Highly active catalysis of methanol oxidative carbonylation over nano Cu2O supported on micropore-rich mesoporous carbon
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 yiel...
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Veröffentlicht in: | Applied catalysis. B, Environmental Environmental, 2022-04, Vol.303, p.120890, Article 120890 |
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Sprache: | eng |
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Zusammenfassung: | 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 34.2ggCu−1h−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 well-dispersed 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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•Micropore-rich mesoporous carbon supporting Cu catalyst is highly active in methanol oxidation carbonylation.•Introducing micropores to carbon support causes under-coordinated carbon atoms.•These atoms serve to immobilize Cu nanoparticles at micropore mouths.•Auto-reduction of CuO to active Cu2O is accelerated by increasing microporosity.•An electron-deficient environment of Cu2O sites favors high intrinsic activity. |
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ISSN: | 0926-3373 1873-3883 |
DOI: | 10.1016/j.apcatb.2021.120890 |