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Title: | Non-fluorinated ethers to mitigate electrode surface reactivity in high-voltage NCM811-Li batteries | Authors: | Wang, Z Che, X Wang, D Wang, Y He, X Zhu, Y Zhang, B |
Issue Date: | 17-Jun-2024 | Source: | Angewandte chemie international edition, 17 June 2024, v. 63, no. 25, e202404109 | Abstract: | Lithium (Li) metal batteries (LMBs) with nickel (Ni)-rich layered oxide cathodes exhibit twice the energy density of conventional Li-ion batteries. However, their lifespan is limited by severe side reactions caused by high electrode reactivity. Fluorinated solvent-based electrolytes can address this challenge, but they pose environmental and biological hazards. This work reports on the molecular engineering of fluorine (F)-free ethers to mitigate electrode surface reactivity in high-voltage Ni-rich LMBs. By merely extending the alkyl chains of traditional ethers, we effectively reduce the catalytic reactivity of the cathode towards the electrolyte at high voltages, which suppresses the oxidation decomposition of the electrolyte, microstructural defects and rock-salt phase formation in the cathode, and gas release issues. The high-voltage Ni-rich NCM811-Li battery delivers capacity retention of 80 % after 250 cycles with a high Coulombic efficiency of 99.85 %, even superior to that in carbonate electrolytes. Additionally, this strategy facilitates passivation of the Li anode by forming a robust solid-electrolyte interphase, boosting the Li reversibility to 99.11 % with a cycling life of 350 cycles, which outperforms conventional F-free ether electrolytes. Consequently, the lifespan of practical LMBs has been prolonged by over 100 % and 500 % compared to those in conventional carbonate- and ether-based electrolytes, respectively. | Keywords: | Cathode surface reactivity High-voltage batteries Ni−O bond covalency Non-fluorinated ethers Rock-salt phase formation |
Publisher: | Wiley-VCH | Journal: | Angewandte chemie international edition | ISSN: | 1433-7851 | EISSN: | 1521-3773 | DOI: | 10.1002/anie.202404109 | Rights: | © 2024 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH. This is an open access article under the terms of the Creative Commons Attribution Non-Commercial License (https://creativecommons.org/licenses/by-nc/4.0/), which permits use, distribution and reproduction in any medium, provided the original work is properly cited and is not used for commercial purposes. The following publication Z. Wang, X. Che, D. Wang, Y. Wang, X. He, Y. Zhu, B. Zhang, Angew. Chem. Int. Ed. 2024, 63, e202404109 is available at https://doi.org/10.1002/anie.202404109. |
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