Selective Functionalization Blended with Scaffold Conductivity in Graphene Acid Promotes H₂O₂ Electrochemical Sensing

The widespread industrial use of H₂O₂ has provoked great interest in the development of new and more efficient materials for its detection. Enzymatic electrochemical sensors have drawn particular attention, primarily because of their excellent selectivity. However, their high cost, instability, complex immobilization, and inherent tendency toward denaturation of the enzyme significantly limit their practical usefulness. Inspired by the powerful proton-catalyzed H₂O₂ reduction mechanism of peroxidases, we have developed a well-defined and densely functionalized carboxylic graphene derivative (graphene acid, GA) that serves as a proton source and conductive electrode for binding and detecting H₂O₂. An unprecedented H₂O₂ sensitivity of 525 μA cm^-2 mM^-1 is achieved by optimizing the balance between the carboxyl group content and scaffold conductivity of GA. Importantly, the GA sensor greatly outperforms all reported carbon-based H₂O₂ sensors and is superior to enzymatic ones because of its simple immobilization, low cost, and uncompromised sensitivity even after continuous operation for 7 days. In addition, GA-based sensing electrodes remain highly selective in the presence of interferents such as ascorbic acid, paracetamol, and glucose, as well as complex matrices such as milk. GA-based sensors thus have considerable potential for use in practical industrial sensing technologies.