Journal
NANO ENERGY
Volume 93, Issue -, Pages -Publisher
ELSEVIER
DOI: 10.1016/j.nanoen.2021.106809
Keywords
Photocatalysis; CO2 reduction; ZnIn2S4; ZnS; Interfacial charge transfer; Z-Scheme
Categories
Funding
- Ministry of Science and Technology (MOST) in Taiwan [107-2745-M-002-001-ASP, 108-2119-M-002-030, 109-2123-M-002-004]
- MOST [106-2112-M-008-003-MY3]
- Academia Sinica [AS-iMATE-108-31, AS-SS-106-02-3]
- Center of Atomic Initiative for New Materials (AI-Mat), National Taiwan University [108L9008, 109 L9008]
- Featured Areas Research Center Program within the Ministry of Education (MOE) in Taiwan
- Science and Engineering Research Board (SERB), New Delhi, India [CRG/2021/003355]
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The research successfully prepared a ZnS/ZnIn2S4 heterostructure, achieving high photochemical quantum efficiency by optimizing the Zn:In ratio. Electronic levels and band alignments were deduced from ultraviolet photoemission spectroscopy and UV-Vis. Finally, evidence of the direct Z-scheme and CO2 adsorption during the photocatalytic reaction was verified through various experimental methods.
Employing direct Z-scheme semiconductor heterostructures in photocatalysis offers efficient charge carrier separation and isolation of both redox reactions, thus beneficial to reduce CO2 into solar fuels. Here, a ZnS/ ZnIn2S4 heterostructure, comprising cubic ZnS nanocrystals on hexagonal ZnIn2S4 (ZIS) nanosheets, is successfully fabricated in a single-pot hydrothermal approach. The composite ZnS/ZnIn2S4 exhibits microstrain at its interface with an electric field favorable for Z-scheme. At an optimum ratio of Zn:In (similar to 1:0.5), an excellent photochemical quantum efficiency of around 0.8% is reached, nearly 200-fold boost compared with pristine ZnS. Electronic levels and band alignments are deduced from ultraviolet photoemission spectroscopy and UV-Vis. Evidence of the direct Z-scheme and carrier dynamics is verified by photo-reduction experiment, along with photoluminescence (PL) and time-resolved PL. Finally, diffuse-reflectance infrared Fourier transformed spectroscopy explores the CO2 and related intermediate species adsorbed on the catalyst during the photocatalytic reaction. This microstrain-induced direct Z-scheme approach opens a new pathway for developing nextgeneration photocatalysts for CO2 reduction.
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