Journal
ACS NANO
Volume 13, Issue 7, Pages 8356-8363Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.9b03826
Keywords
defect-mediated hole dynamics; CdS/ZnS nanorods; photocatalyst; type I band alignment; core/mesoporous-shell structure; hydrogen evolution
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Funding
- JSPS KAKENHI [JP16H06520, JP17H05257]
- SENTAN JST
- JSPS [JP17J09073]
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Controlling the carrier dynamics in a semiconductor nanoparticulate photocatalyst is the key to developing catalytic activity. Generally, type I band alignment is unsuitable for photocatalysts because the photoinduced carriers accumulate in the narrow bandgap semiconductor. To avoid the termination of reactions and/or photocorrosion of materials caused by carrier accumulation, it is common to employ type II band alignment for photoenergy conversion systems instead of type I. However, CdS/ZnS core/mesoporous-shell heterostructures show superior photocatalytic activity despite having type I band alignment that is generally unfavorable for photocatalytic reactions. Transient absorption spectroscopy and time-resolved microwave conductivity revealed efficient photoinduced hole transfer from the CdS phase to the ZnS phase. The defect-mediated hole transfer from the CdS to the ZnS phase resulted in long-lived charge separation (>2.4 ms) leading to high photocatalytic performance. This study provides insight into defect-mediated carrier transfer in nanoparticulate photocatalysts, which could be used as a guideline for the design of highly active and stable nanoparticulate photocatalysts.
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