Electride support boosts nitrogen dissociation over ruthenium catalyst and shifts the bottleneck in ammonia synthesis

Masaaki Kitano, Shinji Kanbara, Yasunori Inoue, Navaratnarajah Kuganathan, Peter V. Sushko, Toshiharu Yokoyama, Michikazu Hara () and Hideo Hosono ()
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Masaaki Kitano: Materials Research Center for Element Strategy, Tokyo Institute of Technology
Shinji Kanbara: Materials and Structures Laboratory, Tokyo Institute of Technology
Yasunori Inoue: Materials and Structures Laboratory, Tokyo Institute of Technology
Navaratnarajah Kuganathan: University College London
Peter V. Sushko: Fundamental and Computational Sciences Directorate, Pacific Northwest National Laboratory
Toshiharu Yokoyama: Materials Research Center for Element Strategy, Tokyo Institute of Technology
Michikazu Hara: Materials and Structures Laboratory, Tokyo Institute of Technology
Hideo Hosono: Materials Research Center for Element Strategy, Tokyo Institute of Technology

Nature Communications, 2015, vol. 6, issue 1, 1-9

Abstract: Abstract Novel approaches to efficient ammonia synthesis at an ambient pressure are actively sought out so as to reduce the cost of ammonia production and to allow for compact production facilities. It is accepted that the key is the development of a high-performance catalyst that significantly enhances dissociation of the nitrogen–nitrogen triple bond, which is generally considered a rate-determining step. Here we examine kinetics of nitrogen and hydrogen isotope exchange and hydrogen adsorption/desorption reactions for a recently discovered efficient catalyst for ammonia synthesis—ruthenium-loaded 12CaO·7Al2O3 electride (Ru/C12A7:e−)—and find that the rate controlling step of ammonia synthesis over Ru/C12A7:e− is not dissociation of the nitrogen–nitrogen triple bond but the subsequent formation of N–Hn species. A mechanism of ammonia synthesis involving reversible storage and release of hydrogen atoms on the Ru/C12A7:e− surface is proposed on the basis of observed hydrogen absorption/desorption kinetics.

Date: 2015
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DOI: 10.1038/ncomms7731

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