Ordered macroporous superstructure of bifunctional cobalt phosphide with heteroatomic modification for paired hydrogen production and polyethylene terephthalate plastic recycling

The integration of cathodic hydrogen evolution reaction (HER) with thermodynamically favorable anodic oxidation reactions offers a sustainable alternative for electrochemical valorization. Herein, the atomic Ni modified CoP electrocatalyst featuring an elaborate ordered macroporous superstructure with abundant built-in mesopores has been developed from the ordered macroporous ZIF-67 single crystals, of which the distinctive structural advantages lead to a high HER performance. When the catalyst further underwent an electrochemical reconstruction, an outstanding activity with high Faradaic efficiency up to 96% of formate for ethylene glycol oxidation reaction (EGOR) can be afforded in alkaline electrolyte, as well as in the complex electrolyte of polyethylene terephthalate (PET) plastic hydrolysate. Remarkably, an exotic energy-saving pair-electrolysis system coupling HER and EGOR was explored in the PET plastic hydrolysate by employing this bifunctional electrocatalyst for concurrent H 2 and commodity chemical production. Our work may showcase the rational structural engineering of advanced electrocatalysts for multiple electrochemical applications. • Atomic Ni-modified CoP electrocatalyst with ordered macroporous superstructure was prepared. • A low overpotential of 119 mV @ 10 mA cm −2 for alkaline HER can be achieved. • A high formate Faradaic efficiency of 96 % for EGOR can be obtained. • An energy-saving pair-electrolysis system was explored for concurrent H 2 production and PET plastic upcycling.