Deep eutectic solvents (DESs) are emerging as tunable and sustainable electrolytic media for electrochemical applications due to their low volatility, high ionic conductivity, and environmental compatibility. In this study, a series of acidic DESs was systematically evaluated through physicochemical characterizations (e.g., viscosity, density, conductivity) and electrochemical techniques (e.g., cyclic voltammetry) to determine their electrochemical potential windows and stability. Among the formulations tested, a selection of high-performing DESs was screened using ferrocene as a model redox couple to assess their compatibility and redox behavior. The most promising DESs were employed for the exfoliation of activated carbon derived from sustainable biomass sources. This green exfoliation approach was used to synthesize two-dimensional carbon nanomaterials: graphene (EG) and nitrogen-doped graphene (N-EG). In parallel, nitrogen doped carbon nanotubes (CNTs) were prepared via a chemical process to compare their performances with N-EG. These modifiers were deposited onto carbon cloth substrates via cathodic electrophoretic deposition (EPD), forming high-surface-area, conductive electrodes. Further, the coated electrodes were evaluated in a three-electrode cell configuration using the positive electrolyte of the all-vanadium redox flow battery (RFB) as well as a functionalized benzoquinone-based electrolyte, a promising class of redox-active organic molecules for aqueous RFB systems. Key electrochemical performance metrics, such as cyclic voltammetry and electrochemical impedance spectroscopy were used to optimize the most effective electrode–electrolyte combinations. This work established a sustainable, DES-enabled pathway for producing advanced carbon-based electrocatalysts. The best-performing electrode materials from this study will be further investigated as catalytic electrodes in full-cell hydrogen/quinone regenerative fuel cells aiming to enhance the efficiency and scalability of next-generation organic energy storage systems.

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Development of DES-Processed Graphene-Based Electrocatalysts for Quinone Redox Flow Battery Applications

  • Shamik Chaudhuri,
  • Züleyha Kudaş,
  • Reza Afshar Ghotli,
  • Nadir Deniz Akgül,
  • Mustafa Kemal Bayazıt,
  • Serap Hayat Soytaş,
  • Tülay Yılmaz İnan,
  • Farouq Sabri Mjalli,
  • Andres Parra-Puerto,
  • Stefan Spirk,
  • Barun Kumar Chakrabarti

摘要

Deep eutectic solvents (DESs) are emerging as tunable and sustainable electrolytic media for electrochemical applications due to their low volatility, high ionic conductivity, and environmental compatibility. In this study, a series of acidic DESs was systematically evaluated through physicochemical characterizations (e.g., viscosity, density, conductivity) and electrochemical techniques (e.g., cyclic voltammetry) to determine their electrochemical potential windows and stability. Among the formulations tested, a selection of high-performing DESs was screened using ferrocene as a model redox couple to assess their compatibility and redox behavior. The most promising DESs were employed for the exfoliation of activated carbon derived from sustainable biomass sources. This green exfoliation approach was used to synthesize two-dimensional carbon nanomaterials: graphene (EG) and nitrogen-doped graphene (N-EG). In parallel, nitrogen doped carbon nanotubes (CNTs) were prepared via a chemical process to compare their performances with N-EG. These modifiers were deposited onto carbon cloth substrates via cathodic electrophoretic deposition (EPD), forming high-surface-area, conductive electrodes. Further, the coated electrodes were evaluated in a three-electrode cell configuration using the positive electrolyte of the all-vanadium redox flow battery (RFB) as well as a functionalized benzoquinone-based electrolyte, a promising class of redox-active organic molecules for aqueous RFB systems. Key electrochemical performance metrics, such as cyclic voltammetry and electrochemical impedance spectroscopy were used to optimize the most effective electrode–electrolyte combinations. This work established a sustainable, DES-enabled pathway for producing advanced carbon-based electrocatalysts. The best-performing electrode materials from this study will be further investigated as catalytic electrodes in full-cell hydrogen/quinone regenerative fuel cells aiming to enhance the efficiency and scalability of next-generation organic energy storage systems.