Single Zinc Atom Aggregates: Synergetic Interaction to Boost Fast Polysulfide Conversion in Lithium-Sulfur Batteries

Single-atom catalysts (SACs) pave new possibilities to improve the utilization efficiency of sulfur electrodes arising from polysulfide shuttle effects and sluggish kinetics due to their excellent applicability in atomic-scale reaction mechanisms and structure-activity relationships. Herein, nitrogen (N)-anchored SACs on the highly ordered N-doped carbon nanotube arrays are reported as the sulfur host for fast redox conversion in lithium-sulfur (Li-S) batteries. The cube structure of the aligned carbon nanotubes can promote the rapid mass transfer under high sulfur loadings, and abundant single-atom active sites further accelerate the conversion of lithium polysulfides (LiPSs). The synergistic enhancement effect induced by adjacent single atoms with interatomic distances <1 nm further accelerates the rapid multi-step reaction of sulfur at high sulfur loadings. As a result, the obtained Li-S batteries exhibit outstanding cycle stability with a high areal capacity of 5.6 mAh cm(-2) after 100 cycles under a high sulfur loading of 7.2 mg cm(-2) (electrolyte to sulfur ratio is approximate to 3.7 mL g(-1)). Even assembled into a pouch cell, it still delivers a high capacity of 953.4 mAh g(-1) after 100 cycles at 0.1 C, contributing to the development of the practically viable Li-S batteries.

Automated summary

This study reports nitrogen (N)-anchored single-atom catalysts (SACs) on highly ordered N-doped carbon nanotube arrays as the sulfur host for fast redox conversion in lithium-sulfur (Li-S) batteries. The synergistic enhancement effect induced by adjacent single atoms with interatomic distances <1 nm further accelerates the rapid multi-step reaction of sulfur at high sulfur loadings. The obtained Li-S batteries exhibit outstanding cycle stability and high capacity, contributing to the development of practically viable Li-S batteries.