Journal
NANO LETTERS
Volume 19, Issue 2, Pages 1234-1241Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.8b04768
Keywords
Solar water splitting; hydrogen fuel; graphene; interfacial interaction; interfacial charge transfer; dual-band-gap systems
Categories
Funding
- National Natural Science Foundation of China [21422303, 21573049, 21872043, 81602643]
- National Key R&D Program nanotechnology special focus [2016YFA0201600]
- Beijing Natural Science Foundation [2142036]
- Knowledge Innovation Program, Youth Innovation Promotion Association
- Special Program of One Belt One Road of CAS
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Dual-band-gap systems are promising for solar water splitting due to their excellent light-harvesting capability and high charge-separation efficiency. However, a fundamental understanding of interfacial charge-transfer behavior in the dual-band-gap configuration is still incomplete. Taking CdS/reduced graphene oxide (CdS/RGO) nanoheterojunctions as a model solar water splitting system, we attempt here to highlight the interaction-dependent interfacial charge-transfer behavior based on both experimental observations and theoretical calculations. Experimental evidence points to charge transfer at the CdS-RGO interface playing a dominant role in the photocatalytic hydrogen production activity. By tuning the degree of reduction of RGO, the interfacial interaction, and, thereby, the charge transfer can be controlled at the CdS-RGO interface. This observation is supported by theoretical analysis, where we find that the interfacial charge transfer is a balance between the effective single-electron- and hole-transfer probability and the surface free electron and hole concentration, both of which are related to the surface potential and tailored by interfacial interaction. This mechanism is applicable to all systems for solar water splitting, providing a useful guidance for the design and study of heterointerfaces for high-efficiency energy conversion.
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