Noncovalently functionalized organic graphene aerogel composite for high-performance proton storage

doi:10.1016/j.cjche.2024.11.018

Abstract

Abstract: Although organic compounds are considered to be promising electrode materials with their remarkable characteristics such as diverse structures, design controllability, and environmental friendliness, their low charge-transfer capability and limited cycling durability hinder their application in aqueous proton batteries. Herein, we prepared a noncovalent phenazine-based graphene aerogel (H/G) composite for aqueous proton storage, which is realized by redox-active Hexaazatrinaphthalene (HATN) organic compound combined with conductive reduced graphene oxide (rGO). The integration of rGO into HATN not only effectively optimizes the electronic structure of the H/G composite to enhance its electrochemical activity, but also the favorable noncovalent π–π interaction existed between HATN and rGO provides a stable structure for fast electron transportation. The obvious electron transfer in the aerogel composite promotes fast and reversible redox reactions occurred with the imino-active HATN in the composite electrode for proton uptake/removal in an aqueous acidic electrolyte, which are demonstrated by in-situ Fourier transform infrared (FTIR) investigation, theoretical calculations and experimental measurements. Therefore, it can deliver a fast, stable and efficient aqueous proton storage behavior with a large specific capacity of 274 mA·h·g^-1 and considerable calendar life with ～100% capacity retention after 3000 cycles, surpassing previously reported proton-based organic electrodes in aqueous acidic electrolytes. Furthermore, an outstanding soft-package aqueous proton (APB) has been fabricated with considerable long-term cycling stability.

Key words: Organic compounds, Composite materials, Noncovalent interactions, Energy storage, Aqueous proton batteries

摘要： Although organic compounds are considered to be promising electrode materials with their remarkable characteristics such as diverse structures, design controllability, and environmental friendliness, their low charge-transfer capability and limited cycling durability hinder their application in aqueous proton batteries. Herein, we prepared a noncovalent phenazine-based graphene aerogel (H/G) composite for aqueous proton storage, which is realized by redox-active Hexaazatrinaphthalene (HATN) organic compound combined with conductive reduced graphene oxide (rGO). The integration of rGO into HATN not only effectively optimizes the electronic structure of the H/G composite to enhance its electrochemical activity, but also the favorable noncovalent π–π interaction existed between HATN and rGO provides a stable structure for fast electron transportation. The obvious electron transfer in the aerogel composite promotes fast and reversible redox reactions occurred with the imino-active HATN in the composite electrode for proton uptake/removal in an aqueous acidic electrolyte, which are demonstrated by in-situ Fourier transform infrared (FTIR) investigation, theoretical calculations and experimental measurements. Therefore, it can deliver a fast, stable and efficient aqueous proton storage behavior with a large specific capacity of 274 mA·h·g^-1 and considerable calendar life with ～100% capacity retention after 3000 cycles, surpassing previously reported proton-based organic electrodes in aqueous acidic electrolytes. Furthermore, an outstanding soft-package aqueous proton (APB) has been fabricated with considerable long-term cycling stability.

关键词: Organic compounds, Composite materials, Noncovalent interactions, Energy storage, Aqueous proton batteries

Jing He, Maoding Cheng, Qinglong Jiang, Subramania Angaiah, Minjie Shi, Chao Yan. Noncovalently functionalized organic graphene aerogel composite for high-performance proton storage[J]. Chinese Journal of Chemical Engineering, 2025, 79(3): 260-268.

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