UV-Cross-Linked Composite Polymer Electrolyte for High-Rate, Ambient Temperature Lithium Batteries

We report an innovative cross-linked composite polymer electrolyte (CPE) based on the garnet-type ceramic super Li+ ion conductor, Li7La3Zr2O12 (LLZO), that is encompassed in a supersoft poly(ethylene oxide)/tetraglyme matrix. UV-induced, facile and solvent-free cross-linking process ensures flexible and self-standing CPEs, which are nonflammable and perfectly shape-retaining under thermal/mechanical stress. The CPEs exhibit high ionic conductivity, exceeding 0.1 mS cm–1 at 20 °C, suitable for ambient and subambient temperature operation. Lab-scale lithium metal polymer cells assembled with LiFePO4-based composite cathode and the optimized CPE deliver full capacity at low current rates and outstanding specific discharge capacity of 115 mAh g–1 at 1C rate and ambient temperature. Remarkably, the lithium metal cell can run for hundreds of galvanostatic cycles (>400) with low overpotential, limited fading, and excellent Coulombic efficiency (>99%), which postulates the practical application of the newly deve...

[1]  P. V. Wright,et al.  Complexes of alkali metal ions with poly(ethylene oxide) , 1973 .

[2]  F. Jiang,et al.  Elucidating the Performance Limitations of Lithium-ion Batteries due to Species and Charge Transport through Five Characteristic Parameters , 2016, Scientific Reports.

[3]  S. Passerini,et al.  Hybrid electrolytes for lithium metal batteries , 2018, Journal of Power Sources.

[4]  Scott J. Litzelman,et al.  Status and challenges in enabling the lithium metal electrode for high-energy and low-cost rechargeable batteries , 2022, Nature Energy.

[5]  Candace K. Chan,et al.  Nanostructured Garnet-type Li7La3Zr2O12: Synthesis, Properties, and Opportunities as Electrolytes for Li-ion Batteries , 2017 .

[6]  Alain Guyot,et al.  Polymer electrolytes , 1985, Polymer Bulletin.

[7]  Yutao Li,et al.  Electrochemical Nature of the Cathode Interface for a Solid-State Lithium-Ion Battery: Interface between LiCoO2 and Garnet-Li7La3Zr2O12 , 2016 .

[8]  J. Nowiński,et al.  Crystalline phases, morphology and conductivity of PEO:LiTFSI electrolytes in the eutectic region , 2006 .

[9]  David P. Wilkinson,et al.  Recent advances in all-solid-state rechargeable lithium batteries , 2017 .

[10]  Rui Zhang,et al.  An anion-immobilized composite electrolyte for dendrite-free lithium metal anodes , 2017, Proceedings of the National Academy of Sciences.

[11]  Yan‐Bing He,et al.  Challenges and perspectives of garnet solid electrolytes for all solid-state lithium batteries , 2018, Journal of Power Sources.

[12]  M. Armand,et al.  Issues and challenges facing rechargeable lithium batteries , 2001, Nature.

[13]  Diana Golodnitsky,et al.  The sei model—application to lithium-polymer electrolyte batteries , 1995 .

[14]  Miao Zhang,et al.  Flexible and ion-conducting membrane electrolytes for solid-state lithium batteries: Dispersion of garnet nanoparticles in insulating polyethylene oxide , 2016 .

[15]  B. Scrosati,et al.  Lithium batteries: Status, prospects and future , 2010 .

[16]  N. Brandon,et al.  Peculiarities of ion transport in confined-in-ceramics concentrated polymer electrolytes , 2016 .

[17]  Yue Qi,et al.  Simulation of the effect of contact area loss in all-solid-state Li-ion batteries , 2017 .

[18]  Venkataraman Thangadurai,et al.  Fast Lithium Ion Conduction in Garnet‐Type Li7La3Zr2O12 , 2007 .

[19]  N. Zhao,et al.  Composite electrolytes of polyethylene oxides/garnets interfacially wetted by ionic liquid for room-temperature solid-state lithium battery , 2017 .

[20]  Jin Zheng,et al.  New Insights into the Compositional Dependence of Li-Ion Transport in Polymer-Ceramic Composite Electrolytes. , 2018, ACS applied materials & interfaces.

[21]  Lucienne Buannic,et al.  Investigating the Dendritic Growth during Full Cell Cycling of Garnet Electrolyte in Direct Contact with Li Metal. , 2017, ACS applied materials & interfaces.

[22]  F. Bella,et al.  Super Soft All-Ethylene Oxide Polymer Electrolyte for Safe All-Solid Lithium Batteries , 2016, Scientific Reports.

[23]  Steven D. Lacey,et al.  Toward garnet electrolyte–based Li metal batteries: An ultrathin, highly effective, artificial solid-state electrolyte/metallic Li interface , 2017, Science Advances.

[24]  Biyi Xu,et al.  Stability of garnet-type Li ion conductors: An overview , 2017 .