 4-methylenehex-5-enal [CH2=CHC(=CH2)CH2CH2CHO], (3Z)- and (3E)-4-methylhexa-3,5-dienal [CH2=CHC(CH3)=CHCH2CHO] and 4-methylcyclohex-3-en-1-one, which are products of the atmospheric degradations of myrcene, Z- and E-ocimene and terpinolene, respectively, have been measured at 296 ± 2 K and atmospheric pressure of air using relative rate methods. The rate constants obtained (in cm3 molecule–1 s–1 units) were: for 4-methylenehex-5-enal, (1.55 ± 0.15) × 10–10, (4.75 ± 0.35) × 10–13 and (1.46 ± 0.12) × 10–17 for the OH radical, NO3 radical and O3 reactions, respectively; for (3Z)-4-methylhexa-3,5-dienal: (1.61 ± 0.35) × 10–10, (2.17 ± 0.30) × 10–12, and (4.13 ± 0.81) × 10–17 for the OH radical, NO3 radical and O3 reactions, respectively; for (3E)-4-methylhexa-3,5-dienal: (2.52 ± 0.65) × 10–10, (1.75 ± 0.27) × 10–12, and (5.36 ± 0.28) × 10–17 for the OH radical, NO3 radical and O3 reactions, respectively; and for 4-methylcyclohex-3-en-1-one: (1.10 ± 0.19) × 10–10, (1.81 ± 0.35) × 10–12, and (6.98 ± 0.40) × 10–17 for the OH radical, NO3 radical and O3 reactions, respectively. These carbonyl compounds are all reactive in the troposphere, with daytime reaction with the OH radical and nighttime reaction with the NO3 radical being predicted to dominate as loss processes and with estimated lifetimes of about an hour or less. 相似文献
28.
Controls on metamorphic equilibration: the importance of intergranular solubilities mediated by fluid composition
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W. D. Carlson J. D. Hixon J. M. Garber R. J. Bodnar 《Journal of Metamorphic Geology》2015,33(2):123-146
A dramatic demonstration of the role of intergranular solubility in promoting chemical equilibration during metamorphism is found in the unusual zoning of garnet in pelitic schist exposed at Harpswell Neck, Maine, USA. Many garnet crystals have irregular, patchy distributions of Mn, Cr, Fe and Mg in their inclusion‐rich interiors, transitioning to smooth, concentric zoning in their inclusion‐poor outer rims; in contrast, zoning of Ca and Y is comparatively smooth and concentric throughout. We re‐assess the disputed origin of these zoning features by examining garnet growth in the context of the thermal and structural history of the rocks, and by evaluating the record of fluid–rock interaction revealed in outcrop‐scale veining and fluid‐inclusion assemblages. The transition in the character of garnet zoning correlates with the onset of a synkinematic, simple‐shear‐dominated phase of garnet growth and with a shift in the composition of the intergranular fluid from CO2‐rich to H2O‐rich. Compositional variations in garnet are therefore best explained by a two‐stage growth history in which intergranular diffusive fluxes reflect differences in the concentration of dissolved species in these two contrasting fluids. Interiors of garnet crystals grew in the presence of a CO2‐rich fluid, in which limited solubility for Mn and Cr (and perhaps Fe and Mg) produced patchy disequilibrium overprint zoning, while appreciable solubility for Ca and Y permitted their rock‐wide equilibration. Rims grew in the presence of an H2O‐rich fluid, in which high intergranular concentrations for all elements except Cr enabled diffusion over length scales sufficient for rock‐wide equilibration. This striking example of partial chemical equilibrium during reaction and porphyroblast growth implies that thermal effects may commonly be subsidiary in importance to solubilities in the intergranular medium as determinants of length scales for metamorphic equilibration. 相似文献
29.
热液金属矿床成因研究过程中,观测与实验始终是密切结合的。上世纪70年代,平衡热力学的实验数据的快速积累,使人们用热力学理论计算可以预测和反演矿石和岩石的成因。但是,没有矿物-水溶液的反应速率数据,又没有与流体力学的结合,搞清楚矿石成因是困难的。七、八十年代,开始研究矿物与水溶液的反应动力学实验。科学家们开始瞄准了从平衡-封闭-静态转向非平衡-开放-动力学研究的这个大方向。1992年我们建立地球化学动力学开放研究实验室。研究高温高压矿物与水反应速率,发现固液的开放体系的自组织现象。实验发现温度影响矿物的各个元素反应速率改变,发现在跨越水临界态时矿物与水反应速率涨落、在近临界的气-液两相不混溶区一些金属进入气相、超临界流体的氧化作用及特别的溶剂性能影响矿物溶解性质。实验证实:临界态区流体与矿石成因有关。水岩相互作用的反应动力学实验温度从低温到550度,揭示矿石的金属来源、迁移、金属与蚀变分带机制。一大批大于300度的矿物与水反应动力学实验在国际界是少有报道的。九十年代,超高压的科学发展,与同步辐射光源的技术进步的结合,使固体地球科学又迈向了地球深内部。我们发展了高温高压流体性质的原位直测(测量850℃水溶液)红外谱,发现深部流体的新性质:气液两相流体的新结构,在临界温度区(300~400℃),水分子氢键网络的破坏受压力影响不大(23MPa~3GPa),同时,出现水的高电导率。研发新仪器为开放-流动-非平衡的反应动力学实验与极端条件下物质性质的直接观测结合,在科学前沿领域开辟了创新道路。 相似文献
30.
Sulphate reduction is a key reaction to remove acidity from water bodies affected by acid mine drainage. In this study, 35SSO42− reduction rates determined in sediments from a variety of acidic lignite pit lakes have been compiled. The rates decreased with pH and are strongly dependent on carbon substrate. The rates were fitted to a Monod model adapted to the specific conditions of acidic pit lakes (APL) sediments: i) sulphate reduction rate is independent from sulphate concentration due to the high concentration typically observed in APL systems (10–30 mM), ii) the observed pH dependency of sulphate reduction was accounted for by an inhibition function Finihibt which considers the occurrence of low cell numbers of sulphate reducing bacteria at pH values < 4.75. Simulated steady-state sulphate reduction rates are predicting measured rates at carbon substrate concentrations of <10 μM. Estimated steady-state reaction time scales range between 2.4 h at pH 7 and 41 h at pH 3 at a carbon half-saturation constant of KC−S = 100 μM and are increasing with increasing KC−S values. Time scales at low pH are too long to allow for significant generation of alkalinity during the time of residence of groundwater passing through the top and hence most reactive zone of APL sediments which has important implications for the remediation of acidic pit lakes. 相似文献