Reactant-Sustained Dynamically Stable Interfacial Hydrogen-Bond Network for Highly Selective, Ampere-Level Ethylene Glycol Electrooxidation.

The catalyst-electrolyte interfacial microenvironment fundamentally governs the activity and selectivity of electrochemical reactions. However, engineering a dynamically stable interface capable of sustaining continuous reactant delivery and facilitating proton-coupled electron transfer remains challenging, particularly under ampere-level current densities. Herein, a reactant-enhanced hydrogen-bond network constructed on an ultrathin metal-organic framework (MOF)-derived electrocatalyst (Co-PET@NF) enables highly selective ethylene glycol electrooxidation (EGOR). Mechanistic investigations reveal that abundant exposed unsaturated Co sites promote preferential EG adsorption for increased EG surface coverage and accelerated replenishment dynamics, ensuring the connectivity and integrity of the interfacial hydrogen-bond network. This dynamically reinforced network facilitates rapid proton transfer from the catalyst surface into the bulk electrolyte, stabilizing the dehydrogenated active sites while preserving a localized alkaline surface microenvironment. Consequently, Co‑PET@NF achieves a high Faradaic efficiency for formate (FE