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Nearly 100% selective and visible-light-driven methane conversion to formaldehyde via. single-atom Cu and Wδ
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Nearly 100% selective and visible-light-driven methane conversion to formaldehyde via. single-atom Cu and Wδ
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Journal Article
Nearly 100% selective and visible-light-driven methane conversion to formaldehyde via. single-atom Cu and Wδ
2023
Overview
Direct solar-driven methane (CH
4
) reforming is highly desirable but challenging, particularly to achieve a value-added product with high selectivity. Here, we identify a synergistic ensemble effect of atomically dispersed copper (Cu) species and partially reduced tungsten (W
δ+
), stabilised over an oxygen-vacancy-rich WO
3
, which enables exceptional photocatalytic CH
4
conversion to formaldehyde (HCHO) under visible light, leading to nearly 100% selectivity, a very high yield of 4979.0 μmol·g
−1
within 2 h, and the normalised mass activity of 8.5 × 10
6
μmol·g
-1
Cu
·h
−1
of HCHO at ambient temperature. In-situ EPR and XPS analyses indicate that the Cu species serve as the electron acceptor, promoting the photo-induced electron transfer from the conduction band to O
2
, generating reactive •OOH radicals. In parallel, the adjacent W
δ+
species act as the hole acceptor and the preferred adsorption and activation site of H
2
O to produce hydroxyl radicals (•OH), and thus activate CH
4
to methyl radicals (•CH
3
). The synergy of the adjacent dual active sites boosts the overall efficiency and selectivity of the conversion process.
Direct solar-driven methane (CH
4
) reforming is highly desirable but challenging. Here, the synergy of atomic Cu species and partially reduced tungsten (W
δ+
), stabilized over an oxygen-vacancy-rich WO
3
, enables exceptional CH
4
conversion to formaldehyde (HCHO) under visible light.
