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Bifunctional flame retardant solid-state electrolyte toward safe li metal batteries

能源化学:英文版 2023年第6期81卷 613-622,I0014页

作者： Qiang Lv Yajie Song Bo Wang Shangjie Wang Bochen Wu Yutong Jing Huaizheng Ren Shengbo Yang Lei Wang lihui Xiao Dianlong Wang Huakun liu Shixue Dou MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage State Key Laboratory of Urban Water Resource and EnvironmentSchool of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina School of Chemistry and Chemical Engineering Harbin Institute of TechnologyHarbin 150001HeilongjiangChina Institute for Superconducting&Electronic Materials Australian Institute of Innovative MaterialsUniversity of WollongongWollongongNSW 2500Australia Institute of Energy Material Science University of Shanghai for Science and TechnologyShanghai 200093China

Solid polymer electrolytes(SPEs)are one of the most promising alternatives to flammable liquid electrolytes for building safe li metal batteries.Nevertheless,the poor ionic conductivity at room temperature(RT)and low resistance to li dendrites seriously hinder the commercialization of SPEs.Herein,we design a bifunctional flame retardant SPE by combining hydroxyapatite(HAP)nanomaterials with Nmethyl pyrrolidone(NMP)in the PVDF-HFP matrix.The addition of HAP generates a hydrogen bond network with the PVDF-HFP matrix and cooperates with NMP to facilitate the dissociation of li TFSI in the PVDF-HFP matrix.Consequently,the prepared SPE demonstrates superior ionic conductivity at RT,excellent fireproof properties,and strong resistance to li dendrites.The assembled li symmetric cell with prepared SPE exhibits a stable cycling performance of over 1200 h at 0.2 m A cm^(-2),and the solid-state liFePO_4||li cell shows excellent capacity retention of 85.3%over 600 cycles at 0.5 C.

关键词： Solid polymer electrolytes safe li metal batteries li dendrites Hydroxyapatite N-methyl pyrrolidone PVDF-HFP Fireproof property

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Synergistic coupling among Mg_(2)B_(2)O_(5),polycarbonate and N,Ndimethylformamide enhances the electrochemical performance of PVDF-HFP-based solid electrolyte

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Journal of Energy Chemistry 2024年第7期94卷 158-168页

作者： Yutong Jing Qiang Lv Yujia Chen Bo Wang Bochen Wu Cheng li Shengbo Yang Zhipeng He Dianlong Wang Huakun liu Shixue Dou MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage State Key Laboratory of Urban Water Resource and EnvironmentSchool of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina Institute of Energy Material Science University of Shanghai for Science and TechnologyShanghai 200093China Institute for Superconducting&Electronic Materials Australian Institute of Innovative MaterialsUniversity of WollongongWollongongNSW 2500Australia

Polymer solid electrolytes(SPEs)based on the[solvate-li+]complex structure have promising prospects in lithium metal batteries(LMBs)due to their unique ion transport mechanism.However,the solvation structure may compromise the mechanical performance and safety,hindering practical application of SPEs.In this work,a composite solid electrolyte(CSE)is designed through the organic-inorganic syner-gistic interaction among N,N-dimethylformamide(DMF),polycarbonate(PC),and Mg_(2)B_(2)O_(5) in poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP).Flame-retardant Mg_(2)B_(2)O_(5) nanowires provide non-flammability to the prepared CSEs,and the addition of PC improves the dispersion of Mg_(2)B_(2)O_(5) nanowires.Simultaneously,the organic-inorganic synergistic action of PC plasticizer and Mg_(2)B_(2)O_(5) nanowires pro-motes the dissociation degree of liTFSI and reduces the crystallinity of PVDF-HFP,enabling rapid li ion transport.Additionally,Raman spectroscopy and DFT calculations confirm the coordination between Mg atoms in Mg_(2)B_(2)O_(5) and N atoms in DMF,which exhibits Lewis base-like behavior attacking adjacent C-F and C-H bonds in PVDF-HFP while inducing dehydrofluorination of PVDF-HFP.Based on the syner-gistic coupling of Mg_(2)B_(2)O_(5),PC,and DMF in the PVDF-HFP matrix,the prepared CSE exhibits superior ion conductivity(9.78×10^(-4) s cm^(-1)).The assembled li symmetric cells cycle stably for 3900 h at a current density of 0.1 mA cm^(-2) without short circuit.The LFP||li cells assembled with PDL-Mg_(2)B_(2)O_(5)/PC CSEs show excellent rate capability and cycling performance,with a capacity retention of 83.3%after 1000 cycles at 0.5 C.This work provides a novel approach for the practical application of organic-inorganic Synergistic CSEs in LMBs.

关键词： Composite solid electrolytes safe li metal batteries Synergistic coupling effect Poly(vinylidene fluoride-co-hexafluoropro pylene)

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