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Polysiloxane‐Based Single‐Ion Conducting Polymer Blend Electrolyte Comprising Small‐Molecule Organic Carbonates for High‐Energy and High‐Power Lithium‐Metal Batteries
Author(s) -
Liang HaiPeng,
Zarrabeitia Maider,
Chen Zhen,
Jovanovic Sven,
Merz Steffen,
Granwehr Josef,
Passerini Stefano,
Bresser Dominic
Publication year - 2022
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.202200013
Subject(s) - materials science , electrolyte , electrochemistry , polymer , chemical engineering , hexafluoropropylene , cathode , lithium (medication) , electrochemical window , ionic conductivity , membrane , battery (electricity) , inorganic chemistry , electrode , composite material , chemistry , copolymer , medicine , biochemistry , tetrafluoroethylene , engineering , endocrinology , power (physics) , physics , quantum mechanics
Single‐ion conducting polymer electrolytes are considered particularly attractive for realizing high‐performance solid‐state lithium‐metal batteries. Herein, a polysiloxane‐based single‐ion conductor (PSiO) is investigated. The synthesis is performed via a simple thiol‐ene reaction, yielding flexible and self‐standing polymer electrolyte membranes (PSiOM) when blended with poly(vinylidene fluoride‐ co ‐hexafluoropropylene) (PVdF‐HFP). When incorporating 57 wt% of organic carbonates, these polymer membranes provide a Li + conductivity of >0.4 mS cm −1 at 20 °C and a wide electrochemical stability window of more than 4.8 V. This excellent electrochemical stability allows for the highly reversible cycling of symmetric Li||Li cells as well as high‐energy Li||LiNi 0.6 Mn 0.2 Co 0.2 O 2 (NMC 622 ) and Li||LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC 811 ) cells for several hundred cycles at relatively high discharge and charge rates. Remarkably, Li||NMC 811 cells with high mass loading cathodes provide more than 76% capacity retention at a high current density of 1.44 mA cm −2 , thus rendering this polymer electrolyte suitable for high‐performance battery applications.