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<p>Nanoscale metal/semiconductor heterostructures are critical components for a variety of light energy conversion applications. Herein, with plasmonic hafnium nitride (HfN) as a model system, we show that spinodal decomposition can be exploited as a unique means to produce the lattice-coherent metal/semiconductor heterostructure between HfN and its native oxynitride semiconductor—Hf<sub>2</sub>ON<sub>2</sub>. Atomic-resolution electron microscopy imaging provides direct visualization of the complete lattice coherency over the interface region with precisely controlled spatial modulation. The light-harvesting HfN component exhibits a broadband plasmonic absorption covering visible and near-infrared regions, and the plasmonically excited hot electrons can be efficiently injected into neighboring Hf<sub>2</sub>ON<sub>2</sub> across interface. When combined with a small amount of Pt co-catalyst, the coherent HfN/Hf<sub>2</sub>ON<sub>2</sub> heterostructure achieves high-efficiency photocatalytic H<sub>2</sub> production from methanol decomposition under visible and NIR light illumination, with apparent quantum yields of 27% at 600 nm and 13.9% at 850 nm, respectively. This performance contributes to the efficient utilization of a broad solar spectrum in photocatalysis and solar energy conversion applications.</p>

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Spinodal decomposition enables coherent plasmonic metal/semiconductor heterostructure for full spectrum photocatalysis

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月14日

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  • Lisha Lu,
  • Muhua Sun,
  • Aomiao Zhi,
  • Hao Ling,
  • Yingying Lan,
  • Hongbo Han,
  • Jianlin Wang,
  • Xiaowei Zhang,
  • Yu Zhao,
  • Meiyun Li,
  • Lejuan Cai,
  • Xiaomin Li,
  • Xuedong Bai,
  • Wenlong Wang

摘要

Nanoscale metal/semiconductor heterostructures are critical components for a variety of light energy conversion applications. Herein, with plasmonic hafnium nitride (HfN) as a model system, we show that spinodal decomposition can be exploited as a unique means to produce the lattice-coherent metal/semiconductor heterostructure between HfN and its native oxynitride semiconductor—Hf2ON2. Atomic-resolution electron microscopy imaging provides direct visualization of the complete lattice coherency over the interface region with precisely controlled spatial modulation. The light-harvesting HfN component exhibits a broadband plasmonic absorption covering visible and near-infrared regions, and the plasmonically excited hot electrons can be efficiently injected into neighboring Hf2ON2 across interface. When combined with a small amount of Pt co-catalyst, the coherent HfN/Hf2ON2 heterostructure achieves high-efficiency photocatalytic H2 production from methanol decomposition under visible and NIR light illumination, with apparent quantum yields of 27% at 600 nm and 13.9% at 850 nm, respectively. This performance contributes to the efficient utilization of a broad solar spectrum in photocatalysis and solar energy conversion applications.