Evolution of multiple spillover hydrogen species on anatase titanium dioxide

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Author(s)Liu, Kairui
Author(s)Hou, Guangjin
Author(s)Gao, Pan
Author(s)Nie, Xuezhong
Author(s)Bai, Shi
Author(s)Janik, Michael J.
Author(s)Zhang, Z. Conrad
Date Accessioned2023-02-16T19:23:35Z
Date Available2023-02-16T19:23:35Z
Publication Date2022-12-21
DescriptionThis article was originally published in Cell Reports Physical Science. The version of record is available at: https://doi.org/10.1016/j.xcrp.2022.101190
AbstractHydrogen spillover is a widespread phenomenon on reducible metal oxide surfaces, with numerous observations confirming its occurrence. However, direct physical characterization of the spillover hydrogen species on an oxide catalyst support remains challenging. Differentiating the binding sites of specific spillover hydrogen species has been elusive. Herein, we vary temperature and reductive conditions, then quench and detect the physicochemical character of three distinct spillover hydrogen species on anatase titanium dioxide (TiO2-A) by deuterium magic-angle-spinning (MAS) nuclear magnetic resonance (NMR) spectroscopy, aided by density functional theory. Fast cooling during the sample preparation is crucial in quenching the spillover deuterium species to enable MAS NMR detection. Energetically favorable spillover deuterium species evolve from deuteron to deuteride states with increasing reduction temperature. Prevailing deuteron species reside on the 2-fold-coordinated O2c site of the TiO2-A (101) surface at low reduction temperature. At high reduction temperature, deuterides residing at oxygen vacancies (Ti6c–D–Ti5c) are formed.
SponsorThis work was supported by the Global Expert program funding of China; National Natural Science Foundation of China no. 21932005, 21721004, and 22172164; DICP I201936; and by the State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences. The 2H MAS NMR measurements at the University of Delaware were made possible by the Delaware COBRE program, supported by a grant from the National Institute of General Medical Sciences (NIGMS) (5 P30 GM110758-02) from the National Institutes of Health.
CitationLiu, Kairui, Guangjin Hou, Pan Gao, Xuezhong Nie, Shi Bai, Michael J. Janik, and Z. Conrad Zhang. “Evolution of Multiple Spillover Hydrogen Species on Anatase Titanium Dioxide.” Cell Reports Physical Science 3, no. 12 (December 21, 2022): 101190. https://doi.org/10.1016/j.xcrp.2022.101190.
ISSN2666-3864
URLhttps://udspace.udel.edu/handle/19716/32307
Languageen_US
PublisherCell Reports Physical Science
Keywordshydrogen spillover
Keywords2H MAS NMR
Keywordsfast cooling
Keywordsoxygen vacancy
Keywordshydride species
KeywordsAnatase titanium oxide
TitleEvolution of multiple spillover hydrogen species on anatase titanium dioxide
TypeArticle
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