期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 57, 期 7, 页码 1836-1840出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201710605
关键词
core-shell structures; copper; heterogeneous catalysis; methanol dehydrogenation; reaction mechanisms
资金
- National Natural Science Foundation of China [21303240, 21573270, U1510104, 21773281]
- Shanxi Youth Science Foundation [2014021014-5]
- Talent Scientific and Technological Innovation Program [201605D211001]
- CAS/SAFEA International Partnership Program for Creative Research Teams [2015YC901]
Identification of the active copper species, and further illustration of the catalytic mechanism of Cu-based catalysts is still a challenge because of the mobility and evolution of Cu-0 and Cu+ species in the reaction process. Thus, an unprecedentedly stable Cu-based catalyst was prepared by uniformly embedding Cu nanoparticles in a mesoporous silica shell allowing clarification of the catalytic roles of Cu-0 and Cu+ in the dehydrogenation of methanol to methyl formate by combining isotope-labeling experiment, in situ spectroscopy, and DFT calculations. It is shown that Cu-0 sites promote the cleavage of the O-H bond in methanol and of the C-H bond in the reaction intermediates CH3O and H2COOCH3 which is formed from CH3O and HCHO, whereas Cu+ sites cause rapid decomposition of formaldehyde generated on the Cu-0 sites into CO and H-2.
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