Selective electrosynthesis of urea from nitrate and carbon dioxide with low overpotential

利用低过电位从硝酸盐和二氧化碳选择性电合成尿素

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Abstract

Reducing the energy cost and CO(2) emission of traditional urea synthesis through alternative strategy is crucial for the sustainable social development. Herein, we report the electrosynthesis of urea from nitrate and CO(2) on Ag/CdO heterostructured catalyst with low overpotential. The optimized Ag(0.07)/CdO catalyst demonstrates a high urea yield rate of 111.6 ± 3.1 mmol g(cat.)(-1) h(-1) with 50.0 ± 2.7% Faradaic efficiency at -0.15 V vs. RHE in a flow cell, and can further achieve a urea yield rate of 427.0 ± 30.2 mmol g(cat.)(-1) h(-1) in an optimized two-electrode cell with stable response for 1000 h. Operando spectroscopy and theoretical calculations indicate that Ag attracts *NO(2) intermediate as well as promotes the reconstruction of CdO into low coordinated CdCO(3) that facilitate the activation of CO(2), thus benefits *CO/*NO(2) adsorption and coupling at low overpotential as well as suppresses the generation of CO and NH(3) by-products.

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