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Angew Chem Int Ed Engl. 2019 Apr 23;58(18):6001-6006. doi: 10.1002/anie.201901582. Epub 2019 Mar 26.

Stable Conversion Chemistry-Based Lithium Metal Batteries Enabled by Hierarchical Multifunctional Polymer Electrolytes with Near-Single Ion Conduction.

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Centre for Clean Energy Technology, School of Mathematical and Physical Sciences, University of Technology Sydney, Sydney, NSW, 2007, Australia.
CIC ENERGIGUNE, Parque Tecnológico de Álava, Miñano, 01510, Spain.
College of Material Science and Engineering, Nanjing University of Aeronautics and Astronautics, Nanjing, 210006, P. R. China.


The low Coulombic efficiency and serious safety issues resulting from uncontrollable dendrite growth have severely impeded the practical applications of lithium (Li) metal anodes. Herein we report a stable quasi-solid-state Li metal battery by employing a hierarchical multifunctional polymer electrolyte (HMPE). This hybrid electrolyte was fabricated via in situ copolymerizing lithium 1-[3-(methacryloyloxy)propylsulfonyl]-1-(trifluoromethanesulfonyl)imide (LiMTFSI) and pentaerythritol tetraacrylate (PETEA) monomers in traditional liquid electrolyte, which is absorbed in a poly(3,3-dimethylacrylic acid lithium) (PDAALi)-coated glass fiber membrane. The well-designed HMPE simultaneously exhibits high ionic conductivity (2.24×10-3  S cm-1 at 25 °C), near-single ion conducting behavior (Li ion transference number of 0.75), good mechanical strength and remarkable suppression for Li dendrite growth. More intriguingly, the cation permselective HMPE efficiently prevents the migration of negatively charged iodine (I) species, which provides the as-developed Li-I batteries with high capacity and long cycling stability.


hierarchical structure; iodine cathode; lithium metal battery; near-single ion conduction; polymer electrolyte


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