Temperature-induced low-coordinate Ni single-atom catalyst for boosted CO₂ electroreduction activity
Single-atom catalysts (SACs) exhibit remarkable potential for electrochemical reduction of CO2 to value-added products. However, the commonly pursued methods for preparing SACs are hard to scale up, and sometimes, lack general applicability because of expensive raw materials and complex synthetic pr...
| Main Authors: | , , , , , |
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| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2023
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| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/170336 |
| _version_ | 1811687106241626112 |
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| author | Wang, Na Li, Haoyue Wang, Haojing Yang, Huanhuan Ren, Ziqiu Xu, Rong |
| author2 | School of Chemistry, Chemical Engineering and Biotechnology |
| author_facet | School of Chemistry, Chemical Engineering and Biotechnology Wang, Na Li, Haoyue Wang, Haojing Yang, Huanhuan Ren, Ziqiu Xu, Rong |
| author_sort | Wang, Na |
| collection | NTU |
| description | Single-atom catalysts (SACs) exhibit remarkable potential for electrochemical reduction of CO2 to value-added products. However, the commonly pursued methods for preparing SACs are hard to scale up, and sometimes, lack general applicability because of expensive raw materials and complex synthetic procedures. In addition, the fine tuning of coordination environment of SACs remains challenging due to their structural vulnerability. Herein, a simple and universal strategy is developed to fabricate Ni SACs with different nitrogen coordination numbers through one-step pyrolysis of melamine, Ni(NO3 )∙6H2 O, and polyvinylpyrrolidone at different temperatures. Experimental measurements and theoretical calculations reveal that the low-coordinate Ni SACs exhibit outstanding CO2 reduction performance and stability, achieving a Faradic efficiency (FECO ) of 98.5% at -0.76 V with CO current density of 24.6 mA cm-2 , and maintaining FECO of over 91.0% at all applied potential windows from -0.56 to -1.16 V, benefiting from its coordinatively unsaturated structure to afford high catalytic activity and low barrier for the formation of *COOH intermediate. No significant performance degradation is observed over 50 h of continuous operation. Additionally, several other metallic single-atom catalysts are successfully prepared by this synthetic method, demonstrating the universality of this strategy. |
| first_indexed | 2024-10-01T05:11:02Z |
| format | Journal Article |
| id | ntu-10356/170336 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2024-10-01T05:11:02Z |
| publishDate | 2023 |
| record_format | dspace |
| spelling | ntu-10356/1703362023-09-08T01:18:47Z Temperature-induced low-coordinate Ni single-atom catalyst for boosted CO₂ electroreduction activity Wang, Na Li, Haoyue Wang, Haojing Yang, Huanhuan Ren, Ziqiu Xu, Rong School of Chemistry, Chemical Engineering and Biotechnology National Research Foundation Engineering::Chemical engineering Coordination Environments Universality Single-atom catalysts (SACs) exhibit remarkable potential for electrochemical reduction of CO2 to value-added products. However, the commonly pursued methods for preparing SACs are hard to scale up, and sometimes, lack general applicability because of expensive raw materials and complex synthetic procedures. In addition, the fine tuning of coordination environment of SACs remains challenging due to their structural vulnerability. Herein, a simple and universal strategy is developed to fabricate Ni SACs with different nitrogen coordination numbers through one-step pyrolysis of melamine, Ni(NO3 )∙6H2 O, and polyvinylpyrrolidone at different temperatures. Experimental measurements and theoretical calculations reveal that the low-coordinate Ni SACs exhibit outstanding CO2 reduction performance and stability, achieving a Faradic efficiency (FECO ) of 98.5% at -0.76 V with CO current density of 24.6 mA cm-2 , and maintaining FECO of over 91.0% at all applied potential windows from -0.56 to -1.16 V, benefiting from its coordinatively unsaturated structure to afford high catalytic activity and low barrier for the formation of *COOH intermediate. No significant performance degradation is observed over 50 h of continuous operation. Additionally, several other metallic single-atom catalysts are successfully prepared by this synthetic method, demonstrating the universality of this strategy. Nanyang Technological University National Research Foundation (NRF) This work is supported by the National Natural Science Foundation of China (NSFC) (No. 22105178, 52103237), the Nanyang Technological University, and the National Research Foundation (NRF), Singapore, under its Campus for Research Excellence and Technological Enterprise (CREATE) program through the Carbon Reduction in Chemical Technology (C4T) program. 2023-09-08T01:18:47Z 2023-09-08T01:18:47Z 2023 Journal Article Wang, N., Li, H., Wang, H., Yang, H., Ren, Z. & Xu, R. (2023). Temperature-induced low-coordinate Ni single-atom catalyst for boosted CO₂ electroreduction activity. Small, 19(35), 2301469-. https://dx.doi.org/10.1002/smll.202301469 1613-6810 https://hdl.handle.net/10356/170336 10.1002/smll.202301469 37098645 2-s2.0-85153365527 35 19 2301469 en Small © 2023 Wiley-VCH GmbH. All rights reserved. |
| spellingShingle | Engineering::Chemical engineering Coordination Environments Universality Wang, Na Li, Haoyue Wang, Haojing Yang, Huanhuan Ren, Ziqiu Xu, Rong Temperature-induced low-coordinate Ni single-atom catalyst for boosted CO₂ electroreduction activity |
| title | Temperature-induced low-coordinate Ni single-atom catalyst for boosted CO₂ electroreduction activity |
| title_full | Temperature-induced low-coordinate Ni single-atom catalyst for boosted CO₂ electroreduction activity |
| title_fullStr | Temperature-induced low-coordinate Ni single-atom catalyst for boosted CO₂ electroreduction activity |
| title_full_unstemmed | Temperature-induced low-coordinate Ni single-atom catalyst for boosted CO₂ electroreduction activity |
| title_short | Temperature-induced low-coordinate Ni single-atom catalyst for boosted CO₂ electroreduction activity |
| title_sort | temperature induced low coordinate ni single atom catalyst for boosted co₂ electroreduction activity |
| topic | Engineering::Chemical engineering Coordination Environments Universality |
| url | https://hdl.handle.net/10356/170336 |
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