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Abstract:
The selective partial oxidation of methane to methanol using molecular oxygen (O-2) represents a long-standing challenge, inspiring extensive study for many decades. However, considerable challenges still prevent low-temperature methane activation via the aerobic route. Here we report a precipitated Pd-containing phosphomolybdate, which, after activation by molecular hydrogen (H2), converts methane and O-2 almost exclusively to methanol at room temperature. The highest activity reaches 67.4 mu mol gcat(-1) h(-1). Pd enables rapid H-2 activation and H spillover to phosphomolybdate for Mo reduction, while facile O-2 activation and subsequent methane activation occur on the reduced phosphomolybdate sites. Continuous production of methanol from methane was also achieved by concurrently introducing H-2, O-2 and methane into the system, where H-2 assists in maintaining a moderately reduced state of phosphomolybdate. This work reveals the underexplored potential of such a Mo-based catalyst for aerobic methane oxidation and highlights the importance of regulating the chemical valence state to construct methane active sites.
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NATURE CATALYSIS
ISSN: 2520-1158
Year: 2023
4 2 . 9
JCR@2023
4 2 . 9 0 0
JCR@2023
JCR Journal Grade:1
CAS Journal Grade:1
Cited Count:
WoS CC Cited Count: 0
SCOPUS Cited Count: 49
ESI Highly Cited Papers on the List: 0 Unfold All
WanFang Cited Count:
Chinese Cited Count:
30 Days PV: 0
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