Charge Confinement in an Ordered High-Entropy Intermetallic Breaks the Activity-Poisoning Trade‑Off for Glycolic Acid Electrosynthesis From Polyethylene Terephthalate.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 42671276.
- Also identified by DOI 10.1002/adma.74877.
- No licence information is recorded for this record.
- Because redistribution is not established, this page shows the abstract only. Follow the links below for the full text.
Abstract
Selective electrooxidation of ethylene glycol (EG) from polyethylene terephthalate (PET) hydrolysate to glycolic acid (GA) offers a sustainable route for plastic upcycling but is hindered by insufficient activity at industrially relevant current densities and severe catalyst deactivation caused by poisoning intermediates. Here, we design a two-dimensional ordered high-entropy intermetallic, HEI (PdPtRh)(InBi)ene, based on a Pd<sub>1</sub>In<sub>1</sub>-type body-centered-cubic framework. The ordered lattice induces pronounced p--d hybridization and charge redistribution, giving rise to a charge-confinement effect at the active sites. Operando infrared spectroscopy, CO stripping, and theoretical calculations reveal that this confined electronic environment precisely regulates the evolution of the key poisoning intermediate *COCH<sub>2</sub>OH, weakening its accumulation while preserving efficient EG activation. As a result, HEI (PdPtRh)(InBi)ene achieves a current density of 554.21 mA cm<sup>-2</sup> at 0.9 V in PET hydrolysate (PETH). Furthermore, it maintains stable operation for 90 h in a flow cell at an industrially relevant current density of 200 mA cm<sup>-2</sup>, delivering an average GA Faradaic efficiency of 99.22% and an average GA production rate of 1.85 mmol h<sup>-1</sup> cm<sup>-2</sup>. These findings demonstrate charge-confinement engineering as an effective route to regulate poisoning-intermediate behavior in electrocatalytic alcohol oxidation.