Journal
ACS CATALYSIS
Volume 5, Issue 10, Pages 6200-6208Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.5b01678
Keywords
Cu catalyst; hydrogenation; Cu-0/Cu+ active sites; methyl acetate; alcohol; balancing effect
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Funding
- National Natural Science Foundation of China [91434127, 21325626, 21276186]
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Hydrogenation of carbon oxygen (C-O) bonds plays a significant role in organic synthesis. Cu-based catalysts have been extensively investigated because of their high selectivity in C-O hydrogenation. However, no consensus has been reached on the precise roles of Cu-0 and Cu+ species for C-O hydrogenation reactions. Here we resolve this long-term dispute with a series of highly comparable Cu/SiO2 catalysts. All catalysts represent the full-range distribution of the Cu species and have similar general morphologies, which are detected and mutually corroborated by multiple characterizations. The results demonstrate that, when the accessible metallic Cu surface area is below a certain value, the catalytic activity of hydrogenation linearly increases with increasing Cu-0 surface area, whereas it is primarily affected by the Cu+ surface area. Furthermore, the balancing effect of these two active Cu sites on enhancing the catalytic performance is demonstrated: the Cu+ sites adsorb the methoxy and acyl species, while the Cu-0 facilitates the H-2 decomposition. This insight into the precise roles of active species can lead to new possibilities in the rational design of catalysts for hydrogenation of C-O bonds.
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