Redox-driven confinement of quinone with imidazole in sub-nanometer sized porous carbon space mitigating chemical degradation for aqueous energy storage

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 i...

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Veröffentlicht in:Journal of materials chemistry. A, Materials for energy and sustainability Materials for energy and sustainability, 2024-03, Vol.12 (1), p.5778-5792
Hauptverfasser: Yang, Jeehae, Park, Anseong, Kwon, Taesung, Lee, Yongkyu, Lee, Won Bo, Nam, Ki Min, Kim, YongJoo, Chang, Jinho
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Sprache:eng
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Zusammenfassung: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 ∼97% capacity retention rate over the 100 th 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.
ISSN:2050-7488
2050-7496
DOI:10.1039/d3ta07180d