Electrocatalytic synthesis of ammonia by surface proton hopping

R. Manabe, H. Nakatsubo, A. Gondo, Kota Murakami, Shuhei Ogo, H. Tsuneki, M. Ikeda, A. Ishikawa, Hiromi Nakai, Yasushi Sekine

Research output: Contribution to journalArticle

22 Citations (Scopus)

Abstract

Highly efficient ammonia synthesis at a low temperature is desirable for future energy and material sources. We accomplished efficient electrocatalytic low-temperature ammonia synthesis with the highest yield ever reported. The maximum ammonia synthesis rate was 30099 μmol gcat -1 h-1 over a 9.9 wt% Cs/5.0 wt% Ru/SrZrO3 catalyst, which is a very high rate. Proton hopping on the surface of the heterogeneous catalyst played an important role in the reaction, revealed by in situ IR measurements. Hopping protons activate N2 even at low temperatures, and they moderate the harsh reaction condition requirements. Application of an electric field to the catalyst resulted in a drastic decrease in the apparent activation energy from 121 kJ mol-1 to 37 kJ mol-1. N2 dissociative adsorption is markedly promoted by the application of the electric field, as evidenced by DFT calculations. The process described herein opens the door for small-scale, on-demand ammonia synthesis.

Original languageEnglish
Pages (from-to)5434-5439
Number of pages6
JournalChemical Science
Volume8
Issue number8
DOIs
Publication statusPublished - 2017

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Ammonia
Protons
Catalysts
Electric fields
Discrete Fourier transforms
Temperature
Activation energy
Adsorption

ASJC Scopus subject areas

  • Chemistry(all)

Cite this

Manabe, R., Nakatsubo, H., Gondo, A., Murakami, K., Ogo, S., Tsuneki, H., ... Sekine, Y. (2017). Electrocatalytic synthesis of ammonia by surface proton hopping. Chemical Science, 8(8), 5434-5439. https://doi.org/10.1039/c7sc00840f

Electrocatalytic synthesis of ammonia by surface proton hopping. / Manabe, R.; Nakatsubo, H.; Gondo, A.; Murakami, Kota; Ogo, Shuhei; Tsuneki, H.; Ikeda, M.; Ishikawa, A.; Nakai, Hiromi; Sekine, Yasushi.

In: Chemical Science, Vol. 8, No. 8, 2017, p. 5434-5439.

Research output: Contribution to journalArticle

Manabe, R, Nakatsubo, H, Gondo, A, Murakami, K, Ogo, S, Tsuneki, H, Ikeda, M, Ishikawa, A, Nakai, H & Sekine, Y 2017, 'Electrocatalytic synthesis of ammonia by surface proton hopping', Chemical Science, vol. 8, no. 8, pp. 5434-5439. https://doi.org/10.1039/c7sc00840f
Manabe R, Nakatsubo H, Gondo A, Murakami K, Ogo S, Tsuneki H et al. Electrocatalytic synthesis of ammonia by surface proton hopping. Chemical Science. 2017;8(8):5434-5439. https://doi.org/10.1039/c7sc00840f
Manabe, R. ; Nakatsubo, H. ; Gondo, A. ; Murakami, Kota ; Ogo, Shuhei ; Tsuneki, H. ; Ikeda, M. ; Ishikawa, A. ; Nakai, Hiromi ; Sekine, Yasushi. / Electrocatalytic synthesis of ammonia by surface proton hopping. In: Chemical Science. 2017 ; Vol. 8, No. 8. pp. 5434-5439.
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