Nearly 100% selective and visible-light-driven methane conversion to formaldehyde via. single-atom Cu and Wδ+

Lei Luo, Xiaoyu Han, Keran Wang, Youxun Xu, Lunqiao Xiong, Jiani Ma, Zhengxiao Guo () and Junwang Tang ()
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Lei Luo: Northwest University
Xiaoyu Han: The University of Manchester
Keran Wang: Northwest University
Youxun Xu: University College London
Lunqiao Xiong: University College London
Jiani Ma: Northwest University
Zhengxiao Guo: The University of Hong Kong
Junwang Tang: University College London

Nature Communications, 2023, vol. 14, issue 1, 1-13

Abstract: Abstract Direct solar-driven methane (CH4) 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 (Wδ+), stabilised over an oxygen-vacancy-rich WO3, which enables exceptional photocatalytic CH4 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 × 106 μmol·g-1Cu·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 O2, generating reactive •OOH radicals. In parallel, the adjacent Wδ+ species act as the hole acceptor and the preferred adsorption and activation site of H2O to produce hydroxyl radicals (•OH), and thus activate CH4 to methyl radicals (•CH3). The synergy of the adjacent dual active sites boosts the overall efficiency and selectivity of the conversion process.

Date: 2023
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DOI: 10.1038/s41467-023-38334-7

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