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<p>TiO<sub>2</sub>/BiVO<sub>4</sub> heterojunctions are considered to be one of the most promising materials for photocatalysts due to their extended carrier lifetime, high visible light response, and good stability. However, while Type-II TiO<sub>2</sub>/BiVO<sub>4</sub> heterojunctions are well-studied, the fundamental mechanism behind the Type-I configurations remains unclear, particularly regarding their unexpected high photocatalytic activity despite theoretically unfavorable band alignment. Herein, we reveal that localized polaronic mid-gap states (SP states) can mediate efficient charge transfer and recombination in TiO<sub>2</sub>/BiVO<sub>4</sub> using time-resolved photoluminescence (PL) spectroscopy and transient absorption spectroscopy (TAS), providing direct experimental evidence of this mechanism. The existence of SP states enables exceptional methyl orange degradation efficiency (nearly 100% in 1&#xa0;h under visible light) despite the theoretically unfavorable Type-I alignment. This work redefines the potential of Type-I systems for visible-light photocatalysis by demonstrating how polaron engineering overcomes the limitations of traditional band structures, advancing their applications in solar utilization.</p>

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Unveiling the role of localized polaronic mid-gap states in enhanced carrier transfer in TiO2/BiVO4 heterojunctions under visible light irradiation

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月8日

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  • Zixi Yin,
  • Xingchen Liu,
  • Guijie Liang,
  • Yin Wang

摘要

TiO2/BiVO4 heterojunctions are considered to be one of the most promising materials for photocatalysts due to their extended carrier lifetime, high visible light response, and good stability. However, while Type-II TiO2/BiVO4 heterojunctions are well-studied, the fundamental mechanism behind the Type-I configurations remains unclear, particularly regarding their unexpected high photocatalytic activity despite theoretically unfavorable band alignment. Herein, we reveal that localized polaronic mid-gap states (SP states) can mediate efficient charge transfer and recombination in TiO2/BiVO4 using time-resolved photoluminescence (PL) spectroscopy and transient absorption spectroscopy (TAS), providing direct experimental evidence of this mechanism. The existence of SP states enables exceptional methyl orange degradation efficiency (nearly 100% in 1 h under visible light) despite the theoretically unfavorable Type-I alignment. This work redefines the potential of Type-I systems for visible-light photocatalysis by demonstrating how polaron engineering overcomes the limitations of traditional band structures, advancing their applications in solar utilization.