Lithium-sulfur (Li-S) batteries are attracting substantial attention because of their high-energy densities and potential applications in portable electronics. However, an intrinsic property of Li-S systems, that is, the solubility of lithium polysulfides (LiPSs), hinders the commercialization of Li-S batteries. Herein, a new material, that is, carbon nitride phosphorus (CNP), is designed and synthesized as a superior LiPS adsorbent to overcome the issues of Li-S batteries. Both the experimental results and the density functional theory (DFT) calculations confirm that CNP possesses the highest binding energy with LiPS at a P concentration of ∼22% (CNP22). The DFT calculations explain the simultaneous existence of Li-N bonding and P-S coordination in the sulfur cathode when CNP22 interacts with LiPS. By introducing CNP22 into the Li-S systems, a sufficient charging capacity at a low cutoff voltage, that is, 2.45 V, is effectively implemented, to minimize the side reactions, and therefore, to prolong the cycling life of Li-S systems. After 700 cycles, a Li-S cell with CNP22 gives a high discharge capacity of 850 mA h g-1 and a cycling stability with a decay rate of 0.041% cycle-1. The incorporation of CNP22 can achieve high performance in Li-S batteries without concerns regarding the LiPS shuttling phenomenon.
Keywords: DFT calculation; P−S bond; adsorbent; carbon nitride phosphorus; lithium polysulfides; lithium−sulfur batteries; shuttling phenomenon.