Interfacial Microgel Self-Assembly Engineered for Superionic Conduction in PVDF Electrolyte
Yanping Chen1, Chengdong Fang1, Qingquan Lin1
1State Key Laboratory For Physical Chemistry of Solid Surfaces, Innovation Laboratory for Sciences and Technologies of Energy Materials of Fujian Province (IKKEM), Collaborative Innovation Center of Chemistry for Energy Materials (iChem), Engineering Research Center of Electrochemical Technologies of Ministry of Education, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, Fujian, 361005, China.
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In this work, we propose an ion-mediated interfacial microgel self-assembly strategy, enabling the construction of a conduction network with optimized ion coordination to overcome the intrinsic limitations of PVDF-based electrolytes. As prepared M(D)-PVDF-HFP electrolyte shows remarkable ionic conductivity (4.54 × 10-4 S cm-1 at room temperature), high Li+ transference number (0.63), and a 4.8 V-wide operating window. Galvanostatic electrochemical impedance spectroscopy and finite element method simulations demonstrate rapid response and a high and uniform Li+ flux under operating conditions. Consequently, symmetric cells display stable Li plating/stripping for >5,000 h with an overpotential of only 136.4 mV at 0.1 mA cm-2 (25 °C). Furthermore, all-solid-state cells employing a LiNi0.8Co0.1Mn0.1O2 cathode delivered an initial reversible specific capacity of 181.08 mAh g-1, even under a high areal capacity load of approximately 2.0 mAh cm-2. Our work is an innovative exploration to induce uniform Li+ flux in heterogeneous polymer electrolyte and highlights the importance of internal interface behavior in solid-state polymer electrolytes.
