Polysiloxane‐Based Single‐Ion Conducting Polymer Blend Electrolyte Comprising Small‐Molecule Organic Carbonates for High‐Energy and High‐Power Lithium‐Metal Batteries

Advanced Energy Materials, vol. 12

Abstract

Abstract 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||LiNi0.6Mn0.2Co0.2O2 (NMC622) and Li||LiNi0.8Mn0.1Co0.1O2 (NMC811) cells for several hundred cycles at relatively high discharge and charge rates. Remarkably, Li||NMC811 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.

Authors 8

1. Hai‐Peng Liang

   Karlsruhe Institute of Technology · Helmholtz-Institute Ulm

   Affiliation as printed

   Helmholtz Institute Ulm (HIU) Helmholtzstrasse 11 89081 Ulm Germany

   Karlsruhe Institute of Technology (KIT) P.O. Box 3640 76021 Karlsruhe Germany

   Helmholtz Institute Ulm (HIU), Helmholtzstrasse 11, 89081 Ulm, Germany

   Karlsruhe Institute of Technology (KIT), P.O. Box 3640, 76021 Karlsruhe, Germany

2. Maider Zarrabeitia

   Karlsruhe Institute of Technology · Helmholtz-Institute Ulm

   Affiliation as printed

   Helmholtz Institute Ulm (HIU) Helmholtzstrasse 11 89081 Ulm Germany

   Karlsruhe Institute of Technology (KIT) P.O. Box 3640 76021 Karlsruhe Germany

   Helmholtz Institute Ulm (HIU), Helmholtzstrasse 11, 89081 Ulm, Germany

   Karlsruhe Institute of Technology (KIT), P.O. Box 3640, 76021 Karlsruhe, Germany

3. Zhen Chen

   Karlsruhe Institute of Technology · Helmholtz-Institute Ulm

   Affiliation as printed

   Helmholtz Institute Ulm (HIU) Helmholtzstrasse 11 89081 Ulm Germany

   Karlsruhe Institute of Technology (KIT) P.O. Box 3640 76021 Karlsruhe Germany

   Helmholtz Institute Ulm (HIU), Helmholtzstrasse 11, 89081 Ulm, Germany

   Karlsruhe Institute of Technology (KIT), P.O. Box 3640, 76021 Karlsruhe, Germany

4. Sven Jovanovic Aachen Institute of Technical and Macromolecular Chemistry

   Forschungszentrum Jülich · RWTH Aachen University

   Affiliation as printed

   IEK‐9 Forschungszentrum Jülich Wilhelm‐Johnen Straße 52425 Jülich Germany

   Institute of Technical and Macromolecular Chemistry RWTH Aachen University 52074 Aachen Germany

   Institute of Technical and Macromolecular Chemistry, RWTH Aachen University, 52074 Aachen, Germany

5. Steffen Merz

   Forschungszentrum Jülich

   Affiliation as printed

   IEK‐9 Forschungszentrum Jülich Wilhelm‐Johnen Straße 52425 Jülich Germany

6. Josef Granwehr Aachen Institute of Technical and Macromolecular Chemistry

   Forschungszentrum Jülich · RWTH Aachen University

   Affiliation as printed

   IEK‐9 Forschungszentrum Jülich Wilhelm‐Johnen Straße 52425 Jülich Germany

   Institute of Technical and Macromolecular Chemistry RWTH Aachen University 52074 Aachen Germany

   Institute of Technical and Macromolecular Chemistry, RWTH Aachen University, 52074 Aachen, Germany

7. Stefano Passerini corresponding

   Karlsruhe Institute of Technology · Helmholtz-Institute Ulm

   Affiliation as printed

   Helmholtz Institute Ulm (HIU) Helmholtzstrasse 11 89081 Ulm Germany

   Karlsruhe Institute of Technology (KIT) P.O. Box 3640 76021 Karlsruhe Germany

   Helmholtz Institute Ulm (HIU), Helmholtzstrasse 11, 89081 Ulm, Germany

   Karlsruhe Institute of Technology (KIT), P.O. Box 3640, 76021 Karlsruhe, Germany

8. Dominic Bresser corresponding

   Karlsruhe Institute of Technology · Helmholtz-Institute Ulm

   Affiliation as printed

   Helmholtz Institute Ulm (HIU) Helmholtzstrasse 11 89081 Ulm Germany

   Karlsruhe Institute of Technology (KIT) P.O. Box 3640 76021 Karlsruhe Germany

   Helmholtz Institute Ulm (HIU), Helmholtzstrasse 11, 89081 Ulm, Germany

   Karlsruhe Institute of Technology (KIT), P.O. Box 3640, 76021 Karlsruhe, Germany