Boosting photocatalytic CO2 reduction in a ZnS/ZnIn2S4 heterostructure through strain-induced direct Z-scheme and a mechanistic study of molecular CO2 interaction thereon
- Citation:
- Sabbah, A, Shown I, Qorbani M, Fu F-Y, Lin T-Y, Wu H-L, Chung P-W, Wu C-I, Santiago SRM, Shen J-L, Chen K-H, Chen L-C. 2022. Boosting photocatalytic CO2 reduction in a ZnS/ZnIn2S4 heterostructure through strain-induced direct Z-scheme and a mechanistic study of molecular CO2 interaction thereon, 2022. Nano Energy. 93:106809.
Abstract:
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 (~ 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 next-generation photocatalysts for CO2 reduction.
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