Dual Li ion transport channels in a dynamical supramolecular solid electrolyte toward safety and high-performance Li metal batteries

The polymer based quasi-solid electrolyte (QSE), which combines the high ionic conductivity of the liquid electrolytes with the excellent mechanical flexibility of the polymer matrix, is highly desired and most promising for Li metal batteries (LMBs). However, the Li⁺ transfer pathways in QSE is not clear enough, and the practical applications in LMBs are also hindered by safety hazards arising from risks of mechanical damage, flammability and high voltage instability. Here, a dynamical supramolecular QSE with abundant hydrogen bonds to fabricate stable and safety LMBs, is reported. In this designed electrolyte, both thermal stability and superior interface stability with anode/cathode electrodes were achieved. Notably, the dual Li⁺ transport channels in QSE were investigated using in-situ FTIR technology and DFT calculations, providing insights into both the “wet” liquid phase and “dry” polymer chain channels. Benefiting from this design, the Li||NCM622 full batteries based on this QSE exhibit excellent long-term cycling stability.