Tuning Intermediates Adsorption and CâN Coupling for Efficient Urea Electrosynthesis Via Doping Ni into Cu.
Small Methods
; 8(3): e2300811, 2024 Mar.
Article
em En
| MEDLINE
| ID: mdl-37997184
ABSTRACT
Simultaneous electrochemical reduction of nitrite and carbon dioxide (CO2 ) under mild reaction conditions offers a new sustainable and low-cost approach for urea synthesis. However, the development of urea electrosynthesis thus far still suffers from low selectivity due to the high energy barrier of * CO formation and the subsequent CâN coupling. In this work, a highly active dendritic Cu99 Ni1 catalyst is developed to enable the highly selective electrosynthesis of urea from co-reduction of nitrite and CO2 , reaching a urea Faradaic efficiency (FE) and production rate of 39.8% and 655.4 µg h-1 cm-2 , respectively, at -0.7 V versus reversible hydrogen electrode (RHE). In situ Fourier-transform infrared spectroscopy (FT-IR) measurements together with density functional theory (DFT) calculations demonstrate that Ni doping into Cu can significantly enhance the adsorption energetics of the key reaction intermediates and facilitate the CâN coupling. This work not only provides a new strategy to design efficient electrocatalysts for urea synthesis but also offers deep insights into the mechanism of CâN coupling during the co-reduction of nitrite and CO2 .
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MEDLINE
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En
Ano de publicação:
2024
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Article