4.6 Article

Spatial Management of CO Diffusion on Tandem Electrode Promotes NH2 Intermediate Formation for Efficient Urea Electrosynthesis

Journal

ACS ENERGY LETTERS
Volume 8, Issue 8, Pages 3373-3380

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.3c00824

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Researchers have developed a Cu/ZnO stacked tandem gas-diffusion electrode for selective urea synthesis from electrocatalytic CO2 and nitrate reduction reactions. The electrode promotes the conversion of NO3(-) to *NH2 by providing a high CO concentration, resulting in accelerated C-N coupling for urea synthesis. Experimental results demonstrate the high efficiency of urea synthesis under ambient conditions using the optimized ZnO/Cu electrode.
Electrocatalytic urea synthesis is a promising alternativeto theenergy-intensive conventional industrial process. However, it lackshighly active and selective catalyst systems. Herein, we report aCu/ZnO stacked tandem gas-diffusion electrode (GDE) for selectiveurea synthesis from electrocatalytic CO2 and nitrate reductionreactions. The ZnO catalyst layer (CL) segment at the inlet providesa high CO concentration to the downstream Cu CL segment, promotingthe conversion of NO3 (-) to *NH2. The CO-mediated NH2 formation accelerates the C-Ncoupling rate for urea synthesis. As a result, the stacked GDE withan optimal ZnO/Cu CL area ratio achieves a high Faradaic efficiencyof 37.4% and a high yield of 3.2 & mu;mol h(-1) cm(-2) for urea at -0.3 V vs RHE under ambient conditions.This work expands the application of tandem electrodes and realizesthe cascade C-N coupling reaction.

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