Anisotropically Hybridized Porous Crystalline Li‐S Battery Separators

Anisotropically hybridized porous crystalline Li-S battery separators based on porous crystalline materials that can meet the multiple functionalities of both anodic and cathodic sides are much desired for Li-S battery yet still challenging in directional design. Here, an anisotropically hybridized separator (CPM) based on an ionic liquid-modified porphyrin-based covalent-organic framework (COF-366-OH-IL) and catalytically active metal-organic framework (Ni3 (HITP)2 ) that can integrate the lithium-polysulfides (LiPSs) adsorption/catalytic conversion and ion-conduction sites together to directionally meet the requirements of electrodes is reported. Remarkably, the-obtained separator exhibits an exceptional high Li+ transference-number (tLi+ = 0.8), ultralow polarization-voltage (<30 mV), high initial specific-capacity (921.38 mAh g-1 at 1 C), and stable cycling-performance, much superior to polypropylene and monolayer-modified separators. Moreover, theoretical calculations confirm the anisotropic effect of CPM on the anodic side (e.g., Li+ transfer, LiPSs adsorption, and anode-protection) and cathodic side (e.g., LiPSs adsorption/catalysis). This work might provide a new perspective for separator exploration.