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Interfacial “Single-Atom-in-Defects” Catalysts Accelerating Li+ Desolvation Kinetics for Long-Lifespan Lithium-Metal Batteries.
Adv. Mater. 35 (2023)
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+, Li0 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 Co1−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. Paired with the LiFePO4 cathode, the full cell (10.7 mg cm−2) stabilizes a capacity retention of 90.3% after 300 cycles at 0.5 C, signifying the feasibility of using interfacial catalysts for modulating Li behaviors toward practical applications.
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Publication type
Article: Journal article
Document type
Scientific Article
Keywords
Dendrite-free Lithium Plating ; In situ Sum Frequency Generation (sfg) ; Li-ion Desolvation ; Lithium-metal Batteries ; Single-atomic Catalysts
Language
english
Publication Year
2023
HGF-reported in Year
2023
ISSN (print) / ISBN
0935-9648
e-ISSN
1521-4095
Journal
Advanced materials
Quellenangaben
Volume: 35,
Issue: 39
Publisher
Wiley
Publishing Place
Weinheim
Reviewing status
Peer reviewed
Institute(s)
Helmholtz AI - KIT (HAI - KIT)
Scopus ID
85166952666
Erfassungsdatum
2023-10-18