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Solvation Sheath Engineering by Multivalent Cations Enabling Multifunctional SEI for Fast-Charging Lithium-Metal Batteries

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ACS APPLIED MATERIALS & INTERFACES
卷 15, 期 49, 页码 57110-57118

出版社

AMER CHEMICAL SOC
DOI: 10.1021/acsami.3c13306

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lithium-metal batteries; fast-charging; multifunctional SEI; solvation sheath; LiNO3; aluminum ethoxide

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Researchers have successfully established an ideal solid electrolyte interface by tuning the solvation structure of Li+ ions, enabling the uniform deposition of lithium metal and improving the Coulombic efficiency and cycling performance of lithium metal batteries.
With the pursuit of high energy and power density, the fast-charging capability of lithium-metal batteries has progressively been the primary focus of attention. To prevent the formation of lithium dendrites during fast charging, the ideal solid electrolyte interphase should be capable of concurrent fast Li+ transport and uniform nucleation sites; however, its construction in a facile manner remains a challenge. Here, as Al3+ has a higher charge and Al metal is lithiophilic, we tuned the Li+ solvation structure by introducing LiNO3 and aluminum ethoxide together, resulting in the dissolution of LiNO3 and the simultaneous generation of fast ionic conductor and lithiophilic sites. Consequently, our approach facilitated the deposition of lithium metal in a uniform and chunky way, even at a high current density. As a result, the Coulombic efficiency of the Li||Cu cell increased to over 99%. Moreover, the Li||LiFePO4 full cell demonstrated significantly enhanced cycling performance with a remarkable capacity retention of 94.5% at 4 C, far superior to the 46.1% capacity retention observed with the base electrolyte.

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