Negative PO3-implanted bionic ion transport channels for promoting Li-S battery
摘要
Lithium-sulfur (Li-S) battery, as a promising next-generation high-energy-density battery, suffers from lithium polysulfides (LPSs) shuttle and Li dendrites issues. Porous crystalline framework-based membranes as separator can effectively absorb and restrain LPSs but without precise structural design principal exploration and mechanism studies. Herein, bio-inspired 1D oriented lithium-ion transport channels with molecular negatively charged PO3(−1) have been developed in hybrid tetrazole frameworks for promoting the transmission of Li+ ions. The theoretical calculations and in situ spectroscopy demonstrated the higher binding energy and inhibited diffusion of LPSs in PO3. The assembled PP@PO3 Janus separator in Li-S coin cell delivered a high initial capacity of 1410.9 mAh g−1 at 0.1 C and a low attenuation rate of 0.038% per cycle over 500 cycles at 5 C. Besides, the high capacities of 862, 542 and 409 mAh g−1 based on high-sulfur-loading cathodes of 2.6, 3.8 and 5.0 mg cm−2 at 0.5 C were achieved, respectively. Moreover, the punch battery of PO3@PP separator with S-cathode of 1.2 mg cm−2 has been developed for demonstrating its potentials commercial application, which displays impressive capacity of 873.4 mAh g−1 with the retention of ∼78.9% over 50 cycles.