Journal
CHEMICAL ENGINEERING JOURNAL
Volume 430, Issue -, Pages -Publisher
ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.132784
Keywords
CO2 hydrogenation; Methanol; Catalytic active site; Hollow nanosphere; First-principle
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Funding
- National Natural Science Foundation of China [21808105, 22178163, 21722606, 21878149, 22078155]
- Natural Science Foundation of Jiangsu Province [BK20180709]
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This study introduces unified first-principle calculations to investigate the catalytic active sites over the universal Cu-ZnO based catalysts for CO2 hydrogenation to methanol. The study reveals that Cu/ZnO interfaces and Zn-doped Cu sites play significant roles among the catalytic active sites, and can successively participate in the CO2 conversion process.
The catalytic active sites over the universal Cu-ZnO based catalysts for CO2 hydrogenation to methanol are still the subject of intense debate. Herein, unified first-principle calculations for the CO2 conversion processes over the controversial catalytic active sites, i.e., Cu crystal steps, Zn-doped Cu sites, Cu/ZnO interfaces, and the Cu and Zn closest packing crystal facets, are implemented, which is verified with the experimental facts based on support-free catalysts of porous hollow nanospheres that eliminate the interferences from the catalyst supports. We discover that the enhanced catalytic activity corresponds to the uplifted and spin-polarized density of states owing to the hybridization of Cu and Zn species, and prove that Cu/ZnO interfaces and Zn-doped Cu sites play significant roles among the catalytic active sites, and successively participate in the CO2 conversion, of which initial step should primarily be the hydrogen-free CO2 dissociation, differing from the preconceived viewpoint of hydrogen-assisted dissociation of CO2.
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