ORS6-0129
Engineering Single-Ion Conducting Poly(ionic liquids) via Novel Ionic Monomers and Polymer Architectures for Solid-State Batteries and Piezoionic Sensors
When and Where
Nov 30, -0001
12:00am - 12:00am
Presenter(s)
Alexander Shaplov (Functional Polymeric and Particulate Materials Unit, Luxembourg Institute of Science and Technology (LIST))
Co-Author(s)
Abstract
The realization of safe, high-performance solid-state Li batteries and piezoionic sensors demands polyelectrolytes combining high ionic conductivity (>10⁻⁵ S/cm at 25°C) with robust thermal and electrochemical stability. Poly(ionic liquid)s, as macromolecular counterparts of ionic liquids, offer promising platform, yet their development is limited by the intrinsic trade-off between ion transport and glass transition temperature, which constrains mechanical integrity and device performance. Here, we present a set of design strategies based on ionic random and block copolymers, as well as polymer networks.
First, block copolymers poly[TMCₙ-b-(LiMₘ-r-PEGM)ₖ] were synthesized via ROP of trimethylene carbonate followed by RAFT copolymerization of ionic monomer LiM with PEGM. These materials form hexagonally packed cylinders and exhibit improved viscoelastic properties, ionic conductivity 3.7×10⁻⁶ S/cm (70°C), high tLi⁺=0.91 and wide electrochemical stability (4.8V vs. Li⁺/Li). Li/LFP and Li/NMC cells deliver stable cycling with capacities up to 145 and 118 mAh/g (C/20, 70°C). Second, block copolymers comprising a conductive LiM/PEGM random segment and a rigid poly(2-phenylethyl methacrylate) block display lamellar ordering, enhanced mechanical strength, and σ=3.8×10⁻⁷ S/cm at 25°C, with tLi⁺=0.96 and ESW≈4.4V. Li/LFP cells show stable cycling up to 150 mAh/g.
Third, random copolymers incorporating a new ionic monomer with PEG spacer achieve σ= 3.0×10⁻⁶ S/cm at 25°C, ESW≈4.5V, and efficient dendrite suppression. Cells retain 100 mAh/g (200 cycles at C/5, 70 °C). Finally, crosslinked networks from ionic monomers, PEGM, and PEGDM reach 1.0×10⁻⁶ S/cm at 25°C and exhibit a piezoionic response of 290 mV under 80 kPa pressure, enabling unique, self-powered, soft electronic sensors.
Supported by Luxembourg National Research Fund (FNR) through the FNRS–FNR project INFINITE (INTER/FNRS/21/16555380).
First, block copolymers poly[TMCₙ-b-(LiMₘ-r-PEGM)ₖ] were synthesized via ROP of trimethylene carbonate followed by RAFT copolymerization of ionic monomer LiM with PEGM. These materials form hexagonally packed cylinders and exhibit improved viscoelastic properties, ionic conductivity 3.7×10⁻⁶ S/cm (70°C), high tLi⁺=0.91 and wide electrochemical stability (4.8V vs. Li⁺/Li). Li/LFP and Li/NMC cells deliver stable cycling with capacities up to 145 and 118 mAh/g (C/20, 70°C). Second, block copolymers comprising a conductive LiM/PEGM random segment and a rigid poly(2-phenylethyl methacrylate) block display lamellar ordering, enhanced mechanical strength, and σ=3.8×10⁻⁷ S/cm at 25°C, with tLi⁺=0.96 and ESW≈4.4V. Li/LFP cells show stable cycling up to 150 mAh/g.
Third, random copolymers incorporating a new ionic monomer with PEG spacer achieve σ= 3.0×10⁻⁶ S/cm at 25°C, ESW≈4.5V, and efficient dendrite suppression. Cells retain 100 mAh/g (200 cycles at C/5, 70 °C). Finally, crosslinked networks from ionic monomers, PEGM, and PEGDM reach 1.0×10⁻⁶ S/cm at 25°C and exhibit a piezoionic response of 290 mV under 80 kPa pressure, enabling unique, self-powered, soft electronic sensors.
Supported by Luxembourg National Research Fund (FNR) through the FNRS–FNR project INFINITE (INTER/FNRS/21/16555380).
