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Breaking the Activity-Stability Trade-Off via Synergistic Integration of Surface Hydroxyl Coverage and Dynamic
Kai Deng1, Rui Shen1, Ya Zhou1
1State Key Laboratory of Green Chemical Synthesis and Conversion, Zhejiang Key Laboratory of Surface and Interface Science and Engineering for Catalysts, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, People's Republic of China.
Abstract:
The electrocatalytic valorization of waste polyethylene terephthalate (PET)-derived ethylene glycol (EG) into glycolic acid (GA) represents a promising route for plastic upcycling. Palladium (Pd) catalysts are widely employed for the selective production of GA via the EG electrooxidation reaction (EGOR); however, they are typically constrained by an intrinsic activity-stability trade-off. Herein, we report a porous (PtPd)2SnGa intermetallic metallene (denoted as PI-(PtPd)2SnGa-ene) coupled with a pulsed electrocatalysis (PE) strategy to achieve efficient GA synthesis. The unique p-d orbital hybridization and high oxophilicity of PI-(PtPd)2SnGa-ene facilitate the desorption of the key *O═C─CH2OH intermediate and the adsorption of OH- species. Moreover, dynamic potential modulation effectively removes the accumulated PdOx passivation layer formed at high potentials. The as-prepared PI-(PtPd)2SnGa-ene catalyst achieves a Faradaic efficiency (FE) for GA production exceeding 90% over a broad potential window from 0.8 to 1.2 V. When integrated with the PE strategy in a membrane-free flow electrolyzer (MFE) system, the catalytic system operates stably for 100 h, successfully reconciling high activity with long-term stability. This study provides new insights into the efficient and stable electrocatalytic upcycling of PET waste into GA.
