期刊
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
卷 48, 期 2, 页码 586-599出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.ijhydene.2022.09.277
关键词
Methane photooxidation; FRET; Donor-acceptor (D-A); heterojunction; STF; AQE
Researchers have developed a novel FRET-active ZnO/Ag@Ag4V2O7 hybrid material for promoting the photocatalytic oxidation of methane. This hybrid material enhances the photoredox ability through FRET and has a higher positive potential, facilitating the methane oxidation reaction. Experimental results show that the photocurrent density of this material under visible illumination is 300 times higher than that of the individual materials, and it exhibits good apparent quantum efficiency and solar-to-fuel efficiency.
Direct photoelectrochemical oxidation of methane gas into oxygenates derivatives through pristine photocatalysts is a great challenge. Suitable band potential(eV) energy with a large charge carrier life span is required to break the C-H bond. Herein, a novel Fo euro rster Resonance Energy Transfer (FRET) active ZnO/Ag@Ag4V2O7 hybrid is employed to drive this photoredox reaction. FRET-enabled dipole-dipole charge transfer between ZnO donor and Ag4V2O7 acceptor chromophore for enhancing the photoredox ability of the heterojunction. DFT study also unveils the electronic density defect into ZnO, Zn-s orbital, and V-p orbital of Ag4V2O7 photo center which induces FRET into heterojunction. Meanwhile, LSPR increases the charge density into the heterojunction observed through Pl quenching. The higher positive potential of heterojunction (2.36eV) facilitated the exergonic methane oxidation. The photocurrent density of heterojunction upon visible illumination is found to be 300 times greater than the bare materials. The apparent quantum efficiency for methane photooxidation is found to be 11% along with 1.2 mW/cm2 of power production. The solar to fuel efficiency is more than 13.2% providing an opportunity to oxidise the methane under the ambient environment into energy-rich derivatives along with electricity generation.(c) 2022 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
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