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High-performance artificial nitrogen fixation at ambient conditions using a metal-free electrocatalyst

Conversion of naturally abundant nitrogen to ammonia is a key (bio)chemical process to sustain life and represents a major challenge in chemistry and biology. Electrochemical reduction is emerging as a sustainable strategy for artificial nitrogen fixation at ambient conditions by tackling the hydrog...

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Autores principales: Qiu, Weibin, Xie, Xiao-Ying, Qiu, Jianding, Fang, Wei-Hai, Liang, Ruping, Ren, Xiang, Ji, Xuqiang, Cui, Guanwei, Asiri, Abdullah M., Cui, Ganglong, Tang, Bo, Sun, Xuping
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2018
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6113289/
https://www.ncbi.nlm.nih.gov/pubmed/30154483
http://dx.doi.org/10.1038/s41467-018-05758-5
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author Qiu, Weibin
Xie, Xiao-Ying
Qiu, Jianding
Fang, Wei-Hai
Liang, Ruping
Ren, Xiang
Ji, Xuqiang
Cui, Guanwei
Asiri, Abdullah M.
Cui, Ganglong
Tang, Bo
Sun, Xuping
author_facet Qiu, Weibin
Xie, Xiao-Ying
Qiu, Jianding
Fang, Wei-Hai
Liang, Ruping
Ren, Xiang
Ji, Xuqiang
Cui, Guanwei
Asiri, Abdullah M.
Cui, Ganglong
Tang, Bo
Sun, Xuping
author_sort Qiu, Weibin
collection PubMed
description Conversion of naturally abundant nitrogen to ammonia is a key (bio)chemical process to sustain life and represents a major challenge in chemistry and biology. Electrochemical reduction is emerging as a sustainable strategy for artificial nitrogen fixation at ambient conditions by tackling the hydrogen- and energy-intensive operations of the Haber–Bosch process. However, it is severely challenged by nitrogen activation and requires efficient catalysts for the nitrogen reduction reaction. Here we report that a boron carbide nanosheet acts as a metal-free catalyst for high-performance electrochemical nitrogen-to-ammonia fixation at ambient conditions. The catalyst can achieve a high ammonia yield of 26.57 μg h(–1) mg(–1)(cat.) and a fairly high Faradaic efficiency of 15.95% at –0.75 V versus reversible hydrogen electrode, placing it among the most active aqueous-based nitrogen reduction reaction electrocatalysts. Notably, it also shows high electrochemical stability and excellent selectivity. The catalytic mechanism is assessed using density functional theory calculations.
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spelling pubmed-61132892018-08-30 High-performance artificial nitrogen fixation at ambient conditions using a metal-free electrocatalyst Qiu, Weibin Xie, Xiao-Ying Qiu, Jianding Fang, Wei-Hai Liang, Ruping Ren, Xiang Ji, Xuqiang Cui, Guanwei Asiri, Abdullah M. Cui, Ganglong Tang, Bo Sun, Xuping Nat Commun Article Conversion of naturally abundant nitrogen to ammonia is a key (bio)chemical process to sustain life and represents a major challenge in chemistry and biology. Electrochemical reduction is emerging as a sustainable strategy for artificial nitrogen fixation at ambient conditions by tackling the hydrogen- and energy-intensive operations of the Haber–Bosch process. However, it is severely challenged by nitrogen activation and requires efficient catalysts for the nitrogen reduction reaction. Here we report that a boron carbide nanosheet acts as a metal-free catalyst for high-performance electrochemical nitrogen-to-ammonia fixation at ambient conditions. The catalyst can achieve a high ammonia yield of 26.57 μg h(–1) mg(–1)(cat.) and a fairly high Faradaic efficiency of 15.95% at –0.75 V versus reversible hydrogen electrode, placing it among the most active aqueous-based nitrogen reduction reaction electrocatalysts. Notably, it also shows high electrochemical stability and excellent selectivity. The catalytic mechanism is assessed using density functional theory calculations. Nature Publishing Group UK 2018-08-28 /pmc/articles/PMC6113289/ /pubmed/30154483 http://dx.doi.org/10.1038/s41467-018-05758-5 Text en © The Author(s) 2018 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
Qiu, Weibin
Xie, Xiao-Ying
Qiu, Jianding
Fang, Wei-Hai
Liang, Ruping
Ren, Xiang
Ji, Xuqiang
Cui, Guanwei
Asiri, Abdullah M.
Cui, Ganglong
Tang, Bo
Sun, Xuping
High-performance artificial nitrogen fixation at ambient conditions using a metal-free electrocatalyst
title High-performance artificial nitrogen fixation at ambient conditions using a metal-free electrocatalyst
title_full High-performance artificial nitrogen fixation at ambient conditions using a metal-free electrocatalyst
title_fullStr High-performance artificial nitrogen fixation at ambient conditions using a metal-free electrocatalyst
title_full_unstemmed High-performance artificial nitrogen fixation at ambient conditions using a metal-free electrocatalyst
title_short High-performance artificial nitrogen fixation at ambient conditions using a metal-free electrocatalyst
title_sort high-performance artificial nitrogen fixation at ambient conditions using a metal-free electrocatalyst
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6113289/
https://www.ncbi.nlm.nih.gov/pubmed/30154483
http://dx.doi.org/10.1038/s41467-018-05758-5
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