Deciphering nickel-catalyzed electrochemical ammonia synthesis from nitric oxide
Electrochemical nitric oxide (NO) reduction to ammonia (NH3) is an attractive nitrogen fixation way; however, the poor mechanistic understanding and unsatisfied NH3 selectivity strongly impede its practical applications. Here, we screened a suite of transition-metal electrocatalysts, in which Ni out...
| Main Authors: | , , , , , , , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2024
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| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/173335 |
| _version_ | 1826117137490509824 |
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| author | Zhao, Siwen Liu, Jiyuan Zhang, Zhibin Zhu, Chenyuan Shi, Guoshuai Wu, Jing Yang, Chunlei Wang, Qinghe Chang, Mingwei Liu, Kaihui Li, Shuzhou Zhang, Liming |
| author2 | School of Materials Science and Engineering |
| author_facet | School of Materials Science and Engineering Zhao, Siwen Liu, Jiyuan Zhang, Zhibin Zhu, Chenyuan Shi, Guoshuai Wu, Jing Yang, Chunlei Wang, Qinghe Chang, Mingwei Liu, Kaihui Li, Shuzhou Zhang, Liming |
| author_sort | Zhao, Siwen |
| collection | NTU |
| description | Electrochemical nitric oxide (NO) reduction to ammonia (NH3) is an attractive nitrogen fixation way; however, the poor mechanistic understanding and unsatisfied NH3 selectivity strongly impede its practical applications. Here, we screened a suite of transition-metal electrocatalysts, in which Ni outperformed others at the top of a volcano-shaped plot. We rationally fabricated five monocrystalline Ni electrocatalysts and observed higher productivities on high-index facets. In particular, Ni(210) demonstrates a unique NH3 selectivity with a yield rate 2-fold higher than those of low-index facets. The energy required for key intermediates switching from hollow-to-bridge sites was established as a descriptor for NH3 production. Electrochemical measurements on Ni nanoparticle ensembles evidenced a high NH3 selectivity of over 85% with a decent production rate, along with a stable running over 50 h. This work guides the rational design of NO reduction electrocatalysts and establishes a paradigm to understand the structure-function correlation in catalysis. |
| first_indexed | 2024-10-01T04:22:45Z |
| format | Journal Article |
| id | ntu-10356/173335 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T04:22:45Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1733352024-01-29T01:03:16Z Deciphering nickel-catalyzed electrochemical ammonia synthesis from nitric oxide Zhao, Siwen Liu, Jiyuan Zhang, Zhibin Zhu, Chenyuan Shi, Guoshuai Wu, Jing Yang, Chunlei Wang, Qinghe Chang, Mingwei Liu, Kaihui Li, Shuzhou Zhang, Liming School of Materials Science and Engineering Engineering::Materials Electrocatalysis Nitrogen Fixation Electrochemical nitric oxide (NO) reduction to ammonia (NH3) is an attractive nitrogen fixation way; however, the poor mechanistic understanding and unsatisfied NH3 selectivity strongly impede its practical applications. Here, we screened a suite of transition-metal electrocatalysts, in which Ni outperformed others at the top of a volcano-shaped plot. We rationally fabricated five monocrystalline Ni electrocatalysts and observed higher productivities on high-index facets. In particular, Ni(210) demonstrates a unique NH3 selectivity with a yield rate 2-fold higher than those of low-index facets. The energy required for key intermediates switching from hollow-to-bridge sites was established as a descriptor for NH3 production. Electrochemical measurements on Ni nanoparticle ensembles evidenced a high NH3 selectivity of over 85% with a decent production rate, along with a stable running over 50 h. This work guides the rational design of NO reduction electrocatalysts and establishes a paradigm to understand the structure-function correlation in catalysis. Ministry of Education (MOE) This research was supported by the National Natural Science Foundation of China (grants 21872039, 22072030, and 52025023), the Fundamental Research Funds for the Central Universities (20720220008), the Science and Technology Commission of Shanghai Municipality (grants 18JC1411700, 19DZ2270100, and 22520711100), the National Key R&D Program of China (2022YFA1505200), and the Key R&D Program of Guangdong Province (grant 2020B010189001). S.L. thanks funding support from the Singapore Academic Research Fund Tier 1 (RG8/20 and RG10/21). C.Z. thanks funding support from the China Postdoctoral Science Foundation (2021M700810). 2024-01-29T01:03:15Z 2024-01-29T01:03:15Z 2023 Journal Article Zhao, S., Liu, J., Zhang, Z., Zhu, C., Shi, G., Wu, J., Yang, C., Wang, Q., Chang, M., Liu, K., Li, S. & Zhang, L. (2023). Deciphering nickel-catalyzed electrochemical ammonia synthesis from nitric oxide. Chem, 9(12), 3555-3572. https://dx.doi.org/10.1016/j.chempr.2023.08.001 2451-9308 https://hdl.handle.net/10356/173335 10.1016/j.chempr.2023.08.001 2-s2.0-85179605078 12 9 3555 3572 en RG8/20 RG10/21 Chem © 2023 Elsevier Inc. All rights reserved. |
| spellingShingle | Engineering::Materials Electrocatalysis Nitrogen Fixation Zhao, Siwen Liu, Jiyuan Zhang, Zhibin Zhu, Chenyuan Shi, Guoshuai Wu, Jing Yang, Chunlei Wang, Qinghe Chang, Mingwei Liu, Kaihui Li, Shuzhou Zhang, Liming Deciphering nickel-catalyzed electrochemical ammonia synthesis from nitric oxide |
| title | Deciphering nickel-catalyzed electrochemical ammonia synthesis from nitric oxide |
| title_full | Deciphering nickel-catalyzed electrochemical ammonia synthesis from nitric oxide |
| title_fullStr | Deciphering nickel-catalyzed electrochemical ammonia synthesis from nitric oxide |
| title_full_unstemmed | Deciphering nickel-catalyzed electrochemical ammonia synthesis from nitric oxide |
| title_short | Deciphering nickel-catalyzed electrochemical ammonia synthesis from nitric oxide |
| title_sort | deciphering nickel catalyzed electrochemical ammonia synthesis from nitric oxide |
| topic | Engineering::Materials Electrocatalysis Nitrogen Fixation |
| url | https://hdl.handle.net/10356/173335 |
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