High‐Throughput Carbon Scaffold and Liquid Metal Enable High‐Flux Li + Transport, Improved Interface Wettability, Dendrite Suppression, and Polysulfide Control in Li–S Batteries

ABSTRACT Lithium metal holds immense promise for next‐generation high‐energy‐density batteries; however, its practical deployment is impeded by sluggish kinetics and intricate interfacial chemistry. To address these challenges, we engineered a high‐throughput carbon scaffold (HTCS) via bio‐alkaline treatment, serving as a host for both sulfur cathodes (HTCS/S) and lithiophilic HTCS/Li–GaIn anodes fabricated through in situ melt‐infusion. This porous, interconnected 3D architecture effectively mitigates local current density and interfacial resistance, thereby suppressing polarization and enhancing wettability, the ultrahigh fluid flux of this HTCS reached 9.0×10 5 L m −2 h −1 bar −1 . Furthermore, the incorporation of liquid GaIn alloy buffers lithium reactivity, inhibits dendrite growth, and ensures uniform deposition. Consequently, symmetric HTCS/Li–GaIn cells exhibit exceptional stability for over 5000 h with a low polarization of approximately 65 mV. When paired in a full cell configuration, the HTCS/S||HTCS/Li–GaIn system delivers a specific capacity of 1586.9 mAh g −1 at 0.1 C after 100 cycles. Corroborating these results, ab initio molecular dynamics (AIMD) simulations reveal a robust binding energy of −2.81 eV between Li and GaIn motifs within amorphous Li–GaIn alloys, confirming strong metallic interactions. This synergistic integration of the conductive HTCS framework with the self‐healing liquid metal facilitates rapid Li + transport while effectively curtailing polysulfide dissolution and the shuttle effect.