Synergizing Polysulfide Trapping and Fast Ion Kinetics Enabled by Poly(Acrylamide‐co‐Lithium Acrylate) Aqueous Binder for High‐Sulfur‐Loading Lithium–Sulfur Batteries

ABSTRACT Although lithium–sulfur (Li–S) batteries offer high theoretical energy density, their practical implementation is impeded by the polysulfide shuttle effect and mechanical disintegration of sulfur cathodes, particularly under high‐sulfur‐loading conditions. To overcome these limitations, a multifunctional aqueous binder, poly(acrylamide‐co‐lithium acrylate) (AmLA), is proposed to synergistically enhance electrode integrity and suppress lithium polysulfide (LiPS) migration. The copolymer architecture integrates polar amide and lithium carboxylate groups, which establish a robust hydrogen‐bonding network for mechanical stability while simultaneously providing strong chemical anchoring sites for LiPS confinement. In situ UV‐visible spectroscopy corroborates the significant retardation of LiPS dissolution, confirming the suppression of shuttle reactions. Consequently, AmLA‐based sulfur cathodes exhibit superior electrochemical kinetics, delivering a 3.4‐fold enhancement in rate capability at 2 C compared to the polyvinylidene fluoride binder. With a high sulfur content of 75 wt% and an areal loading of 3.2 mg cm ⁻² , the cathode retains a high reversible capacity of 777 mAh g ⁻¹ after 200 cycles, accompanied by reduced polarization. Furthermore, stable cycling is preserved even at a high sulfur loading of 6 mg cm ⁻² (7 mAh cm ⁻² ). Thus, AmLA offers a viable strategy for resolving the chemical and mechanical bottlenecks of high‐energy‐density Li–S batteries.