期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 61, 期 18, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202117851
关键词
Carbon-Neutral; Hydrogenation; Mechanochemistry; Internal Field NMR; Solid-Gas Reaction
资金
- National Research Foundation (NRF) of Korea [2014R1A3A2069102, 2016R1A5A1009405]
- UK Brand Project of UNIST [1.200096.01]
- Paris Region
- European Union [754387]
- National Natural Science Foundation of China [21403092]
- Marie Curie Actions (MSCA) [754387] Funding Source: Marie Curie Actions (MSCA)
In this study, a mechanochemical method was used to enhance the reaction rate of carbon hydrogasification and improve its selectivity. The findings of this work have the potential to advance research in carbon hydrogasification and other solid-gas reactions.
Carbon hydrogasification is the slowest reaction among all carbon-involved small-molecule transformations. Here, we demonstrate a mechanochemical method that results in both a faster reaction rate and a new synthesis route. The reaction rate was dramatically enhanced by up to 4 orders of magnitude compared to the traditional thermal method. Simultaneously, the reaction exhibited very high selectivity (99.8 % CH4, versus 80 % under thermal conditions) with a cobalt catalyst. Our study demonstrated that this extreme increase in reaction rate originates from the continuous activation of reactive carbon species via mechanochemistry. The high selectivity is intimately related to the activation at low temperature, at which higher hydrocarbons are difficult to form. This work is expected to advance studies of carbon hydrogasification, and other solid-gas reactions.
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