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<p>The simultaneous utilization of methane and carbon dioxide via dry reforming holds promise for sustainable syngas production, yet conventional thermocatalytic processes suffer from energy-intensive operation and catalyst deactivation. Here, we report a light-driven methane dry reforming strategy utilizing sinter-resistant nano-island alloys catalyst, which are dynamically evolved from partially oxidized NiIr nanoclusters anchored on TiO<sub>2</sub> under photoexcitation. In situ characterization reveals interfacial charge oscillations on the catalyst induce a support-Ni-Ir electron transfer pathway, stabilizing oxidized Ni linkages while electronically modulating surface Ir sites. This dual functionality promotes CH<sub>x</sub>O* intermediate formation, suppressing coking during 100-h operation under intermittent illumination. By decoupling photoelectric and photothermal contributions, we demonstrate that localized photogenerated electrons dominate balanced syngas production, whereas photothermal effects enhance molecular vibrations. The optimized catalyst achieves a syngas rate of 10841 mmol g<sub>cat</sub><sup>-1</sup> h<sup>-1</sup> with 25.0% light-to-fuel efficiency, establishing a design paradigm for solar-driven alloy catalysts in greenhouse gas valorization.</p>

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Light-driven restructuring generates nanoisland NiIr alloy for efficient methane dry reforming

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年1月15日

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  • Chengxuan He,
  • Ruijie Yang,
  • Chenggui Zhong,
  • Zhicheng Ye,
  • Yuan Dong,
  • Weihao Chen,
  • Lingyun Chen,
  • Zhihan Wang,
  • Shiqun Wu,
  • Jinlong Zhang

摘要

The simultaneous utilization of methane and carbon dioxide via dry reforming holds promise for sustainable syngas production, yet conventional thermocatalytic processes suffer from energy-intensive operation and catalyst deactivation. Here, we report a light-driven methane dry reforming strategy utilizing sinter-resistant nano-island alloys catalyst, which are dynamically evolved from partially oxidized NiIr nanoclusters anchored on TiO2 under photoexcitation. In situ characterization reveals interfacial charge oscillations on the catalyst induce a support-Ni-Ir electron transfer pathway, stabilizing oxidized Ni linkages while electronically modulating surface Ir sites. This dual functionality promotes CHxO* intermediate formation, suppressing coking during 100-h operation under intermittent illumination. By decoupling photoelectric and photothermal contributions, we demonstrate that localized photogenerated electrons dominate balanced syngas production, whereas photothermal effects enhance molecular vibrations. The optimized catalyst achieves a syngas rate of 10841 mmol gcat-1 h-1 with 25.0% light-to-fuel efficiency, establishing a design paradigm for solar-driven alloy catalysts in greenhouse gas valorization.