High-Performance Sustainable Electrochromic Devices Based on Carrageenan Solid Polymer Electrolytes with Ionic Liquid

[Image: see text] The development of sustainable functional materials with strong potential to be applied in different areas has been growing and gaining increasing interest to address the environmental impact of current materials and technologies. In this scope, this work reports on sustainable functional materials with electrochromic properties, based on their increasing interest for a variety of applications, including sensing technologies. The materials have been developed based on a natural derived polymer, carrageenan, in which different amounts of the ionic liquid (IL) 1-ethyl-3-methylimidazolium thiocyanate ([EMIM][SCN]) were blended. It is shown that the addition of different amounts of IL to the carrageenan matrix does not affect the properties of the samples in terms of morphology or physicochemical and thermal properties, the most significant difference being the increase of the ionic conductivity with increasing IL content, ranging from 2.3 × 10(–11) S·cm(–1) for pristine carrageenan to 4.6 × 10(–4) S·cm(–1) for the samples with 5 and 60 wt % IL content, respectively. A electrochromic device has been developed based on the different IL/carrageenan samples as electrolyte and poly(3,4-ethylenedioxythiophene) polystyrenesulfonate (PEDOT:PSS) as electrodes. Spectroelectrochemistry testing demonstrates functional devices at low voltages between 0.3 and −0.9 V. Among the different samples, the one with 15 wt % IL content presents the best conditions for application, presenting an oxidation time of 6 s, a reduction time of 8 s, and a charge density of 1150 and 1050 μC·cm(–2) for oxidation and reduction, respectively. The same sample also presents excellent optical density as a function of load density, presenting an optical switch (Δ%Tx) of 99%. Thus, it is demonstrated that it is possible to develop high efficiency and sustainable electrochromic devices based on natural polymers and ionic liquids.