Nanofillers’ applicability in gel polymer electrolyte
(GPE)-based
devices skyrocketed in the last decade as soon as their remarkable
benefits were realized. However, their applicability in GPE-based
electrochromic devices (ECDs) has hardly seen any development due
to challenges such as optical inhomogeneity brought by incompetent
nanofiller sizes, transmittance drop due to higher filler loading
(usually required), and poor methodologies of electrolyte fabrication.
To address such issues, herein, we demonstrate a reinforced polymer
electrolyte tailored through poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP),1-butyl-3-methylimidazolium tetrafluoroborate
(BMIMBF4), and four types of mesoporous SiO2 nanofillers, porous (distinct morphologies) and nonporous, two each.
The synthesized electrochromic species 1,1′-bis(4-fluorobenzyl)-4,4′-bipyridine-1,1′-diium
tetrafluoroborate (BzV, 0.05 M), counter redox species ferrocene (Fc,
0.05 M), and supporting electrolyte (TBABF4, 0.5 M) were
first dissolved in propylene carbonate (PC) and then immobilized in
an electrospun PVDF-HFP/BMIMBF4/SiO2 host. We
distinctly observed that spherical (SPHS) and hexagonal pore (MCMS)
morphologies of fillers endowed higher transmittance change (ΔT) and coloration efficiency (CE) in utilized ECDs; particularly
for the MCMS-incorporated ECD (GPE-MCMS/BzV-Fc ECD), ΔT reached ∼62.5% and CE soared to 276.3 cm2/C at 603 nm. The remarkable benefit of filler’s hexagonal
morphology was also seen in the GPE-MCMS/BzV-Fc ECD, which not only
marked an astounding ionic conductivity (σ) of ∼13.5
× 10–3 S cm–1 at 25 °C,
thus imitating the solution-type ECD’s behavior, but also retained
∼77% of initial ΔT after 5000 switching
cycles. The enhancement in ECD’s performance resulted from
merits brought by filler geometries such as the proliferation of Lewis
acid–base interaction sites due to the high surface-to-volume
ratio, the creation of percolating tunnels, and the emergence of capillary
forces triggering facile ion transportation in the electrolyte matrix.