文献类型：期刊文献

英文题名：Engineering spatially proximate redox sites in Pd-In/TiO2 photocatalyst for selective CO2 photoreduction

作者：Khan, Mazhar[1];Akmal, Zeeshan[1];Tayyab, Muhammad[2];Mansoor, Seemal[1];Zeb, Muhammad Adnan[1];Zeeshan, Amir[3];Khan, Muhammad Mubashir[4];Ye, Ziwei[1];Zhang, Jinlong[1];Wu, Shiqun[1];Wang, Lingzhi[1]

机构：[1]East China Univ Sci & Technol, Inst Fine Chem, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn,Key Lab Adv Mat & Joint Int Re, Shanghai 200237, Peoples R China;[2]Tsinghua Univ, Inst Mat Res, Tsinghua Shenzhen Int Grad Sch, Shenzhen 518055, Guangdong, Peoples R China;[3]Lahore Garrison Univ, Dept Chem, Lahore 54920, Pakistan;[4]Univ Agr Faisalabad, Dept Phys, Faisalabad 38000, Pakistan

年份：2025

卷号：709

外文期刊名：APPLIED SURFACE SCIENCE

收录：;EI(收录号：20252218535905);WOS:【SCI-EXPANDED(收录号:WOS:001504772700001)】；

基金：This study was supported by National Key R & D Program of China (2021YFC2103500) , National Natural Science Foundation of China (22472056 and 22202070) , the Science and Technology Commission of Shanghai Municipality (24ZR1491000) , the Innovation Program of Shanghai Municipal Education Commission (2021-01-07-00-02-E00106) , the Fundamental Research Funds for the Central Universities (222201717003) , the Postdoctoral Innovative Talent Support Program (BX20220107) , the Shanghai Rising-Star Program (22YF1410200) , and the Shanghai Super Postdoctoral Fellow.

语种：英文

外文关键词：Photocatalysis; CO 2 photoreduction; Redox reaction; MOFs

摘要：The synergistic integration of redox reactions in the photocatalyst poses a significant challenge for CO2 photoreduction. Addressing this issue requires the design of spatially proximate redox sites while effectively suppressing charge recombination at these sites. This work offers a pioneering tactic that exploits synergistic redox reactions in close atomic proximity. The deliberate incorporation of palladium and indium into TiO2, where the Pd site assists in hole accumulation, accelerates water dissociation, and generates highly active H* species. Meanwhile, adjacent In sites capture photogenerated electrons from TiO2, producing reactive intermediates by activating CO2. The synergistic incorporation of Pd and In accelerates redox functionality, boosts charge carrier separation, and mitigates recombination at closely situated redox sites. Comprehensive characterizations, including in-situ XPS and FTIR, strengthen these innovative outcomes. The optimized Pd0.5-In1/TiO2 photocatalyst achieves nearly 100 % selectivity of CH4 with a production rate of 30.5 mu mol g-1h- 1 without the use of any sacrificial reagent, demonstrating a 25-fold improvement compared to pristine TiO2. In-situ infrared spectroscopy further validates that the synergistic doping of metal ions promotes the formation of *CH3O and *CHO, key intermediates in the production of CH4. This investigation provides valuable insight into the intricate design of coupled redox active sites.