The photocatalytic reduction of CO_(2) into value-added chemicals is of great significance for the utilization of carbon resources,but it also faces the problem of low solar energy efficiency and inefficient charge se...The photocatalytic reduction of CO_(2) into value-added chemicals is of great significance for the utilization of carbon resources,but it also faces the problem of low solar energy efficiency and inefficient charge separation.Herein,a CuSCN-loaded CoS_(2) photocatalyst was prepared via a one-pot molten-salt method,and the optimal CO generation rate could reach 289.8μmol g^(−1) h^(−1)(selectivity 92.0%),approximately 32 times that of bare CoS_(2) under a visible-light excitation of λ≥420 nm.In situ X-ray photoelectron spectroscopy(XPS)results indicate that CuSCN acts as a hole acceptor,and photoelectrochemical tests and density functional theory(DFT)calculations demonstrate that CuSCN/CoS_(2) has higher efficiency in the separation and transfer of photogenerated carriers than CoS_(2).CuSCN was proved to be a strong carrier for CO_(2) mass transfer through Brunauer–Emmett–Teller(BET)physical adsorption.Mechanistic studies show that CuSCN/CoS_(2) is more conducive to the conversion of adsorbed CO_(2) into the key reactive intermediate ^(*)COOH,for which the Co sites of CuSCN/CoS_(2) exhibit a lower formation energy,in comparison with CoS_(2) and CuSCN alone.As such,the combined action of CuSCN/CoS_(2) was a synergistic effect that enhances CO_(2) chemisorption and hole transfer,resulting in increased photocatalytic activity for CO_(2) reduction.展开更多
基金supported by the National Natural Science Foundation of China(22366018,5236005,22272034)Key Projects of Jiangxi Provincial Natural Science Foundation(20232ACB203022,20224ACB213010)+3 种基金Jiangxi Province“Double Thousand”Talent Training Plan(jxsq2023201086,jxsq2023102141,jxsq2023102142,jxsq2023102143)Program of Qingjiang Excellent Young Talents,JXUST(JXUSTQJBJ2020005)Jiangxi Provincial Natural Science Foundation(20224BAB203018)Jiangxi Province Graduate Innovation Special Fund Project(YC2022-S659).
文摘The photocatalytic reduction of CO_(2) into value-added chemicals is of great significance for the utilization of carbon resources,but it also faces the problem of low solar energy efficiency and inefficient charge separation.Herein,a CuSCN-loaded CoS_(2) photocatalyst was prepared via a one-pot molten-salt method,and the optimal CO generation rate could reach 289.8μmol g^(−1) h^(−1)(selectivity 92.0%),approximately 32 times that of bare CoS_(2) under a visible-light excitation of λ≥420 nm.In situ X-ray photoelectron spectroscopy(XPS)results indicate that CuSCN acts as a hole acceptor,and photoelectrochemical tests and density functional theory(DFT)calculations demonstrate that CuSCN/CoS_(2) has higher efficiency in the separation and transfer of photogenerated carriers than CoS_(2).CuSCN was proved to be a strong carrier for CO_(2) mass transfer through Brunauer–Emmett–Teller(BET)physical adsorption.Mechanistic studies show that CuSCN/CoS_(2) is more conducive to the conversion of adsorbed CO_(2) into the key reactive intermediate ^(*)COOH,for which the Co sites of CuSCN/CoS_(2) exhibit a lower formation energy,in comparison with CoS_(2) and CuSCN alone.As such,the combined action of CuSCN/CoS_(2) was a synergistic effect that enhances CO_(2) chemisorption and hole transfer,resulting in increased photocatalytic activity for CO_(2) reduction.
