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H2-reduced phosphomolybdate promotes room-temperature aerobic oxidation of methane to methanol
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H2-reduced phosphomolybdate promotes room-temperature aerobic oxidation of methane to methanol
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Journal Article
H2-reduced phosphomolybdate promotes room-temperature aerobic oxidation of methane to methanol
2023
Overview
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 (H
2
), converts methane and O
2
almost exclusively to methanol at room temperature. The highest activity reaches 67.4 μmol g
cat
−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.
The partial oxidation of methane to methanol is a very attractive yet challenging process. Now, a H
2
-reduced Pd-containing phosphomolybdate catalyst is reported to convert methane and O
2
to methanol with nearly 100% selectivity at room temperature.
Publisher
Nature Publishing Group UK,Nature Publishing Group
Subject
