A porous hydrogen-bonded organic framework (HOF) structure was explored for the first time in the design of high-performance electrochromic devices (ECDs) using polyoxometalate (POM)-based charge-balancing layers as counter electrodes (CEs). The novelty of this work lies in the facile construction of films using small molecule-based EC materials to form a porous HOF structure. A full-cell model of an ECD was constructed by utilizing a POM-based CE to optimize the voltage distribution on the HOF-coated working electrode (WE). The addition of PWO (PW) on CE significantly enhanced the voltage distribution on EC electrodes and decreased the overvoltage on the WE, further preventing the formation of non-EC species and resulting in a 3.3-fold increase in the lifetime of the ECD. The optical contrast was enhanced from 47% (TiO only) to 68%, and the coloration efficiency was enhanced from 185 (TiO only) to 373 cm C. The optimized voltage distribution on the WE, leading to the fast response time and high optical EC contrast, could be explained by the charge-balancing effect. Overall, this new finding provides a robust framework for designing high-performance ECDs, taking advantage of the porous morphology and potential matching of the HOF and PW.
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