Akademik Veri Yönetim Sistemi
Materials Chemistry and Physics, cilt.358, 2026 (SCI-Expanded, Scopus)
This study delineates the design, synthesis, and electrochemical evaluation of a novel series of biarylcarbaldehyde-based organic materials. These substances function as high-performance, metal-free electrocatalysts for hydrazine oxidation (HzOR). Notably, compound 1a emerged as the most effective, achieving a peak current density of 40.76 mA/cm2 in 1.0 M KOH containing 0.5 M hydrazine. Its performance markedly surpasses that of numerous recent non-noble metal hybrid catalysts and advanced organic molecular catalysts. Furthermore, 1a exhibits a remarkably low onset potential of approximately 0.02 V versus RHE (0.421 V versus Ag/AgCl), aligning with the kinetic efficiency characteristics of complex metallic interfaces. Density Functional Theory (DFT) calculations were employed to analyze the structure-activity relationships. The results demonstrate that the high activity of 1a is attributable to its planar-conjugated structure, which facilitates electron delocalization, and its highly electrophilic carbonyl group, thereby promoting efficient hydrazine adsorption. Furthermore, geometric investigations confirmed that 1a adopts an optimized Bürgi-Dunitz trajectory, thus reducing the activation energy required for nucleophilic attack. Chronoamperometry assessments indicated remarkable long-term stability, with catalytic activity remaining consistent over a period of 4000 s. This work establishes a new benchmark for organic electrocatalysts, demonstrating that meticulously designed, metal-free small molecules can compete with transition-metal systems. These findings offer a sustainable, cost-efficient, and environmentally friendly approach to the development of advanced materials for direct hydrazine fuel cells and comparable energy conversion technologies.