[en] Polycarbonates bearing linear carbonate linkages and polyether segments have demonstrated to be highly attractive solid electrolyte candidates for the design of safe energy storage devices, e.g. lithium metal batteries. In this contribution, we are studying the influence of the introduction of some cyclic carbonate linkages within the polymer backbone on the electrolyte properties. We first describe the synthesis of polycarbonates/polyethers containing different contents of both linear and cyclic carbonate linkages within the chain by the copolymerization of a highly reactive CO2-based monomer (bis(-alkylidene cyclic carbonate)) with poly(ethylene glycol) diol and a dithiol at room temperature. We then explore the influence of the content of the cyclic carbonates and the loading of the polymer by lithium bis(trifluoromethane) sulfonimide (LiTFSI) on the electrolyte properties (glass transition and melting temperatures, ion conductivity and diffusivity). The best electrolyte candidate is characterized by a linear/cyclic carbonate linkage ratio of 82/18 when loaded with 30 wt% LiTFSI. It exhibits an ion conductivity of 5.6 10-5 S cm-1 at 25°C (7.9 10-4 S cm-1 at 60 °C), which surpasses by 150 % (424 % at 60 °C) the conductivity measured for a similar polymers bearing linear carbonate linkages only. It is also characterized by a high oxidation stability up to 5.6 V (vs. Li/Li+). A self-standing membrane is then constructed by impregnating a glass fiber filter by this optimal polymer, LiTFSI and a small amount of a plasticizer (tetraglyme). Cells are then assembled by sandwiching the membrane between a C-coated LiFePO4 (LFP) as the cathode and lithium as the anode and counter electrode. The cycling performances are evaluated at 0.1 C at 60 °C and room temperature for 40 cycles. Excellent cycling performances are noted with 100 % of the theoretical capacity (170 mAh g-1) at 60 °C, and 73.5 % of the theoretical capacity (125 mAh g-1) at 25 °C.
Research Center/Unit :
Center for Education and Research on Macromolecules (CERM) Complex and Entangled Systems from Atoms to Materials (CESAM) Research Unit
Disciplines :
Chemistry Materials science & engineering
Author, co-author :
Ouhib, Farid ; University of Liège (ULiège), Complex and Entangled Systems from Atoms to Materials (CESAM) Research Unit, Center for Education and Research on Macromolecules (CERM), Belgium
Meabe, Leire; University of the Basque Country, POLYMAT, Donostia/SanSebastian, Spain
Mahmoud, Abdelfattah ; University of Liège (ULiège), Complex and Entangled Systems from Atoms to Materials (CESAM), Group of Research in Energy and ENvironment from MATerials (Greenmat) and Laboratory of Structural Inorganic Chemistry (LCIS), 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
Thomassin, Jean-Michel ; University of Liège (ULiège), Complex and Entangled Systems from Atoms to Materials (CESAM) Research Unit, Center for Education and Research on Macromolecules (CERM), Belgium
Boschini, Frédéric ; University of Liège (ULiège), Complex and Entangled Systems from Atoms to Materials (CESAM), Group of Research in Energy and ENvironment from MATerials (Greenmat) and Laboratory of Structural Inorganic Chemistry (LCIS), Belgium
Zhu, Haijin; Deakin University, Institute for Frontier Materials (IFM), Waurn Ponds, Australia
Forsyth, Maria; Deakin University, Institute for Frontier Materials (IFM), Waurn Ponds, Australia > IKERBASQUE Basque Foundation for Science, Bilbao, Spain
Mecerreyes, David; University of the Basque Country, POLYMAT, Donostia/SanSebastian, Spain
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
Language :
English
Title :
Influence of the cyclic vs. linear carbonate segments in the properties and performance of CO2-sourced polymer electrolytes for lithium batteries
Publication date :
14 February 2020
Journal title :
ACS Applied Polymer Materials
eISSN :
2637-6105
Publisher :
American Chemical Society (ACS), Washington, United States - District of Columbia
Volume :
2
Issue :
2
Pages :
922-931
Peer reviewed :
Peer Reviewed verified by ORBi
Funders :
EC - European Commission Région wallonne ERC - European Research Council Gobierno Vasco FWO - Fonds Wetenschappelijk Onderzoek Vlaanderen EOS - The Excellence Of Science Program
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