Journal
APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 303, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.apcatb.2021.120890
Keywords
Micropore-rich mesoporous carbon; Methanol; Oxidative carbonylation; Dimethyl carbonate
Funding
- National Natural Science Foundation of China [U1510203]
- Key Research and Development Project of Shanxi Province (International Science and Technology Cooperation Program) [201803D421011]
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A micropore-rich mesoporous carbon (MMC) derived from ordered mesoporous carbon (OMC) is used as a support to prepare a highly active nano Cu2O catalyst for methanol oxidation carbonylation. The well-dispersed Cu nanoparticles with high purity of Cu2O are obtained, leading to significantly enhanced performance in terms of space-time yield and turnover frequency of DMC. The introduction of plentiful under-coordinated carbon atoms in the micropores plays a key role in immobilizing Cu precursors and accelerating the auto-reduction of CuO to form high-purity Cu2O, thereby enhancing the intrinsic activity of the catalyst.
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.
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