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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...
Autores principales: | , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Royal Society of Chemistry
2017
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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. |
format | Online Article Text |
id | pubmed-5609515 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2017 |
publisher | Royal Society of Chemistry |
record_format | MEDLINE/PubMed |
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
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title_full | Electrocatalytic synthesis of ammonia by surface proton hopping
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title_fullStr | Electrocatalytic synthesis of ammonia by surface proton hopping
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title_full_unstemmed | Electrocatalytic synthesis of ammonia by surface proton hopping
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title_short | Electrocatalytic synthesis of ammonia by surface proton hopping
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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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