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Catalytic anode surface enabling in situ polymerization of gel polymer electrolyte for stable Li metal batteries

Nano Research 2024年第6期17卷 5216-5223页

作者： Guocheng Li Kang Liang Yuanjian Li Xiangrui Duan Lin Fu Zhao Cai Zhaofu Zhang Jiangnan Dai Yongming Sun Wuhan National Laboratory for Optoelectronics Huazhong University of Science and TechnologyWuhan 430074China The Institute of Technological Sciences Wuhan UniversityWuhan 430074China Faculty of Materials Science and Chemistry China University of Geoscience(Wuhan)Wuhan 430074China

Employing quasi-solid-state gel polymer electrolyte(GPE)instead of the liquid counterpart has been regarded as a promising strategy for improving the electrochemical performance of Li metal batteries.However,the poor and uneven interfacial contact between Li metal anode and GPE could cause large interfacial resistance and electrochemical Li stripping/plating inhomogeneity,deteriorating the electrochemical performance.Herein,we proposed that the functional component of composite anode could work as the catalyst to promote the in situ polymerization reaction,and we experimentally realized the integration of polymerized-dioxolane electrolyte and Li/Li_(22)Sn_(5)/LiF composite electrode with low interfacial resistance and good stability by in situ catalyzation polymerization.Thus,the reaction kinetics and stability of metallic Li anode were significantly enhanced.As a demonstration,symmetric cell using such a GPE-Li/Li_(22)Sn_(5)/LiF integration achieved stable cycling beyond 250 cycles with small potential hysteresis of 25 mV at 1 mA·cm^(−2)and 1 mAh·cm^(−2),far outperforming the counterpart regular GPE on pure Li.Paired with LiNi0.5Co0.3Mn0.2O2,the full cell with the GPE-Li/Li_(22)Sn_(5)/LiF integration maintained 85.7%of the original capacity after 100 cycles at 0.5 C(1 C=200 mA·g^(−1)).Our research provides a promising strategy for reducing the resistance between GPE and Li metal anode,and realizes Li metal batteries with enhance electrochemical performance.

关键词： catalyzation polymerization interface resistance interfacial stability Li metal batteries electrochemical performance

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A lithium–tin fluoride anode enabled by ionic/electronic conductive paths for garnet-based solid-state lithium metal batteries

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Rare Metals 2024年第2期43卷 575-587页

作者： Lei Zhang Qian-Kun Meng Xiang-Ping Feng Ming Shen Yu-Qing Zhang Quan-Chao Zhuang Run-Guo Zheng Zhi-Yuan Wang Yan-Hua Cui Hong-Yu Sun Yan-Guo Liu School of Materials Science and Engineering Northeastern UniversityShenyang110819China School of Resources and Materials Northeastern University at QinhuangdaoQinhuangdao066004China School of Materials and Physics China University of Mining&TechnologyXuzhou221116China Institute of Electronic Engineering China Academy of Engineering PhysicsMianyang621900China

The high energy density and stability of solid-state lithium metal batteries(SSLMBs)have garnered great ***-type oxides,especially Li_(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO),with high ionic conductivity,wide electrochemical window,and stability to Li metal anode,are promising solid-state electrolyte(SSEs)materials for SSLMBs.However,Li/LLZTO interface issues including high interface resistance,inhomogeneous Li deposition,and Li dendrite growth have hindered the practical application of SSLMBs.Herein,a multi-functional Li–SnF_(2) composite anode with Li,LiF,and Li-Sn alloy was specifically designed and prepared.The composite anode improves the wettability to LLZTO,constructing an intimate contact interface between it and LLZTO.Meanwhile,ionic/electronic conductive paths in situ formed at the interface can effectively uniform Li deposition and suppress Li dendrite.The solid-state symmetric cell exhibits low interface resistance(11Ω·cm^(2)) and high critical current density(1.3 mA·cm^(−2))at 25℃.The full SSLMB based on LiFePO_(4) or LiNi_(0.5)Co_(0.2)Mn_(0.3)O_(2) cathode also shows stable cycling performance and high rate capability.This work provides a new composite anode strategy for achieving high-energy density and high-safety SSLMBs.

关键词： Solid-state lithium metal batteries(SSLMBs) Lithium-tin fluoride anode Ionic/electronic conductive interface resistance Lithium dendrite

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