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<p>A transfer-free strategy is reported to fabricate FeS<sub>2−x</sub>/graphene heterostructures by direct chemical vapor deposition (CVD) growth of graphene on sapphire followed by sulfurization of a pre-deposited Fe film. We uncover a thickness-dependent phase evolution mechanism, in which graphene acts as a structural template that promotes the preferential formation of sulfur-vacancy-rich FeS<sub>2−x</sub> at an optimal Fe precursor thickness of 10&#xa0;nm. Experimental characterization and mechanistic analysis reveal that these engineered sulfur vacancies-related donor states contribute to n-type doping, improving the apparent optical absorption behavior and increasing the carrier concentration of FeS<sub>2−x</sub>. Furthermore, the sulfur-vacancy-rich interface acts as active charge-transfer centers, amplifying adsorption-induced modulation and facilitating charge transfer upon gas adsorption. As a result, the optimized sensor exhibits competitive room-temperature sensing performance toward NO<sub>2</sub>, featuring a high response of 10.27% to 100 ppb NO<sub>2</sub>, a remarkable calculated detection limit of 1.08 ppb, and rapid response/recovery kinetics. In addition, excellent stability, reproducibility, selectivity, and favorable humidity tolerance are achieved. This work elucidates the synergistic interplay between vacancy engineering and heterointerface modulation in 2D sensing systems and provides a scalable pathway toward advanced high-performance chemiresistive sensors.</p> Graphical abstract <p></p>

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Sulfur vacancy-engineered FeS2−x /graphene heterostructures for ultrasensitive ppb-level NO2 sensing

  • 期刊论文

  • 发表日期：

    2026年7月16日

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  • Hao Yu,
  • Ding Ai,
  • Qi Che,
  • Ziteng Li,
  • Yuting Han,
  • Yanhao Ma,
  • Xin Ji,
  • Hong Zheng,
  • Yonghong Cheng,
  • Chengye Dong

摘要

A transfer-free strategy is reported to fabricate FeS2−x/graphene heterostructures by direct chemical vapor deposition (CVD) growth of graphene on sapphire followed by sulfurization of a pre-deposited Fe film. We uncover a thickness-dependent phase evolution mechanism, in which graphene acts as a structural template that promotes the preferential formation of sulfur-vacancy-rich FeS2−x at an optimal Fe precursor thickness of 10 nm. Experimental characterization and mechanistic analysis reveal that these engineered sulfur vacancies-related donor states contribute to n-type doping, improving the apparent optical absorption behavior and increasing the carrier concentration of FeS2−x. Furthermore, the sulfur-vacancy-rich interface acts as active charge-transfer centers, amplifying adsorption-induced modulation and facilitating charge transfer upon gas adsorption. As a result, the optimized sensor exhibits competitive room-temperature sensing performance toward NO2, featuring a high response of 10.27% to 100 ppb NO2, a remarkable calculated detection limit of 1.08 ppb, and rapid response/recovery kinetics. In addition, excellent stability, reproducibility, selectivity, and favorable humidity tolerance are achieved. This work elucidates the synergistic interplay between vacancy engineering and heterointerface modulation in 2D sensing systems and provides a scalable pathway toward advanced high-performance chemiresistive sensors.

Graphical abstract