Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 145, Issue 48, Pages 26144-26151Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.3c08359
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This study reports the coupling reaction between CO2RR and NO3RR using molecular copper boron-imidazolate cages, resulting in high selectivity and activity for urea production. The mechanism involves tandem reactions at separate copper sites and condensation between *CO and NH2OH to produce urea.
Electrocatalysis expands the ability to generate industrially relevant chemicals locally and on-demand with intermittent renewable energy, thereby improving grid resiliency and reducing supply logistics. Herein, we report the feasibility of using molecular copper boron-imidazolate cages, BIF-29-(Cu), to enable coupling between the electroreduction reaction of CO2 (CO2RR) with NO3 (-) reduction (NO3RR) to produce urea with high selectivity of 68.5% and activity of 424 mu A cm(-2). Remarkably, BIF-29-(Cu) is among the most selective systems for this multistep C-N coupling to-date, despite possessing isolated single-metal sites. The mechanism for C-N bond formation was probed with a combination of electrochemical analysis, in situ spectroscopy, and atomic-scale simulations. We found that NO3RR and CO2RR occur in tandem at separate copper sites with the most favorable C-N coupling pathway following the condensation between *CO and NH2OH to produce urea. This work highlights the utility of supramolecular metal-organic cages with atomically discrete active sites to enable highly efficient coupling reactions.
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