Harnessing Cu-Doped isorhamnetin carbon dots for adsorption-enhanced nitrate electroreduction to ammonia
摘要
Electrochemical nitrate reduction offers a promising route for both nitrate remediation and sustainable ammonia synthesis, yet its efficiency and selectivity are strongly limited by sluggish reaction kinetics and insufficient reactant adsorption. Herein, Cu-loaded carbon dots (Iso-CuCDs) were synthesized using the natural product isorhamnetin as a carbon precursor, in which ultrasmall Cu species were uniformly anchored on oxygen-rich carbon dots. Structural characterizations reveal that Cu is highly dispersed in an amorphous or low-valence state through Cu–O–C interfacial interactions, effectively modulating the electronic structure of the carbon matrix. Benefiting from enhanced nitrate/nitrite adsorption and improved charge-transfer kinetics, Iso-CuCDs exhibit efficient electrocatalytic nitrate reduction, delivering a maximum NH3 production rate of 1.56 mmol h− 1 mgcat−1 with a Faradaic efficiency of 94.6% at − 0.1 V vs. RHE. Moreover, the catalyst maintains stable current density and Faradaic efficiency during long-term electrolysis exceeding 16 h. This work demonstrates that coupling highly dispersed Cu species with functional carbon dots provides an effective strategy for regulating interfacial chemistry and promoting selective electrochemical nitrate-to-ammonia conversion.