Applied Catalysis2022,Vol.30314.DOI:10.1016/j.apcatb.2021.120890

Highly active catalysis of methanol oxidative carbonylation over nano Cu2O supported on micropore-rich mesoporous carbon

Wang, Jiajun Fu, Tingjun Meng, Fanhui Zhao, Dan Chuang, Steven S. . C. Li, Zhong
Applied Catalysis2022,Vol.30314.DOI:10.1016/j.apcatb.2021.120890

Highly active catalysis of methanol oxidative carbonylation over nano Cu2O supported on micropore-rich mesoporous carbon

Wang, Jiajun 1Fu, Tingjun 1Meng, Fanhui 1Zhao, Dan 1Chuang, Steven S. . C. 2Li, Zhong1
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作者信息

  • 1. Taiyuan Univ Technol
  • 2. Univ Akron
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Abstract

A micropore-rich mesoporous carbon (MMC) derived from ordered mesoporous carbon (OMC) is fabricated as support to prepare a highly active nano Cu2O catalyst for methanol oxidation carbonylation. The well-dispersed -3.3 nm Cu nanoparticles with ca. 90% purity of Cu2O are obtained. The space-time yield and turnover frequency of DMC are significantly enhanced to 34.2 g g-Cu1 h-1 and 89.1 h-1, both of which are greater than that over the mesoporous-only Cu/OMC catalyst. It is found that plentiful under-coordinated carbon atoms are formed in the introduced micropores, which serve as binding sites to immobilize Cu precursors to form the welldispersed Cu nanoparticles. A large number of these atoms are favorable to accelerate auto-reduction of CuO to Cu2O in kinetics and further promote to form high-purity Cu2O. Besides, the electrons of Cu2O are forced to transfer to the micropore surrounding, forming an electron-deficient Cu+ site in favor of intrinsic activity enhancement.

Key words

Micropore-rich mesoporous carbon/Methanol/Oxidative carbonylation/Dimethyl carbonate/DENSITY-FUNCTIONAL THEORY/DIMETHYL CARBONATE/KOH ACTIVATION/SURFACE/MECHANISM/ADSORPTION/REACTIVITY/REDUCTION/CLUSTERS/EXAFS

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出版年

2022
Applied Catalysis

Applied Catalysis

ISSN:0926-3373
被引量17
参考文献量50
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