Tailoring Antibonding-Orbital Occupancy State of Selenium in Se-Enriched ReSe_(2+x) Cocatalyst for Exceptional H_2 Evolution of TiO_2 Photocatalyst

Duoduo Gao; Haoyu Long; Xuefei WangJiaguo YuHuogen Yu

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Tailoring Antibonding-Orbital Occupancy State of Selenium in Se-Enriched ReSe_(2+x) Cocatalyst for Exceptional H_2 Evolution of TiO_2 Photocatalyst

机译：Tailoring Antibonding-Orbital Occupancy State of Selenium in Se-Enriched ReSe_(2+x) Cocatalyst for Exceptional H_2 Evolution of TiO_2 Photocatalyst

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Electron density regulation of active sites can realize an optimal hydrogenbindingstrength, whereas the underlying regulation mechanism is still indistinct.Herein, a new concept of antibonding-orbital occupancy state is firstproposed to unveil the fundamental influence mechanism of electron densityon the Se-H_(ads) bond strength for achieving first-rank adsorption energytoward atomic hydrogen by constructing Se-enriched surrounding to formelectron-deficient Se~((2-δ)-) active sites in ReSe_(2+x) nanodots. To this end, the SerichReSe_(2+x) nanodots (0.3-1 nm) can be dexterously fabricated onto the TiO_2to prepare Se-rich ReSe_(2+x)/TiO_2 by an ingenious one-step photosynthesisroute. In a surprise, a large number of visual H_2 bubbles are continuouslyproduced on the resultant ReSe_(2+x)/TiO_2(0.7 wt.) with an ultrahigh rate of12 490.4 μmol h~(?1) g~(?1) and an apparent quantum efficiency of 60.0, whichis 5.0 times higher than that of traditional ReSe2/TiO_2, even comparablewith benchmark Pt/TiO_2(0.7 wt.). In situ/ex situ XPS characterizationscoupled with density functional theory (DFT) calculations corroborate that aSe-enriched environment can induce the formation of electron-deficientSe~((2-δ)?) and then reduce its antibonding-orbital occupancy state, thusincreasing the stability of H 1s-p antibonding and accordingly reinforcing theSe-H_(ads) bonds. This holistic study identifies the dominant role of antibondingorbitaloccupancy states in the optimization of hydrogen-binding energy.

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来源
《Advanced functional materials》 |2023年第6期|2209994.1-2209994.10|共10页
作者
Duoduo Gao; Haoyu Long; Xuefei WangJiaguo YuHuogen Yu;
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作者单位

State Key Laboratory of Silicate Materials for Architectures and School of Chemistry Chemical Engineering and Life Science Wuhan University of Technology Wuhan 430070, P. R. China;

Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China University of Geosciences Wuhan 430074, P. R. China;

State Key Laboratory of Silicate Materials for Architectures and School of Chemistry Chemical Engineering and Life Science Wuhan University of Technology Wuhan 430070, P. R. China,Laboratory of Solar Fuel Faculty of Materials Science and Chemistry China U;

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antibonding-orbital occupancy states; cocatalysts; electron-deficient Se; H-binding strength; photocatalyses;

Tailoring Antibonding-Orbital Occupancy State of Selenium in Se-Enriched ReSe_(2+x) Cocatalyst for Exceptional H_2 Evolution of TiO_2 Photocatalyst

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