Efficient Ammonia Electrosynthesis from Nitrate on Strained Ruthenium Nanoclusters
The limitations of the Haber–Bosch reaction, particularly high-temperature operation, have ignited new interests in low-temperature ammonia-synthesis scenarios. Ambient N2 electroreduction is a compelling alternative but is impeded by a low ammonia production rate (mostly <10 mmol gcat –1 h–1), a...
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| Published in | Journal of the American Chemical Society Vol. 142; no. 15; pp. 7036 - 7046 |
|---|---|
| Main Authors | , , , , , , , , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
United States
American Chemical Society
15.04.2020
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| Subjects | |
| Online Access | Get full text |
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| Abstract | The limitations of the Haber–Bosch reaction, particularly high-temperature operation, have ignited new interests in low-temperature ammonia-synthesis scenarios. Ambient N2 electroreduction is a compelling alternative but is impeded by a low ammonia production rate (mostly <10 mmol gcat –1 h–1), a small partial current density (<1 mA cm–2), and a high-selectivity hydrogen-evolving side reaction. Herein, we report that room-temperature nitrate electroreduction catalyzed by strained ruthenium nanoclusters generates ammonia at a higher rate (5.56 mol gcat –1 h–1) than the Haber–Bosch process. The primary contributor to such performance is hydrogen radicals, which are generated by suppressing hydrogen–hydrogen dimerization during water splitting enabled by the tensile lattice strains. The radicals expedite nitrate-to-ammonia conversion by hydrogenating intermediates of the rate-limiting steps at lower kinetic barriers. The strained nanostructures can maintain nearly 100% ammonia-evolving selectivity at >120 mA cm–2 current densities for 100 h due to the robust subsurface Ru–O coordination. These findings highlight the potential of nitrate electroreduction in real-world, low-temperature ammonia synthesis. |
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| AbstractList | The limitations of the Haber–Bosch reaction, particularly high-temperature operation, have ignited new interests in low-temperature ammonia-synthesis scenarios. Ambient N₂ electroreduction is a compelling alternative but is impeded by a low ammonia production rate (mostly <10 mmol gcₐₜ–¹ h–¹), a small partial current density (<1 mA cm–²), and a high-selectivity hydrogen-evolving side reaction. Herein, we report that room-temperature nitrate electroreduction catalyzed by strained ruthenium nanoclusters generates ammonia at a higher rate (5.56 mol gcₐₜ–¹ h–¹) than the Haber–Bosch process. The primary contributor to such performance is hydrogen radicals, which are generated by suppressing hydrogen–hydrogen dimerization during water splitting enabled by the tensile lattice strains. The radicals expedite nitrate-to-ammonia conversion by hydrogenating intermediates of the rate-limiting steps at lower kinetic barriers. The strained nanostructures can maintain nearly 100% ammonia-evolving selectivity at >120 mA cm–² current densities for 100 h due to the robust subsurface Ru–O coordination. These findings highlight the potential of nitrate electroreduction in real-world, low-temperature ammonia synthesis. The limitations of the Haber-Bosch reaction, particularly high-temperature operation, have ignited new interests in low-temperature ammonia-synthesis scenarios. Ambient N electroreduction is a compelling alternative but is impeded by a low ammonia production rate (mostly <10 mmol g h ), a small partial current density (<1 mA cm ), and a high-selectivity hydrogen-evolving side reaction. Herein, we report that room-temperature nitrate electroreduction catalyzed by strained ruthenium nanoclusters generates ammonia at a higher rate (5.56 mol g h ) than the Haber-Bosch process. The primary contributor to such performance is hydrogen radicals, which are generated by suppressing hydrogen-hydrogen dimerization during water splitting enabled by the tensile lattice strains. The radicals expedite nitrate-to-ammonia conversion by hydrogenating intermediates of the rate-limiting steps at lower kinetic barriers. The strained nanostructures can maintain nearly 100% ammonia-evolving selectivity at >120 mA cm current densities for 100 h due to the robust subsurface Ru-O coordination. These findings highlight the potential of nitrate electroreduction in real-world, low-temperature ammonia synthesis. The limitations of the Haber-Bosch reaction, particularly high-temperature operation, have ignited new interests in low-temperature ammonia-synthesis scenarios. Ambient N2 electroreduction is a compelling alternative but is impeded by a low ammonia production rate (mostly <10 mmol gcat-1 h-1), a small partial current density (<1 mA cm-2), and a high-selectivity hydrogen-evolving side reaction. Herein, we report that room-temperature nitrate electroreduction catalyzed by strained ruthenium nanoclusters generates ammonia at a higher rate (5.56 mol gcat-1 h-1) than the Haber-Bosch process. The primary contributor to such performance is hydrogen radicals, which are generated by suppressing hydrogen-hydrogen dimerization during water splitting enabled by the tensile lattice strains. The radicals expedite nitrate-to-ammonia conversion by hydrogenating intermediates of the rate-limiting steps at lower kinetic barriers. The strained nanostructures can maintain nearly 100% ammonia-evolving selectivity at >120 mA cm-2 current densities for 100 h due to the robust subsurface Ru-O coordination. These findings highlight the potential of nitrate electroreduction in real-world, low-temperature ammonia synthesis.The limitations of the Haber-Bosch reaction, particularly high-temperature operation, have ignited new interests in low-temperature ammonia-synthesis scenarios. Ambient N2 electroreduction is a compelling alternative but is impeded by a low ammonia production rate (mostly <10 mmol gcat-1 h-1), a small partial current density (<1 mA cm-2), and a high-selectivity hydrogen-evolving side reaction. Herein, we report that room-temperature nitrate electroreduction catalyzed by strained ruthenium nanoclusters generates ammonia at a higher rate (5.56 mol gcat-1 h-1) than the Haber-Bosch process. The primary contributor to such performance is hydrogen radicals, which are generated by suppressing hydrogen-hydrogen dimerization during water splitting enabled by the tensile lattice strains. The radicals expedite nitrate-to-ammonia conversion by hydrogenating intermediates of the rate-limiting steps at lower kinetic barriers. The strained nanostructures can maintain nearly 100% ammonia-evolving selectivity at >120 mA cm-2 current densities for 100 h due to the robust subsurface Ru-O coordination. These findings highlight the potential of nitrate electroreduction in real-world, low-temperature ammonia synthesis. The limitations of the Haber–Bosch reaction, particularly high-temperature operation, have ignited new interests in low-temperature ammonia-synthesis scenarios. Ambient N2 electroreduction is a compelling alternative but is impeded by a low ammonia production rate (mostly <10 mmol gcat –1 h–1), a small partial current density (<1 mA cm–2), and a high-selectivity hydrogen-evolving side reaction. Herein, we report that room-temperature nitrate electroreduction catalyzed by strained ruthenium nanoclusters generates ammonia at a higher rate (5.56 mol gcat –1 h–1) than the Haber–Bosch process. The primary contributor to such performance is hydrogen radicals, which are generated by suppressing hydrogen–hydrogen dimerization during water splitting enabled by the tensile lattice strains. The radicals expedite nitrate-to-ammonia conversion by hydrogenating intermediates of the rate-limiting steps at lower kinetic barriers. The strained nanostructures can maintain nearly 100% ammonia-evolving selectivity at >120 mA cm–2 current densities for 100 h due to the robust subsurface Ru–O coordination. These findings highlight the potential of nitrate electroreduction in real-world, low-temperature ammonia synthesis. |
| Author | Quan, Fengjiao Zhang, Lizhi Xu, Liangpang Wang, Jianfang Lei, Fengcai Shi, Yanbiao Yu, Jimmy C Yang, Jianhua Hao, Weichang Li, Lejing Liu, Yang Wong, Po Keung Wang, Bo Mao, Chengliang Li, Jie Chan, Alice W. M Zhan, Guangming Du, Yi Dou, Shi-Xue |
| AuthorAffiliation | Department of Chemistry Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry School of Physics, BUAA-UOW Joint Research Centre School of Life Sciences Institute for Superconducting and Electronic Materials (ISEM), Australian Institute for Innovative Materials (AIIM) Department of Physics |
| AuthorAffiliation_xml | – name: Department of Chemistry – name: School of Physics, BUAA-UOW Joint Research Centre – name: Institute for Superconducting and Electronic Materials (ISEM), Australian Institute for Innovative Materials (AIIM) – name: Department of Physics – name: School of Life Sciences – name: Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry |
| Author_xml | – sequence: 1 givenname: Jie surname: Li fullname: Li, Jie – sequence: 2 givenname: Guangming surname: Zhan fullname: Zhan, Guangming organization: Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry – sequence: 3 givenname: Jianhua surname: Yang fullname: Yang, Jianhua – sequence: 4 givenname: Fengjiao surname: Quan fullname: Quan, Fengjiao organization: Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry – sequence: 5 givenname: Chengliang surname: Mao fullname: Mao, Chengliang organization: Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry – sequence: 6 givenname: Yang surname: Liu fullname: Liu, Yang – sequence: 7 givenname: Bo surname: Wang fullname: Wang, Bo – sequence: 8 givenname: Fengcai surname: Lei fullname: Lei, Fengcai – sequence: 9 givenname: Lejing orcidid: 0000-0001-7144-9305 surname: Li fullname: Li, Lejing – sequence: 10 givenname: Alice W. M surname: Chan fullname: Chan, Alice W. M – sequence: 11 givenname: Liangpang surname: Xu fullname: Xu, Liangpang – sequence: 12 givenname: Yanbiao surname: Shi fullname: Shi, Yanbiao organization: Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry – sequence: 13 givenname: Yi surname: Du fullname: Du, Yi organization: School of Physics, BUAA-UOW Joint Research Centre – sequence: 14 givenname: Weichang orcidid: 0000-0002-1597-7151 surname: Hao fullname: Hao, Weichang organization: School of Physics, BUAA-UOW Joint Research Centre – sequence: 15 givenname: Po Keung orcidid: 0000-0003-3081-960X surname: Wong fullname: Wong, Po Keung – sequence: 16 givenname: Jianfang orcidid: 0000-0002-2467-8751 surname: Wang fullname: Wang, Jianfang – sequence: 17 givenname: Shi-Xue surname: Dou fullname: Dou, Shi-Xue organization: School of Physics, BUAA-UOW Joint Research Centre – sequence: 18 givenname: Lizhi orcidid: 0000-0002-6842-9167 surname: Zhang fullname: Zhang, Lizhi email: zhanglz@mail.ccnu.edu.cn organization: Key Laboratory of Pesticide & Chemical Biology of Ministry of Education, Institute of Environmental & Applied Chemistry, College of Chemistry – sequence: 19 givenname: Jimmy C orcidid: 0000-0001-9886-3725 surname: Yu fullname: Yu, Jimmy C email: jimyu@cuhk.edu.hk |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/32223152$$D View this record in MEDLINE/PubMed |
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| Snippet | The limitations of the Haber–Bosch reaction, particularly high-temperature operation, have ignited new interests in low-temperature ammonia-synthesis... The limitations of the Haber-Bosch reaction, particularly high-temperature operation, have ignited new interests in low-temperature ammonia-synthesis... |
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| Title | Efficient Ammonia Electrosynthesis from Nitrate on Strained Ruthenium Nanoclusters |
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