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<p>This study presents the synthesis, characterization, and electrochemical assessment of a new fluorinated sulfonamide-based organic catalyst, FBS⁻, which is immobilized on a glassy carbon electrode (GCE) using Nafion for the electrocatalytic oxidation of hydrazine (N₂H₄) in an alkaline environment. Structural analysis through <sup>1</sup>H and <sup>13</sup>C NMR, including 2D COSY, confirms the anticipated substitution pattern on the aromatic ring, which includes a fluorine atom that enhances electronic stability and oxidative resistance. Density Functional Theory (DFT) calculations- including HOMO–LUMO analysis, Electron Localization Function (ELF), Localization of Orbitals (LOL), Average Local Ionization Energy (ALIE), and Molecular Electrostatic Potential (MEP) maps- demonstrate a weak HOMO–LUMO gap (2.122 eV), substantial electron density concentration on the sulfonamide part, and significant redox activity of the anionic form. Electrochemical tests reveal that FBS⁻ serves as a bifunctional catalyst, facilitating electron transfer and local deprotonation of hydrazine. Cyclic voltammetry demonstrates a significant increase in current density (up to 33.33 mA/cm<sup>2</sup>) in the presence of hydrazine, while chronoamperometry and electrochemical impedance spectroscopy (EIS) corroborate its outstanding stability and low charge transfer resistance. The analysis of the scan rate-dependent CV reveals a linear relationship between peak current and the square root of the scan rate (R<sup>2</sup> = 0.993), suggesting a diffusion-controlled mechanism. Relative to other organic and noble-metal-based systems, FBS⁻ exhibits superior performance, merging high catalytic activity, chemical durability, and straightforward synthetic accessibility. These results position FBS⁻ as a promising, metal-free electrocatalyst for hydrazine oxidation and related energy and environmental, analytical, and electroanalytical applications.</p>

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Electrochemical and computational study of novel 5-fluoro-2-(methylamino) benzenesulfonamide as an organic catalyst for hydrazine electrooxidation

  • 期刊论文

  • 发表日期：

    2025年6月10日

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  • Katia Mohand Saidi,
  • Nafila Bouider,
  • Bassam A. Najri,
  • Kamel Harrouche,
  • Hilal Kivrak,
  • Arif Kivrak,
  • Smail Khelili

摘要

This study presents the synthesis, characterization, and electrochemical assessment of a new fluorinated sulfonamide-based organic catalyst, FBS⁻, which is immobilized on a glassy carbon electrode (GCE) using Nafion for the electrocatalytic oxidation of hydrazine (N₂H₄) in an alkaline environment. Structural analysis through 1H and 13C NMR, including 2D COSY, confirms the anticipated substitution pattern on the aromatic ring, which includes a fluorine atom that enhances electronic stability and oxidative resistance. Density Functional Theory (DFT) calculations- including HOMO–LUMO analysis, Electron Localization Function (ELF), Localization of Orbitals (LOL), Average Local Ionization Energy (ALIE), and Molecular Electrostatic Potential (MEP) maps- demonstrate a weak HOMO–LUMO gap (2.122 eV), substantial electron density concentration on the sulfonamide part, and significant redox activity of the anionic form. Electrochemical tests reveal that FBS⁻ serves as a bifunctional catalyst, facilitating electron transfer and local deprotonation of hydrazine. Cyclic voltammetry demonstrates a significant increase in current density (up to 33.33 mA/cm2) in the presence of hydrazine, while chronoamperometry and electrochemical impedance spectroscopy (EIS) corroborate its outstanding stability and low charge transfer resistance. The analysis of the scan rate-dependent CV reveals a linear relationship between peak current and the square root of the scan rate (R2 = 0.993), suggesting a diffusion-controlled mechanism. Relative to other organic and noble-metal-based systems, FBS⁻ exhibits superior performance, merging high catalytic activity, chemical durability, and straightforward synthetic accessibility. These results position FBS⁻ as a promising, metal-free electrocatalyst for hydrazine oxidation and related energy and environmental, analytical, and electroanalytical applications.