Cationic Covalent Organic Framework with Ultralow HOMO Energy Used as Scaffolds for 5.2 V Solid Polycarbonate Electrolytes
Abstract Solid polymer electrolytes (SPEs) have become promising candidate to replace common liquid electrolyte due to highly improved security. However, the practical use of SPEs is still restricted by their decomposition and breakage at the electrode interfacial layer especially at high voltage. H...
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| Format: | Article |
| Language: | English |
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Wiley
2022-07-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202200390 |
| _version_ | 1818043592108670976 |
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| author | Jie Liu Yuhao Zhang Haoqing Ji Jing Zhang Pinxin Zhou Yufeng Cao Jinqiu Zhou Chenglin Yan Tao Qian |
| author_facet | Jie Liu Yuhao Zhang Haoqing Ji Jing Zhang Pinxin Zhou Yufeng Cao Jinqiu Zhou Chenglin Yan Tao Qian |
| author_sort | Jie Liu |
| collection | DOAJ |
| description | Abstract Solid polymer electrolytes (SPEs) have become promising candidate to replace common liquid electrolyte due to highly improved security. However, the practical use of SPEs is still restricted by their decomposition and breakage at the electrode interfacial layer especially at high voltage. Herein, a new cationic covalent organic framework (COF) is designed and synthesized as a reinforced skeleton to resist the constant oxidative decomposition of solid polycarbonate electrolyte, which can stabilize cathode electrolyte interphase layer to develop long‐term cycle solid lithium metal battery. The ultralow HOMO energy (−12.55 eV according to density functional theory (DFT) calculations), reflecting its oxidation resistance at positive potential, would be responsible for the high decomposition voltage of 5.2 V versus Li+/Li of solid polycarbonate electrolyte. Furthermore, the smooth surface of interfacial layer and inhibited decomposition reaction at cathode side is confirmed in solid LiCoO2 cell, which realizes high initial capacity up to 160.3 mAh g−1 at 0.1 C and greatly improved stability in 4.5 V class solid polymer lithium metal battery with high capacity retention over 200 cycles. This new type of high‐voltage resistant solid polymer electrolyte promotes the realization of high‐voltage cathode materials and higher energy density lithium metal battery. |
| first_indexed | 2024-12-10T09:04:39Z |
| format | Article |
| id | doaj.art-e00a82ad40074eaca41c87d83d259c8e |
| institution | Directory Open Access Journal |
| issn | 2198-3844 |
| language | English |
| last_indexed | 2024-12-10T09:04:39Z |
| publishDate | 2022-07-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj.art-e00a82ad40074eaca41c87d83d259c8e2022-12-22T01:55:10ZengWileyAdvanced Science2198-38442022-07-01921n/an/a10.1002/advs.202200390Cationic Covalent Organic Framework with Ultralow HOMO Energy Used as Scaffolds for 5.2 V Solid Polycarbonate ElectrolytesJie Liu0Yuhao Zhang1Haoqing Ji2Jing Zhang3Pinxin Zhou4Yufeng Cao5Jinqiu Zhou6Chenglin Yan7Tao Qian8School of Chemistry and Chemical Engineering Nantong University Nantong 226019 ChinaKey Laboratory of Core Technology of High Specific Energy Battery and Key Materials for Petroleum and Chemical Industry College of Energy Soochow University Suzhou 215006 ChinaKey Laboratory of Core Technology of High Specific Energy Battery and Key Materials for Petroleum and Chemical Industry College of Energy Soochow University Suzhou 215006 ChinaState Key Laboratory of Space Power‐sources Technology Shanghai Institute of Space Power‐Sources Shanghai 200245 ChinaState Key Laboratory of Space Power‐sources Technology Shanghai Institute of Space Power‐Sources Shanghai 200245 ChinaSchool of Chemistry and Chemical Engineering Nantong University Nantong 226019 ChinaSchool of Chemistry and Chemical Engineering Nantong University Nantong 226019 ChinaKey Laboratory of Core Technology of High Specific Energy Battery and Key Materials for Petroleum and Chemical Industry College of Energy Soochow University Suzhou 215006 ChinaSchool of Chemistry and Chemical Engineering Nantong University Nantong 226019 ChinaAbstract Solid polymer electrolytes (SPEs) have become promising candidate to replace common liquid electrolyte due to highly improved security. However, the practical use of SPEs is still restricted by their decomposition and breakage at the electrode interfacial layer especially at high voltage. Herein, a new cationic covalent organic framework (COF) is designed and synthesized as a reinforced skeleton to resist the constant oxidative decomposition of solid polycarbonate electrolyte, which can stabilize cathode electrolyte interphase layer to develop long‐term cycle solid lithium metal battery. The ultralow HOMO energy (−12.55 eV according to density functional theory (DFT) calculations), reflecting its oxidation resistance at positive potential, would be responsible for the high decomposition voltage of 5.2 V versus Li+/Li of solid polycarbonate electrolyte. Furthermore, the smooth surface of interfacial layer and inhibited decomposition reaction at cathode side is confirmed in solid LiCoO2 cell, which realizes high initial capacity up to 160.3 mAh g−1 at 0.1 C and greatly improved stability in 4.5 V class solid polymer lithium metal battery with high capacity retention over 200 cycles. This new type of high‐voltage resistant solid polymer electrolyte promotes the realization of high‐voltage cathode materials and higher energy density lithium metal battery.https://doi.org/10.1002/advs.202200390cationic covalent organic frameworkhigh decomposition voltagelithium metal batterysolid polymer electrolyte |
| spellingShingle | Jie Liu Yuhao Zhang Haoqing Ji Jing Zhang Pinxin Zhou Yufeng Cao Jinqiu Zhou Chenglin Yan Tao Qian Cationic Covalent Organic Framework with Ultralow HOMO Energy Used as Scaffolds for 5.2 V Solid Polycarbonate Electrolytes Advanced Science cationic covalent organic framework high decomposition voltage lithium metal battery solid polymer electrolyte |
| title | Cationic Covalent Organic Framework with Ultralow HOMO Energy Used as Scaffolds for 5.2 V Solid Polycarbonate Electrolytes |
| title_full | Cationic Covalent Organic Framework with Ultralow HOMO Energy Used as Scaffolds for 5.2 V Solid Polycarbonate Electrolytes |
| title_fullStr | Cationic Covalent Organic Framework with Ultralow HOMO Energy Used as Scaffolds for 5.2 V Solid Polycarbonate Electrolytes |
| title_full_unstemmed | Cationic Covalent Organic Framework with Ultralow HOMO Energy Used as Scaffolds for 5.2 V Solid Polycarbonate Electrolytes |
| title_short | Cationic Covalent Organic Framework with Ultralow HOMO Energy Used as Scaffolds for 5.2 V Solid Polycarbonate Electrolytes |
| title_sort | cationic covalent organic framework with ultralow homo energy used as scaffolds for 5 2 v solid polycarbonate electrolytes |
| topic | cationic covalent organic framework high decomposition voltage lithium metal battery solid polymer electrolyte |
| url | https://doi.org/10.1002/advs.202200390 |
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