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<p>Achieving efficient carrier separation in transition-metal-oxide semiconductors is crucial for their applications in optoelectronic and catalytic devices. However, the substantial disparity in mobility between holes and electrons heavily limits device performance. Here we develop a general strategy for enhancing hole mobility via reducing their effective mass through metal vacancy (V<sub>M</sub>) management. The introduction of V<sub>M</sub> yields remarkable improvements in hole mobility: 430% for WO<sub>3</sub>, 350% for TiO<sub>2</sub> and 270% for Bi<sub>2</sub>O<sub>3</sub>. To illustrate the importance of this finding, we applied the V<sub>M</sub> concept to photoelectrochemical water splitting, where efficient carrier separation is highly coveted. In particular, V<sub>M</sub>-WO<sub>3</sub> achieves a 4.4-fold enhancement in photo-to-current efficiency, yielding a performance of 4.8 mA cm<sup>−2</sup> for both small- and large-scale photoelectrodes with exceptional stability for over 120 h.</p><p></p>

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Metal vacancies in semiconductor oxides enhance hole mobility for efficient photoelectrochemical water splitting

  • 期刊论文

  • 发表日期：

    2025年2月25日

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  • Jun Wang,
  • Kang Liu,
  • Wanru Liao,
  • Yicui Kang,
  • Hanrui Xiao,
  • Yingkang Chen,
  • Qiyou Wang,
  • Tao Luo,
  • Jiawei Chen,
  • Hongmei Li,
  • Ting-Shan Chan,
  • Shanyong Chen,
  • Evangelina Pensa,
  • Liyuan Chai,
  • Fangyang Liu,
  • Liangxing Jiang,
  • Changxu Liu,
  • Junwei Fu,
  • Emiliano Cortés,
  • Min Liu

摘要

Achieving efficient carrier separation in transition-metal-oxide semiconductors is crucial for their applications in optoelectronic and catalytic devices. However, the substantial disparity in mobility between holes and electrons heavily limits device performance. Here we develop a general strategy for enhancing hole mobility via reducing their effective mass through metal vacancy (VM) management. The introduction of VM yields remarkable improvements in hole mobility: 430% for WO3, 350% for TiO2 and 270% for Bi2O3. To illustrate the importance of this finding, we applied the VM concept to photoelectrochemical water splitting, where efficient carrier separation is highly coveted. In particular, VM-WO3 achieves a 4.4-fold enhancement in photo-to-current efficiency, yielding a performance of 4.8 mA cm−2 for both small- and large-scale photoelectrodes with exceptional stability for over 120 h.