Synchronously Consolidating Li, Se, S, and C for Robust Li–SeS Batteries
S-redox involving solvated polysulfides is accompanied by volumetric change and structural decay of the S-based cathodes. Here, we propose a synchronous construction strategy for consolidating Li, Se, S, and C elements within a composite cathode via a paradigm reaction of 8Li+2Se+CS<sub>2</sub> = 2Li<sub>4</sub>SeS+C. The obtained composite features crystalline Li<sub>4</sub>SeS encapsulated in a carbon nanocage (Li<sub>4</sub>SeS@C), exhibiting ultrahigh electrical conductivity, ultralow activation barrier, and excellent structural integrity, accordingly enabling large specific capacity (615 mAh g<sup>-1</sup>) and high capacity retention (87.3% after 350 cycles) at 10 A g<sup>-1</sup>. TOF-SIMS demonstrates its superior volumetric efficiency to a similar derivative SeS@C (2Se+CS<sub>2</sub> = 2SeS+C), and DFT reveals its lower activation barrier than Li<sub>2</sub>S@C and Li<sub>2</sub>Se@C. This consolidation design significantly improves the electrochemical performance of S-based cathodes, and the paradigm reaction guarantees structural diversity and flexibility. Moreover, employing a synchronous construction mechanism to maximize the synergistic effect between element consolidation and carbon encapsulation opens up a new approach for developing robust S or chalcogenide cathodes.
Authors
- Yifei Yuan (ORCID: https://orcid.org/0000-0002-2360-8794)
- Longlong Fan (ORCID: https://orcid.org/0000-0002-1748-1192)
- Junfan Zhang (ORCID: https://orcid.org/0000-0003-4547-5651)
- Duanyun Cao (ORCID: https://orcid.org/0000-0002-3989-959X)
- Jia‐Qi Huang (ORCID: https://orcid.org/0000-0001-7394-9186)
- Mengmeng Qian
- Guoqiang Tan (ORCID: https://orcid.org/0000-0002-3254-3865)
- Tinglu Song (ORCID: https://orcid.org/0000-0003-3907-7956)
- Feng Wu (ORCID: https://orcid.org/0000-0003-3504-8576)
- Jing Wang (ORCID: https://orcid.org/0000-0002-7264-8266)
- Chongteng Wu
- Yun Li (ORCID: https://orcid.org/0009-0004-4732-0471)
Institutions
- Beijing Institute of Technology (CN)
- Wenzhou University (CN)
- Chinese Academy of Sciences (CN)
- Institute of High Energy Physics (CN)
- Chongqing University of Technology (CN)
Publication Details
- Journal
- Nano Letters
- Published
- 2024-09-23
- DOI
- https://doi.org/10.1021/acs.nanolett.4c01388
- Citations
- 8
- Primary Topic
- Advancements in Battery Materials
- Type
- article
- Field-Weighted Citation Impact
- 1.67
Funders
- National Natural Science Foundation of China