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Electron-Delocalization-Stabilized Photoelectrocatalytic Coupling of Methane by NiO-Polyoxometalate Sub-1 nm Heterostructures
- Source :
- Journal of the American Chemical Society; November 2023, Vol. 145 Issue: 43 p23681-23690, 10p
- Publication Year :
- 2023
-
Abstract
- The oxidative coupling of methane to C2 oxygenates merits great scientific and technological potential yet remains a challenge due to its inferior selectivity. Subnanomaterials (SNMs) with “p–n–p–n”-type heteroconstructions feature enhanced external field coupling properties and tunable electronic structures, serving as promising catalysts for the selective partial oxidation of methane. Here we develop NiO–polyoxometalate (POM) subnanocoils with a thickness of 1.8 nm, showing excellent catalytic activity toward photoelectrochemical coupling of methane into a C2 product under mild conditions (1 bar, 25 °C) with a notable productivity (up to 4.48 mmol gcat–1h–1) and a high selectivity (>99%). Under photoelectrochemical coupling, C–H bonds can be activated by NiO, and the resulted *COOH intermediates are stabilized by the delocalized electrons in POM clusters. The contiguous active sites of NiO and POM at the molecular level allow the in situcoupling of *COOH into oxalate. This work points out an economic way for the oxidation of methane under mild conditions and may enlighten the design of functional SNMs from fundamental standpoints.
Details
- Language :
- English
- ISSN :
- 00027863 and 15205126
- Volume :
- 145
- Issue :
- 43
- Database :
- Supplemental Index
- Journal :
- Journal of the American Chemical Society
- Publication Type :
- Periodical
- Accession number :
- ejs64289506
- Full Text :
- https://doi.org/10.1021/jacs.3c07984