Single Mo Atom Supported on Defective Boron Nitride Monolayer as an Efficient Electrocatalyst for Nitrogen Fixation: A Computational Study
The production of ammonia (NH3) from molecular dinitrogen (N2) under mild conditions is one of the most attractive and challenging processes in chemistry. Here by means of density functional theory (DFT) computations, we systematically investigated the potential of single transition metal atoms (Sc...
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| Published in | Journal of the American Chemical Society Vol. 139; no. 36; pp. 12480 - 12487 |
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| Main Authors | , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
13.09.2017
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| Subjects | |
| Online Access | Get full text |
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| Abstract | The production of ammonia (NH3) from molecular dinitrogen (N2) under mild conditions is one of the most attractive and challenging processes in chemistry. Here by means of density functional theory (DFT) computations, we systematically investigated the potential of single transition metal atoms (Sc to Zn, Mo, Ru, Rh, Pd, and Ag) supported on the experimentally available defective boron nitride (TM–BN) monolayer with a boron monovacancy as a N2 fixation electrocatalyst. Our computations revealed that the single Mo atom supported by a defective BN nanosheet exhibits the highest catalytic activity for N2 fixation at room temperature through an enzymatic mechanism with a quite low overpotential of 0.19 V. The high spin-polarization, selective stabilization of N2H* species, or destabilizing NH2* species are responsible for the high activity of the Mo-embedded BN nanosheet for N2 fixation. This finding opens a new avenue of NH3 production by single-atom electrocatalysts under ambient conditions. |
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| AbstractList | The production of ammonia (NH
) from molecular dinitrogen (N
) under mild conditions is one of the most attractive and challenging processes in chemistry. Here by means of density functional theory (DFT) computations, we systematically investigated the potential of single transition metal atoms (Sc to Zn, Mo, Ru, Rh, Pd, and Ag) supported on the experimentally available defective boron nitride (TM-BN) monolayer with a boron monovacancy as a N
fixation electrocatalyst. Our computations revealed that the single Mo atom supported by a defective BN nanosheet exhibits the highest catalytic activity for N
fixation at room temperature through an enzymatic mechanism with a quite low overpotential of 0.19 V. The high spin-polarization, selective stabilization of N
H* species, or destabilizing NH
* species are responsible for the high activity of the Mo-embedded BN nanosheet for N
fixation. This finding opens a new avenue of NH
production by single-atom electrocatalysts under ambient conditions. The production of ammonia (NH₃) from molecular dinitrogen (N₂) under mild conditions is one of the most attractive and challenging processes in chemistry. Here by means of density functional theory (DFT) computations, we systematically investigated the potential of single transition metal atoms (Sc to Zn, Mo, Ru, Rh, Pd, and Ag) supported on the experimentally available defective boron nitride (TM–BN) monolayer with a boron monovacancy as a N₂ fixation electrocatalyst. Our computations revealed that the single Mo atom supported by a defective BN nanosheet exhibits the highest catalytic activity for N₂ fixation at room temperature through an enzymatic mechanism with a quite low overpotential of 0.19 V. The high spin-polarization, selective stabilization of N₂H* species, or destabilizing NH₂* species are responsible for the high activity of the Mo-embedded BN nanosheet for N₂ fixation. This finding opens a new avenue of NH₃ production by single-atom electrocatalysts under ambient conditions. The production of ammonia (NH3) from molecular dinitrogen (N2) under mild conditions is one of the most attractive and challenging processes in chemistry. Here by means of density functional theory (DFT) computations, we systematically investigated the potential of single transition metal atoms (Sc to Zn, Mo, Ru, Rh, Pd, and Ag) supported on the experimentally available defective boron nitride (TM-BN) monolayer with a boron monovacancy as a N2 fixation electrocatalyst. Our computations revealed that the single Mo atom supported by a defective BN nanosheet exhibits the highest catalytic activity for N2 fixation at room temperature through an enzymatic mechanism with a quite low overpotential of 0.19 V. The high spin-polarization, selective stabilization of N2H* species, or destabilizing NH2* species are responsible for the high activity of the Mo-embedded BN nanosheet for N2 fixation. This finding opens a new avenue of NH3 production by single-atom electrocatalysts under ambient conditions.The production of ammonia (NH3) from molecular dinitrogen (N2) under mild conditions is one of the most attractive and challenging processes in chemistry. Here by means of density functional theory (DFT) computations, we systematically investigated the potential of single transition metal atoms (Sc to Zn, Mo, Ru, Rh, Pd, and Ag) supported on the experimentally available defective boron nitride (TM-BN) monolayer with a boron monovacancy as a N2 fixation electrocatalyst. Our computations revealed that the single Mo atom supported by a defective BN nanosheet exhibits the highest catalytic activity for N2 fixation at room temperature through an enzymatic mechanism with a quite low overpotential of 0.19 V. The high spin-polarization, selective stabilization of N2H* species, or destabilizing NH2* species are responsible for the high activity of the Mo-embedded BN nanosheet for N2 fixation. This finding opens a new avenue of NH3 production by single-atom electrocatalysts under ambient conditions. The production of ammonia (NH3) from molecular dinitrogen (N2) under mild conditions is one of the most attractive and challenging processes in chemistry. Here by means of density functional theory (DFT) computations, we systematically investigated the potential of single transition metal atoms (Sc to Zn, Mo, Ru, Rh, Pd, and Ag) supported on the experimentally available defective boron nitride (TM–BN) monolayer with a boron monovacancy as a N2 fixation electrocatalyst. Our computations revealed that the single Mo atom supported by a defective BN nanosheet exhibits the highest catalytic activity for N2 fixation at room temperature through an enzymatic mechanism with a quite low overpotential of 0.19 V. The high spin-polarization, selective stabilization of N2H* species, or destabilizing NH2* species are responsible for the high activity of the Mo-embedded BN nanosheet for N2 fixation. This finding opens a new avenue of NH3 production by single-atom electrocatalysts under ambient conditions. |
| Author | Zhao, Jingxiang Chen, Zhongfang |
| AuthorAffiliation | Department of Chemistry Harbin Normal University University of Puerto Rico Key Laboratory of Photonic and Electronic Bandgap Materials, Ministry of Education, and College of Chemistry and Chemical Engineering |
| AuthorAffiliation_xml | – name: Harbin Normal University – name: Department of Chemistry – name: University of Puerto Rico – name: Key Laboratory of Photonic and Electronic Bandgap Materials, Ministry of Education, and College of Chemistry and Chemical Engineering |
| Author_xml | – sequence: 1 givenname: Jingxiang orcidid: 0000-0001-6023-8887 surname: Zhao fullname: Zhao, Jingxiang email: xjz_hmily@163.com organization: Harbin Normal University – sequence: 2 givenname: Zhongfang orcidid: 0000-0002-1445-9184 surname: Chen fullname: Chen, Zhongfang email: zhongfangchen@gmail.com organization: University of Puerto Rico |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/28800702$$D View this record in MEDLINE/PubMed |
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| ContentType | Journal Article |
| Copyright | Copyright © 2017 American Chemical Society |
| Copyright_xml | – notice: Copyright © 2017 American Chemical Society |
| DBID | AAYXX CITATION NPM 7X8 7S9 L.6 |
| DOI | 10.1021/jacs.7b05213 |
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| Snippet | The production of ammonia (NH3) from molecular dinitrogen (N2) under mild conditions is one of the most attractive and challenging processes in chemistry. Here... The production of ammonia (NH ) from molecular dinitrogen (N ) under mild conditions is one of the most attractive and challenging processes in chemistry. Here... The production of ammonia (NH₃) from molecular dinitrogen (N₂) under mild conditions is one of the most attractive and challenging processes in chemistry. Here... |
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| SubjectTerms | ambient temperature ammonia boron boron nitride catalytic activity density functional theory molybdenum nanosheets nitrogen nitrogen fixation palladium rhodium ruthenium scandium silver zinc |
| Title | Single Mo Atom Supported on Defective Boron Nitride Monolayer as an Efficient Electrocatalyst for Nitrogen Fixation: A Computational Study |
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