High‐Energy LiNiO2 Li Metal Batteries Enabled by Hybrid Electrolyte Consisting of Ionic Liquid and Weakly Solvating Fluorinated Ether
Abstract In pursuit of the highest possible energy density, researchers shift their focus to the ultimate anode material, lithium metal (Li0), and high‐capacity cathode materials with high nickel content (Ni > 80%). The combination of these aggressive electrodes presents unprecedented challenges...
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Wiley
2024-12-01
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| Online Access: | https://doi.org/10.1002/advs.202409662 |
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| author | Qian Liu Jiayi Xu Wei Jiang Jihyeon Gim Adam P. Tornheim Rajesh Pathak Qijia Zhu Peng Zuo Zhenzhen Yang Krzysztof Z. Pupek Eungje Lee Chongmin Wang Cong Liu Jason R. Croy Kang Xu Zhengcheng Zhang |
| author_facet | Qian Liu Jiayi Xu Wei Jiang Jihyeon Gim Adam P. Tornheim Rajesh Pathak Qijia Zhu Peng Zuo Zhenzhen Yang Krzysztof Z. Pupek Eungje Lee Chongmin Wang Cong Liu Jason R. Croy Kang Xu Zhengcheng Zhang |
| author_sort | Qian Liu |
| collection | DOAJ |
| description | Abstract In pursuit of the highest possible energy density, researchers shift their focus to the ultimate anode material, lithium metal (Li0), and high‐capacity cathode materials with high nickel content (Ni > 80%). The combination of these aggressive electrodes presents unprecedented challenges to the electrolyte. Here, we report a hybrid electrolyte consisting of a highly fluorinated ionic liquid and a weakly solvating fluorinated ether, whose hybridization structure enables the reversible operation of a battery chemistry based on Li0 and LiNiO2 (Ni = 100%), delivering nearly theoretical capacity of the latter (up to 249 mAh g−1) for >300 cycles with retention of 78.6% and in absence of unwanted morphological changes in both electrodes. Extensive characterization assisted by molecular dynamic simulation and density functional theory calculations reveals the function of the fluorinated ether to be far more profound than simple dilution and viscosity reduction. Instead, it induces drastic changes in Li+‐solvation environment, the consequence of which engenders simultaneous stabilization of electrode/electrolyte and interfacing via formation of respective interfacial chemistries. This study further unlocks fundamental knowledge underneath the prevailing “diluent strategy” that is extensively applied by the electrolyte researchers and opens more design space for the next‐generation electrolytes and interphases for these coveted battery chemistries. |
| format | Article |
| id | doaj-art-af44ce126dd145fe95f594f7641bd72c |
| institution | Kabale University |
| issn | 2198-3844 |
| language | English |
| publishDate | 2024-12-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj-art-af44ce126dd145fe95f594f7641bd72c2024-12-11T16:00:49ZengWileyAdvanced Science2198-38442024-12-011146n/an/a10.1002/advs.202409662High‐Energy LiNiO2 Li Metal Batteries Enabled by Hybrid Electrolyte Consisting of Ionic Liquid and Weakly Solvating Fluorinated EtherQian Liu0Jiayi Xu1Wei Jiang2Jihyeon Gim3Adam P. Tornheim4Rajesh Pathak5Qijia Zhu6Peng Zuo7Zhenzhen Yang8Krzysztof Z. Pupek9Eungje Lee10Chongmin Wang11Cong Liu12Jason R. Croy13Kang Xu14Zhengcheng Zhang15Chemical Sciences and Engineering Division Argonne National Laboratory 9700 S. Cass Ave. Lemont IL 60439 USAChemical Sciences and Engineering Division Argonne National Laboratory 9700 S. Cass Ave. Lemont IL 60439 USAComputational Science Division Argonne National Laboratory 9700 S. Cass Ave. Lemont IL 60439 USAChemical Sciences and Engineering Division Argonne National Laboratory 9700 S. Cass Ave. Lemont IL 60439 USAChemical Sciences and Engineering Division Argonne National Laboratory 9700 S. Cass Ave. Lemont IL 60439 USAApplied Material Division Argonne National Laboratory 9700 S. Cass Ave. Lemont IL 60439 USAChemical Sciences and Engineering Division Argonne National Laboratory 9700 S. Cass Ave. Lemont IL 60439 USAEnvironmental Molecular Sciences Laboratory Pacific Northwest National Laboratory Richland WA 99352 USAChemical Sciences and Engineering Division Argonne National Laboratory 9700 S. Cass Ave. Lemont IL 60439 USAApplied Material Division Argonne National Laboratory 9700 S. Cass Ave. Lemont IL 60439 USAChemical Sciences and Engineering Division Argonne National Laboratory 9700 S. Cass Ave. Lemont IL 60439 USAEnvironmental Molecular Sciences Laboratory Pacific Northwest National Laboratory Richland WA 99352 USAChemical Sciences and Engineering Division Argonne National Laboratory 9700 S. Cass Ave. Lemont IL 60439 USAChemical Sciences and Engineering Division Argonne National Laboratory 9700 S. Cass Ave. Lemont IL 60439 USABattery Science Branch Energy Science Division Sensor and Electron Devices Directorate U.S. Army Research Laboratory Adelphi MD 20783 USAChemical Sciences and Engineering Division Argonne National Laboratory 9700 S. Cass Ave. Lemont IL 60439 USAAbstract In pursuit of the highest possible energy density, researchers shift their focus to the ultimate anode material, lithium metal (Li0), and high‐capacity cathode materials with high nickel content (Ni > 80%). The combination of these aggressive electrodes presents unprecedented challenges to the electrolyte. Here, we report a hybrid electrolyte consisting of a highly fluorinated ionic liquid and a weakly solvating fluorinated ether, whose hybridization structure enables the reversible operation of a battery chemistry based on Li0 and LiNiO2 (Ni = 100%), delivering nearly theoretical capacity of the latter (up to 249 mAh g−1) for >300 cycles with retention of 78.6% and in absence of unwanted morphological changes in both electrodes. Extensive characterization assisted by molecular dynamic simulation and density functional theory calculations reveals the function of the fluorinated ether to be far more profound than simple dilution and viscosity reduction. Instead, it induces drastic changes in Li+‐solvation environment, the consequence of which engenders simultaneous stabilization of electrode/electrolyte and interfacing via formation of respective interfacial chemistries. This study further unlocks fundamental knowledge underneath the prevailing “diluent strategy” that is extensively applied by the electrolyte researchers and opens more design space for the next‐generation electrolytes and interphases for these coveted battery chemistries.https://doi.org/10.1002/advs.202409662ionic liquidLi metalLiNiO2MD simulation |
| spellingShingle | Qian Liu Jiayi Xu Wei Jiang Jihyeon Gim Adam P. Tornheim Rajesh Pathak Qijia Zhu Peng Zuo Zhenzhen Yang Krzysztof Z. Pupek Eungje Lee Chongmin Wang Cong Liu Jason R. Croy Kang Xu Zhengcheng Zhang High‐Energy LiNiO2 Li Metal Batteries Enabled by Hybrid Electrolyte Consisting of Ionic Liquid and Weakly Solvating Fluorinated Ether Advanced Science ionic liquid Li metal LiNiO2 MD simulation |
| title | High‐Energy LiNiO2 Li Metal Batteries Enabled by Hybrid Electrolyte Consisting of Ionic Liquid and Weakly Solvating Fluorinated Ether |
| title_full | High‐Energy LiNiO2 Li Metal Batteries Enabled by Hybrid Electrolyte Consisting of Ionic Liquid and Weakly Solvating Fluorinated Ether |
| title_fullStr | High‐Energy LiNiO2 Li Metal Batteries Enabled by Hybrid Electrolyte Consisting of Ionic Liquid and Weakly Solvating Fluorinated Ether |
| title_full_unstemmed | High‐Energy LiNiO2 Li Metal Batteries Enabled by Hybrid Electrolyte Consisting of Ionic Liquid and Weakly Solvating Fluorinated Ether |
| title_short | High‐Energy LiNiO2 Li Metal Batteries Enabled by Hybrid Electrolyte Consisting of Ionic Liquid and Weakly Solvating Fluorinated Ether |
| title_sort | high energy linio2 li metal batteries enabled by hybrid electrolyte consisting of ionic liquid and weakly solvating fluorinated ether |
| topic | ionic liquid Li metal LiNiO2 MD simulation |
| url | https://doi.org/10.1002/advs.202409662 |
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