A Thiol Branched 3D Network Quasi Solid-State Polymer Electrolyte Reinforced by Covalent Organic Frameworks for...

Quasi solid-state polymer electrolytes (QSPEs) are particularly attractive due to their high ionic conductivity and excellent safety for lithium metal batteries (LMBs). However, it is still a great challenge for QSPEs to achieve strong mechanical strength and high electrochemical performance simultaneously. Herein, a QSPE (SCOF-PEP-PEA) using a covalent organic framework (COF) containing abundant allyl groups (SCOF) as a rigid porous filler as well as a cross-linker to reinforce the polymer network is reported. Benefitting from the unique 3D nanonetwork structure and abundant lithiophilic functional groups, SCOF-PEP-PEA QSPE exhibits high ionic conductivity (4.0 × 10^-4 S cm^-1) and high lithium-ion transference number (0.82) at room temperature. Moreover, SCOF-PEP-PEA QSPE displays much improved mechanical strength compared to PEP-PEA QSPE (AFM Young's modulus: 453 vs 36 MPa). As a result, the Li/LFP full cell with SCOF-PEP-PEA QSPE shows great rate performance of 141 mAh g^-1 at 1C and delivers a high specific capacity retention of 92% after 220 cycles at 0.5 C (60 °C). This work provides a new strategy to design and prepare high-performance QSPEs with COFs as porous organic filler, and further expand the application of COFs for energy storage applications.