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<p>Developing hydrogen sensors with high performances is imperative for facilitating H<sub>2</sub>-related industries. Metal oxide semiconductor (MOS) based gas sensors are simple structures with low cost that are a promising approach for H<sub>2</sub> detection. However, detection speed and selectivity of MOS-based sensors currently face great challenges. Herein, we design palladium single atoms (SAs) doped tin oxide (SnO<sub>2</sub>/Pd<sub>atom</sub>) for H<sub>2</sub> detection. Actual sensing tests show an ultrafast response speed toward H<sub>2</sub> (3s to 10 ppm H<sub>2</sub>), with detection limit of 50 ppb and superior selectivity. Using in-situ THz time-domain spectroscopy and density functional theory calculations, it proves that an extra energy band near Fermi level appeared in SnO<sub>2</sub>/Pd<sub>atom</sub>, and Pd SAs doped on SnO<sub>2</sub> enhance signally concentration of free carrier in SnO<sub>2</sub>/Pd<sub>atom</sub>. Partial density of states reveals that coupling hybridization between Pd 4d orbital and O 2p orbital promotes electron injection from Pd 4d orbital into O π2p orbital, improving production of more O<sup>-</sup> ions on sensing surfaces. Consequentially, the sensing dynamics involving O<sup>-</sup> ions spillover at SnO<sub>2</sub>-Pd<sub>atom</sub> interface is discussed.</p>

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Hydrogen sensing with high-performance via O- ion spillover at Pd single atoms stabilized SnO2 interface

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月4日

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  • Yunxiao Qian,
  • Guorui Zhao,
  • Changming Zhang,
  • Shengjie Yin,
  • Junwei Chen,
  • Yuanyuan Luo,
  • Zhengfeng Huang,
  • Bo Liu,
  • Guotao Duan

摘要

Developing hydrogen sensors with high performances is imperative for facilitating H2-related industries. Metal oxide semiconductor (MOS) based gas sensors are simple structures with low cost that are a promising approach for H2 detection. However, detection speed and selectivity of MOS-based sensors currently face great challenges. Herein, we design palladium single atoms (SAs) doped tin oxide (SnO2/Pdatom) for H2 detection. Actual sensing tests show an ultrafast response speed toward H2 (3s to 10 ppm H2), with detection limit of 50 ppb and superior selectivity. Using in-situ THz time-domain spectroscopy and density functional theory calculations, it proves that an extra energy band near Fermi level appeared in SnO2/Pdatom, and Pd SAs doped on SnO2 enhance signally concentration of free carrier in SnO2/Pdatom. Partial density of states reveals that coupling hybridization between Pd 4d orbital and O 2p orbital promotes electron injection from Pd 4d orbital into O π2p orbital, improving production of more O- ions on sensing surfaces. Consequentially, the sensing dynamics involving O- ions spillover at SnO2-Pdatom interface is discussed.