Guoxing Jiang, Wenwu Zou, Weifeng Zhang, Zhaoyuan Ou, Shengguang Qi, Tongmei Ma, Zhiming Cui, Zhenxing Liang, Li Du
{"title":"局部共价有机框架纳米片的锂离子加速调节器","authors":"Guoxing Jiang, Wenwu Zou, Weifeng Zhang, Zhaoyuan Ou, Shengguang Qi, Tongmei Ma, Zhiming Cui, Zhenxing Liang, Li Du","doi":"10.1002/aenm.202303672","DOIUrl":null,"url":null,"abstract":"<p>Rational regulation of the Li-ion (Li<sup>+</sup>) migration behaviors and charge distribution at the electrolyte–electrode interface is of great significance in pursuit of high-performance lithium metal battery (LMB) chemistry. Herein, unique locally-zwitterionic covalent organic framework nanosheets (ziCOFNs) are developed as Li<sup>+</sup> accelerated regulators, whose functions include not only kinetics-boosted Li<sup>+</sup> migration but also induces uniform charge distribution in LMBs. The zwitterions act as “dissociation enhancers” to trigger efficient Li<sup>+</sup> desolvation, while the abundant ─COO<sup>−</sup> units within the nanopores favor rapid Li<sup>+</sup> diffusion. In addition, the ordered ionic skeleton dynamically homogenizes the interfacial charge, thereby inhibiting Li dendrite growth and stabilizing the Li-interface chemistry. When implemented as a functional interlayer in the cell configuration, ziCOFNs display ultrahigh transfer number (0.84) and ionic conductivity beyond 4.5 mS cm<sup>−1</sup>. With such a layer, stable Li plating/stripping (over 6500 h) at 3 mA cm<sup>−2</sup> in symmetric cells, and superior long-term cycle performance in high-loading LiFePO<sub>4</sub> (9.4 mg cm<sup>−2</sup>) full cells are achieved. Detailed experimental characterizations combined with theoretical calculations elucidate the mechanism of the zwitterionic framework tuning Li<sup>+</sup> migration behaviors. This work is anticipated to shed fresh light on the exploration of zwitterionic crystalline materials in next-generation LMBs.</p>","PeriodicalId":111,"journal":{"name":"Advanced Energy Materials","volume":null,"pages":null},"PeriodicalIF":24.4000,"publicationDate":"2024-01-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Lithium-Ion Accelerated Regulators by Locally-Zwitterionic Covalent Organic Framework Nanosheets\",\"authors\":\"Guoxing Jiang, Wenwu Zou, Weifeng Zhang, Zhaoyuan Ou, Shengguang Qi, Tongmei Ma, Zhiming Cui, Zhenxing Liang, Li Du\",\"doi\":\"10.1002/aenm.202303672\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Rational regulation of the Li-ion (Li<sup>+</sup>) migration behaviors and charge distribution at the electrolyte–electrode interface is of great significance in pursuit of high-performance lithium metal battery (LMB) chemistry. Herein, unique locally-zwitterionic covalent organic framework nanosheets (ziCOFNs) are developed as Li<sup>+</sup> accelerated regulators, whose functions include not only kinetics-boosted Li<sup>+</sup> migration but also induces uniform charge distribution in LMBs. The zwitterions act as “dissociation enhancers” to trigger efficient Li<sup>+</sup> desolvation, while the abundant ─COO<sup>−</sup> units within the nanopores favor rapid Li<sup>+</sup> diffusion. In addition, the ordered ionic skeleton dynamically homogenizes the interfacial charge, thereby inhibiting Li dendrite growth and stabilizing the Li-interface chemistry. When implemented as a functional interlayer in the cell configuration, ziCOFNs display ultrahigh transfer number (0.84) and ionic conductivity beyond 4.5 mS cm<sup>−1</sup>. With such a layer, stable Li plating/stripping (over 6500 h) at 3 mA cm<sup>−2</sup> in symmetric cells, and superior long-term cycle performance in high-loading LiFePO<sub>4</sub> (9.4 mg cm<sup>−2</sup>) full cells are achieved. Detailed experimental characterizations combined with theoretical calculations elucidate the mechanism of the zwitterionic framework tuning Li<sup>+</sup> migration behaviors. This work is anticipated to shed fresh light on the exploration of zwitterionic crystalline materials in next-generation LMBs.</p>\",\"PeriodicalId\":111,\"journal\":{\"name\":\"Advanced Energy Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":24.4000,\"publicationDate\":\"2024-01-02\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Advanced Energy Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/aenm.202303672\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Advanced Energy Materials","FirstCategoryId":"88","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/aenm.202303672","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Lithium-Ion Accelerated Regulators by Locally-Zwitterionic Covalent Organic Framework Nanosheets
Rational regulation of the Li-ion (Li+) migration behaviors and charge distribution at the electrolyte–electrode interface is of great significance in pursuit of high-performance lithium metal battery (LMB) chemistry. Herein, unique locally-zwitterionic covalent organic framework nanosheets (ziCOFNs) are developed as Li+ accelerated regulators, whose functions include not only kinetics-boosted Li+ migration but also induces uniform charge distribution in LMBs. The zwitterions act as “dissociation enhancers” to trigger efficient Li+ desolvation, while the abundant ─COO− units within the nanopores favor rapid Li+ diffusion. In addition, the ordered ionic skeleton dynamically homogenizes the interfacial charge, thereby inhibiting Li dendrite growth and stabilizing the Li-interface chemistry. When implemented as a functional interlayer in the cell configuration, ziCOFNs display ultrahigh transfer number (0.84) and ionic conductivity beyond 4.5 mS cm−1. With such a layer, stable Li plating/stripping (over 6500 h) at 3 mA cm−2 in symmetric cells, and superior long-term cycle performance in high-loading LiFePO4 (9.4 mg cm−2) full cells are achieved. Detailed experimental characterizations combined with theoretical calculations elucidate the mechanism of the zwitterionic framework tuning Li+ migration behaviors. This work is anticipated to shed fresh light on the exploration of zwitterionic crystalline materials in next-generation LMBs.
期刊介绍:
Established in 2011, Advanced Energy Materials is an international, interdisciplinary, English-language journal that focuses on materials used in energy harvesting, conversion, and storage. It is regarded as a top-quality journal alongside Advanced Materials, Advanced Functional Materials, and Small.
With a 2022 Impact Factor of 27.8, Advanced Energy Materials is considered a prime source for the best energy-related research. The journal covers a wide range of topics in energy-related research, including organic and inorganic photovoltaics, batteries and supercapacitors, fuel cells, hydrogen generation and storage, thermoelectrics, water splitting and photocatalysis, solar fuels and thermosolar power, magnetocalorics, and piezoelectronics.
The readership of Advanced Energy Materials includes materials scientists, chemists, physicists, and engineers in both academia and industry. The journal is indexed in various databases and collections, such as Advanced Technologies & Aerospace Database, FIZ Karlsruhe, INSPEC (IET), Science Citation Index Expanded, Technology Collection, and Web of Science, among others.