Coupling N 2 and CO 2 in H 2 O to synthesize urea under ambient conditions

NATURE CHEMISTRY(2020)

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摘要
The use of nitrogen fertilizers has been estimated to have supported 27% of the world’s population over the past century. Urea (CO(NH 2 ) 2 ) is conventionally synthesized through two consecutive industrial processes, N 2 + H 2 → NH 3 followed by NH 3 + CO 2 → urea. Both reactions operate under harsh conditions and consume more than 2% of the world’s energy. Urea synthesis consumes approximately 80% of the NH 3 produced globally. Here we directly coupled N 2 and CO 2 in H 2 O to produce urea under ambient conditions. The process was carried out using an electrocatalyst consisting of PdCu alloy nanoparticles on TiO 2 nanosheets. This coupling reaction occurs through the formation of C–N bonds via the thermodynamically spontaneous reaction between *N=N* and CO. Products were identified and quantified using isotope labelling and the mechanism investigated using isotope-labelled operando synchrotron-radiation Fourier transform infrared spectroscopy. A high rate of urea formation of 3.36 mmol g –1 h –1 and corresponding Faradic efficiency of 8.92% were measured at –0.4 V versus reversible hydrogen electrode.
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Electrochemistry,Environmental chemistry,Green chemistry,Chemistry/Food Science,general,Analytical Chemistry,Organic Chemistry,Physical Chemistry,Inorganic Chemistry,Biochemistry
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