Abstract

Electrochemically tunable devices based on reversible metal electrodeposition have attracted extensive attention for energy-saving smart windows, information displays, digital signage, and variable reflectance mirrors, owing to their excellent optical modulation characteristics, low operation voltage, and superb electrochemical stability. Here, we study the effects of ionic liquid (IL)-based electrolytes on electrodeposition of the reversible electrochemical mirrors (REMs) by changing the organic cations of the ILs to obtain devices with the desired spectroelectrochemical and electrodeposited properties. Spectroelectrochemical measurements and scanning electron microscopy images show that organic cations drastically affect the switching speed and cycling durability, which we proposed on the basis of the difference in the absorption energies between cations and Ag(111) surfaces. Higher adsorption energy indicates strong adhesion between organic cations and Ag(111) surfaces, and this strong adsorption would prevent aggregation and agglomeration during the nucleation of Ag nanoparticles (AgNPs), leading to a denser and more compact electrodeposited Ag film and faster switching speeds (3.3 s for coloring and 14.3 s for bleaching). These findings allow us to fabricate dynamic devices that exhibit reversibly switchable light modulation at fast switching speeds and excellent cycling stability over thousands of cycles without attenuation. The combination of rapid switching and durable cycling stability enables tunable windows, which are based on reversible electrodeposition of metal Ag and IL-based electrolytes, make REM devices a competitive and promising alternative to traditional intelligent response materials.

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