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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| Published in | Nature communications Vol. 9; no. 1; pp. 3485 - 8 |
|---|---|
| Main Authors | , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
28.08.2018
Nature Publishing Group Nature Portfolio |
| Subjects | |
| Online Access | Get full text |
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| Abstract | 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.
Electrochemical reduction of nitrogen is a promising route to industrial-scale nitrogen fixation at ambient conditions, but is challenged by activation of inert nitrogen. Here the authors report a metal-free catalyst that selectively reduces nitrogen to ammonia with high efficiency and stability. |
|---|---|
| AbstractList | 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.
Electrochemical reduction of nitrogen is a promising route to industrial-scale nitrogen fixation at ambient conditions, but is challenged by activation of inert nitrogen. Here the authors report a metal-free catalyst that selectively reduces nitrogen to ammonia with high efficiency and stability. 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–1cat. 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. 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. 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 mg 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. Electrochemical reduction of nitrogen is a promising route to industrial-scale nitrogen fixation at ambient conditions, but is challenged by activation of inert nitrogen. Here the authors report a metal-free catalyst that selectively reduces nitrogen to ammonia with high efficiency and stability. 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-1cat. 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.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-1cat. 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. |
| ArticleNumber | 3485 |
| Author | Cui, Ganglong Tang, Bo Fang, Wei-Hai Xie, Xiao-Ying Qiu, Jianding Sun, Xuping Ren, Xiang Liang, Ruping Ji, Xuqiang Asiri, Abdullah M. Cui, Guanwei Qiu, Weibin |
| Author_xml | – sequence: 1 givenname: Weibin orcidid: 0000-0002-2648-4221 surname: Qiu fullname: Qiu, Weibin organization: Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, College of Chemistry, Nanchang University – sequence: 2 givenname: Xiao-Ying surname: Xie fullname: Xie, Xiao-Ying organization: Key Laboratory of Theoretical and Computational Photochemistry, Ministry of Education, College of Chemistry, Beijing Normal University – sequence: 3 givenname: Jianding orcidid: 0000-0002-6793-9499 surname: Qiu fullname: Qiu, Jianding organization: College of Chemistry, Nanchang University – sequence: 4 givenname: Wei-Hai surname: Fang fullname: Fang, Wei-Hai organization: Key Laboratory of Theoretical and Computational Photochemistry, Ministry of Education, College of Chemistry, Beijing Normal University – sequence: 5 givenname: Ruping surname: Liang fullname: Liang, Ruping organization: College of Chemistry, Nanchang University – sequence: 6 givenname: Xiang surname: Ren fullname: Ren, Xiang organization: Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China – sequence: 7 givenname: Xuqiang surname: Ji fullname: Ji, Xuqiang organization: Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China – sequence: 8 givenname: Guanwei surname: Cui fullname: Cui, Guanwei organization: College of Chemistry, Chemical Engineering and Materials Science, Shandong Normal University – sequence: 9 givenname: Abdullah M. orcidid: 0000-0001-7905-3209 surname: Asiri fullname: Asiri, Abdullah M. organization: Chemistry Department, Faculty of Science and Center of Excellence for Advanced Materials Research, King Abdulaziz University – sequence: 10 givenname: Ganglong surname: Cui fullname: Cui, Ganglong email: ganglong.cui@bnu.edu.cn organization: Key Laboratory of Theoretical and Computational Photochemistry, Ministry of Education, College of Chemistry, Beijing Normal University – sequence: 11 givenname: Bo surname: Tang fullname: Tang, Bo email: tangb@sdnu.edu.cn organization: College of Chemistry, Chemical Engineering and Materials Science, Shandong Normal University – sequence: 12 givenname: Xuping orcidid: 0000-0002-5326-3838 surname: Sun fullname: Sun, Xuping email: xpsun@uestc.edu.cn organization: Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/30154483$$D View this record in MEDLINE/PubMed |
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| ContentType | Journal Article |
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| Snippet | 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 of nitrogen is a promising route to industrial-scale nitrogen fixation at ambient conditions, but is challenged by activation of... |
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| SubjectTerms | 140/131 140/133 140/146 147/135 147/143 639/301/299/161 639/638/77/886 Ammonia Boron Boron carbide Catalysis Catalysts Chemical reduction Density functional theory Electrocatalysts Electrochemistry Humanities and Social Sciences Hydrogen-based energy multidisciplinary Nitrogen Nitrogen fixation Organic chemistry Science Science (multidisciplinary) Stability analysis |
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| Title | High-performance artificial nitrogen fixation at ambient conditions using a metal-free electrocatalyst |
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