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Bipolar Polymeric Protective Layer for Dendrite-Free and Corrosion-Resistant Lithium Metal Anode in Ethylene Carbonate Electrolyte
Authors:Dr. Chenglong Deng  Dr. Binbin Yang  Dr. Yaohui Liang  Dr. Yi Zhao  Boshun Gui  Dr. Chuanyu Hou  Dr. Yanxin Shang  Jinxiang Zhang  Dr. Tinglu Song  Prof. Xuzhong Gong  Prof. Nan Chen  Prof. Feng Wu  Prof. Renjie Chen
Affiliation:1. Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 China

Advanced Technology Research Institute, Beijing Institute of Technology, Jinan, 250300 China

Contribution: Conceptualization (lead), Data curation (lead), Formal analysis (lead), Project administration (equal), Software (lead), Writing - original draft (lead), Writing - review & editing (lead);2. Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 China

Contribution: Data curation (supporting), Software (supporting);3. Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 China

Contribution: Conceptualization (supporting), Data curation (supporting);4. Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 China

Advanced Technology Research Institute, Beijing Institute of Technology, Jinan, 250300 China

Contribution: Writing - original draft (supporting);5. Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 China

Contribution: Software (supporting);6. Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 China

Contribution: Data curation (equal), Software (supporting);7. Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 China

Advanced Technology Research Institute, Beijing Institute of Technology, Jinan, 250300 China

Contribution: Data curation (supporting);8. Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 China

Contribution: Data curation (supporting);9. School of Chemical Engineering, University of Chinese Academy of Sciences, Beijing, 100049 China;10. Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 China;11. Beijing Key Laboratory of Environmental Science and Engineering, School of Materials Science and Engineering, Beijing Institute of Technology, Beijing, 100081 China

Advanced Technology Research Institute, Beijing Institute of Technology, Jinan, 250300 China

Collaborative Innovation Center of Electric Vehicles in Beijing, Beijing, 100081 China

Contribution: Funding acquisition (supporting)

Abstract:The unstable interface between Li metal and ethylene carbonate (EC)-based electrolytes triggers continuous side reactions and uncontrolled dendrite growth, significantly impacting the lifespan of Li metal batteries (LMBs). Herein, a bipolar polymeric protective layer (BPPL) is developed using cyanoethyl (−CH2CH2C≡N) and hydroxyl (−OH) polar groups, aiming to prevent EC-induced corrosion and facilitating rapid, uniform Li+ ion transport. Hydrogen-bonding interactions between −OH and EC facilitates the Li+ desolvation process and effectively traps free EC molecules, thereby eliminating parasitic reactions. Meanwhile, the −CH2CH2C≡N group anchors TFSI anions through ion-dipole interactions, enhancing Li+ transport and eliminating concentration polarization, ultimately suppressing the growth of Li dendrite. This BPPL enabling Li|Li cell stable cycling over 750 cycles at 10 mA cm−2 for 2 mAh cm−2. The Li|LiNi0.8Mn0.1Co0.1O2 and Li|LiFePO4 full cells display superior electrochemical performance. The BPPL provides a practical strategy to enhanced stability and performance in LMBs application.
Keywords:Lithium metal anode  Bipolar polymeric protective layer  Hydrogen bond interaction  Ion-dipole interaction  Li+ desolvation
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