Optimizing Aqueous Zinc‐Sulfur Battery Performance via Regulating Acetonitrile Co‐Solvents and Carbon Nanotube Carriers

Rechargeable aqueous zinc-sulfur batteries (AZSBs) are gaining attention due to their high energy density, ultra-stable discharge platform, and safety. However, poor liquid/solid reaction processes at the anode and cathode reduce reaction kinetics, and the severe dissolution of polysulfides causes shuttle effects during discharge/charge cycles, hindering practical applications. Improving performance requires optimizing both the cathode and electrolyte. Herein, we design an organic-inorganic hybrid electrolyte (zinc trifluoromethanesulfonate and trace iodine monomer dissolved in an acetonitrile/water co-solvent (AN-X)) and a partially exfoliated multi-walled carbon nanotube (PECNT) hosted sulfur (S@PECNTs) cathode for AZSBs. The sulfur is highly dispersed along the PECNTs with appropriate wettability at the electrode/electrolyte interface using AN-3 as the electrolyte. Meanwhile, this electrolyte inhibits hydrogen evolution at negative potentials and promotes uniform Zn ion stripping/plating. Expressively, the AN-3-based AZSB exhibits a high discharge capacity of 1370 mAh g^-1 with excellent Coulombic efficiency (79.9 %), outstanding rate capability, and cycling performance. These improvements are attributed to the synergistic effect between the S@PECNTs and the AN-3 electrolyte, which reduces R_ct to enhance reaction kinetics and blocks the dissolution and shuttle effect of polysulfides, ensuring a reversible reaction between zinc and sulfur.