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71.
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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
74.
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
75.
76.
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
77.
The chemistry of glycolaldehyde (hydroxyacetaldehyde) relevant to the troposphere has been investigated using UV absorption spectrometry and FTIR absorption spectrometry in an environmental chamber. Quantitative UV absorption spectra have been obtained for the first time. The UV spectrum peaks at 277 nm with a maximum cross section of (5.5± 0.7)×10–20 cm2 molecule–1. Studies of the ultraviolet photolysis of glycolaldehyde ( = 285 ± 25 nm) indicated that the overall quantum yield is > 0.5 in one bar of air, with the major products being CH2OH and HCO radicals. Rate coefficients for the reactions of Cl atoms and OH radicals with glycolaldehyde have been determined to be (7.6± 1.5)×10–11 and (1.1± 0.3)×10–11 cm3 molecule–1 s–1, respectively, in good agreement with the only previous study. The lifetime of glycolaldehyde in the atmosphere is about 1.0 day for reaction with OH, and > 2.5 days for photolysis, although both wet and dry deposition should also be considered in future modeling studies. 相似文献
78.
Kinetic study of the hydrocarbon generation from Upper Paleozoic coals in Ordos Basin 总被引:6,自引:0,他引:6
When organic matter during geological processes is affected by a variety of factors such as paleotemperature, and time, complicated chemical reactions will occur, finally resulting in the generation of petroleum and natural gas. These reactions leading to… 相似文献
79.
An electrochemical model is proposed, which considers the redox conditions and the electrode kinetics at the mineral surface. Advanced modelling of self-potential (SP) anomalies over ore deposits takes into account the course of the redox potential distribution with depth and the oxidation-reduction processes acting at the mineral-electrolyte interface. The application of this model to a SP anomaly in the vicinity of the German Continental Deep Drilling Program (KTB) can explain the surface and borehole data and gives an estimation of the prevailing thermodynamical conditions in the ground.Exclusively, this paper deals with SP anomalies, which are associated with high conductive graphitic layers. It can be concluded that SP-anomalies give an important hint to electronical conducting structures in the earth's crust. 相似文献
80.
This paper compares the performance of analytical and numerical approaches for modeling DNAPL dissolution with biodecay. A solution derived from a 1-D advective transport formulation (“Parker” model) is shown to agree very closely with high resolution numerical solutions. A simple lumped source mass balance solution in which with decay is assumed proportional to DNAPL mass (“Falta1” model) over- or underpredicts aqueous phase biodecay depending on the magnitude of the exponential factor governing the relationship between dissolution rate and DNAPL mass. A modification of the Falta model that assumes decay proportional to the source exit concentration is capable of accurately simulating source behavior with strong aqueous phase biodecay if model parameters are appropriately selected or calibrated (“Falta2” model). However, parameters in the lumped models exhibit complex interdependencies that cannot be quantified without consideration of transport processes within the source zone. Combining the Falta2 solution with relationships derived from the Parker model was found to resolve these limitations and track the numerical model results. A method is presented to generalize the analytical solutions to enable simulation of partial mass removal with changes in source parameters over time due to various remedial actions. The algorithm is verified by comparison with numerical simulation results. An example application is presented that demonstrates the interactions of partial mass removal, enhanced biodecay, enhanced mass transfer and source zone flow reduction applied at various time periods on contaminant flux reduction. Increasing errors that arise in numerical solutions with coarse discretization and high decay rates are shown to be controlled by using an adjusted decay coefficient derived from the Parker analytical solution. 相似文献