In:
Environmental Science: Nano, Royal Society of Chemistry (RSC), Vol. 9, No. 6 ( 2022), p. 1996-2005
Abstract:
Ammonia (NH 3 ) is one of the fundamental pillars of the chemical industry nowadays. Compared with the traditional Haber–Bosch process that requires high energy consumption, the photocatalytic conversion of N 2 to NH 3 under mild conditions is recognized as a sustainable and environmentally-friendly technology. However, the photocatalytic breakage of the NN bond in nitrogen (N 2 ) is a kinetically difficult process. Here, based on density functional theory (DFT) calculations, we report a novel and viable strategy to markedly boost the photocatalytic nitrogen fixation efficiency of InVO 4 by tailoring its oxygen vacancies (V O ). InVO 4 containing constructed V O (V O -InVO 4 ) shows enhanced ammonia production rate, which can be attributed to the promoted N 2 adsorption, improved N 2 activation and decreased reaction barriers on the InVO 4 surface, as evidenced by DFT simulations. Remarkably, the NH 3 yield rate of the optimal V O -InVO 4 achieves up to 139.03 μmol g cat −1 h −1 , which is 5.33 times higher than that of InVO 4 without additional V O fabrication. The introduction of V O largely suppresses the photogenerated charge carrier recombination and enhances visible light utilization, as revealed by photoluminescence and UV-vis absorption spectra, respectively, which correlate well with simulations. Notably, the low-valence V 4+ induced by V O is a more favorable active reaction site for N 2 adsorption, as revealed by the simulation results. This study not only provides a simple yet robust strategy to craft catalysts of high efficiency for photocatalysis, but also expands the mechanistic understanding about defect-mediated catalysis.
Type of Medium:
Online Resource
ISSN:
2051-8153
,
2051-8161
Language:
English
Publisher:
Royal Society of Chemistry (RSC)
Publication Date:
2022
detail.hit.zdb_id:
2758235-8
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