铜价态对TiO基异质结光催化剂导带位置及还原选择性的影响。
Effect of Cu valence states on conduction band position and reduction selectivity of TiO-based heterojunction photocatalysts.
作者信息
Qian Hong, Yuan Binxia, Liu Yuhao, Wang Li, Zhu Rui, Dong Pengyu
机构信息
College of Energy and Mechanical Engineering, Shanghai University of Electric Power, Shanghai 201306, P.R. China.
Key Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province, Yancheng Institute of Technology, Yancheng 224051, P.R. China.
出版信息
iScience. 2025 May 19;28(6):112697. doi: 10.1016/j.isci.2025.112697. eCollection 2025 Jun 20.
TiO has low photocatalytic activity due to its easy recombination of photogenerated charges and low visible light utilization efficiency. This study utilized the keto-enol tautomerism principle of fructose in an alkaline environment to successfully obtain CuO/TiO (CT), CuO/TiO/Cu (CTC), and TiO/Cu (TC) catalysts. As Cu(I) transformed into Cu(0), the bandgap narrowed, significantly enhancing visible light absorption. Photocatalytic tests showed that CT-0.15 exhibited the highest hydrogen production rate (279.53 μmol g h), which was 25.18 times higher than that of TC-2. However, CTC-1 had the highest CO production rate (10.58 μmol g h). Optoelectronic test revealed that CT-0.15 and CTC-1 had higher separation efficiency of photogenerated exciton. Density functional theory (DFT) calculations indicated that the change in the valence state of Cu influenced the reaction mechanism, with CT being favorable for the adsorption of H in HER and CTC promoting the adsorption of CO in carbon dioxide reduction reaction (CO2RR).
由于光生电荷易于复合且可见光利用效率低，TiO的光催化活性较低。本研究利用果糖在碱性环境中的酮 - 烯醇互变异构原理，成功获得了CuO/TiO（CT）、CuO/TiO/Cu（CTC）和TiO/Cu（TC）催化剂。随着Cu（I）转变为Cu（0），带隙变窄，显著增强了可见光吸收。光催化测试表明，CT - 0.15表现出最高的产氢速率（279.53 μmol g⁻¹ h⁻¹），比TC - 2高25.18倍。然而，CTC - 1具有最高的CO产率（10.58 μmol g⁻¹ h⁻¹）。光电测试表明，CT - 0.15和CTC - 1具有更高的光生激子分离效率。密度泛函理论（DFT）计算表明，Cu价态的变化影响了反应机理，CT有利于析氢反应（HER）中H的吸附，而CTC促进了二氧化碳还原反应（CO2RR）中CO的吸附。
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