Tang Kunlin, Wang Zhiqiang, Zou Weixin, Guo Hongyu, Wu Yuchao, Pu Yu, Tong Qing, Wan Haiqin, Gu Xianrui, Dong Lin, Rong Junfeng, Chen Yu-Wen
State Key Laboratory of Pollution Control and Resource Reuse, School of the Environment, School of Chemistry and Chemical Engineering, Center of Modern Analysis, Jiangsu Key Laboratory of Vehicle Emissions Control, Nanjing University, Nanjing 210023, China.
Department of Chemistry, The University of Texas at Austin, Austin, Texas 78712-1224, United States.
ACS Appl Mater Interfaces. 2021 Feb 10;13(5):6219-6228. doi: 10.1021/acsami.0c19233. Epub 2021 Jan 26.
Ir-based heterogeneous catalysts for photocatalytic CO reduction have rarely been reported and are worthy of investigation. In this work, TiO nanosheets with a higher specific surface area and more oxygen vacancies were employed to support Ir metal by impregnation (Imp) and ethylene glycol (EG) reduction methods. In comparison with Ir/TiO (Imp) and TiO, Ir/TiO (EG) exhibited excellent photocatalytic performance toward CO reduction, especially for CH production on account of the oxygen defect of TiO and rich surface hydroxyl groups produced from the interaction between TiO nanosheets and metallic Ir. ESR suggested that the oxygen defect was significant for CO adsorption/activation. Furthermore, metallic Ir was beneficial for photogenerated electron transfer, surface hydroxyl generation, and adsorption of the CO intermediate, generating more available electrons and reducing agents for CH production. CO DRIFTS confirmed the key synergistic interaction between the oxygen defect and metallic Ir in the photoreduction from CO to CH.
用于光催化CO还原的Ir基非均相催化剂鲜有报道,值得研究。在本工作中,采用具有较高比表面积和更多氧空位的TiO纳米片,通过浸渍(Imp)和乙二醇(EG)还原法负载Ir金属。与Ir/TiO(Imp)和TiO相比,Ir/TiO(EG)对CO还原表现出优异的光催化性能,特别是由于TiO的氧缺陷以及TiO纳米片与金属Ir之间相互作用产生的丰富表面羟基,其对CH生成尤为显著。电子自旋共振(ESR)表明氧缺陷对CO吸附/活化具有重要意义。此外,金属Ir有利于光生电子转移、表面羟基生成以及CO中间体的吸附,为CH生成产生更多可用电子和还原剂。CO漫反射红外傅里叶变换光谱(CO DRIFTS)证实了氧缺陷与金属Ir在CO光还原为CH过程中的关键协同作用。