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, Hideo Hosono

Research output: Contribution to journalArticlepeer-review

536 Citations (Scopus)
110 Downloads (Pure)

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·7Al 2 O 3 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-H n 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.

Original languageEnglish
Article number6731
Number of pages9
JournalNature Communications
Volume6
DOIs
Publication statusPublished - 30 Mar 2015
Externally publishedYes

Bibliographical note

CC-BY This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/

ASJC Scopus subject areas

  • Chemistry(all)
  • Biochemistry, Genetics and Molecular Biology(all)
  • Physics and Astronomy(all)

Fingerprint

Dive into the research topics of 'Electride support boosts nitrogen dissociation over ruthenium catalyst and shifts the bottleneck in ammonia synthesis'. Together they form a unique fingerprint.

Cite this