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Boosting selective nitrogen reduction to ammonia on electron-deficient copper nanoparticles

Production of ammonia is currently realized by the Haber–Bosch process, while electrochemical N(2) fixation under ambient conditions is recognized as a promising green substitution in the near future. A lack of efficient electrocatalysts remains the primary hurdle for the initiation of potential ele...

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Autores principales: Lin, Yun-Xiao, Zhang, Shi-Nan, Xue, Zhong-Hua, Zhang, Jun-Jun, Su, Hui, Zhao, Tian-Jian, Zhai, Guang-Yao, Li, Xin-Hao, Antonietti, Markus, Chen, Jie-Sheng
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2019
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6763479/
https://www.ncbi.nlm.nih.gov/pubmed/31558716
http://dx.doi.org/10.1038/s41467-019-12312-4
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author Lin, Yun-Xiao
Zhang, Shi-Nan
Xue, Zhong-Hua
Zhang, Jun-Jun
Su, Hui
Zhao, Tian-Jian
Zhai, Guang-Yao
Li, Xin-Hao
Antonietti, Markus
Chen, Jie-Sheng
author_facet Lin, Yun-Xiao
Zhang, Shi-Nan
Xue, Zhong-Hua
Zhang, Jun-Jun
Su, Hui
Zhao, Tian-Jian
Zhai, Guang-Yao
Li, Xin-Hao
Antonietti, Markus
Chen, Jie-Sheng
author_sort Lin, Yun-Xiao
collection PubMed
description Production of ammonia is currently realized by the Haber–Bosch process, while electrochemical N(2) fixation under ambient conditions is recognized as a promising green substitution in the near future. A lack of efficient electrocatalysts remains the primary hurdle for the initiation of potential electrocatalytic synthesis of ammonia. For cheaper metals, such as copper, limited progress has been made to date. In this work, we boost the N(2) reduction reaction catalytic activity of Cu nanoparticles, which originally exhibited negligible N(2) reduction reaction activity, via a local electron depletion effect. The electron-deficient Cu nanoparticles are brought in a Schottky rectifying contact with a polyimide support which retards the hydrogen evolution reaction process in basic electrolytes and facilitates the electrochemical N(2) reduction reaction process under ambient aqueous conditions. This strategy of inducing electron deficiency provides new insight into the rational design of inexpensive N(2) reduction reaction catalysts with high selectivity and activity.
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spelling pubmed-67634792019-09-30 Boosting selective nitrogen reduction to ammonia on electron-deficient copper nanoparticles Lin, Yun-Xiao Zhang, Shi-Nan Xue, Zhong-Hua Zhang, Jun-Jun Su, Hui Zhao, Tian-Jian Zhai, Guang-Yao Li, Xin-Hao Antonietti, Markus Chen, Jie-Sheng Nat Commun Article Production of ammonia is currently realized by the Haber–Bosch process, while electrochemical N(2) fixation under ambient conditions is recognized as a promising green substitution in the near future. A lack of efficient electrocatalysts remains the primary hurdle for the initiation of potential electrocatalytic synthesis of ammonia. For cheaper metals, such as copper, limited progress has been made to date. In this work, we boost the N(2) reduction reaction catalytic activity of Cu nanoparticles, which originally exhibited negligible N(2) reduction reaction activity, via a local electron depletion effect. The electron-deficient Cu nanoparticles are brought in a Schottky rectifying contact with a polyimide support which retards the hydrogen evolution reaction process in basic electrolytes and facilitates the electrochemical N(2) reduction reaction process under ambient aqueous conditions. This strategy of inducing electron deficiency provides new insight into the rational design of inexpensive N(2) reduction reaction catalysts with high selectivity and activity. Nature Publishing Group UK 2019-09-26 /pmc/articles/PMC6763479/ /pubmed/31558716 http://dx.doi.org/10.1038/s41467-019-12312-4 Text en © The Author(s) 2019 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.
spellingShingle Article
Lin, Yun-Xiao
Zhang, Shi-Nan
Xue, Zhong-Hua
Zhang, Jun-Jun
Su, Hui
Zhao, Tian-Jian
Zhai, Guang-Yao
Li, Xin-Hao
Antonietti, Markus
Chen, Jie-Sheng
Boosting selective nitrogen reduction to ammonia on electron-deficient copper nanoparticles
title Boosting selective nitrogen reduction to ammonia on electron-deficient copper nanoparticles
title_full Boosting selective nitrogen reduction to ammonia on electron-deficient copper nanoparticles
title_fullStr Boosting selective nitrogen reduction to ammonia on electron-deficient copper nanoparticles
title_full_unstemmed Boosting selective nitrogen reduction to ammonia on electron-deficient copper nanoparticles
title_short Boosting selective nitrogen reduction to ammonia on electron-deficient copper nanoparticles
title_sort boosting selective nitrogen reduction to ammonia on electron-deficient copper nanoparticles
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6763479/
https://www.ncbi.nlm.nih.gov/pubmed/31558716
http://dx.doi.org/10.1038/s41467-019-12312-4
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