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Inhibiting effect of carbonate on the photoinduced flatband potential shifts during water photooxidation at TiO2/solution interface

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Abstract

The TiO2/solution interfacial junction is of scientific and practical importance in the field of photoelectrochemical water splitting. Illumination of this interface usually induces unwanted positive shifts in the flatband potential of TiO2 photoelectrode. In this paper, the inhibiting effect of carbonate on the flatband potential shifts during water oxidation at the illuminated TiO2/solution interface was investigated in pH 6–14 solutions by using Mott-Schottky measurement technique. The footprints of the photohole trapping at the TiO2 surface were traced. Most significant effects of the carbonate additive on the flatband potential shifts and on the interfacial charge densities of surface-trapped holes (STHs) were observed in pH < 12 near-neutral and weak-basic solutions. Based on a generalized surface-OH oxidation mechanism of water photooxidation, the experimental results were interpreted. Some novel features and/or properties for the photohole transport kinetics, such as the preferential surface-OH sites for initial hole trapping into TiO2 surface, pH- and carbonate-dependent charge density of STHs, and the kinetic rate determining step (RDS), were revealed and discussed by correlating the differentiated long-lived and short-lived STHs with photogenerated surface intermediate species of water oxidation. The results and discussion reported in this work provide new physical insights for understanding the mechanisms of water photooxidation.

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Acknowledgements

Scientific Research Foundation for Young Scientist of Shandong Province (no. BS2011NJ009) and National Natural Science Foundation (no. 21303094) are gratefully acknowledged.

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Authors and Affiliations

  1. Key Laboratory of Life-Organic Analysis of Shandong, Department of Chemistry, Qufu Normal University, Qufu, Shandong, 273165, People’s Republic of China

    Xin Cheng, De-Sheng Kong, Ze Wang, Yuan-Yuan Feng & Wen-Juan Li

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  1. Xin Cheng
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  2. De-Sheng Kong
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  3. Ze Wang
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  4. Yuan-Yuan Feng
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  5. Wen-Juan Li
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Correspondence to De-Sheng Kong.

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Cheng, X., Kong, DS., Wang, Z. et al. Inhibiting effect of carbonate on the photoinduced flatband potential shifts during water photooxidation at TiO2/solution interface. J Solid State Electrochem 21, 1467–1475 (2017). https://doi.org/10.1007/s10008-016-3500-4

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  • DOI: https://doi.org/10.1007/s10008-016-3500-4

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