期刊
SMALL
卷 17, 期 31, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/smll.202100496
关键词
band alignment; CZTS; CdS; fuel product selectivity; heat treatment; photoelectrochemical CO; (2) reduction; sulfur vacancies
类别
资金
- Australian Research Council (ARC) Training Centre for the Global Hydrogen Economy [IC200100023]
- Australian Renewable Energy Agency (ARENA) [2017/RND006]
- Australian Research Council (ARC) Future Fellowship Programme [FT190100756]
- Australian Centre for Advanced Photovoltaics (ACAP) postdoctoral fellowship programme [RG172864-B]
Copper-based chalcogenides are considered potential photocathode materials for PEC CO2 reduction due to their photovoltaic performance and band alignment. A heat treatment of Cu2ZnSnS4 (CZTS)/CdS photocathode significantly improves photocurrent density by enhancing charge transfer and band alignment. Tailoring sulfur vacancies through heat treatment in different atmospheres allows for selective CO2 reduction pathways.
Copper-based chalcogenides have been considered as potential photocathode materials for photoelectrochemical (PEC) CO2 reduction due to their excellent photovoltaic performance and favorable conduction band alignment with the CO2 reduction potential. However, they suffer from low PEC efficiency due to the sluggish charge transfer kinetics and poor selectivity, resulting from random CO2 reduction reaction pathways. Herein, a facile heat treatment (HT) of a Cu2ZnSnS4(CZTS)/CdS photocathode is demonstrated to enable significant improvement in the photocurrent density (-0.75 mA cm(-2) at -0.6 V vs RHE), tripling that of pristine CZTS, as a result of the enhanced charge transfer and promoted band alignment originating from the elemental inter-diffusion at the CZTS/CdS interface. In addition, rationally regulated CO2 reduction selectivity toward CO or alcohols can be obtained by tailoring the surficial sulfur vacancies by HT in different atmospheres (air and nitrogen). Sulfur vacancies replenished by O-doping is shown to favor CO adsorption and the C-C coupling pathway, and thereby produce methanol and ethanol, whilst the CdS surface with more S vacancies promotes CO desorption capability with higher selectivity toward CO. The strategy in this work rationalizes the interface charge transfer optimization and surface vacancy engineering simultaneously, providing a new insight into PEC CO2 reduction photocathode design.
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