Modulating the coordination environment of Co single-atom catalysts: impact on lithium-sulfur battery performance
The coordination environment is crucial to the electrocatalytic activity of single-atom catalysts (SACs). Although substituting N atoms in traditional transition metal-nitrogen (TM-N4) configuration with other non-metal atoms has been reported, its specific role in sulfur electrochemical reactions h...
| 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/10356/180376 |
| _version_ | 1824454281329115136 |
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| author | Li, Yi Chen, Zhaoyang Zhong, Xin-Yu Mei, Tiehan Li, Zhao Yue, Liang Yang, Jin-Lin Fan, Hong Jin Xu, Maowen |
| author2 | School of Physical and Mathematical Sciences |
| author_facet | School of Physical and Mathematical Sciences Li, Yi Chen, Zhaoyang Zhong, Xin-Yu Mei, Tiehan Li, Zhao Yue, Liang Yang, Jin-Lin Fan, Hong Jin Xu, Maowen |
| author_sort | Li, Yi |
| collection | NTU |
| description | The coordination environment is crucial to the electrocatalytic activity of single-atom catalysts (SACs). Although substituting N atoms in traditional transition metal-nitrogen (TM-N4) configuration with other non-metal atoms has been reported, its specific role in sulfur electrochemical reactions has not been sufficiently investigated. Herein, a Co-P2N2 SACs configuration is fabricated to investigate the mechanistic differences compared to Co-N4 in sulfur reduction/oxidation. This configuration enhances the electron transfer with Li2S6, where the electrons tend to aggregate between P and Li atoms as two separate parts rather than a single merged zone as observed in symmetric Co-N4 SACs. This process facilitates polysulfide decomposition and promotes Li2S nucleation/oxidation. Furthermore, the CoPNC interlayer effectively suppresses cell self-discharge and Li anode corrosion due to polysulfide shuttling. Li-Li symmetrical cell incorporated with the CoPNC interlayer achieves a prolonged lifespan exceeding 1000 h, and Li-S full cell delivers a discharge capacity of more than 1500 mAh g−1. This research provides insights into how the geometric configuration of SACs influences the performance of conversion-type batteries. |
| first_indexed | 2025-02-19T03:19:49Z |
| format | Journal Article |
| id | ntu-10356/180376 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2025-02-19T03:19:49Z |
| publishDate | 2024 |
| record_format | dspace |
| spelling | ntu-10356/1803762024-10-07T15:34:55Z Modulating the coordination environment of Co single-atom catalysts: impact on lithium-sulfur battery performance Li, Yi Chen, Zhaoyang Zhong, Xin-Yu Mei, Tiehan Li, Zhao Yue, Liang Yang, Jin-Lin Fan, Hong Jin Xu, Maowen School of Physical and Mathematical Sciences Physics Atomic coordination Lithium metal The coordination environment is crucial to the electrocatalytic activity of single-atom catalysts (SACs). Although substituting N atoms in traditional transition metal-nitrogen (TM-N4) configuration with other non-metal atoms has been reported, its specific role in sulfur electrochemical reactions has not been sufficiently investigated. Herein, a Co-P2N2 SACs configuration is fabricated to investigate the mechanistic differences compared to Co-N4 in sulfur reduction/oxidation. This configuration enhances the electron transfer with Li2S6, where the electrons tend to aggregate between P and Li atoms as two separate parts rather than a single merged zone as observed in symmetric Co-N4 SACs. This process facilitates polysulfide decomposition and promotes Li2S nucleation/oxidation. Furthermore, the CoPNC interlayer effectively suppresses cell self-discharge and Li anode corrosion due to polysulfide shuttling. Li-Li symmetrical cell incorporated with the CoPNC interlayer achieves a prolonged lifespan exceeding 1000 h, and Li-S full cell delivers a discharge capacity of more than 1500 mAh g−1. This research provides insights into how the geometric configuration of SACs influences the performance of conversion-type batteries. Submitted/Accepted version This work is financially supported by grants from the National Natural Science Foundation of China (No. 22179109) and the Chongqing Doctoral Research and Innovation Project (CYB22120). 2024-10-06T08:17:54Z 2024-10-06T08:17:54Z 2024 Journal Article Li, Y., Chen, Z., Zhong, X., Mei, T., Li, Z., Yue, L., Yang, J., Fan, H. J. & Xu, M. (2024). Modulating the coordination environment of Co single-atom catalysts: impact on lithium-sulfur battery performance. Advanced Functional Materials. https://dx.doi.org/10.1002/adfm.202412279 1616-301X https://hdl.handle.net/10356/180376 10.1002/adfm.202412279 2-s2.0-85202776113 en Advanced Functional Materials © 2024 Wiley-VCH GmbH. All rights reserved. This article may be downloaded for personal use only. Any other use requires prior permission of the copyright holder. The Version of Record is available online at http://doi.org/10.1002/adfm.202412279. application/pdf |
| spellingShingle | Physics Atomic coordination Lithium metal Li, Yi Chen, Zhaoyang Zhong, Xin-Yu Mei, Tiehan Li, Zhao Yue, Liang Yang, Jin-Lin Fan, Hong Jin Xu, Maowen Modulating the coordination environment of Co single-atom catalysts: impact on lithium-sulfur battery performance |
| title | Modulating the coordination environment of Co single-atom catalysts: impact on lithium-sulfur battery performance |
| title_full | Modulating the coordination environment of Co single-atom catalysts: impact on lithium-sulfur battery performance |
| title_fullStr | Modulating the coordination environment of Co single-atom catalysts: impact on lithium-sulfur battery performance |
| title_full_unstemmed | Modulating the coordination environment of Co single-atom catalysts: impact on lithium-sulfur battery performance |
| title_short | Modulating the coordination environment of Co single-atom catalysts: impact on lithium-sulfur battery performance |
| title_sort | modulating the coordination environment of co single atom catalysts impact on lithium sulfur battery performance |
| topic | Physics Atomic coordination Lithium metal |
| url | https://hdl.handle.net/10356/180376 |
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