Ammonia synthesis using a stable electride as an electron donor and reversible hydrogen store

  • Masaaki Kitano
  • , Yasunori Inoue
  • , Youhei Yamazaki
  • , Fumitaka Hayashi
  • , Shinji Kanbara
  • , Satoru Matsuishi
  • , Toshiharu Yokoyama
  • , Sung Wng Kim
  • , Michikazu Hara
  • , Hideo Hosono

Research output: Contribution to journalArticlepeer-review

1327 Scopus citations

Abstract

Industrially, the artificial fixation of atmospheric nitrogen to ammonia is carried out using the Haber-Bosch process, but this process requires high temperatures and pressures, and consumes more than 1% of the world's power production. Therefore the search is on for a more environmentally benign process that occurs under milder conditions. Here, we report that a Ru-loaded electride [Ca 24Al 28O 64] 4+(e -) 4(Ru/C12A7:e -), which has high electron-donating power and chemical stability, works as an efficient catalyst for ammonia synthesis. Highly efficient ammonia synthesis is achieved with a catalytic activity that is an order of magnitude greater than those of other previously reported Ru-loaded catalysts and with almost half the reaction activation energy. Kinetic analysis with infrared spectroscopy reveals that C12A7:e - markedly enhances N 2 dissociation on Ru by the back donation of electrons and that the poisoning of ruthenium surfaces by hydrogen adatoms can be suppressed effectively because of the ability of C12A7:e - to store hydrogen reversibly.

Original languageEnglish
Pages (from-to)934-940
Number of pages7
JournalNature Chemistry
Volume4
Issue number11
DOIs
StatePublished - Nov 2012

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