Enabling Wide-Temperature Range Li-S Batteries via Asymmetric-Coordinated Titanium Sites-Implanted Graphene Single-Atom Electrocatalysts

Abstract

High-performance lithium-sulfur batteries capable of operating under harsh environmental conditions have garnered significant attention, yet they still confront two critical challenges: sluggish polysulfide redox reaction kinetics at low temperatures and the persistent shuttle effect of lithium polysulfides at elevated temperatures. Herein, a single-atom catalyst featuring an asymmetric Ti₁-O₅ configuration (Ti-rGO) supported by reduced graphene oxide is designed to act as an efficient host catalyst for lithium-sulfur batteries. Experimental and theoretical calculations reveal that the Ti₁-O₅ configuration in Ti-rGO is capable of tuning the electronic properties of rGO. Such a tailored electronic structure with an optimized Fermi level accelerates charge transfer and further enhances adsorption energy and conversion kinetics for lithium polysulfides. The 2D porous nanostructure of Ti-rGO provides a physical barrier for the shuttle effect and an open framework to efficiently boost the utilization of sulfur species. Lithium-sulfur batteries employing Ti-rGO/S cathodes demonstrate exceptional rate capability (761 mAh g⁻¹ at 5 C) and cycling stability (low capacity decay of 0.018% per cycle over 1000 cycles at 2 C) under ambient conditions. With a high sulfur loading of 9.2 mg cm⁻² and lean electrolyte usage of 5.8 μL mg⁻¹, the Ti-rGO/S cathodes still achieve a remarkable areal capacity of 10.65 mAh cm⁻². Notably, even over a wide temperature range (−25°C–70°C), the lithium-sulfur batteries based on Ti-rGO/S cathodes still maintain stable cyclic performance at 2 C. This research demonstrates that Ti-rGO-based electrocatalyst systems can facilitate the realization of temperature-resilient lithium-sulfur batteries capable of withstanding both cryogenic and elevated temperature conditions.

Keywords

coordination structure / Li-S batteries / reaction kinetics / single atom catalyst / wide temperature

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