Twin S-Scheme g-C3N4/CuFe2O4/ZnIn2S4 Heterojunction with a Self-Supporting Three-Phase System for Photocatalytic CO2 Reduction: Mechanism Insight and DFT Calculations

文献类型： 外文期刊

第一作者： Liu, Dongdong

作者： Liu, Dongdong;Jiang, Lipeng;Chen, Dengqian;Hao, Zhengkai;Deng, Bowen;Chen, Limei;Sun, Yunyun;Liu, Huitao;Liu, Xin;Jia, Boyin

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关键词： g-C3N4/CuFe2O4/ZnIn2S4 photocatalyst; twin S-scheme heterojunction; self-supporting three-phase system; photocatalytic CO2 reduction; DFT calculations

期刊名称：ACS CATALYSIS （ 影响因子：12.9； 五年影响因子：13.3 ）

ISSN： 2155-5435

年卷期： 2024 年 14 卷 7 期

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收录情况： SCI

摘要： The use of photocatalytic solar energy to drive CO2 reduction is beneficial for addressing fossil fuel shortages and environmental pollution issues. We synthesized a twin S-scheme g-C3N4/CuFe2O4/ZnIn2S4 heterojunction, which was used to construct a self-supporting three-phase system for photocatalytic CO2 reduction. Two built-in electric fields in this heterojunction induced effective migration of photogenerated carriers, resulting in a wide light response range and strong oxidation ability. This twin S-scheme photocatalytic system without a sacrificial agent had high CH4 selectivity (96.8%) and surprise production rate of CH4 (267.4 mu mol g(-1) h(-1)), and still maintained an excellent cycle rate (249-267.4 mu mol g(-1) h(-1)) during five cycles. In addition, g-C3N4/CuFe2O4/ZnIn2S4 heterojunction possessed both hydrophilicity and hydrophobicity, which achieved an efficient transformation of CO2 into CH4 by controlling interface wettability. g-C3N4 as a hydrophobic layer promoted CO2 mass transfer to achieve the enrichment of CO2 on the heterojunction surface; ZnIn2S4 as a hydrophilic layer could well adsorb H2O, which was further oxidized by the photogenerated holes into many protons (H+). Finally, DFT calculations found that Fe-N bonds located between g-C3N4 and CuFe2O4 played a crucial role during the photocatalytic CO2 reduction. They served as a bridge for electron transfer to induce the bending adsorption of CO2, which enhanced the adsorption of *CO and stabilization of *H.

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