Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 120, Issue 10, Pages -Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.2206619120
Keywords
coordinatively unsaturated Cu(I) sites; selective oxidation of methane; Cu-BTC; surface hydrophobic coating; catalysts
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By using magnesium hydride as a support and combining it with a Cu(I) salt solution under the synergistic action of sodium hydroxide and cupric acetate, a Cu2-block catalyst was successfully formed. This catalyst exhibits high activity and stability for the selective oxidation of methane to C1 organic oxygenates at low temperatures.
Selective oxidation of methane to organic oxygenates over metal-organic frameworks (MOFs) catalysts at low temperature is a challenging topic in the field of C1 chemistry because of the inferior stability of MOFs. Modifying the surface of Cu-BTC via hydro-phobic polydimethylsiloxane (PDMS) at 235 degrees C under vacuum not only can dramati-cally improve its catalytic cycle stability in a liquid phase but also generate coordinatively unsaturated Cu(I) sites, which significantly enhances the catalytic activity of Cu-BTC catalyst. The results of spectroscopy characterizations and theoretical calculation proved that the coordinatively unsaturated Cu(I) sites made H2O2 dissociative into center dot OH, which formed Cu(II)-O active species by combining with coordinatively unsaturated Cu(I) sites for activating the C-H bond of methane. The high productivity of C1 oxygenates (CH3OH and CH3OOH) of 10.67 mmol gcat. -1h-1 with super high selectivity of 99.6% to C1 oxygenates was achieved over Cu-BTC-P-235 catalyst, and the catalyst possessed excellent reusability.
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