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Title: High-temperature illite dissolution kinetics

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Research Org.:
Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
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Conference: Presented at: Stanford Geothermal Workshop, Stanford, CA, United States, Jan 26 - Jan 28, 2015
Country of Publication:
United States

Citation Formats

Smith, M M, and Carroll, S A. High-temperature illite dissolution kinetics. United States: N. p., 2015. Web.
Smith, M M, & Carroll, S A. High-temperature illite dissolution kinetics. United States.
Smith, M M, and Carroll, S A. 2015. "High-temperature illite dissolution kinetics". United States. doi:.
title = {High-temperature illite dissolution kinetics},
author = {Smith, M M and Carroll, S A},
abstractNote = {},
doi = {},
journal = {},
number = ,
volume = ,
place = {United States},
year = 2015,
month = 1

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  • Summary Sheet silicates and clays are ubiquitous in geothermal environments. Their dissolution is of interest because this process contributes to scaling reactions along fluid pathways and alteration of fracture surfaces, which could affect reservoir permeability. In order to better predict the geochemical impacts on long-term performance of engineered geothermal systems, we have measured chlorite, biotite, illite, and muscovite dissolution and developed generalized kinetic rate laws that are applicable over an expanded range of solution pH and temperature for each mineral. This report summarizes the rate equations for layered silicates where data were lacking for geothermal systems.
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  • The enthalpy of oxygen dissolution in liquid zirconium occurring during the combustion of Zr particles is estimated. The analysis presented uses direct experimental measurements of the temperature, size, and composition histories of burning Zr particles. The dissolution enthalpy is limited by the range of 700--830 kJ/mol and is somewhat less than that of Zr oxidation. This forms out of the supersaturated Zr/O solution. Stoichiometric ZrO{sub 2} is formed near the end of combustion and the additional energy released at that time causes a rapid temperature increase which can trigger a particle explosion.
  • Physical processes that govern the growth kinetics of carbon clusters at high pressure and high temperature are: (a) thermodynamics and structural sp?-to- sp? bonding) changes and (b) cluster diffusion. Our study on item (a) deals with ab initio and semi-empirical quantum mechanical calculations to examine effects of cluster size on the relative stability of graphite and diamond clusters and the energy barrier between the two. We have also made molecular dynamics simulations using the Brenner bond order potential. Kesults show that the melting line of diamond based on the Brenner potential is reasonable and that the liquid structure changes frommore » mostly sp-bonded carbon chains to mostly sp?-bonding over a relatively narrow density interval. Our study on item (b) uses the time-dependent clustor size distribution function obtained from the relevant Smoluchowski equations. The resulting surface contribution to the Gibbs free energy of carbon clusters was implemented in a thermochemical code.« less
  • Kinetic studies of the dolomite sulfidation reaction are carried out at high pressure (15 atm) and high temperature (600--900 C) in a differential bed flow-through reactor. The dolomite particles are exposed to simulated coal gas environments and the extent of conversion determined. Experiments are carried out to determine the influence of total pressure, reaction temperature and partial pressure of H{sub 2}S on the extent of fully calcined dolomite (FCD) sulfidation. Based on the grain theory it is found that towards the later stages of the reaction the FCD sulfidation is product layer diffusion controlled. The reaction is found to bemore » first order with respect to H{sub 2}S partial pressure. A low apparent activation energy of 4.6 kcal/gmol for the product layer diffusion controlled reaction is attributed to the presence of porous MgO along with the low porosity CaS product layer. A comparison of the performance of dolomite and limestone as sorbents for desulfurization shows that dolomite is a better sorbent with higher conversions even at higher CO{sub 2} partial pressures. The high pressure sulfidation kinetic data obtained in this study would be useful in understanding and optimizing the in-gasifier H{sub 2}S capture using dolomite sorbents.« less