文献类型：期刊文献

英文题名：Regulating Atomically-Precise Pt Sites for Boosting Light-Driven Dry Reforming of Methane

作者：He, Chengxuan[1,2];Li, Qixin[1,2];Ye, Zhicheng[3];Wang, Lijie[1,2];Gong, Yalin[1,2];Li, Songting[1,2];Wu, Jiaxin[1,2];Lu, Zhaojun[1,2];Wu, Shiqun[1,2];Zhang, Jinlong[1,2]

机构：[1]East China Univ Sci & Technol, Shanghai Engn Res Ctr Multimedia Environm Catalysi, Key Lab Adv Mat, 130 Meilong Rd, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Sch Chem & Mol Engn, Frontiers Sci Ctr Materiobiol & Dynam Chem,Joint I, 130 Meilong Rd, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, State Key Lab Chem Engn, 130 Meilong Rd, Shanghai 200237, Peoples R China

年份：2024

卷号：63

期号：46

外文期刊名：ANGEWANDTE CHEMIE-INTERNATIONAL EDITION

收录：;EI(收录号：20244117171358);WOS:【SCI-EXPANDED(收录号:WOS:001328342100001)】；

基金：This work was supported by National Key Research and Development Program of China (2022YFE0107900), the National Natural Science Foundation of China (22202070), the Innovation Program of Shanghai Municipal Education Commission (2021-01-07-00-02-E00106), the Science and Technology Commission of Shanghai Municipality (22230780200, 20DZ2250400, 2018SHZDZX03), the Postdoctoral Innovative Talent Support Program (BX20220107), China Postdoctoral Science Foundation (2022M720050), the Shanghai Rising-Star Program (22YF1410200), and Fundamental Research Funds for the Central Universities (222201717003). Thanks to the Shanghai Synchrotron Radiation Facility (SSFR, beamline BL14 W1) and National Synchrotron Radiation Laboratory (NSRL, beamline BL11U) for providing beam time. We sincerely thank Prof. Lingzhi Wang and Dr. Qingqing Zhang for designing and providing the flow-type quartz reactor, which enabled us to conduct naturalsunlight experiments.

语种：英文

外文关键词：Photochemistry; Platinum; Nanoclusters; Carbon dioxide; Methane conversion

摘要：Light-driven dry reforming of methane is a promising and mild route to convert two greenhouse gas into valuable syngas. However, developing facile strategy to atomically-precise regulate the active sites and realize balanced and stable syngas production is still challenging. Herein, we developed a spatial confinement approach to precisely control over platinum species on TiO2 surfaces, from single atoms to nanoclusters. The configuration comprising single atoms and sub-nanoclusters engenders pronounced electronic metal-support interactions, with resultant interfacial states prompting surface charge rearrangement. The unique geometric and electronic properties of these atom-cluster assemblies facilitate effective activation of CH4 and CO2, accelerating intermediate coupling and minimizing side reactions. Our catalyst exhibits an outstanding syngas generation rate of 34.41 mol gPt-1 h-1 with superior durability, displaying high apparent quantum yield of 9.1 % at 365 nm and turnover frequency of 1289 h-1. This work provides insightful understanding for exploring more multi-molecule systems at an atomic scale. The synergistic structure of Pt single atoms and sub-nanoclusters facilitates robust electronic interactions with the substrate, providing an optimal spatial and electronic framework for activating and converting CO2-CH4 molecules. Our catalyst exhibits an outstanding syngas generation rate of 34.41 mol gPt-1 h-1 with superior durability, highlighting the critical role of atomically-precise interface adjustment in multi-molecule systems. image