[en] Poly(ethylene glycol) (PEG), despite being the most studied polymer electrolyte, suffers from serious drawbacks, which require fundamental studies behind its underperformance in lithium batteries. Here, we report the effect of the terminal group on triarm PEG stars bearing either hydroxyl (TPEG-OH) or carbonate-ketone (TPEG-Carb-ket) terminal groups. The latter is synthesized by a ring-opening reaction triggered by the -OH end group of TPEG-OH and results in a carbonate-ketone functionality. Indeed, the modified chain end is found to act as a sacrificial group by focusing the reactivity of the chain on the terminal group, protecting the rest of the TPEG molecule, which significantly reduces interfacial degradation and achieves a broader electrochemical stability window of up to 4.47 V, high Coulombic efficiency, and capacity retention. It furthermore demonstrates a stable interface with lithium metal after more than 1200 h of stripping and plating. When those electrolytes are investigated in reference cells based on LiFePO4 cathodes and Li anodes, the change in discharge capacity is observed from 118.7 to 113.8 and 108.9 to 5.03 mAh g-1 for TPEG-Carb-ket and TPEG-OH electrolytes, respectively, from the 1st to 100th cycle. The experimental results are further supported by density functional theory calculations and ab initio molecular dynamics simulations.
Research Center/Unit :
CESAM - Complex and Entangled Systems from Atoms to Materials - ULiège CERM - Center for Education and Research on Macromolecules - ULiège
Disciplines :
Materials science & engineering Chemistry
Author, co-author :
Raj, Ashish; Université Catholique de Louvain [UCLouvain] - Institute of Condensed Matter and Nanoscience [IMCN] - Belgium
Panchireddy, Satyannarayana ; Université Catholique de Louvain [UCLouvain] - Institute of Condensed Matter and Nanoscience [IMCN] - Belgium
Bekaert, Lieven ; Vrije Universiteit Brussel [VUB] - Department of Materials and Chemistry - Electrochemical and Surface Engineering [SURF] - Eenheid Algemene Chemie [ALGC] - Belgium
Grignard, Bruno ; University of Liège [ULiège] - Complex and Entangled Systems from Atoms to Materials [CESAM] Research Unit - Center for Education and Research on Macromolecules [CERM] - Belgium ; University of Liège [ULiège] - FRITCO2T Platform - Belgium
Detrembleur, Christophe ; University of Liège [ULiège] - Complex and Entangled Systems from Atoms to Materials [CESAM] Research Unit - Center for Education and Research on Macromolecules [CERM] - Belgium
Gohy, Jean-François ; Université Catholique de Louvain [UCLouvain] - Institute of Condensed Matter and Nanoscience [IMCN] - Belgium
Language :
English
Title :
Solid Polymer Electrolytes with Sacrificial End Groups for a Wide Oxidative Potential and Stable Interface in Lithium Metal Batteries.
Publication date :
11 September 2024
Journal title :
ACS Applied Materials and Interfaces
ISSN :
1944-8244
eISSN :
1944-8252
Publisher :
American Chemical Society, United States
Volume :
16
Issue :
36
Pages :
47464 - 47476
Peer reviewed :
Peer Reviewed verified by ORBi
Funders :
Innoviris - Institut Bruxellois pour la Recherche et l'Innovation SPW - Service Public de Wallonie F.R.S.-FNRS - Fonds de la Recherche Scientifique
Funding text :
AR and JFG are grateful to INNOVIRIS (BRIDGE project) and to Service Public de Wallonie (Win4Excellence BATFACTORY 310153 project) for supporting this research. C.D. is the F.R.S.-FNRS Research Director. The authors of Liege thank F.N.R.S. for funding.
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