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Machine learning-driven molecular dynamics unveils a bulk phase transformation driving ammonia synthesis on barium hydride

Author

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  • Axel Tosello Gardini

    (Italian Institute of Technology
    Universitá di Milano-Bicocca)

  • Umberto Raucci

    (Italian Institute of Technology)

  • Michele Parrinello

    (Italian Institute of Technology)

Abstract

The modern view of industrial heterogeneous catalysis is evolving from the traditional static paradigm where the catalyst merely provides active sites, to that of a functional material in which dynamics plays a crucial role. Using machine learning-driven molecular dynamics simulations, we confirm this picture for the ammonia synthesis catalysed by BaH2. Recent experiments show that this system acts as a highly efficient catalyst, but only when exposed first to N2 and then to H2 in a chemical looping process. Our simulations reveal that when first exposed to N2, BaH2 undergoes a profound change, transforming into a superionic mixed compound, BaH2−2x(NH)x, characterized by a high mobility of both hydrides and imides. This transformation is not limited to the surface but involves the entire catalyst. When this compound is exposed to H2 in the second step of the looping process, ammonia is readily formed and released, a process greatly facilitated by the high ionic mobility. Once all the nitrogen hydrides are hydrogenated, the system reverts to its initial state, ready for the next looping cycle. Our microscopic analysis underlines the dynamic nature of this heterogeneous catalyst, which does not merely serve as static platform for reactions, rather it is a dynamic entity that evolves under reaction conditions.

Suggested Citation

  • Axel Tosello Gardini & Umberto Raucci & Michele Parrinello, 2025. "Machine learning-driven molecular dynamics unveils a bulk phase transformation driving ammonia synthesis on barium hydride," Nature Communications, Nature, vol. 16(1), pages 1-11, December.
  • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-57688-8
    DOI: 10.1038/s41467-025-57688-8
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    1. Christopher M. Goodwin & Patrick Lömker & David Degerman & Bernadette Davies & Mikhail Shipilin & Fernando Garcia-Martinez & Sergey Koroidov & Jette Katja Mathiesen & Raffael Rameshan & Gabriel L. S. , 2024. "Operando probing of the surface chemistry during the Haber–Bosch process," Nature, Nature, vol. 625(7994), pages 282-286, January.
    2. Masaaki Kitano & Shinji Kanbara & Yasunori Inoue & Navaratnarajah Kuganathan & Peter V. Sushko & Toshiharu Yokoyama & Michikazu Hara & Hideo Hosono, 2015. "Electride support boosts nitrogen dissociation over ruthenium catalyst and shifts the bottleneck in ammonia synthesis," Nature Communications, Nature, vol. 6(1), pages 1-9, November.
    3. Wenbo Gao & Jianping Guo & Peikun Wang & Qianru Wang & Fei Chang & Qijun Pei & Weijin Zhang & Lin Liu & Ping Chen, 2018. "Production of ammonia via a chemical looping process based on metal imides as nitrogen carriers," Nature Energy, Nature, vol. 3(12), pages 1067-1075, December.
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