Enhanced Electron Delocalization within Coherent Nano-Heterocrystal Ensembles for Optimizing Polysulfide Conversion in High-Energy-Density Li-S Batteries
© 2023 Wiley‐VCH GmbH.
| Veröffentlicht in: | Advanced materials (Deerfield Beach, Fla.). - 1998. - 36(2024), 13 vom: 28. März, Seite e2310052 |
|---|---|
| 1. Verfasser: | |
| Weitere Verfasser: | , , , , , , , |
| Format: | Online-Aufsatz |
| Sprache: | English |
| Veröffentlicht: |
2024
|
| Zugriff auf das übergeordnete Werk: | Advanced materials (Deerfield Beach, Fla.) |
| Schlagworte: | Journal Article catalytic conversion coherent nano‐heterocrystal electron delocalization lithium‐sulfur battery polysulfide adsorption |
| Zusammenfassung: | © 2023 Wiley‐VCH GmbH. Commercialization of high energy density Lithium-Sulfur (Li-S) batteries is impeded by challenges such as polysulfide shuttling, sluggish reaction kinetics, and limited Li+ transport. Herein, a jigsaw-inspired catalyst design strategy that involves in situ assembly of coherent nano-heterocrystal ensembles (CNEs) to stabilize high-activity crystal facets, enhance electron delocalization, and reduce associated energy barriers is proposed. On the catalyst surface, the stabilized high-activity facets induce polysulfide aggregation. Simultaneously, the surrounded surface facets with enhanced activity promote Li2S deposition and Li+ diffusion, synergistically facilitating continuous and efficient sulfur redox. Experimental and DFT computations results reveal that the dual-component hetero-facet design alters the coordination of Nb atoms, enabling the redistribution of 3D orbital electrons at the Nb center and promoting d-p hybridization with sulfur. The CNE, based on energy level gradient and lattice matching, endows maximum electron transfer to catalysts and establishes smooth pathways for ion diffusion. Encouragingly, the NbN-NbC-based pouch battery delivers a Weight energy density of 357 Wh kg-1, thereby demonstrating the practical application value of CNEs. This work unveils a novel paradigm for designing high-performance catalysts, which has the potential to shape future research on electrocatalysts for energy storage applications |
|---|---|
| Beschreibung: | Date Revised 28.03.2024 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
| ISSN: | 1521-4095 |
| DOI: | 10.1002/adma.202310052 |