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Programming selective formation of epoxy bond: Carbon dots as multifunctional mediators for steering propylene electro oxidation pathways on Ag-graphene hybrids
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DOI：10.1016/j.cclet.2026.112843.png)
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Abstract
En 中文
Achieving precise control over product selectivity in electrochemical alkene oxidation requires catalysts that can be programmed to favor specific bond-forming pathways. Here, we demonstrate that carbon dots (CDs) serve as programmable interfacial mediators to direct propylene electro oxidation exclusively toward the epoxy bond formation on Ag-graphene hybrids. The engineered Ag-6CDs/G catalyst exhibits a remarkable propylene oxide (PO) Faradaic efficiency of 39.71 % and a production rate of 218.85 mmol g‒1 h‒1. We deconvolute the triple role of CDs in programming this selectivity: (1) As a structural mediator that dictates Ag nanoparticle size and spatial distribution, maximizing active site density; (2) as an electronic mediator that fine tunes the Ag d band center, thereby optimizing the adsorption strength ratio between propylene (C=C) and the crucial *OH intermediate to a value ideal for C–O coupling; and (3) as a local microenvironment mediator whose oxygenated surface facilitates water activation, ensuring an efficient supply of oxygen species. This multifunctional mediation is rigorously verified through in situ spectroscopy, electrochemical diagnostics, and density functional theory (DFT) calculations, which collectively map the reaction coordinate and identify the CD induced shifts in adsorption energetics as the origin of the selective pathway. Our work provides a generalizable blueprint for programming bond forming selectivity in electrocatalysis through rational interfacial design.
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