Development of a novel GO/Fe@TANG composite electrode for green and sustainable electrosynthesis of N-phenylbenzamides via electrocatalytic carbonylation and hydrogenation

Abstract

In this study, a novel GO/Fe@TANG composite catalyst was designed by functionalizing graphene oxide (GO) with iron (Fe) and incorporating a hydrogen (H₂) trapping TANG COF. This catalyst was evaluated under mild conditions using a multifunctional MEA/EDA DES that serves as a solvent, an electrolyte and a CO trapping agent. The system efficiently catalyzed the electrochemical carbonylation and hydrogenation of various substrates, including nitrobenzene derivatives 1(a–j), chlorobenzene derivatives 2(a–d), monoxide carbon (CO) 3(a), and H₂ gas 4(a), to afford N-phenylbenzamide derivatives 5(a–m) in high yields ranging from 91% to 96% under mild conditions (room temperature, 1.5 h, 15 mA). The MOF displayed a high specific surface area of 1105 m² g⁻¹ and maintained its catalytic performance over 9 consecutive reuse cycles. Extensive characterization techniques such as FT-IR, SEM, TEM, EDX mapping, TGA, BET, ¹H NMR, CHN, CV, and XPS confirmed the structural, morphological, thermal, and chemical properties of both the catalyst and synthesized products 5(a–m). This work demonstrates an effective, environmentally friendly electrocatalytic system that integrates iron-based porous materials and multifunctional electrolytes, achieving sustainable synthesis of valuable amide derivatives in a streamlined, high-yielding manner aligned with green chemistry principles.