Journal
CHEMCATCHEM
Volume 12, Issue 21, Pages 5540-5547Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.202000934
Keywords
ZnO nanocrystals; Pd; ZnO catalysts; CO(2)hydrogenation into formic acid; Basicity of support; Catalytic mechanism
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Funding
- Natural Science Foundation of Zhejiang Province [LQ20B030007]
- National Natural Science Foundation of China [21525313, 91745202, 91945301]
- Chinese Academy of Sciences
- Changjiang Scholars Program of the Chinese Ministry of Education
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Pd/ZnO catalysts with ca. 2 wt.% Pd loading employing ZnO nanocrystals with various morphologies as supports, including ZnO nanoplates (p-ZnO) predominantly exposing polar {002} facets, ZnO nanorods (r-ZnO) predominantly exposing nonpolar {100} and {101} facets, and commercial ZnO (c-ZnO) exposing random facets, have been prepared as catalysts for the catalytic reaction of CO(2)hydrogenation into formic acid (FA) without the addition of base under mild conditions. A remarkable morphology-dependence of zinc oxide in the Pd/ZnO catalysts was observed. Catalytic activities of various Pd/ZnO catalysts in CO(2)hydrogenation into FA follow an order of Pd/r-ZnO>Pd/p-ZnO>Pd/c-ZnO, and all the catalysts are stable. Kinetic study, CO2-TPD analysis, and in situ DRIFTS spectra provide evidence that all the Pd/ZnO catalysts follow a similar catalytic mechanism that CO(2)activation is the rate-determining step. Consequently, r-ZnO, possessing a higher density of weak basic sites than p-ZnO and c-ZnO, can act as a superb support to prepare Pd/r-ZnO catalyst, which is more active than Pd/p-ZnO and Pd/c-ZnO catalysts for the production of FA. These findings nicely demonstrate the crystal-plane engineering of the metal oxide support in tuning the catalytic performance of Pd-based catalysts for CO(2)hydrogenation into FA.
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