Breaking Barriers to High-Practical Li-S Batteries with Isotropic Binary Sulfiphilic Electrocatalyst: Creating a Virtuous Cycle for Favorable Polysulfides Redox Environments

Adv Sci (Weinh). 2023 Nov;10(33):e2303916. doi: 10.1002/advs.202303916. Epub 2023 Oct 22.

Abstract

Investigations into lithium-sulfur batteries (LSBs) has focused primarily on the initial conversion of lithium polysulfides (LiPSs) to Li2 S2 . However, the subsequent solid-solid reaction from Li2 S2 to Li2 S and the Li2 S decomposition process should be equally prioritized. Creating a virtuous cycle by balancing all three chemical reaction processes is crucial for realizing practical LSBs. Herein, amorphous Ni3 B in synergy with carbon nanotubes (aNi3 B@CNTs) is proposed to implement the consecutive catalysis of S8(solid) → LiPSs(liquid) → Li2 S(solid) →LiPSs(liquid) . Systematic theoretical simulations and experimental analyses reveal that aNi3 B@CNTs with an isotropic structure and abundant active sites can ensure rapid LiPSs adsorption-catalysis as well as uniform Li2 S precipitation. The uniform Li2 S deposition in synergy with catalysis of aNi3 B enables instant/complete oxidation of Li2 S to LiPSs. The produced LiPSs are again rapidly and uniformly adsorbed for the next sulfur evolution process, thus creating a virtuous cycle for sulfur species conversion. Accordingly, the aNi3 B@CNTs-based cell presents remarkable rate capability, long-term cycle life, and superior cyclic stability, even under high sulfur loading and extreme temperature environments. This study proposes the significance of creating a virtuous cycle for sulfur species conversion to realize practical LSBs.

Keywords: binary sulfiphilic catalyst; isotropic adsorption-catalysis; practical Li-S batteries; virtuous cycle; wide-temperature range application.