Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature
The development of electrocatalysts capable of efficient reduction of nitrate (NO 3 − ) to ammonia (NH 3 ) is drawing increasing interest for the sake of low carbon emission and environmental protection. Herein, we present a CuCo bimetallic catalyst able to imitate the bifunctional nature of copper-...
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| Published in | Nature communications Vol. 13; no. 1; pp. 7899 - 13 |
|---|---|
| Main Authors | , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
22.12.2022
Nature Publishing Group Nature Portfolio |
| Subjects | |
| Online Access | Get full text |
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| Abstract | The development of electrocatalysts capable of efficient reduction of nitrate (NO
3
−
) to ammonia (NH
3
) is drawing increasing interest for the sake of low carbon emission and environmental protection. Herein, we present a CuCo bimetallic catalyst able to imitate the bifunctional nature of copper-type nitrite reductase, which could easily remove NO
2
−
via the collaboration of two active centers. Indeed, Co acts as an electron/proton donating center, while Cu facilitates NO
x
−
adsorption/association. The bio-inspired CuCo nanosheet electrocatalyst delivers a 100 ± 1% Faradaic efficiency at an ampere-level current density of 1035 mA cm
−2
at −0.2 V
vs
. Reversible Hydrogen Electrode. The NH
3
production rate reaches a high activity of 4.8 mmol cm
−2
h
−1
(960 mmol g
cat
−1
h
−1
). A mechanistic study, using electrochemical in situ Fourier transform infrared spectroscopy and shell-isolated nanoparticle enhanced Raman spectroscopy, reveals a strong synergy between Cu and Co, with Co sites promoting the hydrogenation of NO
3
−
to NH
3
via adsorbed *H species. The well-modulated coverage of adsorbed *H and *NO
3
led simultaneously to high NH
3
selectivity and yield.
Electroreduction of NO
3
−
to NH
3
is drawing increasing interest. Here, the authors designed a CuCo catalyst imitating the bifunctional nature of Cu-type nitrite reductase to deliver an ampere-level current density for NH
3
formation. |
|---|---|
| AbstractList | The development of electrocatalysts capable of efficient reduction of nitrate (NO
3
−
) to ammonia (NH
3
) is drawing increasing interest for the sake of low carbon emission and environmental protection. Herein, we present a CuCo bimetallic catalyst able to imitate the bifunctional nature of copper-type nitrite reductase, which could easily remove NO
2
−
via the collaboration of two active centers. Indeed, Co acts as an electron/proton donating center, while Cu facilitates NO
x
−
adsorption/association. The bio-inspired CuCo nanosheet electrocatalyst delivers a 100 ± 1% Faradaic efficiency at an ampere-level current density of 1035 mA cm
−2
at −0.2 V
vs
. Reversible Hydrogen Electrode. The NH
3
production rate reaches a high activity of 4.8 mmol cm
−2
h
−1
(960 mmol g
cat
−1
h
−1
). A mechanistic study, using electrochemical in situ Fourier transform infrared spectroscopy and shell-isolated nanoparticle enhanced Raman spectroscopy, reveals a strong synergy between Cu and Co, with Co sites promoting the hydrogenation of NO
3
−
to NH
3
via adsorbed *H species. The well-modulated coverage of adsorbed *H and *NO
3
led simultaneously to high NH
3
selectivity and yield.
Electroreduction of NO
3
−
to NH
3
is drawing increasing interest. Here, the authors designed a CuCo catalyst imitating the bifunctional nature of Cu-type nitrite reductase to deliver an ampere-level current density for NH
3
formation. The development of electrocatalysts capable of efficient reduction of nitrate (NO ) to ammonia (NH ) is drawing increasing interest for the sake of low carbon emission and environmental protection. Herein, we present a CuCo bimetallic catalyst able to imitate the bifunctional nature of copper-type nitrite reductase, which could easily remove NO via the collaboration of two active centers. Indeed, Co acts as an electron/proton donating center, while Cu facilitates NO adsorption/association. The bio-inspired CuCo nanosheet electrocatalyst delivers a 100 ± 1% Faradaic efficiency at an ampere-level current density of 1035 mA cm at -0.2 V vs. Reversible Hydrogen Electrode. The NH production rate reaches a high activity of 4.8 mmol cm h (960 mmol g h ). A mechanistic study, using electrochemical in situ Fourier transform infrared spectroscopy and shell-isolated nanoparticle enhanced Raman spectroscopy, reveals a strong synergy between Cu and Co, with Co sites promoting the hydrogenation of NO to NH via adsorbed *H species. The well-modulated coverage of adsorbed *H and *NO led simultaneously to high NH selectivity and yield. Electroreduction of NO3 − to NH3 is drawing increasing interest. Here, the authors designed a CuCo catalyst imitating the bifunctional nature of Cu-type nitrite reductase to deliver an ampere-level current density for NH3 formation. The development of electrocatalysts capable of efficient reduction of nitrate (NO 3 − ) to ammonia (NH 3 ) is drawing increasing interest for the sake of low carbon emission and environmental protection. Herein, we present a CuCo bimetallic catalyst able to imitate the bifunctional nature of copper-type nitrite reductase, which could easily remove NO 2 − via the collaboration of two active centers. Indeed, Co acts as an electron/proton donating center, while Cu facilitates NO x − adsorption/association. The bio-inspired CuCo nanosheet electrocatalyst delivers a 100 ± 1% Faradaic efficiency at an ampere-level current density of 1035 mA cm −2 at −0.2 V vs . Reversible Hydrogen Electrode. The NH 3 production rate reaches a high activity of 4.8 mmol cm −2 h −1 (960 mmol g cat −1 h −1 ). A mechanistic study, using electrochemical in situ Fourier transform infrared spectroscopy and shell-isolated nanoparticle enhanced Raman spectroscopy, reveals a strong synergy between Cu and Co, with Co sites promoting the hydrogenation of NO 3 − to NH 3 via adsorbed *H species. The well-modulated coverage of adsorbed *H and *NO 3 led simultaneously to high NH 3 selectivity and yield. The development of electrocatalysts capable of efficient reduction of nitrate (NO3-) to ammonia (NH3) is drawing increasing interest for the sake of low carbon emission and environmental protection. Herein, we present a CuCo bimetallic catalyst able to imitate the bifunctional nature of copper-type nitrite reductase, which could easily remove NO2- via the collaboration of two active centers. Indeed, Co acts as an electron/proton donating center, while Cu facilitates NOx- adsorption/association. The bio-inspired CuCo nanosheet electrocatalyst delivers a 100 ± 1% Faradaic efficiency at an ampere-level current density of 1035 mA cm-2 at -0.2 V vs. Reversible Hydrogen Electrode. The NH3 production rate reaches a high activity of 4.8 mmol cm-2 h-1 (960 mmol gcat-1 h-1). A mechanistic study, using electrochemical in situ Fourier transform infrared spectroscopy and shell-isolated nanoparticle enhanced Raman spectroscopy, reveals a strong synergy between Cu and Co, with Co sites promoting the hydrogenation of NO3- to NH3 via adsorbed *H species. The well-modulated coverage of adsorbed *H and *NO3 led simultaneously to high NH3 selectivity and yield.The development of electrocatalysts capable of efficient reduction of nitrate (NO3-) to ammonia (NH3) is drawing increasing interest for the sake of low carbon emission and environmental protection. Herein, we present a CuCo bimetallic catalyst able to imitate the bifunctional nature of copper-type nitrite reductase, which could easily remove NO2- via the collaboration of two active centers. Indeed, Co acts as an electron/proton donating center, while Cu facilitates NOx- adsorption/association. The bio-inspired CuCo nanosheet electrocatalyst delivers a 100 ± 1% Faradaic efficiency at an ampere-level current density of 1035 mA cm-2 at -0.2 V vs. Reversible Hydrogen Electrode. The NH3 production rate reaches a high activity of 4.8 mmol cm-2 h-1 (960 mmol gcat-1 h-1). A mechanistic study, using electrochemical in situ Fourier transform infrared spectroscopy and shell-isolated nanoparticle enhanced Raman spectroscopy, reveals a strong synergy between Cu and Co, with Co sites promoting the hydrogenation of NO3- to NH3 via adsorbed *H species. The well-modulated coverage of adsorbed *H and *NO3 led simultaneously to high NH3 selectivity and yield. The development of electrocatalysts capable of efficient reduction of nitrate (NO3−) to ammonia (NH3) is drawing increasing interest for the sake of low carbon emission and environmental protection. Herein, we present a CuCo bimetallic catalyst able to imitate the bifunctional nature of copper-type nitrite reductase, which could easily remove NO2− via the collaboration of two active centers. Indeed, Co acts as an electron/proton donating center, while Cu facilitates NOx− adsorption/association. The bio-inspired CuCo nanosheet electrocatalyst delivers a 100 ± 1% Faradaic efficiency at an ampere-level current density of 1035 mA cm−2 at −0.2 V vs. Reversible Hydrogen Electrode. The NH3 production rate reaches a high activity of 4.8 mmol cm−2 h−1 (960 mmol gcat−1 h−1). A mechanistic study, using electrochemical in situ Fourier transform infrared spectroscopy and shell-isolated nanoparticle enhanced Raman spectroscopy, reveals a strong synergy between Cu and Co, with Co sites promoting the hydrogenation of NO3− to NH3 via adsorbed *H species. The well-modulated coverage of adsorbed *H and *NO3 led simultaneously to high NH3 selectivity and yield.Electroreduction of NO3− to NH3 is drawing increasing interest. Here, the authors designed a CuCo catalyst imitating the bifunctional nature of Cu-type nitrite reductase to deliver an ampere-level current density for NH3 formation. |
| ArticleNumber | 7899 |
| Author | Lou, Yao-Yin Akdim, Ouardia Li, Guang Huang, Xiao-Yang Fang, Jia-Yi Zhao, Kuang-Min Hu, Sheng-Nan Sun, Shi-Gang Zheng, Qi-Zheng |
| Author_xml | – sequence: 1 givenname: Jia-Yi orcidid: 0000-0001-5403-5872 surname: Fang fullname: Fang, Jia-Yi organization: State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University – sequence: 2 givenname: Qi-Zheng orcidid: 0000-0002-9508-5822 surname: Zheng fullname: Zheng, Qi-Zheng organization: State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University – sequence: 3 givenname: Yao-Yin orcidid: 0000-0002-2782-2130 surname: Lou fullname: Lou, Yao-Yin email: yylou@suda.edu.cn organization: State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, School of Chemical and Environmental Engineering, College of Chemistry, Chemical Engineering and Materials Science, Soochow University – sequence: 4 givenname: Kuang-Min orcidid: 0000-0002-5533-6199 surname: Zhao fullname: Zhao, Kuang-Min organization: State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University – sequence: 5 givenname: Sheng-Nan orcidid: 0000-0002-3754-8075 surname: Hu fullname: Hu, Sheng-Nan organization: State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University – sequence: 6 givenname: Guang surname: Li fullname: Li, Guang organization: State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University – sequence: 7 givenname: Ouardia surname: Akdim fullname: Akdim, Ouardia organization: Cardiff Catalysis Institute, School of Chemistry, Cardiff University – sequence: 8 givenname: Xiao-Yang surname: Huang fullname: Huang, Xiao-Yang organization: State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Cardiff Catalysis Institute, School of Chemistry, Cardiff University – sequence: 9 givenname: Shi-Gang orcidid: 0000-0003-2327-4090 surname: Sun fullname: Sun, Shi-Gang email: sgsun@xmu.edu.cn organization: State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/36550156$$D View this record in MEDLINE/PubMed |
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| Snippet | The development of electrocatalysts capable of efficient reduction of nitrate (NO
3
−
) to ammonia (NH
3
) is drawing increasing interest for the sake of low... The development of electrocatalysts capable of efficient reduction of nitrate (NO ) to ammonia (NH ) is drawing increasing interest for the sake of low carbon... The development of electrocatalysts capable of efficient reduction of nitrate (NO3−) to ammonia (NH3) is drawing increasing interest for the sake of low carbon... The development of electrocatalysts capable of efficient reduction of nitrate (NO3-) to ammonia (NH3) is drawing increasing interest for the sake of low carbon... Electroreduction of NO3 − to NH3 is drawing increasing interest. Here, the authors designed a CuCo catalyst imitating the bifunctional nature of Cu-type... |
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| SubjectTerms | 119/118 140/131 140/133 140/146 140/58 147/135 147/28 147/3 639/301/299/886 639/638/161/886 704/172/169/896 Adsorption Ammonia Bimetals Carbon Catalysts Chemical synthesis Copper Current density Electrocatalysts Electrochemistry Environmental protection Fourier transforms Humanities and Social Sciences Hydrogenation Infrared spectroscopy multidisciplinary Nanoparticles Nanosheets Nitrates Nitrite reductase Nitrite Reductases Nitrites Nitrogen dioxide Raman spectroscopy Reductases Science Science (multidisciplinary) Selectivity Spectrum analysis |
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| Title | Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature |
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