High-efficiency electrochemical nitrate reduction to ammonia via boron-doped hydroxyl oxide cobalt induced electron delocalization
[Display omitted] Electrochemical nitrate reduction to ammonia is a promising alternative strategy for producing valuable ammonia. This prospective route, however, is subject to a slow electrocatalytic rate, which resulted from the weak adsorption and activation of intermediate species, and the low...
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| Published in | Journal of colloid and interface science Vol. 676; pp. 560 - 568 |
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| Main Authors | , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
Elsevier Inc
15.12.2024
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| Subjects | |
| Online Access | Get full text |
| ISSN | 0021-9797 1095-7103 1095-7103 |
| DOI | 10.1016/j.jcis.2024.07.160 |
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| Abstract | [Display omitted]
Electrochemical nitrate reduction to ammonia is a promising alternative strategy for producing valuable ammonia. This prospective route, however, is subject to a slow electrocatalytic rate, which resulted from the weak adsorption and activation of intermediate species, and the low density electron cloud of active centers. To address this issue, we developed a novel approach by doping boron into metal hydroxyl oxides to adjust the electronic structure of active centers, and consequently, led a significant improvement in the Faraday efficiency upto approaching 100 %, as well as an impressive ammonia yield upto approximately 23 mg/h mgcat−1 at −0.6 V vs. reversible hydrogen electrode (RHE). Experimental data in mechanism demonstrate that the doped boron play a crucial role in modulating the local electronic environment surrounding the active sites Co. In situ Raman and FTIR spectra provide evidences that boron facilitates the formation of deoxidation and hydrogenation intermediates. Additionally, density functional theory (DFT) calculations support the notion that boron doping enhances the adsorption capability of intermediates, reduces the reaction barrier, and facilitates the desorption of NH3. |
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| AbstractList | [Display omitted]
Electrochemical nitrate reduction to ammonia is a promising alternative strategy for producing valuable ammonia. This prospective route, however, is subject to a slow electrocatalytic rate, which resulted from the weak adsorption and activation of intermediate species, and the low density electron cloud of active centers. To address this issue, we developed a novel approach by doping boron into metal hydroxyl oxides to adjust the electronic structure of active centers, and consequently, led a significant improvement in the Faraday efficiency upto approaching 100 %, as well as an impressive ammonia yield upto approximately 23 mg/h mgcat−1 at −0.6 V vs. reversible hydrogen electrode (RHE). Experimental data in mechanism demonstrate that the doped boron play a crucial role in modulating the local electronic environment surrounding the active sites Co. In situ Raman and FTIR spectra provide evidences that boron facilitates the formation of deoxidation and hydrogenation intermediates. Additionally, density functional theory (DFT) calculations support the notion that boron doping enhances the adsorption capability of intermediates, reduces the reaction barrier, and facilitates the desorption of NH3. Electrochemical nitrate reduction to ammonia is a promising alternative strategy for producing valuable ammonia. This prospective route, however, is subject to a slow electrocatalytic rate, which resulted from the weak adsorption and activation of intermediate species, and the low density electron cloud of active centers. To address this issue, we developed a novel approach by doping boron into metal hydroxyl oxides to adjust the electronic structure of active centers, and consequently, led a significant improvement in the Faraday efficiency upto approaching 100 %, as well as an impressive ammonia yield upto approximately 23 mg/h mgcat⁻¹ at −0.6 V vs. reversible hydrogen electrode (RHE). Experimental data in mechanism demonstrate that the doped boron play a crucial role in modulating the local electronic environment surrounding the active sites Co. In situ Raman and FTIR spectra provide evidences that boron facilitates the formation of deoxidation and hydrogenation intermediates. Additionally, density functional theory (DFT) calculations support the notion that boron doping enhances the adsorption capability of intermediates, reduces the reaction barrier, and facilitates the desorption of NH₃. Electrochemical nitrate reduction to ammonia is a promising alternative strategy for producing valuable ammonia. This prospective route, however, is subject to a slow electrocatalytic rate, which resulted from the weak adsorption and activation of intermediate species, and the low density electron cloud of active centers. To address this issue, we developed a novel approach by doping boron into metal hydroxyl oxides to adjust the electronic structure of active centers, and consequently, led a significant improvement in the Faraday efficiency upto approaching 100 %, as well as an impressive ammonia yield upto approximately 23 mg/h mgcat-1 at -0.6 V vs. reversible hydrogen electrode (RHE). Experimental data in mechanism demonstrate that the doped boron play a crucial role in modulating the local electronic environment surrounding the active sites Co. In situ Raman and FTIR spectra provide evidences that boron facilitates the formation of deoxidation and hydrogenation intermediates. Additionally, density functional theory (DFT) calculations support the notion that boron doping enhances the adsorption capability of intermediates, reduces the reaction barrier, and facilitates the desorption of NH3.Electrochemical nitrate reduction to ammonia is a promising alternative strategy for producing valuable ammonia. This prospective route, however, is subject to a slow electrocatalytic rate, which resulted from the weak adsorption and activation of intermediate species, and the low density electron cloud of active centers. To address this issue, we developed a novel approach by doping boron into metal hydroxyl oxides to adjust the electronic structure of active centers, and consequently, led a significant improvement in the Faraday efficiency upto approaching 100 %, as well as an impressive ammonia yield upto approximately 23 mg/h mgcat-1 at -0.6 V vs. reversible hydrogen electrode (RHE). Experimental data in mechanism demonstrate that the doped boron play a crucial role in modulating the local electronic environment surrounding the active sites Co. In situ Raman and FTIR spectra provide evidences that boron facilitates the formation of deoxidation and hydrogenation intermediates. Additionally, density functional theory (DFT) calculations support the notion that boron doping enhances the adsorption capability of intermediates, reduces the reaction barrier, and facilitates the desorption of NH3. Electrochemical nitrate reduction to ammonia is a promising alternative strategy for producing valuable ammonia. This prospective route, however, is subject to a slow electrocatalytic rate, which resulted from the weak adsorption and activation of intermediate species, and the low density electron cloud of active centers. To address this issue, we developed a novel approach by doping boron into metal hydroxyl oxides to adjust the electronic structure of active centers, and consequently, led a significant improvement in the Faraday efficiency upto approaching 100 %, as well as an impressive ammonia yield upto approximately 23 mg/h mgcat at -0.6 V vs. reversible hydrogen electrode (RHE). Experimental data in mechanism demonstrate that the doped boron play a crucial role in modulating the local electronic environment surrounding the active sites Co. In situ Raman and FTIR spectra provide evidences that boron facilitates the formation of deoxidation and hydrogenation intermediates. Additionally, density functional theory (DFT) calculations support the notion that boron doping enhances the adsorption capability of intermediates, reduces the reaction barrier, and facilitates the desorption of NH . |
| Author | Zhang, Yushuo Zhang, Chunfa Wu, Yingjie Kan, Ziwang Liu, Song Chen, Chunxia Xu, Yinghua Wang, Qi Sun, Tantan Hong, Yan Guo, Jing |
| Author_xml | – sequence: 1 givenname: Jing surname: Guo fullname: Guo, Jing organization: College of Chemistry, Chemical Engineering and Resource Utilization, Northeast Forestry University, Harbin 150040, China – sequence: 2 givenname: Qi surname: Wang fullname: Wang, Qi organization: College of Chemistry, Chemical Engineering and Resource Utilization, Northeast Forestry University, Harbin 150040, China – sequence: 3 givenname: Chunxia surname: Chen fullname: Chen, Chunxia email: ccx1759@163.com organization: College of Chemistry, Chemical Engineering and Resource Utilization, Northeast Forestry University, Harbin 150040, China – sequence: 4 givenname: Chunfa surname: Zhang fullname: Zhang, Chunfa organization: Changchun Jiutai District People’s Hospital, Changchun 130500, China – sequence: 5 givenname: Yinghua surname: Xu fullname: Xu, Yinghua organization: Petroleum and Chemical Industry Key Laboratory of Organic Electrochemical Synthesis, State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 311215, China – sequence: 6 givenname: Yushuo surname: Zhang fullname: Zhang, Yushuo organization: College of Chemistry, Chemical Engineering and Resource Utilization, Northeast Forestry University, Harbin 150040, China – sequence: 7 givenname: Yan surname: Hong fullname: Hong, Yan organization: College of Chemistry, Chemical Engineering and Resource Utilization, Northeast Forestry University, Harbin 150040, China – sequence: 8 givenname: Ziwang surname: Kan fullname: Kan, Ziwang organization: College of Chemistry, Chemical Engineering and Resource Utilization, Northeast Forestry University, Harbin 150040, China – sequence: 9 givenname: Yingjie surname: Wu fullname: Wu, Yingjie organization: School of Medicine and Health, Harbin Institute of Technology, Harbin 150001, China – sequence: 10 givenname: Tantan surname: Sun fullname: Sun, Tantan email: suntantan@zju.edu.cn organization: ZJU-Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University, Hangzhou 311215, China – sequence: 11 givenname: Song orcidid: 0000-0002-1792-6016 surname: Liu fullname: Liu, Song email: carlosliusong@nefu.edu.cn organization: College of Chemistry, Chemical Engineering and Resource Utilization, Northeast Forestry University, Harbin 150040, China |
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| Keywords | Electrocatalysis Transition metal catalyst Ammonia synthesis Nitrate reduction Doping strategy |
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Electrochemical nitrate reduction to ammonia is a promising alternative strategy for producing valuable ammonia. This prospective route,... Electrochemical nitrate reduction to ammonia is a promising alternative strategy for producing valuable ammonia. This prospective route, however, is subject to... |
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| SubjectTerms | adsorption ammonia Ammonia synthesis boron cobalt density functional theory desorption Doping strategy Electrocatalysis electrochemistry electrodes hydrogen hydrogenation Nitrate reduction species Transition metal catalyst |
| Title | High-efficiency electrochemical nitrate reduction to ammonia via boron-doped hydroxyl oxide cobalt induced electron delocalization |
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