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Efficiencies of Various in situ Polymerizations of Liquid Electrolytes and the Practical Implications for Quasi Solid-state Batteries
Authors:Dr Peiying Li  Shuya Wang  Jinjin Hao  Xiang Wang  Prof Shu-Meng Hao  Yuhao Lu  Prof Hong Li  Prof Weidong Zhou  Dr Yuliang Li
Institution:1. State Key Laboratory of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 China

These authors contributed equally to this work.

Contribution: Data curation (lead), ​Investigation (lead);2. State Key Laboratory of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 China

These authors contributed equally to this work.

Contribution: ​Investigation (equal);3. State Key Laboratory of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 China

Contribution: ​Investigation (equal);4. Ningde Amperex Technology Limited (ATL), Key Laboratory of Consumer Lithium-Ion Battery in Fujian, Fujian, 352100 China

Contribution: Writing - review & editing (supporting);5. State Key Laboratory of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 China;6. Ningde Amperex Technology Limited (ATL), Key Laboratory of Consumer Lithium-Ion Battery in Fujian, Fujian, 352100 China

Contribution: Writing - review & editing (equal);7. Key Laboratory for Renewable Energy, Institute of Physics, Chinese Academy of Sciences, Beijing, 100190 China

Contribution: Writing - review & editing (equal);8. Key Laboratory of Organic Solids, Institute of Chemistry, Chinese Academy of Sciences, Beijing, 100190 China

Contribution: Supervision (equal), Writing - review & editing (equal)

Abstract:In situ polymerization of liquid electrolytes is currently the most feasible way for constructing solid-state batteries, which, however, is affected by various interfering factors of reactions and so the electrochemical performance of cells. To disclose the effects from polymerization conditions, two types of generally used in situ polymerizing reactions of ring-opening polymerization (ROP) and double bond radical polymerization (DBRP) were investigated on the aspects of monomer conversion and electrochemical properties (Li+-conductivity and interfacial stability). The ROP generated poly-ester and poly-carbonate show a high monomer conversion of ≈90 %, but suffer a poor Li+-conductivity of lower than 2×10−5 S cm−1 at room temperature (RT). Additionally, the terminal alkoxy anion derived from the ROP is not resistant to high-voltage cathodes. While, the DBRP produced poly-VEC(vinyl ethylene carbonate) and poly-VC(vinylene carbonate) show lower monomer conversions of 50–80 %, delivering relatively higher Li+-conductivities of 2×10−4 S cm−1 at RT. Compared two polymerizing reactions and four monomers, the VEC-based F-containing copolymer possesses advantages in Li+-conductivity and antioxidant capacity, which also shows simultaneous stability towards Li-metal with the help of LiF-based passivating layer, allowing a long-term stable cycling of high-voltage quasi solid-state cells.
Keywords:Double Bond Radical Polymerization  In-Situ Solidification  Interface  Ring-Opening Polymerization  Solid-State Batteries
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