Electrochromic and Energy Storage Performance Enhancement by Introducing Jahn–Teller Distortion: Experimental and Theoretical Study

Aqueous electrochromic batteries (ECBs) have recently garnered significant attention within the realm of renewable rechargeable technology due to their potential applicability in diverse multifunctional devices featuring visible-level indicator batteries. However, there exists an imperative to comprehend the underlying structural factors that contribute to achieving an elevated electrochemical performance. In this context, we have synthesized and compared WO3·H2O (HWO) specifically for heightened ECB application as against the performance of a standard anhydrous WO3 (AWO). To unravel the underlying cause, a density functional theory (DFT) investigation is carried out, disclosing a structural deformation of HWO, unlike AWO, due to Jahn–Teller distortion induced by the presence of interlayer water. It results in a fully compatible HWO ion host to devise a zinc-ion aqueous electrolyte electrochromic battery, exhibiting superior redox reactivity, optical modulation (50%), capacity (200 mAh/m2), and cyclic stability. To glean insights into the dynamic structural alterations during the intercalation and deintercalation processes of Zn2+, ex situ X-ray diffraction and Raman spectroscopic studies are carried out. These investigations culminate in the determination that HWO films are better suited for the application than their AWO counterparts. This finding holds promise for advancing the applications of ECBs and represents a significant step forward in this field.