Theoretical Study of Two-Dimensional α-Tellurene with Pseudo-Heterospecies as a Promising Elemental Anchoring Material for Lithium–Sulfur Batteries

Abstract

The main obstacle that impedes the application of lithium–sulfur (Li–S) batteries is the severe shuttle effect, which can be overcome by introducing anchoring materials (AMs) to immobilize soluble lithium polysulfides (LiPSs) without decomposing them. The number of decomposition pathways could be significantly reduced in AMs with a minimum number of species such as graphene which, however, is homoatomic and nonpolar with low affinity to LiPSs. In this study, we investigate the anchoring behavior of another two-dimensional elemental material α-tellurene that is chemically analogous to the 1T transition-metal dichalcogenides, in the framework of density functional theory. We demonstrate that the α-tellurene with pseudo-heterospecies (with positively charged central Te and negatively charged outer layer Te) exhibits an outstanding anchoring performance due to the suitable binding strength of LiPSs in the range of 0.86–2.39 eV, which effectively suppress the shuttle effect but do not cause the decomposition of LiPSs. The moderate binding strength is attributed to the pseudo-heterospecies as well as to the competition between S and Te for capturing electrons from Li. Furthermore, the low Li atom diffusion (0.18 eV) and Li2S catalytic decomposition (0.88 eV) energy barriers guarantee the fast electrochemical process of α-tellurene-integrated Li–S batteries. Given these advantages, it is expected that α-tellurene is a promising AM for Li–S batteries.

Homogeneous Organometallic Catalysts for Improved Electrochemical Kinetics of Li–S Batteries

“…From Table , it is clear that the minimum distance between LiPS and TiCp 2 decreases from 2.674 Å for Li 2 S 8 to 2.435 Å for Li 2 S when the number of S atoms in LiPS decreases. Figure illustrates that the binding energies increase with increasing lithiation, with the lowest binding energy in the case of Li 2 S 8 , and a similar kind of binding behavior is observed in graphene and other two-dimensional (2D) materials. − Furthermore, Figure proves that interactions of S 8 with TiCp 2 do not lead to any structural deformations, whereas the binding of LiPSs results in a slight distortion compared with their isolated structures; however, no chemical dissociations were observed.…”

A review on theoretical models for lithium–sulfur battery cathodes

“…103 Zhang and coauthors explored the possibility of α-tellurene as the host material in Li-S batteries. 104 Xiong's group proposed a novel kind of tungsten (W) single atomic catalyst with high LiPSs adsorption ability and catalytic activity (Figure 6). 105 F I G U R E 6 The application of Lithium-ion diffusion and Li…”

“…Based on these models, Zhao and coauthors predicted that two‐dimensional magnetic Fe 3 GeX 2 (X = S, Se, and Te) monolayers could be potential candidates which possess bifunctional electrocatalytic activity to the SRR and the Li 2 S decomposition reaction 103 . Zhang and coauthors explored the possibility of α ‐tellurene as the host material in Li–S batteries 104 . Xiong's group proposed a novel kind of tungsten (W) single atomic catalyst with high LiPSs adsorption ability and catalytic activity (Figure 6).…”

“…(B) Predicting the possibility of α ‐tellurene as the host material in Li–S batteries. Reproduced with permission of reference 104. Copyright 2021.…”

Tunable Schottky and ohmic contacts in the Ti2NF2/α-Te van der Waals heterostructure

“…42 Moreover, α-Te with pseudo-heterospecies could be applied as the anchoring material to suppress the shuttle effect and achieve enhanced performance of Li–S batteries. 43 Until now, 2D Te was also successfully prepared by many other methods, such as van der Waals (vdW) epitaxy, 44 hydrothermal reduction of sodium tellurite (Na 2 TeO 3 ), 41 liquid phase exfoliation (LPE), 42 etc. The synthesized 2D Te with high quality offers the base to build 2D Te-based devices, which endows it with potential to be utilized in a wide range of applications.…”