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

Nature Synthesis (2026)Cite this article

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Abstract

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.

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Fig. 1: Schematic of reaction mechanisms for ammonia synthesis.
Fig. 2: Preparation and structural characterizations of AlFe/Al.
Fig. 3: Catalytic performance of AlFe/Al for ammonia synthesis.
Fig. 4: Electronic structures of AlFe/Al catalyst for N2 activation.
Fig. 5: Photoinduced N spillover mechanism.
Fig. 6: Mechanism of photoexcited NHx formation and desorption.

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The data supporting the findings of this study are available within the article and its Supplementary Information. Source data are provided with this paper.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (grant nos. 22275121 and 92580124), the National Key R&D Program of China (grant nos. 2023YFA1506300 and 2023YFB4005201), Shanghai Municipal Science and Technology Major Project, Shanghai Municipal Education Commission (grant no. 2024AIYB007), and Fundamental Research Funds for the Central Universities (grant nos. 23×010301599 and 24×010301678). We thank the Shanghai Synchrotron Radiation Facility of BL02B01 (31124.02.SSRF.BL02B01) for the assistance on NAP-XPS measurements.

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  1. These authors contributed equally: Wen-Qian Li, Yijian Chen, Xiaojun Lu.

Authors and Affiliations

  1. Frontiers Science Center for Transformative Molecules, State Key Laboratory of Polyolefins and Catalysis, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Shanghai, China

    Wen-Qian Li, Xiaojun Lu, Zichuang Li, Kailong Qian, Bo Dai, Ruoqian Jiang, Sijia Zheng, Jiaqi Wang, Xin-Hao Li, Jie-Sheng Chen & Tian-Nan Ye

  2. College of Materials Science and Engineering, National Engineering Research Center for Mg Alloys, National Key Laboratory of Advanced Casting Technologies, National Innovation Center for Industry-Education Integration of Energy Storage Technology, Chongqing University, Chongqing, China

    Yijian Chen, Xianzheng Zhao & Yangfan Lu

  3. Chongqing Institute of New Energy Storage Materials and Equipment, Chongqing, China

    Yijian Chen, Xianzheng Zhao & Yangfan Lu

  4. Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, China

    Hui Zhang

  5. School of Physical Science and Technology, ShanghaiTech University, Shanghai, China

    Xiaoning Liu, Zhi Liu & Yanpeng Qi

  6. Institute of Modern Physics, Fudan University, Shanghai, China

    Bin Zhang

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Contributions

T.-N.Y. conceived the idea and directed the project. J.-S.C. supervised the project. W.-Q.L. designed the experiments and conducted most of the synthetic experiments. Y.C., Y.L. and X.-H.L. performed the DFT calculations. X. Lu and J.W. helped conduct in situ FTIR. H.Z., X. Liu and Z. Liu helped perform NAP-XPS measurements. Z. Li provided acquired XPS data. K.Q. and B.D. helped perform the TPD measurements. R.J. and S.Z. provided assistance with XAS data acquisition and analysis. X.Z. provided Rietveld refinement analysis of XRD patterns. Y.Q. helped conduct magnetization measurements. B.Z. provided assistance with the Mössbauer spectra data. T.-N.Y. and W.-Q.L. cowrote the paper. All authors revised and approved the paper.

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Correspondence to Hui Zhang, Yangfan Lu or Tian-Nan Ye.

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Nature Synthesis thanks Laura Collado, Zhenyu Sun and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. Primary Handling Editor: Alexandra Groves, in collaboration with the Nature Synthesis team.

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Li, WQ., Chen, Y., Lu, X. et al. Photoinduced nitrogen spillover enables ammonia synthesis on iron–aluminium dual-site catalysts. Nat. Synth (2026). https://doi.org/10.1038/s44160-026-01013-8

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