Lithium-mediated electrochemical nitrogen reduction: Mechanistic insights to enhance performance
Summary: Green synthesis of ammonia by electrochemical nitrogen reduction reaction (NRR) shows great potential as an alternative to the Haber-Bosch process but is hampered by sluggish production rate and low Faradaic efficiency. Recently, lithium-mediated electrochemical NRR has received renewed att...
| Main Authors: | , , , , , , , , , |
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| Format: | Article |
| Language: | English |
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Elsevier
2021-10-01
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| Series: | iScience |
| Subjects: | |
| Online Access: | http://www.sciencedirect.com/science/article/pii/S2589004221010737 |
| _version_ | 1818585187379838976 |
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| author | Xiyang Cai Cehuang Fu Haldrian Iriawan Fan Yang Aiming Wu Liuxuan Luo Shuiyun Shen Guanghua Wei Yang Shao-Horn Junliang Zhang |
| author_facet | Xiyang Cai Cehuang Fu Haldrian Iriawan Fan Yang Aiming Wu Liuxuan Luo Shuiyun Shen Guanghua Wei Yang Shao-Horn Junliang Zhang |
| author_sort | Xiyang Cai |
| collection | DOAJ |
| description | Summary: Green synthesis of ammonia by electrochemical nitrogen reduction reaction (NRR) shows great potential as an alternative to the Haber-Bosch process but is hampered by sluggish production rate and low Faradaic efficiency. Recently, lithium-mediated electrochemical NRR has received renewed attention due to its reproducibility. However, further improvement of the system is restricted by limited recognition of its mechanism. Herein, we demonstrate that lithium-mediated NRR began with electrochemical deposition of lithium, followed by two chemical processes of dinitrogen splitting and protonation to ammonia. Furthermore, we quantified the extent to which the freshly deposited active lithium lost its activity toward NRR due to a parasitic reaction between lithium and electrolyte. A high ammonia yield of 0.410 ± 0.038 μg s−1 cm−2 geo and Faradaic efficiency of 39.5 ± 1.7% were achieved at 20 mA cm−2 geo and 10 mA cm−2 geo, respectively, which can be attributed to fresher lithium obtained at high current density. |
| first_indexed | 2024-12-16T08:33:05Z |
| format | Article |
| id | doaj.art-5cb5758792264015b765e4c14c22dc51 |
| institution | Directory Open Access Journal |
| issn | 2589-0042 |
| language | English |
| last_indexed | 2024-12-16T08:33:05Z |
| publishDate | 2021-10-01 |
| publisher | Elsevier |
| record_format | Article |
| series | iScience |
| spelling | doaj.art-5cb5758792264015b765e4c14c22dc512022-12-21T22:37:49ZengElsevieriScience2589-00422021-10-012410103105Lithium-mediated electrochemical nitrogen reduction: Mechanistic insights to enhance performanceXiyang Cai0Cehuang Fu1Haldrian Iriawan2Fan Yang3Aiming Wu4Liuxuan Luo5Shuiyun Shen6Guanghua Wei7Yang Shao-Horn8Junliang Zhang9Institute of Fuel Cells, School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, ChinaInstitute of Fuel Cells, School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, ChinaDepartment of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, USA; Department of Materials, Imperial College London, London SW7 5RB, UKInstitute of Fuel Cells, School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, ChinaInstitute of Fuel Cells, School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, ChinaInstitute of Fuel Cells, School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, ChinaInstitute of Fuel Cells, School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, ChinaSJTU-Paris Tech Elite Institute of Technology, Shanghai Jiao Tong University, Shanghai 200240, ChinaDepartment of Materials Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, USA; Department of Mechanical Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, USA; Corresponding authorInstitute of Fuel Cells, School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China; Corresponding authorSummary: Green synthesis of ammonia by electrochemical nitrogen reduction reaction (NRR) shows great potential as an alternative to the Haber-Bosch process but is hampered by sluggish production rate and low Faradaic efficiency. Recently, lithium-mediated electrochemical NRR has received renewed attention due to its reproducibility. However, further improvement of the system is restricted by limited recognition of its mechanism. Herein, we demonstrate that lithium-mediated NRR began with electrochemical deposition of lithium, followed by two chemical processes of dinitrogen splitting and protonation to ammonia. Furthermore, we quantified the extent to which the freshly deposited active lithium lost its activity toward NRR due to a parasitic reaction between lithium and electrolyte. A high ammonia yield of 0.410 ± 0.038 μg s−1 cm−2 geo and Faradaic efficiency of 39.5 ± 1.7% were achieved at 20 mA cm−2 geo and 10 mA cm−2 geo, respectively, which can be attributed to fresher lithium obtained at high current density.http://www.sciencedirect.com/science/article/pii/S2589004221010737Chemical reactionElectrochemistryChemical synthesis |
| spellingShingle | Xiyang Cai Cehuang Fu Haldrian Iriawan Fan Yang Aiming Wu Liuxuan Luo Shuiyun Shen Guanghua Wei Yang Shao-Horn Junliang Zhang Lithium-mediated electrochemical nitrogen reduction: Mechanistic insights to enhance performance iScience Chemical reaction Electrochemistry Chemical synthesis |
| title | Lithium-mediated electrochemical nitrogen reduction: Mechanistic insights to enhance performance |
| title_full | Lithium-mediated electrochemical nitrogen reduction: Mechanistic insights to enhance performance |
| title_fullStr | Lithium-mediated electrochemical nitrogen reduction: Mechanistic insights to enhance performance |
| title_full_unstemmed | Lithium-mediated electrochemical nitrogen reduction: Mechanistic insights to enhance performance |
| title_short | Lithium-mediated electrochemical nitrogen reduction: Mechanistic insights to enhance performance |
| title_sort | lithium mediated electrochemical nitrogen reduction mechanistic insights to enhance performance |
| topic | Chemical reaction Electrochemistry Chemical synthesis |
| url | http://www.sciencedirect.com/science/article/pii/S2589004221010737 |
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