Lattice-Distortion-Driven Electron Delocalization Enables Efficient Electrosynthesis of Glycolic Acid and Terephthalic Acid from Plastic Wastes
Hao Wang, Xiaoxiao Dong, Fulai Liu, Xingchen Chang, Tao Yu, Jinfa Chang, Mingxu Liu, Ruqiang Zou, Yang Yang, Chun-Chao Hou
Abstract
Electrocatalytic upcycling of waste polyethylene terephthalate (PET) plastics into high-value-added C 2 products (GA, etc.), coupled with hydrogen production, presents a promising solution to mitigate plastic pollution. However, the mechanisms by which the adsorption of key reaction intermediates affects the ethylene glycol oxidation reaction are not well understood. Herein, we synthesize two model catalysts: pristine-lattice Pd/NF (p-Pd) and lattice-distorted Pd/NiO x (l-Pd), the latter constructed by controlling the interfacial metal–support interaction. Detailed characterizations and theoretical calculations reveal that lattice distortion of Pd drives interfacial electron delocalization and generates electron-deficient Pd sites, which strongly attract OH – anions via electrostatic interaction and result in enhanced *OH adsorption on Pd. Enriched surface *OH coverage is crucial for weakening *CO–CH 2 OH or other carbonyl intermediate adsorption and promoting C–H bond oxidation, thereby greatly inhibiting surface poisoning and synergistically promoting GA generation. Specifically, l-Pd delivers a current density of 300 mA cm –2 at an ultralow potential of 1.03 V vs RHE, while achieving a maximum GA Faradaic efficiency of 98.3% and a selectivity of 92.8% at 0.8 V vs RHE. Under membrane electrode assembly conditions, only a cell voltage of 1.26 V is needed for l-Pd to deliver an industrial-level current density of 500 mA cm –2, while enabling continuous PET electrolysis for 204 h at 1.2 V. This study unveils new perspectives on the key role of surface-adsorbed intermediates and offers valuable insights for designing efficient catalysts for the electrochemical upcycling of PET plastics.