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. 2016 Jan 21:6:19892.
doi: 10.1038/srep19892.

Super Soft All-Ethylene Oxide Polymer Electrolyte for Safe All-Solid Lithium Batteries

Luca Porcarelli  1 , Claudio Gerbaldi  1 , Federico Bella  1 , Jijeesh Ravi Nair  1
Affiliations

Super Soft All-Ethylene Oxide Polymer Electrolyte for Safe All-Solid Lithium Batteries

Luca Porcarelli et al. Sci Rep. .

Abstract

Here we demonstrate that by regulating the mobility of classic -EO- based backbones, an innovative polymer electrolyte system can be architectured. This polymer electrolyte allows the construction of all solid lithium-based polymer cells having outstanding cycling behaviour in terms of rate capability and stability over a wide range of operating temperatures. Polymer electrolytes are obtained by UV-induced (co)polymerization, which promotes an effective interlinking between the polyethylene oxide (PEO) chains plasticized by tetraglyme at various lithium salt concentrations. The polymer networks exhibit sterling mechanical robustness, high flexibility, homogeneous and highly amorphous characteristics. Ambient temperature ionic conductivity values exceeding 0.1 mS cm(-1) are obtained, along with a wide electrochemical stability window (>5 V vs. Li/Li(+)), excellent lithium ion transference number (>0.6) as well as interfacial stability. Moreover, the efficacious resistance to lithium dendrite nucleation and growth postulates the implementation of these polymer electrolytes in next generation of all-solid Li-metal batteries working at ambient conditions.

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Figures

Figure 1
Figure 1. Sketched representation of ISPE preparation along with used materials, and plausible illustration (right bottom) of interconnected PEO chains with hypothesized branched clusters of tetraglyme oligomers; on the top right, the real aspect of a freshly prepared ISPE.
Figure 2
Figure 2
Micrographs showing the overall morphology of sample PTL-1: cross-section under secondary electron mode (A,B) and top view (C,D), at different magnifications; (E,F) shown the images of the sample PTL-1 (at 25 °C) under stretch and bend mode, demonstrating the mechanical integrity and excellent elasticity.
Figure 3
Figure 3
(a) Differential scanning calorimetry (DSC) curves of the ISPEs PTL-1 to PTL-3 that contains various amounts of LiTFSI salt. (b) Thermogravimetric analysis (TGA) of the same series of ISPEs along with related differential curves (dotted lines of same color code). Taking into account the experimental errors related to the measurement and the sample preparation, all weight losses are consistent with the polymer electrolyte compositions.
Figure 4
Figure 4
(A) Arrhenius plot showing the ionic conductivity vs. temperature for ISPEs prepared with various LiTFSI content. (B–D) VTF fitting of the samples PTL-1 to PTL-3.
Figure 5
Figure 5
(a) 3D Nyquist plot representing the evolution of the interfacial resistance with time for sample PTL-1, using the Li/PTL-1/Li cell configuration. (b) Electrochemical stability window (anodic and cathodic scan) of PTL-1. The tests were performed at 25 °C.
Figure 6
Figure 6. Potential vs. test time of lithium stripping and plating of a symmetrical lithium cell at various current rates (i.e., 0.05, 0.1, 0.2 mA cm−2) at 20 °C.
Figure 7
Figure 7
(a) Photograph of bare TiO2 based electrode and electrolyte before UV curing. (b) Freshly prepared self-supporting multiphase electrode/electrolyte composite obtained by direct hot-pressing and in situ photopolymerisation of the polymer electrolyte over the TiO2-electrode film supported over copper foil. (c) Cross-sectional FESEM images showing the optimum interface achieved after UV curing.
Figure 8
Figure 8
(A) Representative charge/discharge profiles of a cell assembled with the configuration of Li/PTL-1/TiO2. The cycling test was performed at 20 °C at a current density of 0.1 mA cm−2. (B) Graph illustrating the specific capacity vs. number of cycles along with Coulombic efficiency.
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