Engineering d-p Orbital Hybridization with P, S Co-Coordination Asymmetric Configuration of Single Atoms Toward High-Rate and Long-Cycling Lithium-Sulfur Battery.
Adv Mater
; 36(38): e2407070, 2024 Sep.
Article
in En
| MEDLINE
| ID: mdl-39091051
ABSTRACT
Single-atom catalysts (SACs) have been increasingly explored in lithium-sulfur (Li-S) batteries to address the issues of severe polysulfide shuttle effects and sluggish redox kinetics. However, the structure-activity relationship between single-atom coordination structures and the performance of Li-S batteries remain unclear. In this study, a P, S co-coordination asymmetric configuration of single atoms is designed to enhance the catalytic activity of Co central atoms and promote d-p orbital hybridization between Co and S atoms, thereby limiting polysulfides and accelerating the bidirectional redox process of sulfur. The well-designed SACs enable Li-S batteries to demonstrate an ultralow capacity fading rate of 0.027% per cycle after 2000 cycles at a high rate of 5 C. Furthermore, they display excellent rate performance with a capacity of 619 mAh g-1 at an ultrahigh rate of 10 C due to the efficient catalysis of CoSA-N3PS. Importantly, the assembled pouch cell still retains a high discharge capacity of 660 mAh g-1 after 100 cycles at 0.2 C and provides a high areal capacity of 4.4 mAh cm-2 even with a high sulfur loading of 6 mg cm-2. This work demonstrates that regulating the coordination environment of SACs is of great significance for achieving state-of-the-art Li-S batteries.
Full text:
1
Collection:
01-internacional
Database:
MEDLINE
Language:
En
Journal:
Adv Mater
/
Adv. mater. (Weinheim Print)
/
Advanced materials (Weinheim Print)
Journal subject:
BIOFISICA
/
QUIMICA
Year:
2024
Document type:
Article
Country of publication:
Alemania