文献类型：期刊文献

英文题名：Interactions of Oxide Surfaces with Water Revealed with Solid-State NMR Spectroscopy

作者：Chen, Junchao[4,5];Hope, Michael A.[3];Lin, Zhiye[4,5];Wang, Meng[6];Liu, Tao[3];Halat, David M.[3];Wen, Yujie[4,5];Chen, Teng[4,5];Ke, Xiaokang[4,5];Magusin, Pieter C. M. M.[3];Ding, Weiping[4,5];Xia, Xifeng[7];Wu, Xin-Ping[1,2];Gong, Xue-Qing[1,2,5];Grey, Clare P.[3];Peng, Luming[4,5]

机构：[1]East China Univ Sci & Technol, Ctr Computat Chem, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China;[3]Univ Cambridge, Dept Chem, Cambridge CB2 1EW, England;[4]Nanjing Univ, Key Lab Mesoscop Chem MOE, Sch Chem & Chem Engn, Nanjing 210023, Peoples R China;[5]Nanjing Univ, Collaborat Innovat Ctr Chem Life Sci, Sch Chem & Chem Engn, Nanjing 210023, Peoples R China;[6]Peking Univ, Coll Chem & Mol Engn CCME, Beijing 100871, Peoples R China;[7]Nanjing Univ Sci & Technol, Anal & Testing Ctr, Nanjing 210094, Peoples R China

年份：2020

卷号：142

期号：25

起止页码：11173

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20202808904813);WOS:【SCI-EXPANDED(收录号:WOS:000543780500034)】；

基金：This work was supported by the National Natural Science Foundation of China (NSFC) (21972066, 91745202, 21573103, and 21421004), NSFC.Royal Society Joint Program (21661130149), the Fundamental Research Funds for the Central Universities (1124020512), and National Science Fund for Talent Training in Basic Science (J1103310). Xin-Ping Wu thanks the Research Start-up Fund for Distinguished Research Fellow at East China University of Science and Technology (ECUST) under award no. YJ0142208. The ECUST group thanks the Programme of Introducing Talents of Discipline to Universities (B16017). Luming Peng thanks the Royal Society and Newton Fund for a Royal Society.Newton Advanced Fellowship. Clare P. Grey thanks the European Research Council for an Advanced Fellowship. This work was also supported by a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions. Michael A. Hope thanks the Oppenheimer Foundation for funding. David M. Halat acknowledges the Cambridge International Trust for funding and is grateful for support from NECCES, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under award no. DE-SC0012583. We thank Dr. Subhradip Paul in the University of Nottingham for invaluable discussions and help in this work.

语种：英文

外文关键词：Ions - Nanorods - Molecules - Oxygen - Hydration - Nuclear magnetic resonance spectroscopy - Density functional theory - Light polarization

摘要：Hydrous materials are ubiquitous in the natural environment and efforts have previously been made to investigate the structures and dynamics of hydrated surfaces for their key roles in various chemical and physical applications, with the help of theoretical modeling and microscopy techniques. However, an overall atomic-scale understanding of the water-solid interface, including the effect of water on surface ions, is still lacking. Herein, we employ ceria nanorods with different amounts of water as an example and demonstrate a new approach to explore the water-surface interactions by using solid-state NMR in combination with density functional theory. NMR shifts and relaxation time analysis provide detailed information on the local structure of oxygen ions and the nature of water motion on the surface: the amount of molecularly adsorbed water decreases rapidly with increasing temperature (from room temperature to 150 degrees C), whereas hydroxyl groups are stable up to 150 degrees C, and dynamic water molecules are found to instantaneously coordinate to the surface oxygen ions. The applicability of dynamic nuclear polarization for selective detection of surface oxygen species is also compared to conventional NMR with surface selective isotopic-labeling: the optimal method depends on the feasibility of enrichment and the concentration of protons in the sample. These results provide new insight into the interfacial structure of hydrated oxide nanostructures, which is important to improve performance for various applications.