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Abstract. The possibility to use natural polymer as ionic conducting matrix was investigated in this study. Samples of agarbased electrolytes with different ionic liquids were prepared and characterized by physical and chemical analyses. Samples of solvent-free electrolytes were prepared and characterized by ionic conductivity measurements, thermal analysis, electrochemical stability, X-ray diffraction, scanning electron microscopy and Fourier Transform infrared spectroscopy. Electrolyte samples are thermally stable up to approximately 190°C. All the materials synthesized are semicrystalline. The electrochemical stability domain of all samples is about 2.0 V versus Li/Li + . The preliminary studies carried out with electrochromic devices (ECDs) incorporating optimized compositions have confirmed that these materials may perform as satisfactory multifunctional component layers in the field of 'smart windows', as well as ECD-based devices.

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We introduce a bioinspired strategy for the synthesis of green polymer electrolytes (PEs) that relies on the use of silk fibroin (SF). The two series of PEs prepared, doped with lithium bis(trifluoromethanesulfonyl)imide or lithium tetrafluoroborate and incorporating glycerol, exhibited outstanding filmogenic properties, very high transparency, and suitable adhesion to glass substrates. Despite their poor ionic conductivity, the SF‐based films were employed in the construction of glass/ITO/WO3/PE/CeO2–TiO2/ITO/glass electrochromic devices displaying an optical modulation up to 5.5 % at λ=633 nm, a switching speed of about 15 s, stability up to 5160 cycles, and coloration efficiency up to −53.1 m2 C−1. This work, in which we provide the proof‐of‐concept, paves the way for new design approaches for silk‐based materials, which would enlarge the range of applications of SF to the energy field.

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