Quasi-single-ion selective polymer of intrinsic microporosity interface: bifunctional promoter for achieving uniform lithium metal deposition

The relentless pursuit of high-energy-density lithium battery innovation compels the emergence of stable and high-performance anodes, serving as a cornerstone for transformative advancements. However, the rampant dendrites growth and unbridled volumetric expansion of lithium anodes gravely undermine Coulombic efficiency and markedly curtail the cycling longevity. Herein, an exquisite micron-scale artificial film crafting from polymers of intrinsic microporosity (PIMs) combined a rigid structural framework with pliant segments confers extraordinary mechanical strength (5.28 GPa) and outstanding flexibility, which were unveiled to curtail Li dendrite proliferation and mitigate parasitic side reactions. The intrinsic nanoscale pores and electronegative functional groups of the PIM-based film adeptly regulate lithium-ion transport, fostering uniform deposition and stripping with a high Li + transference number of 0.946. Density functional theory (DFT) calculations reveal a strong affinity between the AO-PIM-1 coating and Li + . The AO-PIM-1@Cu anode achieves an impressive Coulombic efficiency of 98.45 % after 180 cycles at 0.5 mA cm −2 . Moreover, the modified Li|Li symmetrical cell demonstrates exceptional stability, sustaining over 8000 h under 10 mA cm −2 at a capacity density of 5 mAh cm −2 . This work profoundly expands the design horizon for artificial SEI, offering a compelling avenue for the practical realization of lithium metal batteries.