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<p>Despite the development of the Haber–Bosch process, ammonia synthesis under mild conditions remains challenging due to the high bond energy (945 kJ mol⁻<sup>1</sup>) of the N≡N triple bond. Both thermal- and photocatalytic processes often suffer from the intrinsic scaling relationship between N<sub>2</sub> activation and NH<sub>3</sub> desorption efficiencies. Here we report that the photocatalytic process over an AlFe nanoalloy catalyst provides a promising solution through a photoinduced nitrogen spillover reaction mechanism. Fe acts as the primary active site for N<sub>2</sub> adsorption and dissociation. The transferred photoexcited electrons from Al to Fe enhance N<sub>2</sub> activation. Al serves as a secondary active site, facilitating N spillover from Fe to Al sites under photoexcitation, promoting NH<sub>3</sub> desorption. This dual-site strategy enables an ammonia synthesis rate of 8.6 mmol g<sub>cat</sub><sup>−1</sup> h<sup>−1</sup> at 4.28 W cm<sup>−2</sup> without additional thermal input under ambient pressure. The performance surpasses that of conventional industrial Fe catalysts under thermocatalytic conditions. This study proposes a photoassisted active site modulation strategy for efficient ammonia synthesis catalyst to circumvent scaling relationships.</p><p></p>

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Photoinduced nitrogen spillover enables ammonia synthesis on iron–aluminium dual-site catalysts

  • 期刊论文

  • 发表日期：

    2026年3月2日

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  • Wen-Qian Li,
  • Yijian Chen,
  • Xiaojun Lu,
  • Hui Zhang,
  • Zichuang Li,
  • Kailong Qian,
  • Bo Dai,
  • Ruoqian Jiang,
  • Sijia Zheng,
  • Jiaqi Wang,
  • Xianzheng Zhao,
  • Yangfan Lu,
  • Xiaoning Liu,
  • Zhi Liu,
  • Yanpeng Qi,
  • Bin Zhang,
  • Xin-Hao Li,
  • Jie-Sheng Chen,
  • Tian-Nan Ye

摘要

Despite the development of the Haber–Bosch process, ammonia synthesis under mild conditions remains challenging due to the high bond energy (945 kJ mol⁻1) of the N≡N triple bond. Both thermal- and photocatalytic processes often suffer from the intrinsic scaling relationship between N2 activation and NH3 desorption efficiencies. Here we report that the photocatalytic process over an AlFe nanoalloy catalyst provides a promising solution through a photoinduced nitrogen spillover reaction mechanism. Fe acts as the primary active site for N2 adsorption and dissociation. The transferred photoexcited electrons from Al to Fe enhance N2 activation. Al serves as a secondary active site, facilitating N spillover from Fe to Al sites under photoexcitation, promoting NH3 desorption. This dual-site strategy enables an ammonia synthesis rate of 8.6 mmol gcat−1 h−1 at 4.28 W cm−2 without additional thermal input under ambient pressure. The performance surpasses that of conventional industrial Fe catalysts under thermocatalytic conditions. This study proposes a photoassisted active site modulation strategy for efficient ammonia synthesis catalyst to circumvent scaling relationships.