Customizing Component Regulated Dense Heterointerfaces for Crafting Robust Lithium‐Sulfur Batteries

Abstract

Lithium–sulfur (Li–S) batteries hold great promise for the next‐generation energy storage system. However, their commercial applications are severely hindered by myriads of drawbacks such as poor electrical conductivity of sulfur, sluggish redox reaction kinetics of sulfur species, “shuttling effect” of soluble lithium polysulfides (LiPSs) and uncontrollable dendritic Li growth. Herein, it is conceptually demonstrated that sluggish conversion kinetics of LiPSs is markedly stimulated by exquisite heterointerface modulation at nanoscale level over transition metal carbides and nitrides. In this scenario, N‐doped carbon coupled with molybdenum nitride/carbide (Mo2N‐MoC/NC) hybrid nanocomposites are designed through a one‐step carbonization‐nitridation process, wherein component regulation induced dense heterointerfaces are in situ produced. Benefiting from high electrical conductivity, strong chemical adsorption, and superior catalytic activity afforded by dense heterointerfaces, the Mo2N‐MoC/NC modified separators significantly restrict the soluble LiPSs shuttling and simultaneously suppress the Li dendrite generation. The assembled Li–S batteries with Mo2N‐MoC/NC modified separators exhibit remarkable electrochemical performance. Integrated experimental and theoretical results substantiate the boosted chemisorption and catalytic conversion of LiPSs endowed by such dense heterointerfaces. The work will open a new vista for rationally constructing multifarious heterostructured materials for the communities of Li‐S batteries.

High Energy Density Aqueous Zinc–Chalcogen (S, Se, Te) Batteries: Recent Progress, Challenges, and Perspective

“…First, the insulating nature of both sulfur (5 × 10 −28 S cm −1 ) or selenium (1 × 10 −3 S cm −1 ), as well as their discharge products lead to the poor electrode conductivity. [83,84] Second, the notable volume change of the chalcogen cathode (e.g., 50.3% of S) during battery dynamic cycling may induce a large mechanical destruction effect. [85,86] Third, the sluggish reaction kinetics of chalcogen species during the direct solid-solid conversion process in water-based electrolyte may bring low energy efficiencies during cycles.…”

Electrolessly tin-plated sulfur nanocomposite for practical lean-electrolyte lithium–sulfur cells with a high-loading sulfur cathode

“…S19 and Table S5, ESI †). 26,[31][32][33][34] The electrocatalytic characteristics of the two samples were first compared in terms of their polysulfide adsorption capacities. With the same content of tin in both composites, the tin-plated sulfur nanocomposite displayed significantly weaker polysulfide peaks in its ultraviolet-visible spectrum than the sulfur/tin composite; moreover, the polysulfide solution of the tin-plated sulfur nanocomposite became transparent after one week of resting, while the sulfur/tin composite remained yellow (Fig.…”

“…This is because of the use of a high-loading sulfur cathode and the realization of high electrochemical utilization of sulfur, which results in a high peak current. 24–26,31–34 During the CV scanning, the tin-plated sulfur nanocomposites showed high lithium-ion diffusion coefficients, which might result from the diffusing polysulfides that are trapped by the conductive tin plating shell and serve as the catholyte to promote the lithium-ion diffusion during cycling. This might be the external mechanism for the high lithium-ion diffusion.…”

Electrochemical performance study of nano-Fe3O4/C modified separator for lithium-sulfur batteries

“…Additionally, the current sulfur loading is insufficient for practical energy storage applications. Furthermore, the poor electronic and ionic conductivity of sulfur and the discharge product, Li 2 S, contribute to sluggish reaction kinetics and substantial polarization, further compromising battery performance [6][7][8][9][10].…”