A Highly Stable Copper‐Based Catalyst for Clarifying the Catalytic Roles of Cu0 and Cu+ Species in Methanol Dehydrogenation |
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| Authors: | Huanhuan Yang Dr. Yanyan Chen Dr. Xiaojing Cui Guofu Wang Youliang Cen Dr. Tiansheng Deng Wenjun Yan Jie Gao Dr. Shanhui Zhu Prof. Unni Olsbye Prof. Jianguo Wang Prof. Weibin Fan |
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| Affiliation: | 1. State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, P. R. China;2. University of Chinese Academy of Sciences, Beijing, P. R. China;3. Department of Chemistry, inGAP Centre of Research-based Innovation, University of Oslo, Oslo, Norway |
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| Abstract: | 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 Cu0 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 Cu0 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 Cu0 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 Cu0 sites into CO and H2. |
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| Keywords: | core– shell structures copper heterogeneous catalysis methanol dehydrogenation reaction mechanisms |
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