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<p>Hydrogen extraction from liquid hydrogen carriers is a promising strategy to address hydrogen storage and transportation challenges for a hydrogen economy. We report a novel heterogeneous catalytic architecture, Ni(Mn)-O-P/GaN nanowires, for efficient, selective, and ultra-stable hydrogen evolution from formic acid (FA). The catalyst achieves a high activity of 29.92 mol H<sub>2</sub>·g<sub>cat</sub><sup>−1</sup>·h<sup>−1</sup> with nearly 100% selectivity and a high turnover frequency (TOF) of 31,019.2 h<sup>−1</sup> at 150 °C. It exhibits exceptional stability over 4000 hours under fluctuated temperatures (55-75 °C) with a turnover numbers (TONs) of 5,023,060, integrable with low-grade industrial waste heat. In-situ characterizations, isotope experiments, and density functional theory calculations collectively reveal that the synergy between Ni(Mn)-O-P and GaN are favorable for the O-H dissociation of FA with an interesting H-exchange mechanism with H<sub>2</sub>O while inhibiting the undesired FA dehydration and coking formation. An industrial prototype test validates practical on-demand hydrogen production using waste heat.</p>

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Highly efficient heterogeneous thermal catalysis for noble-metal-free hydrogen production from formic acid

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年12月27日

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  • Liang Qiu,
  • Lin Yao,
  • Ping Wang,
  • Zhiwei Jiang,
  • Jinglin Li,
  • Ying Li,
  • Yixin Li,
  • Zhaosong Wu,
  • Muhammad Salman Nasir,
  • Ding Wang,
  • Xinqiang Wang,
  • Zhen Huang,
  • Baowen Zhou

摘要

Hydrogen extraction from liquid hydrogen carriers is a promising strategy to address hydrogen storage and transportation challenges for a hydrogen economy. We report a novel heterogeneous catalytic architecture, Ni(Mn)-O-P/GaN nanowires, for efficient, selective, and ultra-stable hydrogen evolution from formic acid (FA). The catalyst achieves a high activity of 29.92 mol H2·gcat−1·h−1 with nearly 100% selectivity and a high turnover frequency (TOF) of 31,019.2 h−1 at 150 °C. It exhibits exceptional stability over 4000 hours under fluctuated temperatures (55-75 °C) with a turnover numbers (TONs) of 5,023,060, integrable with low-grade industrial waste heat. In-situ characterizations, isotope experiments, and density functional theory calculations collectively reveal that the synergy between Ni(Mn)-O-P and GaN are favorable for the O-H dissociation of FA with an interesting H-exchange mechanism with H2O while inhibiting the undesired FA dehydration and coking formation. An industrial prototype test validates practical on-demand hydrogen production using waste heat.