Corrosion Engineering of Part-per-million Single Atom Pt 1 /Ni(OH) 2 Electrocatalyst for PET Upcycling at Ampere-level Current Density.

The plastic waste issue has posed a series of formidable challenges for the ecological environment and human health. While the conventional recycling strategies often led to plastic down-cycling, the electrochemical strategy of recovering valuable monomers enables an ideal, circular plastic economy. Here we report a corrosion synthesized single atom Pt 1 /Ni(OH) 2 electrocatalyst with part-per-million noble Pt loading for highly efficient and selective upcycling of polyethylene terephthalate (PET) into valuable chemicals (potassium diformate and terephthalic acid) and green hydrogen. Electro-oxidation of PET hydrolysate, ethylene glycol (EG), to formate is processed with high Faraday efficiency (FE) and selectivity (> 90%) at the current density close to 1000 mA/cm 2 (1.444 V versus RHE). The in-situ spectroscopy and density functional theory (DFT) calculations provided insights into the mechanism and the understanding of the high efficiency. Remarkably, the electro-oxidation of EG at the ampere-level current density was also successfully illustrated by using an MEA with high FEs to formate integrated with hydrogen production for 500 hours of continuous operation. This process allows valuable chemical production at high space-time yield and is highly profitable (588-700 $ ton -1 PET), showing industrial perspective on single-atom catalysis of electrochemical plastic upcycling. This article is protected by copyright. All rights reserved.