4.6 Article

Visible light-driven H2O2 synthesis over Au/C3N4: medium-sized Au nanoparticles exhibiting suitable built-in electric fields and inhibiting reverse H2O2 decomposition

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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
卷 24, 期 48, 页码 29557-29569

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ROYAL SOC CHEMISTRY
DOI: 10.1039/d2cp04202a

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This study demonstrates the visible light-driven production of H2O2 by modulating the size of Au nanoparticles. It is found that medium-sized Au particles exhibit the highest catalytic activity. The relationship between particle size and catalytic performance is supported by experimental and theoretical methods, showing that medium-sized Au particles promote photon absorption, enhance O-2 adsorption, and inhibit H2O2 decomposition.
Visible light-driven H2O2 production presents the unique merits of sustainability and environmental friendliness. The size of noble metal nanoparticles (NPs) determines their dispersion and electronic structure and greatly affects their photocatalytic activity. In this work, a series of sized Au NPs over C3N4 were modulated for H2O2 production. The results show that there is a volcanic trend in H2O2 with the decrease of Au particle size, and the highest H2O2 production rate of 1052 mu mol g(-1) h(-1) is obtained from medium-sized Au particles (similar to 8.7 nm). The relationship between structure and catalytic performance is supported by experimental and theoretical methods. (1) First, medium-sized Au NPs promote photon absorption, and have a suitable built-in electric field at the heterojunction, which can be successfully tuned to achieve a more efficient h(+)-e(-) spatial separation. (2) Second, medium-sized Au NPs enhance O-2 adsorption, and create selective 2e(-) O-2 reduction reaction sites. (3) Particularly, medium-sized Au NPs promote the desorption of produced H2O2 and inhibit H2O2 decomposition, finally leading to the highest H2O2 selectivity. Excellent catalytic performance will be obtained by finely optimizing the particle size in a certain range. This work provides a new idea for preparing high efficiently photocatalysts for H2O2 production.

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