Abstract
One-pot synthesis of N,N′-dialkylureas were successfully achieved from catalytic carbonylation of aliphatic primary amines with CO2 as the carbon source and Y0.08Zr0.92O1.96 mixed oxide (Yttria-stabilized zirconia, YSZ-8) as the heterogeneous catalyst. The yield of the target product was obtained up to 80.60% from a 48 h reaction with an aliphatic primary amine and 3.0 MPa CO2 in N-methyl-2-pirrolidinone at 160 °C. A multi-pronged mechanistic study was carried out where factors that might influence the reaction efficiency were studied, including catalyst structure, substrates basicity, CO2 pressure, solvent polarity and reaction time. The presence of oxygen vacancies in YSZ-8 was found to be essential for the carbonylation process by creating additional reduction potential for the activation of CO2 which would lead to the key intermediate species.
Highlights
N,N 0 -dialkylureas are widely used in the chemical industry, especially in the manufacture of pesticides, herbicides, pharmaceuticals, resin precursors and plant growth regulators [1].Conventionally, they are prepared from highly toxic reagents depending on methods such as phosgene or isocyanates [2]
It can be concluded that the Yttria-stabilized zirconia (YSZ)-8 (Figure 1a) catalyst prepared in this work possesses exactly the structure of
30.2◦, 55.3◦, and 58.6◦ for YSZ-8 show a slight shift to high angle compared to the standard diffraction
Summary
N,N 0 -dialkylureas are widely used in the chemical industry, especially in the manufacture of pesticides, herbicides, pharmaceuticals, resin precursors and plant growth regulators [1]. They are prepared from highly toxic reagents depending on methods such as phosgene or isocyanates [2]. The stability heterogeneous catalyst resulted in an appreciable yield of N,N -dialkylureas. The stability of of Au@polymer catalyst is not promising, to relatively the relatively chemical bonding between. Y, YSZ-8) was employed as with a heterogeneous catalyst for the production of N,N 0 -dialkylureas via %. The reaction efficiency were studied systematically, where a possible reaction mechanism was proposed Factors was alsoinfluencing proposed. the reaction efficiency were studied systematically, where a possible reaction mechanism was proposed
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