Defective Phosphorene as a Promising Anchoring Material for Lithium–Sulfur Batteries

Abstract

The lithium−sulfur battery, despite having considerable advantages, is still far from its practical applications, which is primarily caused by the dissolution of polysulfide clusters of lithium (LiPSs) into the electrolyte. Entrapping these LiPSs through integration of the anchoring material with the electrode is an effective approach to overcome this problem. In this study, density functional theory and ab initio molecular dynamics have been adopted to systematically examine the anchoring behaviors of two-dimensional phosphorene-based (monovacancy/oxygen-/sulfur-doped) materials, for all the intermediates of polysulfide. The defective sites provide strong adsorption for polysulfide clusters by generating firm chemical bonds together with van der Waals interactions. As a result, the intermediate discharge products could be thermodynamically stabilized on these defective substrates, against the local environment with virtually alike to initial configurations, which cannot be achieved with pristine phosphorene. Moreover, the emerging midgap states in the electronic structures of defective phosphorene and adsorptive systems improve the electrical conductivity of the defective-phosphorene-based electrode, alleviating the low rate capability related with pristine-phosphorene based batteries. It is illustrated that the anchoring ability of pristine phosphorene can be significantly improved by the defects, among which the monovacancy structure demonstrates superior performance for achieving long cycle life.

Arsenene, antimonene and bismuthene as anchoring materials for lithium‐sulfur batteries: A computational study

“…51 The potential applications of defective black phosphorene and blue phosphorene (β-phase of phosphorene) in Li-S batteries have also been proposed through theoretical calculations. 52,53 For arsenene, antimonene and bismuthene allotropes, Zhang et al predicted that all corresponding β phases with the buckled form are the most stable structures. 54 β-arsenene, β-antimonene and β-bismuthene have been testified to exist and successfully isolated from group-VA bulk crystals.…”

Xenes as an Emerging 2D Monoelemental Family: Fundamental Electrochemistry and Energy Applications

“…Defects are thought to have important effects on the electronic structure and electrochemical applications of Xenes. [123,124] Different synthetic methods could induce the different degree of defects in the Xenes. [125,126] Element doping is another important route to induce the formation of defects into the emerging Xenes.…”

Applications of 2D MXenes for Electrochemical Energy Conversion and Storage

“…The increasingly prominent climate changes and limited availability of fossil fuel issues have stimulated a tremendous amount of research interest in highly efficient and clean energy storage and conversion devices [1][2][3][4][5]. The development of new classes of advanced two-dimensional (2D) layered materials, including graphene, MoS 2 , phosphorene, have promoted tremendous technological progress in those energy resources (e.g., supercapacitor, different-type metal ion batteries (MIBs)), which are attributed to their extraordinary properties [2,[6][7][8][9][10][11][12][13][14][15][16][17]. The enhancement in the performance of these devices by incorporating layered materials indicated that the 2D materials commonly possess the following two unique characteristics:…”