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Electrocatalytic synthesis of ammonia by surface proton hopping

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 30 099 μmol g(cat) (–1) h(–1) over a...

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Autores principales: Manabe, R., Nakatsubo, H., Gondo, A., Murakami, K., Ogo, S., Tsuneki, H., Ikeda, M., Ishikawa, A., Nakai, H., Sekine, Y.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Royal Society of Chemistry 2017
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5609515/
https://www.ncbi.nlm.nih.gov/pubmed/28970922
http://dx.doi.org/10.1039/c7sc00840f
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author Manabe, R.
Nakatsubo, H.
Gondo, A.
Murakami, K.
Ogo, S.
Tsuneki, H.
Ikeda, M.
Ishikawa, A.
Nakai, H.
Sekine, Y.
author_facet Manabe, R.
Nakatsubo, H.
Gondo, A.
Murakami, K.
Ogo, S.
Tsuneki, H.
Ikeda, M.
Ishikawa, A.
Nakai, H.
Sekine, Y.
author_sort Manabe, R.
collection PubMed
description 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 30 099 μmol g(cat) (–1) h(–1) over a 9.9 wt% Cs/5.0 wt% Ru/SrZrO(3) 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 N(2) 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). N(2) 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.
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spelling pubmed-56095152017-10-02 Electrocatalytic synthesis of ammonia by surface proton hopping Manabe, R. Nakatsubo, H. Gondo, A. Murakami, K. Ogo, S. Tsuneki, H. Ikeda, M. Ishikawa, A. Nakai, H. Sekine, Y. Chem Sci Chemistry 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 30 099 μmol g(cat) (–1) h(–1) over a 9.9 wt% Cs/5.0 wt% Ru/SrZrO(3) 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 N(2) 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). N(2) 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. Royal Society of Chemistry 2017-08-01 2017-06-05 /pmc/articles/PMC5609515/ /pubmed/28970922 http://dx.doi.org/10.1039/c7sc00840f Text en This journal is © The Royal Society of Chemistry 2017 http://creativecommons.org/licenses/by/3.0/ This is an Open Access article distributed under the terms of the Creative Commons Attribution 3.0 Unported License (http://creativecommons.org/licenses/by/3.0/) which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
spellingShingle Chemistry
Manabe, R.
Nakatsubo, H.
Gondo, A.
Murakami, K.
Ogo, S.
Tsuneki, H.
Ikeda, M.
Ishikawa, A.
Nakai, H.
Sekine, Y.
Electrocatalytic synthesis of ammonia by surface proton hopping
title Electrocatalytic synthesis of ammonia by surface proton hopping
title_full Electrocatalytic synthesis of ammonia by surface proton hopping
title_fullStr Electrocatalytic synthesis of ammonia by surface proton hopping
title_full_unstemmed Electrocatalytic synthesis of ammonia by surface proton hopping
title_short Electrocatalytic synthesis of ammonia by surface proton hopping
title_sort electrocatalytic synthesis of ammonia by surface proton hopping
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5609515/
https://www.ncbi.nlm.nih.gov/pubmed/28970922
http://dx.doi.org/10.1039/c7sc00840f
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