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An Unusual Strong Visible‐Light Absorption Band in Red Anatase TiO2 Photocatalyst Induced by Atomic Hydrogen‐Occupied Oxygen Vacancies
Authors:Yongqiang Yang  Li‐Chang Yin  Yue Gong  Ping Niu  Jian‐Qiang Wang  Lin Gu  Xingqiu Chen  Gang Liu  Lianzhou Wang  Hui‐Ming Cheng
Affiliation:1. Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang, China;2. Laboratory for Advanced Materials & Electron Microscopy, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing, China;3. Key Laboratory of Interfacial Physics and Technology and Shanghai Synchrotron Radiation Facility, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai, China;4. School of Materials Science and Engineering, University of Science and Technology of China, Shenyang, China;5. Nanomaterials Centre, School of Chemical Engineering and AIBN, The University of Queensland, St Lucia, Brisbane, QLD, Australia;6. Low‐Dimensional Material and Device Laboratory, Tsinghua‐Berkeley Shenzhen Institute, Tsinghua University, Shenzhen, China;7. Center of Excellence in Environmental Studies, King Abdulaziz University, Jeddah, Saudi Arabia
Abstract:Increasing visible light absorption of classic wide‐bandgap photocatalysts like TiO2 has long been pursued in order to promote solar energy conversion. Modulating the composition and/or stoichiometry of these photocatalysts is essential to narrow their bandgap for a strong visible‐light absorption band. However, the bands obtained so far normally suffer from a low absorbance and/or narrow range. Herein, in contrast to the common tail‐like absorption band in hydrogen‐free oxygen‐deficient TiO2, an unusual strong absorption band spanning the full spectrum of visible light is achieved in anatase TiO2 by intentionally introducing atomic hydrogen‐mediated oxygen vacancies. Combining experimental characterizations with theoretical calculations reveals the excitation of a new subvalence band associated with atomic hydrogen filled oxygen vacancies as the origin of such band, which subsequently leads to active photo‐electrochemical water oxidation under visible light. These findings could provide a powerful way of tailoring wide‐bandgap semiconductors to fully capture solar light.
Keywords:atomic hydrogen  oxygen vacancies  photocatalysts  red TiO2  visible light
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