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Rational design of ZnIn2S4-COF heterojunction to inhibit photogenerated carrier dynamics for enhanced photocatalytic CO2 reduction
Dongdong Liu, Ziqi Tang, Haoyu Wang, Xinjie Li, Jingyang Li, Chao Zhu, Shan Ding, Yuan-sheng Cheng, Hui Zhang, Peipei Li*, Ju Wu*, Guozan Yuan*
https://doi.org/10.1016/j.cjsc.2025.100762
ABSTRACT
Using solar energy to convert CO2 into chemicals presents an economical, environmentally friendly, and sustainable approach. However, single-component photocatalysts exhibit limitations, including a narrow light absorption range, rapid carrier recombination, and weak reduction capabilities. To mitigate charge carrier recombination and enhance reduction efficiency, this study prepared heterojunction photocatalysts by in situ growing Zinc indium sulfide (ZnIn2S4) on a covalent organic framework (COF) substrate. Under visible light irradiation, the 30% ZIS-COF heterojunction demonstrated the highest CO2 reduction performance (1187.2 μmol g-1) and selectivity exceeding 99%, outperforming the single-component system. The electron transfer mechanism and catalytic process were further explored through photoluminescence, time-resolved fluorescence decay spectra, attenuated total reflection Fourier transform infrared spectroscopy, and spin polarized density functional theory calculations. The results reveal that, upon photoexcitation, electrons in the COF migrate to ZnIn2S4 (ZIS), and the efficient flow of photoexcited electrons is facilitated by the intimate interface contact between COF and ZIS. Moreover, the porous structure of the COF promotes CO2 adsorption and enhances mass transfer. This study establishes a versatile platform for developing various hybrid combinations of CO2-reducing metal semiconductors and photosensitizing COF materials, paving the way for enhanced photocatalytic performance.
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