Accelerating cathode gas detachment and strengthening anode lewis acidity achieves industrial-level benzylamine electrooxidation coupled with hydrogen production

BAOR-HER system is designed to produce high‑value chemicals and hydrogen. • Porous cathode accelerates hydrogen gas detachment and enhances HER kinetics effectively. • Vanadium doping strengthens anode Lewis acidity and improves BAOR activity and selectivity. • The system delivers industrial-grade performance, featuring high product yield and low energy cost at 1.60 V @ 400 mA cm −2 . Coupling the benzylamine oxidation reaction (BAOR) with hydrogen evolution reaction (HER) offers an energy-saving route to simultaneously produce valuable benzonitrile (BN) and clean H 2 . However, its industrial implementation is hindered by insufficient current density and selectivity, stemming from sluggish gas detachment at the cathode and inadequate Lewis acidity at the anode. Herein, we present a synergistic electrode design in which a porous CoP@Ni 2 P heterojunction as cathode and V-doped CoP@Ni 2 P heterojunction as anode. As revealed by combined experimental and theoretical studies, for cathode, the porous CoP@Ni 2 P heterojunction exhibits a hydrophilic-aerophobic surface, which facilitates mass transport and H 2 detachment. Meanwhile, it presents the optimized adsorption of water and H*, boosting HER kinetics. For anode, high-valence V promotes surface reconstruction into CoNiOOH species with strengthened Lewis acidity, which optimizes the adsorption of OH* and benzylamine for elevating BAOR activity. Assembled into a two-electrode flow electrolyzer, it shows an industrial-level current density of 400 mA cm −2 at only 1.6 V with low consumption of 3.86 kW h/Nm 3 . Besides, the 97% BN yield and ∼100% HER Faradaic efficiency are achieved. This work demonstrates a spatially decoupled catalyst-design strategy for scalable co-production of green hydrogen and value-added organics. Download: Download high-res image (170KB) Download: Download full-size image