Electrocatalytic\nAromatic Alcohols Splitting to Aldehydes\nand H<sub>2</sub> Gas

Selective\nelectrocatalytic transformation of alcohols to aldehydes\noffers an efficient and environmentally friendly platform for the\nsimultaneous production of fine chemicals and pure hydrogen gas. However,\ntraditional alcohol oxidation reactions (AORs) in aqueous electrolyte\nunavoidably face competitive reactions (e.g., water oxidation and\noveroxidations reactions) for the presence of active oxygen species\nfrom water oxidation, causing an unwanted decrease in final efficiency\nand selectivity. Here, we developed an integrated all-solid proton\ngenerator-transfer electrolyzer to trigger the pure alcohol splitting\nreaction (ASR). In this splitting process, only O–H and C–H\nbonds can be cleaved at the proton generator (Pt nanoparticles), thereby\ncompletely avoiding all competitive reactions involving oxygen active\nspecies to give a > 99% selectivity to aldehydes. The as-generated\nprotons are transported to the cathode by a three-dimensional (3D)\nconducting network (assemblies of ionomers and carbon spheres) for\nefficient hydrogen production. Unlike the poor selectivity (<22%)\nand durability (<3 h) of a conventional AOR electrolyzer, this\nASR electrolyzer could be continuously operated at a low cell voltage\nof 1.2 V for at least 10 days to give a high Faradaic efficiency of\n80–93% for aldehyde production.