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    Hydrogen-Bond Network Promotes Water Splitting on the TiO2 Surface
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    • Xiaochuan Ma
      Xiaochuan Ma
      Hefei National Research Center for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China
      More by Xiaochuan Ma
      Orcidhttps://orcid.org/0000-0002-9936-1927
    • Yongliang Shi
      Yongliang Shi
      Center for Spintronics and Quantum Systems, State Key Laboratory for Mechanical Behavior of Materials, School of Materials Science and Engineering, Xi’an Jiaotong University, Xi’an, Shaanxi 710049, China
      More by Yongliang Shi
    • Jianyi Liu
      Jianyi Liu
      Hefei National Research Center for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China
      More by Jianyi Liu
    • Xintong Li
      Xintong Li
      Hefei National Research Center for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China
      More by Xintong Li
    • Xuefeng Cui
      Xuefeng Cui
      Hefei National Research Center for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China
      Hefei National Laboratory, University of Science and Technology of China, Hefei 230088, China
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    • Shijing Tan*
      Shijing Tan
      Hefei National Research Center for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China
      Hefei National Laboratory, University of Science and Technology of China, Hefei 230088, China
      *E-mail: [email protected]
      More by Shijing Tan
      Orcidhttps://orcid.org/0000-0002-8537-9528
    • Jin Zhao*
      Jin Zhao
      Hefei National Research Center for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China
      ICQD/Hefei National Research Center for Physical Sciences at the Microscale, and CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, and Department of Physics, University of Science and Technology of China, Hefei, Anhui 230026, China
      *E-mail: [email protected]
      More by Jin Zhao
      Orcidhttps://orcid.org/0000-0003-1346-5280
    • Bing Wang*
      Bing Wang
      Hefei National Research Center for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026, China
      Hefei National Laboratory, University of Science and Technology of China, Hefei 230088, China
      *E-mail: [email protected]
      More by Bing Wang
      Orcidhttps://orcid.org/0000-0002-2953-2196
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2022, 144, 30, 13565–13573
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    https://doi.org/10.1021/jacs.2c03690
    Published July 19, 2022
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    Abstract

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    Breaking the strong covalent O–H bond of an isolated H2O molecule is difficult, but it can be largely facilitated when the H2O molecule is connected with others through hydrogen-bonding. How a hydrogen-bond network forms and performs becomes crucial for water splitting in natural photosynthesis and artificial photocatalysis and is awaiting a microscopic and spectroscopic understanding at the molecular level. At the prototypical photocatalytic H2O/anatase-TiO2(001)-(1×4) interface, we report the hydrogen-bond network can promote the coupled proton and hole transfer for water splitting. The formation of a hydrogen-bond network is controlled by precisely tuning the coverage of water to above one monolayer. Under ultraviolet (UV) light irradiation, the hydrogen-bond network opens a cascaded channel for the transfer of a photoexcited hole, concomitant with the release of the proton to form surface hydroxyl groups. The yielded hydroxyl groups provide excess electrons to the TiO2 surface, causing the reduction of Ti4+ to Ti3+ and leading to the emergence of gap states, as monitored by in situ UV/X-ray photoelectron spectroscopy. The density functional theory calculation reveals that the water splitting becomes an exothermic process through hole oxidation with the assistance of the hydrogen-bond network. In addition to the widely concerned exotic activity from photocatalysts, our study demonstrates the internal hydrogen-bond network, which is ubiquitous at practical aqueous/catalyst interfaces, is also indispensable for water splitting.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.2c03690.

    • Sample preparation; UPS, XPS, ARPES, and STM measurements; DFT calculation details; full and zoom-in UPS spectral features; work function change with H2O adsorption; temperature-dependent adsorption of water at the anatase-TiO2(001)-(1×4) surface; XPS peak fitting of O 1s spectra at the anatase-TiO2(001) surface; extracting the 1π and 3σ contributions of hydroxyl groups in UPS spectra; lattice distortion around OHb at the terrace sites; 3a1 peak splitting in 2D energy-momentum space; additional STM images of H2O at the anatase-TiO2(001)-(1×4) surface obtained at 80 K; proposed H2O configurations and adsorption energies; AIMD simulations; energy change of the transition state and split state by injecting holes; calculated total and partial DOS for valence bands of the anatase-TiO2(001)-(1×4) surface (PDF)

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