3D Interconnected Porous Carbon Aerogels as Sulfur Immobilizers for Sulfur Impregnation for Lithium-Sulfur Batteries with High Rate Capability and Cycling Stability

To eliminate capacity‐fading effects due to the loss of sulfur cathode materials as a result of polysulfide dissolution in lithium–sulfur (Li–S) cells, 3D carbon aerogel (CA) materials with abundant narrow micropores can be utilized as an immobilizer host for sulfur impregnation. The effects of S incorporation on microstructure, surface area, pore size distribution, and pore volume of the S/CA hybrids are studied. The electrochemical performance of the S/CA hybrids is investigated using electrochemical impedance spectroscopy, galvanostatical charge–discharge, and cyclic voltammetry techniques. The 3D porous S/CA hybrids exhibit significantly improved reversible capacity, high‐rate capability, and excellent cycling performance as a cathode electrode for Li–S batteries. The S/CA hybrid with an optimal incorporating content of 27% S shows an excellent reversible capacity of 820 mAhg−1 after 50 cycles at a current density of 100 mAg−1. Even at a current density of 3.2C (5280 mAg−1), the reversible capacity of 27%S/CA hybrid can still maintain at 521 mAhg−1 after 50 cycles. This strategy for the S/CA hybrids as cathode materials to utilize the abundant micropores for sulfur immobilizers for sulfur impregnation for Li–S battery offers a new way to solve the long‐term reversibility obstacle and provides guidelines for designing cathode electrode architectures. 3D carbon aerogel (CA) materials with abundant micropores and mesopores are utilized as an immobilizer host for sulfur impregnation to eliminate capacity‐fading effects due to the loss of sulfur cathode as a result of polysulfide dissolution in lithium‐sulfur cells. The 3D porous S/CA hybrids exhibit significantly improved reversible capacity, high‐rate capability, and cycling performance as a cathode electrode for Li–S batteries.