High-Entropy Metallene Arrays with a Turing Structure for Electrocatalytic Upcycling of Polyethylene Terephthalate Plastics Coupled with Electrosynthesis of Ammonia
Wenxin Wang, Ningxin Xiao, Ruidong Yang, Lin Han, Kai Deng, Jianguo Wang, Hongjing Wang, Hongjie Yu, Liang Wang
Abstract
The electrocatalytic upgrading of polyethylene terephthalate (PET) plastics and nitrate-containing wastewater into value-added chemicals provides a promising sustainable strategy for dual-waste utilization. In this work, metallene arrays with a Turing structure were constructed through the self-assembly of high-entropy alloy (HEA) nanocrystals (PdPtCuNiAg MARs) and applied for the upcycling of PET plastics coupled with the electrosynthesis of ammonia. The electrocatalytic coupled system can achieve a current density of 400 mA cm –2 at a low voltage of 1.18 V and exhibits excellent Faraday efficiencies of glycolic acid and NH 3 (FE GA > 95.8%, FE NH 3 > 93.4%) over a wide potential range. Furthermore, the coupled system remains stable over 120 h, enabling efficient coproduction of GA and NH 3 . The Turing structure provides topological ordering and a high density of exposed active sites, which enhances reaction kinetics. The combination of experimental and density functional theory calculation results indicates that the microstrain effect modulates the electronic environment of the catalyst surface, which regulates the adsorption strength of *OC–CH 2 OH and *NO in the EGOR and NO 3 RR processes, thereby lowering the reactive energy barriers of the rate-determining step.