“…Water electrolysis has emerged as an attractive pathway for hydrogen generation. However, it is severely hindered by the slow anodic oxygen evolution reaction (OER). , Owing to its relatively favorable thermodynamic kinetics, the electrocatalytic amine oxidation reaction (AOR) has the potential to produce high-value-added products coupled with hydrogen generation. , Among the selective electrooxidation products of amines, nitriles have gained more respect due to their wide applications as essential building blocks and intermediates for agrochemicals, pharmaceuticals, and fine chemicals. − Typically, butyronitrile, one of the most common low-carbon nitriles, is a significant intermediate in the chemical and pharmaceutical industries and is also widely used in dye-sensitized solar cells. , Hence, coupling the AOR with the water reduction reaction is beneficial to rationally reduce the activation energy of water electrolysis and has scientific and industrial importance. However, despite the impressive progress in this field, this promising topic has not been fully explored with respect to either catalytic conversion processes or conversion efficiency optimization.…”