Chemistry of hydrogen sulphide under coal liquefaction conditions: 1. Modelling hydrogen transfer catalysis |
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Authors: | Albert S. HirschonKaren Sundback Richard M. Laine |
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Affiliation: | Organometallic Chemistry Program, Physical Organic Chemistry Department, SRI International, Menlo Park, CA 94025, USA |
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Abstract: | The work reported here represents initial attempts to develop a complete kinetic and mechanistic understanding of the reaction chemistry of H2S under coal liquefaction conditions, using both model systems and coal. Hydrogen sulphide was found to promote/catalyse the transfer of hydrogen from tetralin to 2-hydroxyquinoline (2-HOQ). The presence of H2S can increase the rate of hydrogen transfer from tetralin to 2-HOQ by a factor of 10 compared with the same reaction run in the absence of H2S. The energy of activation for hydrogen transfer was found to decrease by ≈5 kcal mol−1 in the presence of H2S. The presence of H2S was also found to promote loss of oxygen from 2-HOQ to form small amounts of quinoline. No evidence of CC or CN bond cleavage in 2-HOQ was noted under any of the reaction conditions studied. These results suggest that the presence of H2S reduces the temperatures necessary to promote effective hydrogen transfer from tetralin by 50–75 °C. Moreover, they imply that similar effects occur in H2S-promoted coal liquefaction. |
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Keywords: | coal liquefaction H2S hydrogen transfer catalysis |
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