文献类型：期刊文献

英文题名：Atomic Design and Fine-Tuning of Subnanometric Pt Catalysts to Tame Hydrogen Generation

作者：Yang, Jie[1,2];Fu, Wenzhao[3];Chen, Chaoqiu[1];Chen, Wenyao[3];Huang, Wugen[4,5];Yang, Ruoou[6];Kong, Qingqiang[5,7];Zhang, Baiyan[1,2];Zhao, Jixiao[1,2];Chen, Chengmeng[7];Luo, Jun[8,9];Yang, Fan[4];Duan, Xuezhi[3];Jiang, Zheng[6,10];Qin, Yong[1,2]

机构：[1]Chinese Acad Ciences, Inst Coal Chem, State Key Lab Coal Convers, Taiyuan 030001, Peoples R China;[2]Univ Chinese Acad Sci, Ctr Mat Sci & Optoelect Engn, Beijing 100049, Peoples R China;[3]East China Univ Sci & Technol, State Key Lab Chem Engn, Shanghai 200237, Peoples R China;[4]Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China;[5]Univ Chinese Acad Sci, Beijing 100049, Peoples R China;[6]Chinese Acad Sci, Shanghai Adv Res Inst, Zhangjiang Natl Lab, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China;[7]Chinese Acad Sci, CAS Key Lab Carbon Mat, Inst Coal Chem, Taiyuan 030001, Peoples R China;[8]Tianjin Univ Technol, Ctr Electron Microscopy, Sch Mat Sci & Engn, Inst New Energy Mat & Low Carbon Technol, Tianjin 300384, Peoples R China;[9]Tianjin Univ Technol, Tianjin Key Lab Adv Funct Porous Mat, Sch Mat Sci & Engn, Inst New Energy Mat & Low Carbon Technol, Tianjin 300384, Peoples R China;[10]Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai 201800, Peoples R China

年份：2021

卷号：11

期号：7

起止页码：4146

外文期刊名：ACS CATALYSIS

收录：;EI(收录号：20211510199171);WOS:【SCI-EXPANDED(收录号:WOS:000637003700035)】；

基金：The authors acknowledge the financial support from the National Natural Science Foundation of China (21872161, U1832208, and 21673269), the National Science Fund for Distinguished Young Scholars (21825204), the National Key R&D Program of China (2017YFA0700101), and Beijing Key Laboratory of Ionic Liquids Clean Process. EXAFS studies were carried out at the BL14W1 beamline at the Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Shanghai, P. R. China.

语种：英文

外文关键词：subnanocatalyst; size effect; atomic layer deposition; active site structure; hydrogen generation

摘要：The rational synthesis of subnanocatalysts with controllable electronic and atomic structures remains a challenge to break the limits of traditional catalysts. Here, we report the atomic-level precise synthesis of Pt/graphene subnanocatalysts (from single atom and dimer to cluster) by atomic layer deposition, achieved by a high-temperature pulsed ozone strategy to controllably pre-create abundant in-plane epoxy groups on graphene as anchoring sites. The specific in-plane epoxy structure endows the deposited Pt species with uniformity, controllability, and stability. Their size-dependent electronic and geometric effects have been observed for ammonia borane hydrolysis, revealing a volcano-type dependence of intrinsic activity on their sizes. Their active site structures have been identified on the basis of extensive characterizations, dynamic compensation effect, kinetic isotope experiments, and density functional theory simulation. The Pt dimers show the highest catalytic activity and better durability than Pt single atoms and nanoparticles, ascribed to the C-Pt-Pt-O (C5Pt2O, metal-metal bond dimer) active site structure. Our work provides insights into the precise tailoring and catalytic mechanism at the subnanometer level.