Electrocatalytic Self-Coupling of N-Heterocyclic Amides for Energy-Efficient Bipolar Hydrogen Production

Replacing anodic oxygen evolution reaction with 3,5-diamino-1,2,4-triazole oxidative coupling enables ultra-low-voltage (0.96 V @10 mA cm − 2 ) dual-electrode H 2 production and simultaneous synthesis of energetic 5,5′-diamino-3,3′-azido-1H-1,2,4-triazole (DAAT), achieving 35.8% energy savings. A Pt single-atom/nanoparticle hybrid on NiS 2 nanosheets (Pt s,n @NiS 2 @CC) exhibits exceptional alkaline hydrogen evolution reaction performance and stability via optimized H* adsorption. Anodic DAAT formation proceeds via an OH*-mediated N–N coupling pathway, enabling stable (> 300 h @500 mA cm − 2 ), industrial-scale bipolar H 2 production coupled with green DAAT synthesis in an anion-exchange membrane water electrolyzer.