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- W4311902511 abstract "The one-step valorization of natural gas remains a challenge. Methane conversion to methanol via chemical looping over copper-containing zeolites is a promising route, and CuMFI is among the earliest successfully applied. However, the structure of the active sites in CuMFI, as well as the effect of copper loading and Si/Al ratio on the copper speciation, are yet to be understood. We found that for CuMFI, the Cu/Al ratio determines the selectivity of methane conversion by governing the structure of the active dicopper sites. At a Cu/Al ratio below 0.3, copper-containing MFI materials host dimeric centers with a Cu–Cu separation of 2.9 Å and a UV/vis absorption band at 27 200 cm–1 capable of selective oxidation of methane to methanol in a wide temperature range (450–550 K). A higher Cu/Al ratio leads to the formation of mono-μ-oxo dicopper sites with Cu–Cu = 3.2 Å, which exhibit a characteristic band at 21 900 cm–1 and react with methane at lower temperatures (<450 K), yielding overoxidation products. Identifying distinctions in the structure of selective and nonselective copper sites will aid in the design of better-performing materials." @default.
- W4311902511 created "2023-01-02" @default.
- W4311902511 creator A5008597064 @default.
- W4311902511 creator A5010083603 @default.
- W4311902511 creator A5054120563 @default.
- W4311902511 date "2022-12-06" @default.
- W4311902511 modified "2023-10-18" @default.
- W4311902511 title "Structure of Selective and Nonselective Dicopper (II) Sites in CuMFI for Methane Oxidation to Methanol" @default.
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- W4311902511 doi "https://doi.org/10.1021/acscatal.2c05299" @default.
- W4311902511 hasPublicationYear "2022" @default.
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