Facile dissociation of molecular nitrogen using lanthanide surfaces: Towards ambient temperature ammonia synthesis

J. R. Chan, S. G. Lambie, H. J. Trodahl, D. Lefebvre, M. Le Ster, A. Shaib, F. Ullstad, S. A. Brown, B. J. Ruck, A. L. Garden, and F. Natali
Phys. Rev. Materials 4, 115003 – Published 30 November 2020
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Abstract

A combined experimental and computational study is reported on a hitherto unrecognised single lanthanide catalyst for the breaking of molecular nitrogen and formation of ammonia at ambient temperature and low pressure. We combine in situ electrical conductance and electron diffraction measurements to track the conversion from the lanthanide metals to the insulating lanthanide nitrides. The efficiency of the conversion is then interpreted using DFT+U calculations, suggesting a molecular nitrogen dissociation pathway separate from that well established for transition metals. Finally, we show that exposure of the lanthanide surfaces to both molecular nitrogen and hydrogen results in the formation of ammonia.

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  • Received 7 May 2020
  • Revised 22 September 2020
  • Accepted 29 October 2020

DOI:https://doi.org/10.1103/PhysRevMaterials.4.115003

©2020 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

J. R. Chan1,*, S. G. Lambie2, H. J. Trodahl1, D. Lefebvre1, M. Le Ster3, A. Shaib1, F. Ullstad1, S. A. Brown3, B. J. Ruck1, A. L. Garden2, and F. Natali1,†

  • 1The MacDiarmid Institute for Advanced Materials and Nanotechnology, School of Chemical and Physical Sciences, Victoria University of Wellington, PO Box 600, Wellington, New Zealand
  • 2The MacDiarmid Institute for Advanced Materials and Nanotechnology, Department of Chemistry, University of Otago, P.O. Box 56, Dunedin 9054, New Zealand
  • 3The MacDiarmid Institute for Advanced Materials and Nanotechnology, School of Physical and Chemical Sciences, University of Canterbury, Private Bag 4800, Christchurch 8140, New Zealand

  • *Jay.Chan@vuw.ac.nz
  • Franck.Natali@vuw.ac.nz

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Issue

Vol. 4, Iss. 11 — November 2020

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