Interfacial "Double-Terminal Binding Sites" Catalysts Synergistically Boosting the Electrocatalytic Li<sub>2</sub>S Redox for Durable Lithium-Sulfur Batteries.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 38465917.
- Also identified by DOI 10.1021/acsnano.3c11903 and PMC identifier 10976959.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
Catalytic conversion of polysulfides emerges as a promising approach to improve the kinetics and mitigate polysulfide shuttling in lithium-sulfur (Li-S) batteries, especially under conditions of high sulfur loading and lean electrolyte. Herein, we present a separator architecture that incorporates double-terminal binding (DTB) sites within a nitrogen-doped carbon framework, consisting of polar Co<sub>0.85</sub>Se and Co clusters (Co/Co<sub>0.85</sub>Se@NC), to enhance the durability of Li-S batteries. The uniformly dispersed clusters of polar Co<sub>0.85</sub>Se and Co offer abundant active sites for lithium polysulfides (LiPSs), enabling efficient LiPS conversion while also serving as anchors through a combination of chemical interactions. Density functional theory calculations, along with <i>in situ</i> Raman and X-ray diffraction characterizations, reveal that the DTB effect strengthens the binding energy to polysulfides and lowers the energy barriers of polysulfide redox reactions. Li-S batteries utilizing the Co/Co<sub>0.85</sub>Se@NC-modified separator demonstrate exceptional cycling stability (0.042% per cycle over 1000 cycles at 2 C) and rate capability (849 mAh g<sup>-1</sup> at 3 C), as well as deliver an impressive areal capacity of 10.0 mAh cm<sup>-2</sup> even in challenging conditions with a high sulfur loading (10.7 mg cm<sup>-2</sup>) and lean electrolyte environments (5.8 μL mg<sup>-1</sup>). The DTB site strategy offers valuable insights into the development of high-performance Li-S batteries.