The high interface impedance between inorganic material electrodes and solid electrolytes results in a high Li+ diffusion energy barrier, which limits the electrochemical performance of active materials. To solve this issue, an integrated configuration of organic active material electrode-solid polymer electrolyte (SPE) is synthesized via in situ polymerization. In the integrated aminoanthraquinone-solid polymer electrolyte (AQ-SPE), the naphthalene urethane bond acts as a bridge that links the organic material electrode and the SPE and acts as a channel for Li+ transport at the electrode/SPE interface. Compared to the activation energy of the conventional aminoanthraquinone/solid polymer electrolyte (AQ/SPE), the activation energy of the charge transfer process for the integrated AQ-SPE decreases from 71.2 to 42.1 kJ mol-1, and the charge transfer impedance decreases from 1140 to 198 Ω at 50 °C. The first and 625th discharge capacity densities of AQ in the integrated AQ-SPE at 0.1 mA cm-1 and 50 °C are 139.7 and 125.3 mAh g-1, respectively. Moreover, pouch batteries with the integrated AQ-SPE show excellent safety performance. The in situ fabrication of integrated electrode-SPE provides an enlightening and extended method for realizing efficient, safe, and environmentally friendly batteries.
Keywords: charge transfer; integrated configuration; interface impedance; ionic conductivity; polymerization.