Cationic polymer-grafted graphene oxide/CNT cathode-coating material for lithium–sulfur batteries

Abstract

A cathode-coating material composed of cationic polymer-grafted graphene oxide (CPGO) and carbon nanotube (CNT) was prepared, where the CPGO was synthesized by grafting quaternized 2-(dimethylamino)ethyl methacrylate (QDMAEMA) onto graphene oxide (GO) via atom transfer radical polymerization (ATRP). GO has good compatibility with carbon black, the main component of the cathode in lithium–sulfur (Li–S) batteries. Here, the cationic polymer having the QDMAEMA unit was intentionally grafted onto GO to decrease the shuttle effect by increasing the chemical adsorption of polysulfide (PS). In addition, when CNT was mixed with CPGO, the compatibility with carbon black was found to be further increased. The lithium–sulfur (Li–S) battery with a sulfur-deposited Super P® carbon black (S/C) cathode coated with a mixture of CPGO and CNT was found to have much improved cell performance compared to those coated without any coating material, with only CPGO, with the mixture of GO and CNT, and with the mixture of PQDMAEMA and CNT. For example, the Li–S battery with the cathode coated using the mixture of CPGO and CNT retained a discharge capacity of 744 mA h g⁻¹ after 50 cycles at 0.2C-rate, while those of the Li–S batteries with bare S/C and CPGO-S/C cathodes were found to be much smaller, i.e., 488 mA h g⁻¹ and 641 mA h g⁻¹, respectively, under the same conditions. Therefore, the mixture of CPGO with CNT as the cathode-coating material showed a synergetic effect to enhance the cell performance of the Li–S battery system.