Sulfur Vapor-Infiltrated 3D Carbon Nanotube Foam for Binder-Free High Areal Capacity Lithium–Sulfur Battery Composite Cathodes

Here, we demonstrate a strategy to produce high areal loading and areal capacity sulfur cathodes by using vapor-phase infiltration of low-density carbon nanotube (CNT) foams preformed by solution processing and freeze-drying. Vapor-phase capillary infiltration of sulfur into preformed and binder-free low-density CNT foams leads to a mass loading of ∼79 wt % arising from interior filling and coating of CNTs with sulfur while preserving conductive CNT–CNT junctions that sustain electrical accessibility through the thick foam. Sulfur cathodes are then produced by mechanically compressing these foams into dense composites (ρ > 0.2 g/cm 3 ), revealing specific capacity of 1039 mAh/g S at 0.1 C, high sulfur areal loading of 19.1 mg/cm 2, and high areal capacity of 19.3 mAh/cm 2 . This work highlights a technique broadly adaptable to a diverse group of nanostructured building blocks where preformed low-density materials can be vapor infiltrated with sulfur, mechanically compressed, and exhibit simultaneous high areal and gravimetric storage properties. This provides a route for scalable, low-cost, and high-energy density sulfur cathodes based on conventional solid electrode processing routes.