文献类型：期刊文献

英文题名：Core-Shell MIL-125(Ti)@In2S3 S-Scheme Heterojunction for Boosting CO2 Photoreduction

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

机构：[1]East China Univ Sci & Technol, State Key Lab Green Chem Engn & Ind Catalysis, Key Lab Adv Mat, Joint Int Res Lab Precis Chem & Mol Engn,Feringa N, 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：17

期号：21

起止页码：30895

外文期刊名：ACS APPLIED MATERIALS & INTERFACES

收录：;EI(收录号：20252118452089);WOS:【SCI-EXPANDED(收录号:WOS:001490423400001)】；

基金：This study was supported by the National Key R&D Program of China (2021YFC2103500), the 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), and the Shanghai Rising-Star Program (22YF1410200).

语种：英文

外文关键词：photocatalysis; CO2 photoreduction; S-scheme heterojunction; MOFs

摘要：Heterojunctions based on metal-organic framework (MOF) materials have emerged as promising systems for CO2 photoreduction under sacrificial agent-free conditions. However, the rational design and precise construction of these heterostructures remain significant challenges. In this study, we report the development of a core-shell heterojunction via the in situ growth of In2S3 nanosheets on MIL-125(Ti) for efficient CO2 photoreduction. Comprehensive characterization elucidates strong interfacial interactions and substantial work function mismatches between MIL-125(Ti) and In2S3, which drive the formation of a robust interfacial electric field (IEF) and facilitate the establishment of an S-scheme heterojunction. The S-scheme heterojunction retains the strong oxidative and reductive potentials of its components, promoting efficient charge separation and transfer. In situ infrared spectroscopy provides evidence that the formation of the S-scheme heterojunction significantly enhances the production of critical intermediates essential for the CO2 reduction process. Moreover, density functional theory calculations reveal that the heterojunction construction significantly facilitates CO2 activation and lowers the energy barrier. The optimized MT-2@IS achieves an exceptional CH4 production rate of 27.65 mu mol g(-1) h(-1) without the use of photosensitizers or sacrificial agents, representing 27-fold and 8.9-fold improvements compared to pristine MIL-125(Ti) and In2S3. This work provides valuable insights into the design of MOF-based heterojunctions and establishes a robust framework for advancing CO2 photoreduction technologies.