Long‐Life and High‐Loading All‐Solid‐State Li–S Batteries Enabled by Acetylene Black with Dispersed Co‐N₄ as Single Atom Catalyst

Abstract

All‐solid‐state Li–S batteries (ASSLSBs) have exhibited great promise as next‐generation energy storage systems due to the elimination of the shuttle effect and flammability. However, the low reactivity of sulfur and poor solid–solid contact in the composite cathode result in limited electrochemical performances. Here, a Co‐N4‐decorated carbon composite is prepared by direct ball milling and serves as a sulfur host for ASSLSBs. The uniform distribution of Co‐N4 can effectively accelerate the redox conversion of sulfur and inhibit the agglomeration of sulfur particles during cycling through strong chemical affinity. Benefiting from these merits, the sulfur cathode with a sulfur content of 40% and a sulfur loading of 1.5 mg cm−2 in ASSLSBs exhibits high reversible capacity (1439 mAh g−1 at 0.1 C) and superior long‐term cyclic performance (capacity fade rate of 0.025% per cycle for 1000 cycles at 0.5 C). Even under a sulfur loading up to 4.5 mg cm−2, the areal capacity can reach 5.13 mAh cm−2 at 60 °C and maintain stable cycling over 300 cycles at 0.3 C. This work offers a promising strategy for enhancing the electrochemical performance of ASSLSBs.

Interface engineering toward stable lithium–sulfur batteries

“…In the system of GPEs, transition metals or transition metal complexes have been introduced to avoid the accumulation of LPSs at the interface and enhance the electrochemical reaction kinetics. 219–222 As seen in Fig. 15b, the high accumulation and clogging of “dead” LPSs on the interface between the cathode and GPEs with intrinsic diffusion limitation is identified as a critical failure cause of GPEs-based ASSLSBs.…”

Bridging the gap between academic research and industrial development in advanced all-solid-state lithium–sulfur batteries

“…192,193 Single-atom catalysts, such as nickel and cobalt, which exhibit a strong chemical affinity with sulfur, accelerated the sulfur conversion and prevented the agglomeration of sulfur particles. 157 In polymer electrolyte-based Li–S batteries, single-atom electrocatalysis has also demonstrated its efficacy in minimizing the formation of dead lithium polysulfides as well. 194…”

Local structural environment of single-atom catalysts

“…15 Therefore, downsizing the catalyst particles or clusters to single-atoms is extremely desirable for catalytic reactions because atomically isolated sites often function as active sites. 14–21…”