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Abstract:
Direct conversion of methane into value-added chemicals, such as methanol under mild conditions, is a promising route for industrial applications. In this work, atomically dispersed Rh on TiO2 suspended in an aqueous solution was used for the oxidation of methane to methanol. Promoted by copper cations (as co-catalyst) in solution, the catalysts exhibited high activity and selectivity for the production of methanol using molecular oxygen with the presence of carbon monoxide at 150 degrees C with a reaction pressure of 31 bar. Millimole level yields of methanol were reached with the selectivity higher than 99 % using the Rh/TiO2 catalysts with the promotion of the copper cation. CO was the reductive agent to generate H-2 from H2O, which led to the formation of H2O2 through the reaction of H-2 and O-2. Atomically dispersed Rh activated the C-H bond in CH4 and catalyzed the oxidation using H2O2. Copper cations maintained the low-valence state of Rh. Moreover, copper acted as a scavenger for suppressing the overoxidation, thus leading to the high selectivity of methanol.
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Source :
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
ISSN: 1433-7851
Year: 2022
Issue: 18
Volume: 61
1 6 . 6
JCR@2022
1 6 . 6 0 0
JCR@2022
ESI Discipline: CHEMISTRY;
ESI HC Threshold:53
JCR Journal Grade:1
CAS Journal Grade:1
Cited Count:
WoS CC Cited Count: 46
SCOPUS Cited Count: 51
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 11
Affiliated Colleges: