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hybrid solid electrolyte enabled dendrite-free Li anodes for high-performance quasi-solid-state lithium-oxygen batteries

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National Science Review 2021年第2期8卷 123-133页

作者： Jin Wang Gang Huang Jun-Min Yan Jin-Ling Ma Tong Liu Miao-Miao Shi Yue Yu Miao-Miao Zhang Ji-Lin Tang Xin-Bo Zhang Key Laboratory of Automobile Materials Ministry of EducationDepartment of Materials Science and EngineeringJilin University State Key Laboratory of Rare Earth Resource Utilization Changchun Institute of Applied ChemistryChinese Academy of Sciences Materials Science and Engineering Physical Science and Engineering DivisionKing Abdullah University of Science and Technology State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of Sciences

The dendrite growth of Li anodes severely degrades the performance of lithium-oxygen(Li-O2) batteries.Recently, hybrid solid electrolyte(HSE) has been regarded as one of the most promising routes to tackle this problem. However, before this is realized, the HSE needs to simultaneously satisfy contradictory requirements of high modulus and even, flexible contact with Li anode, while ensuring uniform Li+distribution. To tackle this complex dilemma, here, an HSE with rigid Li1.5Al0.5Ge1.5(PO4)3(LAGP)core@ultrathin flexible poly(vinylidene fluoride-hexafluoropropylene)(PVDF-HFP) shell interface has been developed. The introduced large amount of nanometer-sized LAGP cores can not only act as structural enhancer to achieve high Young’s modulus but can also construct Li+diffusion network to homogenize Li+distribution. The ultrathin flexible PVDF-HFP shell provides soft and stable contact between the rigid core and Li metal without affecting the Li+distribution, meanwhile suppressing the reduction of LAGP induced by direct contact with Li metal. Thanks to these advantages, this ingenious HSE with ultra-high Young’s modulus of 25 GPa endows dendrite-free Li deposition even at a deposition capacity of 23.6 m Ah.Moreover, with the successful inhibition of Li dendrites, the HSE-based quasi-solid-state Li-O2battery delivers a long cycling stability of 146 cycles, which is more than three times that of gel polymer electrolyte-based Li-O2battery. This new insight may serve as a starting point for further designing of HSE in Li-O2batteries, and can also be extended to various battery systems such as sodium-oxygen batteries.

关键词： lithium-oxygen batteries dendrite suppression Li anodes hybrid solid electrolyte LAGP PVDF-HFP

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