Pulsed Electrolysis Enables Dynamic Interfacial Regulation for Selective Conversion of Waste Plastics into C2 Chemicals

Pd-doped NiCo layered double hydroxide nanosheets were designed for efficient plastic upcycling. • Achieved 94.6% GA Faradaic efficiency with a 0.49 mmol cm -2 h -1 production rate. • Pulsed electrolysis enables dynamic interfacial regulation to mitigate deactivation. • Direct upcycling of PET waste into high-purity value-added GA was demonstrated. The massive accumulation of polyethylene terephthalate (PET) waste necessitates innovative upcycling strategies to recover chemical energy and promote a circular economy. Herein, we report a process intensification strategy for the selective electro-oxidation of PET-derived ethylene glycol (EG) into value-added glycolic acid (GA) using pulsed electrolysis (PE) on a Pd-incorporated NiCo layered double hydroxide (Pd-NiCo-LDH/NF) nanosheet electrocatalyst. Compared with conventional constant-potential electrolysis (CE), the PE mode achieves a superior Faradaic efficiency of 94.6% and a production rate of 0.49 mmol·cm –2 ·h –1 at 1.10 V vs. RHE, representing an 8.2-fold enhancement in yield. In-situ Fourier transform infrared (FTIR) spectroscopy and nuclear magnetic resonance (NMR) analysis were carried out to decipher the enhancement mechanism. Crucially, the practical scalability and industrial potential were demonstrated in a flow electrolyzer using real PET hydrolysates, achieving closed-loop plastic valorization. This work provides a universal paradigm for designing energy-efficient electrocatalytic systems through dynamic interfacial regulation for sustainable chemical production. Download: Download high-res image (177KB) Download: Download full-size image