Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 7, Issue 25, Pages 13915-13924Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.5b02641
Keywords
sulfur vacancy; phase junction; visible light photocatalysis; ZnS; first principle DFT
Funding
- National Natural Science Foundation of China [21473031, 21173046, 21203026]
- National Basic Research Program of China (973 Program) [2013CB632405]
- Science & Technology Plan Project of Fujian Province [2014Y2003]
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ZnS is among the superior photocatalysts for H-2 evolution, whereas the wide bandgap restricts its performance to only UV region. Herein, defect engineering and phase junction architecture from a controllable phase transformation enable ZnS to achieve the conflicting visible-light-driven activities for H-2 evolution. On the basis of first-principle density functional theory calculations, electron spin resonance and photoluminescence results, etc., it is initially proposed that the regulated sulfur vacancies in wurtzite phase of ZnS play the key role of photosensitization units for charge generation in visible light and active sites for effective electron utilization. The symbiotic sphalerite-wurtzite phase junctions that dominate the charge-transfer kinetics for photoexciton separation are the indispensable configuration in the present systems. Neither ZnS samples without phase junction nor those without enough sulfur vacancies conduct visible-light photocatalytic H-2 evolution, while the one with optimized phase junctions and maximum sulfur vacancies shows considerable photocatalytic activity. This work will not only contribute to the realization of visible light photocatalysis for wide-bandgap semiconductors but also broaden the vision on the design of highly efficient transition metal sulfide photocatalysts.
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