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Oxysulfide photocatalyst for visible-light-driven overall water splitting

Nature Materials volume 18, pages 827–832 (2019)Cite this article

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Abstract

Oxysulfide semiconductors have narrow bandgaps suitable for water splitting under visible-light irradiation, because the electronegative sulfide ions negatively shift the valence band edges of the corresponding oxides1,2. However, the instability of sulfide ions during the water oxidation is a critical obstacle to simultaneous evolution of hydrogen and oxygen3. Here, we demonstrate the activation and stabilization of Y2Ti2O5S2, with a bandgap of 1.9 eV, as a photocatalyst for overall water splitting. On loading of IrO2 and Rh/Cr2O3 as oxygen and hydrogen evolution co-catalysts, respectively, and fine-tuning of the reaction conditions, simultaneous production of stoichiometric amounts of hydrogen and oxygen was achieved on Y2Ti2O5S2 during a 20 h reaction. The discovery of the overall water splitting capabilities of Y2Ti2O5S2 extends the range of promising materials for solar hydrogen production.

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Fig. 1: Structure of Y2Ti2O5S2.
Fig. 2: Morphology of Y2Ti2O5S2.
Fig. 3: Band structure of Y2Ti2O5S2.
Fig. 4: Wavelength dependence of photocatalytic activity of Y2Ti2O5S2.
Fig. 5: Photocatalytic performance of Y2Ti2O5S2 for overall water splitting.

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Data availability

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

Q.W. thanks Y. Kuromiya, K. Kato and M. Yamaguchi at The University of Tokyo for performing ICP-AES and elemental analysis, and assisting with the isotopic labelling experiment. S.S. thanks Z. Song at Anhui University for assisting with the theoretical calculations. This work was financially supported by the Artificial Photosynthesis Project of the New Energy and Industrial Technology Development Organization (NEDO) and a Grant-in-Aid for Scientific Research(A) (no. 16H02417) from the Japan Society for the Promotion of Science. M.N. and N.S. performed work at the Advanced Characterization Nanotechnology Platform of the University of Tokyo, supported through the ‘Nanotechnology Platform’ of the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan.

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  1. Qian Wang

    Present address: Department of Chemistry, University of Cambridge, Cambridge, UK

Authors and Affiliations

  1. Department of Chemical System Engineering, School of Engineering, The University of Tokyo, Tokyo, Japan

    Qian Wang, Zhenhua Pan, Taro Yamada & Kazunari Domen

  2. Institute of Engineering Innovation, The University of Tokyo, Tokyo, Japan

    Mamiko Nakabayashi & Naoya Shibata

  3. Center for Energy & Environmental Science, Shinshu University, Nagano, Japan

    Takashi Hisatomi, Zheng Wang, Tsuyoshi Takata & Kazunari Domen

  4. School of Chemistry and Chemical Engineering, Anhui University, Anhui, China

    Song Sun

  5. National Synchrotron Radiation Laboratory, Collaborative Innovation Center of Chemistry for Energy Materials, University of Science & Technology of China, Anhui, China

    Song Sun

  6. Mitsubishi Chemical Corporation, Yokohama R&D center, Kanagawa, Japan

    Seiji Akiyama

  7. Japan Technological Research Association of Artificial Photosynthetic Chemical Process (ARPChem), Tokyo, Japan

    Seiji Akiyama & Xiong Xiao

  8. Department of Applied Chemistry, School of Science and Technology, Meiji University, Kanagawa, Japan

    Xiong Xiao & Tomoaki Watanabe

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Contributions

Q.W. and K.D. designed the research. Q.W. prepared Y2Ti2O5S2 powder and conducted XRD, DRS, XPS, PESA and SEM characterizations, and the water-splitting reactions. Q.W. and T.Y. carried out the isotopic labelling experiment. M.N. and N.S. conducted cross-sectional cutting of particles along with the STEM, STEM-EDS, TEM-EDS, HRTEM and SAED analyses. S.S. performed the theoretical calculations. S.A. carried out the TG analysis. Q.W. and Z.P. fabricated the electrodes by the particle transfer method and conducted the Mott–Schottky measurements. X.X. and T.W. prepared the electrodes using the roll press method. Z.P. and X.X. carried out the photoelectrochemical measurements. T.Y. supervised the elemental analysis. K.D. and T.H. supervised the experimental work. Q.W., T.H., Z.W., T.Y., T.T. and K.D. discussed the results. Q.W., T.H. and K.D. wrote the manuscript with contributions from the other authors.

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Correspondence to Kazunari Domen.

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Supplementary Information

Supplementary Figs. 1–20, Supplementary Table 1, Supplementary references 1–26

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Wang, Q., Nakabayashi, M., Hisatomi, T. et al. Oxysulfide photocatalyst for visible-light-driven overall water splitting. Nat. Mater. 18, 827–832 (2019). https://doi.org/10.1038/s41563-019-0399-z

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