A Hierarchically Porous Multifunctional Current Collector for High‐Performance Li‐S Batteries

ABSTRACT Construction of an advanced current collector with optimized structure and multi‐functionality is critical for solving the thorny problems (e.g., lithium polysulfides (LiPSs) shuttle effect, low conductivity, and sluggish sulfur conversion) of Li‐S batteries. Unlike the use of an conventional pore‐free 2D current collector (low sulfur loading) or the 3D current collector rich in irregular macropores (poor sulfur fixation ability), herein a hierarchically porous current collector (HPCC) with tailored pore architecture and multifunctionality is designed, which is constituted by a large‐pore 3D carbon cloth (CC) substrate (pore size > 50 µm), conjugated microporous conducting polymers (CMPs) filler materials (pore size 0.8–1.6 nm) and Pd nanopaticle catalysts (3–5 nm). The HPCC optimizes the original large‐pore 3D CC structure into a hierarchically porous structure with regularized pore size and uniform catalytic sites, achieving a 2D/3D functional balance. Benefiting from the enhanced Li + /e − transportation, high‐efficiency LiPSs adsorption, and strong catalysis ability for LiPSs, the batteries with HPCC achieve the ultrahigh discharging capacity of 1304 mAh g − 1 at 0.2 C, exceptional stability (0.42% decay/cycle at 10.59 mA·cm − 2 ) even at a high sulfur loading condition of 10.3 mg cm − 2 , and good commercial application potential (driving electric‐car operation). This pore engineering strategy establishes a paradigm for developing a high‐energy‐density battery.