文献类型：期刊文献

英文题名：Integration of CO2 activation and photogenerated electron accumulation at Ti site via dual-tandem electric fields in BiOBr-MIL-125 heterojunction for boosting CO2 photoreduction

作者：Khan, Mazhar[1];Akmal, Zeeshan[1];Tayyab, Muhammad[2];Mansoor, Seemal[1];Liu, Dongni[1];Ye, Ziwei[1];Zhang, Jinlong[1];Wu, Shiqun[1];Wang, Lingzhi[1]

机构：[1]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Key Lab Adv Mat,Joint Int Res Lab Precis Chem & Mo, Shanghai 200237, Peoples R China;[2]Tsinghua Univ, Inst Mat Res, Tsinghua Shenzhen Int Grad Sch, Shenzhen 518055, Guangdong, Peoples R China

年份：2025

卷号：370

外文期刊名：APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY

收录：;EI(收录号：20250817909803);WOS:【SCI-EXPANDED(收录号:WOS:001431623000001)】；

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 Shanghai Rising-Star Program (22YF1410200) .

语种：英文

外文关键词：Photocatalysis; CO 2 photoreduction; Heterojunction; MOFs

摘要：The rational design of heterojunction photocatalysts is crucial for enhancing CO2 photoreduction efficiency, yet precisely channeling photogenerated electrons to the CO2 adsorption sites remains an enormous challenge. In this work, we developed an organic-inorganic heterostructure with continuous inter- and intra-component electric fields. The integration of BiOBr with MIL-125 via chemical bonding established a heterojunction, where the built-in electric field between the two components facilitated the efficient transfer of photogenerated electrons from BiOBr to MIL-125. The intrinsic electric field of MIL-125 further drove the accumulation of photogenerated electrons at Ti sites. This tandem electric field effect, in conjunction with the CO2 adsorption and activation at Ti sites, significantly enhanced the efficiency of CO2 reduction within the heterojunction system. The optimized photocatalyst achieving CO production at a rate of 65.6 mu mol g- 1 h- 1 with nearly 90 % selectivity without the use of sacrificial agents, exhibiting a remarkable 43-fold and 8-fold enhancement in activity compared to pristine MIL-125 and BiOBr, respectively. In-situ infrared spectroscopy and theoretical calculations confirmed the energy optimization effect of the heterostructure on CO2 activation and the hydrogenation reaction, facilitating the formation of the key intermediate *COOH. This work elucidates the mechanism by which tandem built-in electric fields facilitate charge separation.