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Text from PDF Page: 001nanomaterials Article 3D Printable Composite Polymer Electrolytes: Influence of SiO2 Nanoparticles on 3D-Printability Zviadi Katcharava , Anja Marinow, Rajesh Bhandary and Wolfgang H. Binder * Macromolecular Chemistry, Division of Technical and Macromolecular Chemistry, Faculty of Natural Sciences II (Chemistry, Physics, Mathematics), Institute of Chemistry, Martin Luther University Halle-Wittenberg, von-Danckelmann-Platz 4, D-06120 Halle, Germany; email@example.com (Z.K.); firstname.lastname@example.org (A.M.); email@example.com (R.B.) * Correspondence: firstname.lastname@example.org Abstract: We here demonstrate the preparation of composite polymer electrolytes (CPEs) for Li-ion batteries, applicable for 3D printing process via fused deposition modeling. The prepared com- posites consist of modified poly(ethylene glycol) (PEG), lithium bis(trifluoromethylsulfonyl)imide (LiTFSI) and SiO2-based nanofillers. PEG was successfully end group modified yielding telechelic PEG containing either ureidopyrimidone (UPy) or barbiturate moieties, capable to form supramolec- ular networks via hydrogen bonds, thus introducing self-healing to the electrolyte system. Silica nanoparticles (NPs) were used as a filler for further adjustment of mechanical properties of the electrolyte to enable 3D-printability. The surface functionalization of the NPs with either ionic liquid (IL) or hydrophobic alkyl chains is expected to lead to an improved dispersion of the NPs within the polymer matrix. Composites with different content of NPs (5%, 10%, 15%) and LiTFSI salt (EO/Li+ = 5, 10, 20) were analyzed via rheology for a better understanding of 3D printability, and via Broadband Dielectric Spectroscopy (BDS) for checking their ionic conductivity. The composite electrolyte PEG 1500 UPy2/LiTFSI (EO:Li 5:1) mixed with 15% NP-IL was successfully 3D printed, revealing its suitability for application as printable composite electrolytes. Keywords: polymer composite electrolyte; 3D-printing; silica nanoparticles; supramolecular polymers 1. Introduction Since their commercialization in 1990s rechargeable lithium ion batteries (LIBs) are considered the most promising candidates as alternative clean energy sources beyond fossil fuels. Although LIBs exhibit several advantages such as high energy density, low self- discharge and long cycle life, the potential safety issues connected to the wide use of volatile, leachable and highly flammable organic liquid electrolytes, present main bottlenecks hampering their further development. Solid polymer electrolytes (SPEs) displaying low flammability, enhanced electrochemical performance, good processability and flexibility, have the potential to overcome the limitations associated with liquid electrolytes tackling a route towards safe next-generation high energy density batteries [1,2]. Although in the meantime various polymeric materials such as polycarbonates, poly(methacrylate)s, poly(acrylonitrile)s or poly(ionic liquid)s have been investigated as SPEs, poly(ethylene glycol) (PEG) is still the most investigated polymer in this area, due to its relatively low melting- and glass transition temperature and its ability to dissolve large amounts of lithium salts and actively participate in Li-ion transport [1–5]. Nevertheless, low room temperature ionic conductivity (10−8–10−5 S/cm) as well as moderate mechanical integrity of SPEs still makes the development of alternative electrolyte materials desirable. While PEG with molecular weights above 10 kDa displays an insufficient Li-ion conductivity [4,5] one of the promising approaches is the incorporation of inorganic (nano)particles into SPEs, where the synergy of inorganic and organic materials leads to an improvement of material properties and conductivity, such as Li-ion transport. In Citation: Katcharava, Z.; Marinow, A.; Bhandary, R.; Binder, W.H. 3D Printable Composite Polymer Electrolytes: Influence of SiO2 Nanoparticles on 3D-Printability. Nanomaterials 2022, 12, 1859. https://doi.org/10.3390/ nano12111859 Academic Editor: Kambiz Chizari Received: 29 April 2022 Accepted: 26 May 2022 Published: 29 May 2022 Publisher’s Note: MDPI stays neutral with regard to jurisdictional claims in published maps and institutional affil- iations. Copyright: © 2022 by the authors. Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https:// creativecommons.org/licenses/by/ 4.0/). Nanomaterials 2022, 12, 1859. https://doi.org/10.3390/nano12111859 https://www.mdpi.com/journal/nanomaterials
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