Manipulation of Hydrogen Transfer Behaviors by RhCu Alloying Enables an All‐in‐one Sustainable “Furfural‐Nitrate” System

Nitrogen‐oxysalts and biomass‐derived‐aldehydes are typical wastes mainly from industrialization and agriculturalization progresses, and their clean conversions are still very challenging for a green and sustainable future. Nevertheless, scant attention has been devoted to the core issues: the rational integration of two wastes recycling and the targeted manipulation of hydrogen (H*) transfer behaviors to address their sluggish reaction kinetics. Herein, we report an all‐in‐one electrochemical energy system that is thermodynamically designed by coupling nitrate reduction (NO3RR) and furfural oxidation reactions (FOR) together. Particularly, the poor kinetics for both electrode reactions are efficaciously optimized by the as‐fabricated bifunctional electrocatalyst of RhCu alloy nanowires on copper foam (RhCu NW/CF) with highly improved dual‐directional H*‐modulation performances, thus initializing NO3RR for NH3 synthesis at +0.31 V vs. RHE and driving FOR for H2 harvest at an onset potential lower than 0 V. Eventually, such integrated “Furfural‐Nitrate” system can simultaneously effectuate the electricity energy supply (10.76 mW cm−2), wastewater purification, cathodic hydrogen storage (NH3), anodic H2 production, and biomass upgrading, thereby generating economic benefits with multiple non‐mixed valuable products. Hence, it provides a promising perspective of “turning waste into treasure” in a rational manner, justifying its all‐in‐one property in addressing the global challenge of sustainable energy.