Coupling N2 and CO2 in H2O to synthesize urea under ambient conditions
Top Cited Papers
Open Access
- 15 June 2020
- journal article
- research article
- Published by Springer Science and Business Media LLC in Nature Chemistry
- Vol. 12 (8), 717-724
- https://doi.org/10.1038/s41557-020-0481-9
Abstract
The use of nitrogen fertilizers has been estimated to have supported 27% of the world’s population over the past century. Urea (CO(NH2)2) is conventionally synthesized through two consecutive industrial processes, N2 + H2 → NH3 followed by NH3 + CO2 → urea. Both reactions operate under harsh conditions and consume more than 2% of the world’s energy. Urea synthesis consumes approximately 80% of the NH3 produced globally. Here we directly coupled N2 and CO2 in H2O to produce urea under ambient conditions. The process was carried out using an electrocatalyst consisting of PdCu alloy nanoparticles on TiO2 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.Keywords
This publication has 68 references indexed in Scilit:
- Poly(lactic acid)/Poly(ethylene glycol) Polymer Nanocomposites: Effects of Graphene NanoplateletsPolymers, 2013
- Synthesis of ammonia directly from air and water at ambient temperature and pressureScientific Reports, 2013
- Enhanced carbon dioxide capture upon incorporation of N,N′-dimethylethylenediamine in the metal–organic framework CuBTTriChemical Science, 2011
- From greenhouse gas to feedstock: formation of ammonium carbamate from CO2 and NH3 in organic solvents and its catalytic conversion into urea under mild conditionsGreen Chemistry, 2011
- Ammonia Synthesis from First-Principles CalculationsScience, 2005
- Origin of the Overpotential for Oxygen Reduction at a Fuel-Cell CathodeThe Journal of Physical Chemistry B, 2004
- Generalized Gradient Approximation Made SimplePhysical Review Letters, 1996
- Efficient iterative schemes forab initiototal-energy calculations using a plane-wave basis setPhysical Review B, 1996
- Projector augmented-wave methodPhysical Review B, 1994
- Hydrogen bonding in polymers. 4. Infrared temperature studies of a simple polyurethaneMacromolecules, 1986