期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 267, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2020.118698
关键词
Metal-organic framework (MOP); Cu-Zn catalyst; Carbon; Liquid-phase hydrogenation; Ester
资金
- National Natural Science Foundation of China [21878227, U1510203]
- Chinese Scholarship Council [201606255028]
- U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences (BES), Division of Chemical Sciences, Geosciences and Biosciences (Transdisciplinary Approaches to Realize Novel Catalytic Pathways to Energy Carriers) [FWP 47319]
Liquid-phase hydrogenolytic reduction of esters on Cu-based catalysts is a promising approach for synthesis of alcohols. Here, core-shell CuZnx@C materials synthesized via pyrolysis of a Zn(NO3)(2)-loaded metal-organic framework (MOF) were proposed, in which well-defined spacing between Cu species in the parent MOF and the homogeneous loading of a Zn salt leads to an ideal distribution and strong interaction of Cu and Zn after pyrolysis of the precursor. The as-synthesized CuZnx@C showed a much higher catalytic activity than Cu@C. This higher activity is tentatively attributed to the simultaneous presence of Cu-0 and Cu+ sites at ZnO crystal domains. The resulting Cu-O-Zn sites have a high tendency to adsorb the ester in the form of a surface bound species that greatly improves the hydrogenolysis, which is the rate controlling step in the reductive pathway. A theoretical study confirms the ability of this site to bind and catalytically convert fatty acid esters.
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