Interface Engineering\non Heterostructural Nanosheets\nfor Efficient Electrocatalytic-Paired Upcycling of Waste Plastics\nand Nitrate

Developing a coelectrolysis system of the nitrate reduction\nreaction\n(NO<sub>3</sub>RR) and polyethylene terephthalate-derived ethylene\nglycol oxidation reaction (EGOR) is of great significance for the\nelectrocatalytic-paired upcycling of waste plastics and nitrate wastewater.\nHowever, a huge challenge remains in the exploitation of highly active\ncatalytic electrodes. Herein, electrochemical interface engineering\nis developed for the rational synthesis of Cu-modified CoCu layered\ndouble hydroxide heterostructural nanosheets on carbon cloth (Cu@CoCu\nLDH/CC). The membrane electrode assembly (MEA) NO<sub>3</sub>RR||EGOR\nelectrolyzer confirms the promising performance of Cu@CoCu LDH/CC\nwith maximum FEs of formate and NH<sub>3</sub> (98.1%/98.6% at 1.3\nV), a high yield of NH<sub>3</sub> (0.793 mmol h<sup>–1</sup> cm<sup>–2</sup> at 1.6 V), and stability over 120 h at 1.3\nV, which outperforms the other reported coelectrolysis systems. In\nsitu spectroscopy reveals the favorable formation of key reaction\nintermediates and catalytic active species, while the theoretical\ncalculations confirm the optimized electronic structure and energy\nbarriers of both the NO<sub>3</sub>RR and EGOR by constructing a Cu@CoCu\nLDH heterostructure, leading to its high intrinsic activity. Our work\noffers a promising strategy to develop advanced electrodes for coelectrosynthesis\nof value-added chemicals from the upcycling of nitrate wastewater\nand waste plastics.