Redox-driven confinement of quinone with imidazole in sub-nanometer sized porous carbon space mitigating chemical degradation for aqueous energy storage
JOURNAL OF MATERIALS CHEMISTRY A(2024)
摘要
Nanoconfinement of redox molecules influences their molecular interactions and leads to stabilization of a metastable form by alternation of their chemical reactivity, which is not observed in the bulk. Herein, we show that hydro- and benzoquinone can be (electro)chemically confined with imidazole in subnanometer-sized carbon pore regimes, and their chemical degradation induced by nucleophilic attacks was significantly mitigated. On the other hand, the formation of a quinone-imidazole complex became evident in a bulk solution phase containing both benzoquinone and imidazole. Molecular dynamics simulations and density functional theory calculation results clearly elucidated the stabilization of both hydro- and benzoquinone in a sub-nanometer sized carbon space due to their strong interactions with a carbon surface, which was thermodynamically more preferred than the formation of a quinone-imidazole complex. We further experimentally found that imidazole played a central role in stabilizing both hydro- and benzoquinone inside the restrained carbon pore regime. The charge-discharge characteristics associated with redox reactions by confined hydro- and benzoquinone in a microporous carbon regime were investigated and showed an similar to 97% capacity retention rate over the 100th cycle. The enhanced electrode kinetics of the confined quinone redox reaction on a mesoporous carbon electrode was also discussed. This study demonstrated that the physicochemical nature of hydro- and benzoquinone can be altered by their (electro)chemical confinement with imidazole in a subnanometer-sized carbon regime, and their resilience against the nucleophilic attack could impact the development of various quinone-based aqueous energy storage systems for long term cyclability. Hydro- and benzoquinone can be (electro)chemically confined with imidazole in subnanometer-sized carbon pore regimes, and their chemical degradation induced by nucleophilic attacks was significantly mitigated.
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