Atomic Interface Engineering of Pd‐Cu‐NiO Nanosheets Boosts Paired Upcycling of Plastic and Acetonitrile

Abstract Simultaneous valorization of plastic waste and industrial acetonitrile into high‐value chemicals presents an enormous challenge, including high energy demand and poor catalytic selectivity. Herein, this through atomic interface engineering is addressed, constructing Pd single atoms embedded on Cu‐NiO nanosheets as a bifunctional electrocatalyst for paired waste upcycling. The bifunctional electrocatalyst harnesses Pd‐induced hydrogen spillover to accelerate acetonitrile hydrogenation to ethylamine at the cathode, while simultaneously modulating the electronic structure of the oxide support to promote C─C bond cleavage, facilitating ethylene glycol oxidation to formate at the anode. Individual electrode evaluations demonstrate exceptional performance of 95.5% Faradaic efficiency for ethylamine production (918.2 mmol h −1 g −1 ) at −0.4 V potential and 95.1% selectivity for formate generation at 1.4 V potential. The integrated paired system operated at ultralow cell voltage with sustained dual‐product synthesis over 60 h, achieving remarkable energy savings compared to conventional processes. This research establishes a new paradigm for designing atomically precise catalysts where a single active site can synergistically drive disparate redox reactions, paving the way for the integrated upcycling of multiple waste sources.