Fluorine-free water-in-ionomer electrolytes for sustainable lithium-ion batteries

Xin He, Bo Yan, Xin Zhang (), Zigeng Liu, Dominic Bresser, Jun Wang, Rui Wang, Xia Cao, Yixi Su, Hao Jia, Clare P. Grey, Henrich Frielinghaus, Donald G. Truhlar, Martin Winter, Jie Li () and Elie Paillard ()
Additional contact information
Xin He: Helmholtz Institute Münster – Forschungszentrum Jülich GmbH (IEK 12)
Bo Yan: Helmholtz Institute Münster – Forschungszentrum Jülich GmbH (IEK 12)
Xin Zhang: Beijing University of Chemical Technology
Zigeng Liu: University of Cambridge, Lensfield Road
Dominic Bresser: University Grenoble Alpes, CEA, CNRS, SyMMES
Jun Wang: University of Münster
Rui Wang: Forschungszentrum Jülich GmbH
Xia Cao: University of Münster
Yixi Su: Forschungszentrum Jülich GmbH
Hao Jia: University of Münster
Clare P. Grey: University of Cambridge, Lensfield Road
Henrich Frielinghaus: Forschungszentrum Jülich GmbH
Donald G. Truhlar: University of Minnesota
Martin Winter: Helmholtz Institute Münster – Forschungszentrum Jülich GmbH (IEK 12)
Jie Li: University of Münster
Elie Paillard: Helmholtz Institute Münster – Forschungszentrum Jülich GmbH (IEK 12)

Nature Communications, 2018, vol. 9, issue 1, 1-8

Abstract: Abstract The continuously increasing number and size of lithium-based batteries developed for large-scale applications raise serious environmental concerns. Herein, we address the issues related to electrolyte toxicity and safety by proposing a “water-in-ionomer” type of electrolyte which replaces organic solvents by water and expensive and toxic fluorinated lithium salts by a non-fluorinated, inexpensive and non-toxic superabsorbing ionomer, lithium polyacrylate. Interestingly, the electrochemical stability window of this electrolyte is extended greatly, even for high water contents. Particularly, the gel with 50 wt% ionomer exhibits an electrochemical stability window of 2.6 V vs. platinum and a conductivity of 6.5 mS cm−1 at 20 °C. Structural investigations suggest that the electrolytes locally self-organize and most likely switch local structures with the change of water content, leading to a 50% gel with good conductivity and elastic properties. A LiTi2(PO4)3/LiMn2O4 lithium-ion cell incorporating this electrolyte provided an average discharge voltage > 1.5 V and a specific energy of 77 Wh kg−1, while for an alternative cell chemistry, i.e., TiO2/LiMn2O4, a further enhanced average output voltage of 2.1 V and an initial specific energy of 124.2 Wh kg−1 are achieved.

Date: 2018
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DOI: 10.1038/s41467-018-07331-6

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