Mechanistic exploration of Co doping in optimizing the electrochemical performance of 2H-MoS2/N-doped carbon anode for potassium-ion battery

Abstract

The 2H-MoS₂/nitrogen-doped carbon (2H-MoS₂/NC) composite is a promising anode material for potassium-ion batteries (PIBs). Various transition metal doping has been adopted to optimize the poor intrinsic electronic conductivity and lack of active sites in the intralayer of 2H-MoS₂. However, its optimization mechanisms have not been well probed. In this paper, using Cobalt (Co) as an example, we aim to investigate the influence of transition metal doping on the electronic and mechanical properties and electrochemical performance of 2H-MoS₂/NC via first-principles calculation. Co doping is found to be effective in improving the electronic conductivity and the areas of active sites on different positions (C surface, interface, and MoS₂ surface) of 2H-MoS₂/NC. The increased active sites can optimize K adsorption and diffusion capability/processes, where general smaller K adsorption energies and diffusion energy barriers are found after Co doping. This helps improve the rate performance. Especially, the pyridinic N (pyN), pyrrolic N (prN), and graphitic N (grN) are first unveiled to respectively work best in K kinetic adsorption, diffusion, and interfacial stability. These findings are instructive to experimental design of high rate 2H-MoS₂/NC electrode materials. The roles of different N types provide new ideas for optimal design of other functional composite materials.

Keywords: Doping; Electrochemical performance; First-principles study; MoS(2); Potassium-ion battery.