Origin of selectivity switch in Fischer-Tropsch synthesis over Ru and Rh from first-principles statistical mechanics studies.
作者： Jia Chen , Zhi-Pan Liu
DOI: 10.1021/JA7112239
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摘要: For its unique position in chemical industry, Fischer−Tropsch (FT) synthesis has been a hot subject heterogeneous catalysis. Due to great complexity product distribution, it remains unclear how maximally convert syngas long-chain hydrocarbons. By combining extensive DFT calculations with grand canonical Monte Carlo simulations, this work examines the key elementary steps FT over Ru and Rh surfaces, including CO dissociation, C/C coupling, hydrogenations. The origin of relationship between activity selectivity catalysts is revealed based on calculated reaction rate at working temperatures, which catalytic role surface as center accumulating CHx species highlighted. This theoretical demonstrates that ability dissociate under carbon-rich conditions requirement for good catalyst. RC + C (R = alkyl or H) pathway occurring may be general mechanism chain propagation tr...
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