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However, engineering a dynamically stable interface capable of sustaining continuous reactant delivery and facilitating proton\u2010coupled electron transfer remains challenging, particularly under ampere\u2010level current densities. Herein, a reactant\u2010enhanced hydrogen\u2010bond network constructed on an ultrathin metal\u2010organic framework (MOF)\u2010derived electrocatalyst (Co\u2010PET@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\u2010bond 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\u2011PET@NF achieves a high Faradaic efficiency for formate (FE\n                    <jats:sub>FA<\/jats:sub>\n                    ) of 92.8% at 1.0 A cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    . In a coupled hydrogen co\u2011production system, the cell voltage is reduced by 260\u00a0mV at 1.0\u00a0A cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    compared to water electrolysis, with stable operation over 120\u00a0h while delivering an FE\n                    <jats:sub>FA<\/jats:sub>\n                    of 96.9%. Moreover, this mechanism can be extended to other alcohol\u2010based substances (e.g., methanol and glycerol), elucidating the importance of reactant\u2010catalyst interfacial hydrogen\u2010bond interactions in steering alcohol oxidation selectivity and providing a sustainable strategy for biomass and plastic upgrading.\n                  <\/jats:p>","DOI":"10.1002\/anie.7083269","type":"journal-article","created":{"date-parts":[[2026,7,17]],"date-time":"2026-07-17T12:20:21Z","timestamp":1784290821000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Reactant\u2010Sustained Dynamically Stable Interfacial Hydrogen\u2010Bond Network for Highly Selective, Ampere\u2010Level Ethylene Glycol Electrooxidation"],"prefix":"10.1002","volume":"65","author":[{"given":"Li","family":"Yuan","sequence":"first","affiliation":[{"name":"School of Chemical Engineering Sichuan University  Chengdu P. R. 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