Co/Mon Invigorated Bilateral Kinetics Modulation for Advanced Lithium–Sulfur Batteries

Abstract

Sluggish sulfur redox kinetics and Li‐dendrite growth are the main bottlenecks for lithium–sulfur (Li–S) batteries. Separator modification serves as a dual‐purpose approach to address both of these challenges. In this study, the Co/MoN composite is rationally designed and applied as the modifier to modulate the electrochemical kinetics on both sides of the sulfur cathode and lithium anode. Benefiting from its adsorption‐catalysis function, the decorated separators (Co/MoN@PP) not only effectively inhibit polysulfides (LiPSs) shuttle and accelerate their electrochemical conversion but also boost Li+ flux, realizing uniform Li plating/stripping. The accelerated LiPSs conversion kinetics and excellent sulfur redox reversibility triggered by Co/MoN modified separators are evidenced by performance, in‐situ Raman detection and theoretical calculations. The batteries with Co/MoN@PP achieve a high initial discharge capacity of 1570 mAh g−1 at 0.2 C with a low decay rate of 0.39%, uniform Li+ transportation at 1 mA cm−2 over 800 h. Moreover, the areal capacity of 4.62 mAh cm−2 is achieved under high mass loadings of 4.92 mg cm−2. This study provides a feasible strategy for the rational utilization of the synergistic effect of composite with multifunctional microdomains to solve the problems of Li anode and S cathode toward long‐cycling Li–S batteries.

Interfacial “Double-Terminal Binding Sites” Catalysts Synergistically Boosting the Electrocatalytic Li2S Redox for Durable Lithium–Sulfur Batteries

“…In this type of heterojunction composite, it is commonly observed that the metal component plays a crucial role in facilitating fast electron migration, while the presence of polar materials contributes sufficient binding energy. This observation is consistent with previous studies. − …”

Rare Earth Single‐Atom Catalysis for High‐Performance Li−S Full Battery with Ultrahigh Capacity

“…After switching back to the current density of 0.5 C, the high capacity of 1010.2 mAh g À 1 is recovered. The rate performance of Sm-N 3 C 3 significantly exceeded that of NC and Sm 2 O 3 , as well as most of the reported cells using modified separators [52][53][54][55][56][57][58][59] (Figure 4g). Notably, Sm 2 O 3 shows the weakest catalytical effect on LiPSs conversion and poor battery performance, which is probably derived from high internal resistance and charge transfer resistance, as well as the strong adsorption of reactant molecules resulting the difficulty of migration in catalysis processing based on the discussion above.…”

Recent advances in li metal anode protection for high performance lithium-sulfur batteries

“…Moreover, the LiPSs adsorbed on the separator can be reactivated and contribute to capacity retention [225]. In parallel with cathode engineering, extensive research has been conducted on metal compounds, heterostructures, and single-atom catalysts [226,227]. The introduction of these materials possessing both adsorption and catalytic capabilities significantly inhibit the LiPS shuttle effect, thereby preventing the diffusion of LiPSs to the Li metal anode and effectively protecting against Li corrosion caused by LiPS.…”