Corrosion Engineering of Part-Per-Million Single Atom Pt<sub>1</sub>/Ni(OH)<sub>2</sub> Electrocatalyst for PET Upcycling at Ampere-Level Current Density.

Song, Minwei; Wu, Yufeng; Zhao, Ziyi; Zheng, Mengting; Wang, Changlong; Lu, Jun · Adv Mater · 2024

basic_science · Level V

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Abstract

The plastic waste issue has posed a series of formidable challenges for the ecological environment and human health. While conventional recycling strategies often lead to plastic down-cycling, the electrochemical strategy of recovering valuable monomers enables an ideal, circular plastic economy. Here a corrosion synthesized single atom Pt<sub>1</sub>/Ni(OH)<sub>2</sub> 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 is reported. 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<sup>-2</sup> (1.444 V vs RHE). The in situ spectroscopy and density functional theory calculations provide insights into the mechanism and the understanding of the high efficiency. Remarkably, the electro-oxidation of EG at the ampere-level current density is also successfully illustrated by using a membrane-electrode assembly with high FEs to formate integrated with hydrogen production for 500 h of continuous operation. This process allows valuable chemical production at high space-time yield and is highly profitable (588-700 $ ton<sup>-1</sup> PET), showing an industrial perspective on single-atom catalysis of electrochemical plastic upcycling.