文献类型：期刊文献

英文题名：Unveiling the Surface Structure of ZnO Nanorods and H2 Activation Mechanisms with 17O NMR Spectroscopy

作者：Song, Benteng[1,2];Li, Yuhong[7];Wu, Xin-Ping[3];Wang, Fang[1,2];Lin, Ming[4];Sun, Yunhua[1,2];Jia, Ai-ping[5];Ning, Xiang[1,2];Jin, Li[1,2];Ke, Xiaokang[1,2];Yu, Zhiwu[6];Yang, Gang[7];Hou, Wenhua[1,2];Ding, Weiping[1,2];Gong, Xue-Qing[3];Peng, Luming[1,2,8,9]

机构：[1]Nanjing Univ, Sch Chem & Chem Engn, Minist Educ, Key Lab Mesoscop Chem, Nanjing 210023, Peoples R China;[2]Nanjing Univ, Sch Chem & Chem Engn, Collaborat Innovat Ctr Chem Life Sci, Nanjing 210023, Peoples R China;[3]East China Univ Sci & Technol, Res Inst Ind Catalysis, Ctr Computat Chem, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[4]ASTAR, Innovis, Inst Mat Res & Engn IMRE, Singapore 138634, Singapore;[5]Zhejiang Normal Univ, Coll Chem & Life Sci, Key Lab, Minist Educ Adv Catalysis Mat, Jinhua 321004, Peoples R China;[6]Chinese Acad Sci, High Magnet Field Lab, Hefei 230031, Peoples R China;[7]Changshu Inst Technol, Sch Mat Engn, Suzhou Key Lab Funct Ceram Mat, Changshu 215500, Jiangsu, Peoples R China;[8]Nanjing Univ, Jiangsu Key Lab Vehicle Emiss Control, Nanjing 210093, Peoples R China;[9]Nanjing Univ, Frontiers Sci Ctr Crit Earth Mat Cycling FSC CEMa, Nanjing 210023, Jiangsu, Peoples R China

年份：2022

卷号：144

期号：51

起止页码：23340

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20225113265022);WOS:【SCI-EXPANDED(收录号:WOS:000911727500001)】；

基金：This work was supported by National Key R&D Program of China (2021YFA1502803) , the National Natural Science Foundation of China (NSFC) (21972066, 91745202, 21825301, 22003016, and 92145302) , and NSFC-Royal Society Joint Program (21661130149) . The authors thank Dr. F. Blanc and Dr. H. Huo for their help in obtaining the 20.0 T NMR data and Dr. M. Wang for helpful discussions. L.P. thanks the Royal Society and Newton Fund for a Royal Society-Newton Advanced Fellowship. This work was also supported by the Research Funds for the Frontiers Science Center for Critical Earth Material Cycling, Nanjing University, and a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions.

语种：英文

外文关键词：Dissociation - Hydrides - II-VI semiconductors - Nanorods - Nuclear magnetic resonance spectroscopy - Surface reactions - Surface structure - Zinc oxide

摘要：ZnO plays a very important role in many catalytic processes involving H2, yet the details on their interactions and H2 activation mechanism are still missing, owing to the lack of a characterization method that provides resolution at the atomic scale and follows the fate of oxide surface species. Here, we apply 17O solid-state NMR spectroscopy in combination with DFT calculations to unravel the surface structure of ZnO nanorods and explore the H2 activation process. We show that six different types of oxygen ions in the surface and subsurface of ZnO can be distinguished. H2 undergoes heterolytic dissociation on three-coordinated surface zinc and oxygen ions, while the formed hydride species migrate to nearby oxygen species, generating a second hydroxyl site. When oxygen vacancies are present, homolytic dissociation of H2 occurs and zinc hydride species form from the vacancies. Reaction mechanisms on oxide surfaces can be explored in a similar manner.