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Interfacial “Single‐Atom‐in‐Defects” Catalysts Accelerating Li + Desolvation Kinetics for Long‐Lifespan Lithium‐Metal Batteries

Wang, Jian 1; Zhang, Jing; Wu, Jian; Huang, Min; Jia, Lujie; Li, Linge; Zhang, Yongzheng; Hu, Hongfei; Liu, Fangqi; Guan, Qinghua; Liu, Meinan; Adenusi, Henry; Lin, Hongzhen; Passerini, Stefano 1
1 Helmholtz-Institut Ulm (HIU), Karlsruher Institut für Technologie (KIT)

Abstract:

The lithium-metal anode is a promising candidate for realizing high-energy-density batteries owing to its high capacity and low potential. However, several rate-limiting kinetic obstacles, such as the desolvation of Li+ solvation structure to liberate Li$^+$, Li$^0$ nucleation, and atom diffusion, cause heterogeneous spatial Li-ion distribution and fractal plating morphology with dendrite formation, leading to low Coulombic efficiency and depressive electrochemical stability. Herein, differing from pore sieving effect or electrolyte engineering, atomic iron anchors to cation vacancy-rich Co$_{1−xS}$ embedded in 3D porous carbon (SAFe/CVRCS@3DPC) is proposed and demonstrated as catalytic kinetic promoters. Numerous free Li ions are electrocatalytically dissociated from the Li$^+$ solvation complex structure for uniform lateral diffusion by reducing desolvation and diffusion barriers via SAFe/CVRCS@3DPC, realizing smooth dendrite-free Li morphologies, as comprehensively understood by combined in situ/ex situ characterizations. Encouraged by SAFe/CVRCS@3DPC catalytic promotor, the modified Li-metal anodes achieve smooth plating with a long lifespan (1600 h) and high Coulombic efficiency without any dendrite formation. ... mehr


Verlagsausgabe §
DOI: 10.5445/IR/1000161514
Veröffentlicht am 23.08.2023
Originalveröffentlichung
DOI: 10.1002/adma.202302828
Scopus
Zitationen: 36
Web of Science
Zitationen: 32
Dimensions
Zitationen: 43
Cover der Publikation
Zugehörige Institution(en) am KIT Helmholtz-Institut Ulm (HIU)
Publikationstyp Zeitschriftenaufsatz
Publikationsjahr 2023
Sprache Englisch
Identifikator ISSN: 0935-9648, 1521-4095
KITopen-ID: 1000161514
HGF-Programm 38.02.01 (POF IV, LK 01) Fundamentals and Materials
Erschienen in Advanced Materials
Verlag John Wiley and Sons
Band 35
Heft 39
Seiten Art.-Nr.: 2302828
Vorab online veröffentlicht am 21.06.2023
Schlagwörter dendrite-free lithium plating, in situ sum frequency generation (SFG), Li-ion desolvation, lithium-metal batteries, single-atomic catalysts
Nachgewiesen in Scopus
Web of Science
Dimensions
Globale Ziele für nachhaltige Entwicklung Ziel 7 – Bezahlbare und saubere Energie
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