High-voltage aqueous supercapacitors enabled by polysiloxane passivation coating-modified carbon cloth electrode

The voltage window plays a crucial role in determining the energy density of supercapacitors. The limited energy density of carbon-based supercapacitors poses a significant challenge to their widespread adoption. Here, we propose a novel approach to modify carbon cloth by implementing a polysiloxane (PSiO) passivation coating. This forms an ion-conductive and electron-insulating thin film on the surface, effectively impeding electron conduction from electrode surface to electrode/electrolyte interface and suppressing electrolyte electrolysis. Consequently, an expanded voltage window is realized, thereby enhancing the energy density of aqueous carbon-based supercapacitors. The carbon cloth electrode modified with the PSiO passivation coating (CC-A-KH560) exhibits exceptional electrochemical performance, with a significantly increased 78.6 % widened applicable potential range compared to the activated carbon cloth electrode (CC-A). In a two-electrode configuration, the voltage window is broadened from 0.8 V for CC-A to 1.4 V for CC-A-KH560, and the energy density based on CC-A-KH560 is 8 times that based on CC-A. The good stability and durability are also obtained for the firm C–O–Si bonds during PSiO modification. More importantly, this design provides a generic solution of PSiO passivation coating-modified carbon electrode, applicable for diversified silicane couple agents, to realize a high-voltage energy storage performance for aqueous supercapacitors.