التفاصيل البيبلوغرافية
العنوان: |
Quantum chemistry and kinetics of hydrogen sulphide oxidation. |
المؤلفون: |
Monge-Palacios, M., Wang, Q., Alshaarawi, A., Sepulveda, A. C. Cavazos, Sarathy, S. M. |
المصدر: |
Physical Chemistry Chemical Physics (PCCP); 1/28/2024, Vol. 26 Issue 4, p3219-3228, 10p |
مستخلص: |
A fundamental understanding of the acid gas (H2S and CO2) chemistry is key to efficiently implement the desulphurisation process and even the production of clean fuels such as hydrogen or syngas. In this work, we developed a new kinetic model for the pyrolysis and oxidation of hydrogen sulphide by merging two previously reported models with the goal of covering a wider range of conditions and including the effect of carbon dioxide. The resulting model, which consists of 75 species and 514 reactions, was used to conduct rate of production and sensitivity analysis in plug flow reactor simulations, and the results were used to determine the most prominent reactions in which hydrogen sulphide, molecular hydrogen, and sulphur monoxide are involved. The resulting list of important reactions was screened and the kinetics of three of them, i.e., SO2 + S2 → S2O + SO, S2O + S2 → S3 + SO, and SO + SH → S2 + OH, was found to warrant further investigation. With the goal of improving the accurancy of our new kinetic model, we carried out a robust quantum chemistry and Rice–Ramsperger–Kassel–Marcus master equation study to obtain, for the first time, the forward and reverse rate constants for those three reactions at temperatures and pressures of interest for combustion and atmospheric chemistry. This work is the first step of a kinetic study that is aimed at improving the understanding of the chemistry of the pyrolysis and oxidation of H2S, highlighting the importance of sulphur–sulphur interactions and providing a fundamental basis for future kinetic models of H2S not only in the field of combustion, but also in atmospheric chemistry. [ABSTRACT FROM AUTHOR] |
|
Copyright of Physical Chemistry Chemical Physics (PCCP) is the property of Royal Society of Chemistry and its content may not be copied or emailed to multiple sites or posted to a listserv without the copyright holder's express written permission. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.) |
قاعدة البيانات: |
Complementary Index |