New insight into the catalytic mechanism of ester hydrogenation over the Cu/ZnO catalyst: the contribution of hydrogen spillover

被引:3
|
作者
Gao, Lin [1 ,2 ,3 ]
Ding, Guoqiang [3 ]
Zhu, Lei [3 ]
Yu, Zhanqiu [3 ]
Li, Hongju [3 ]
Li, Guoqiang [4 ]
Zhu, Yulei [1 ,3 ]
Xiang, Hongwei [1 ,3 ]
Wen, Xiaodong [1 ,3 ]
Yang, Yong [1 ,3 ]
Li, Yongwang [3 ]
机构
[1] Chinese Acad Sci, State Key Lab Coal Convers, Inst Coal Chem, Taiyuan 030001, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Synfuels China Co Ltd, Beijing, Peoples R China
[4] Synfuels China Inner Mongolia Co Ltd, Ordos, Peoples R China
关键词
DIMETHYL MALEATE; ZINC-OXIDE; SELECTIVE HYDROGENATION; GAMMA-VALEROLACTONE; METHANOL SYNTHESIS; CU/SIO2; CATALYST; GAS-PHASE; COPPER; METHYL; PERFORMANCE;
D O I
10.1039/d3dt04268e
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
The dimethyl maleate hydrogenation activity of Cu, ZnO-X and physically mixed Cu+ZnO-X samples was systematically investigated to probe the essential role of ZnO in ester hydrogenation processes. Cu samples exhibited high C 00000000 00000000 00000000 00000000 11111111 00000000 11111111 00000000 00000000 00000000 C bond hydrogenation ability with dimethyl succinate as the main product. Comparatively, ZnO was inactive in hydrogenation due to its weak ability to dissociate hydrogen while the CO group could be activated and adsorbed on the ZnO surface. Interestingly, physical mixing with ZnO significantly improved the CO hydrogenation activity of Cu samples. The H2-TPD results reveal the origin of "Cu-ZnO synergy": hydrogen atoms formed on the copper surface can spill over to the ZnO surface and react with the adsorbed CO group. Cu+ZnO-X catalysts exhibit a synergistic effect in ester hydrogenation due to the strong adsorption of ester groups by ZnO and H2 activation by metallic Cu, with a proposed mechanism involving hydrogen spillover.
引用
收藏
页码:4048 / 4053
页数:6
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