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Synthesis of Dimethyl Carbonate by Gas-Phase Oxidative Carbonylation of Methanol

Author: ZhangZhaoQing
Tutor: SongYiBing
School: Shantou University
Course: Industrial Catalysis
Keywords: Methanol Dimethyl carbonate Mesoporous molecular sieves Mesoporous Carbon
CLC: TQ323.41
Type: Master's thesis
Year: 2011
Downloads: 76
Quote: 0
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Abstract


Dimethyl carbonate (DMC) is an important green chemical products, with a wide range of applications in environmentally friendly solvents, paints, pharmaceuticals and fuel additives, organic synthesis known as the 21st century - the new base block ‖ its green synthetic route is a research hotspot in recent years. Vapor phase methanol oxidative carbonylation method is an ideal the DMC synthesis method, but the main drawback is the low rate of methanol conversion and catalyst easily deactivation. To this end, the focus of this paper are: the use of template synthesis of mesoporous materials, its as the carrier prepared supported Pd, Cu catalyst visits carbonylation reaction of gas-phase oxidation of methanol on the type of catalyst performance, study the carrier at the same time, help agent and the precursor of the active component factors impact on the performance of the catalyst, and the results are as follows: 1. mesoporous materials synthesis and its load Pd-Cu bimetallic catalyst performance. SBA-15 as a template, sucrose as a carbon source, synthesized mesoporous carbon materials. SEM, XRD and N 2 the physical adsorption test results: mesoporous carbon was rod, loose texture, a good degree of order, a large surface area and uniform pore distribution, the distribution of the aperture set about 4nm. Mesoporous carbon as the carrier applied to the vapor-phase oxidation of methanol carbonylation reaction, the active evaluation results are shown: the initial conversion rate of the methanol is high, reaching about 27%, but the product methanol selectivity is low, only 7 %. As the reaction proceeded, the conversion rate is gradually decreased to 18%, DMC methanol selectivity at 6h was increased to 30%, and to remain stable in the subsequent test period. Comparative performance of the activated carbon supported catalyst reaction can be seen that the changes in the pore structure of the carbon carrier, the aperture is increased and can not effectively improve the catalyst performance, the mass transfer resistance of the reaction system involved is small, affecting the performance of the catalyst reaction the key factor is the degree of dispersion of the active metal species. 2 to the polyhydroxy compound is additive modified activated carbon (AC) load the bimetallic catalyst of Pd-Cu. The active evaluation results are shown: No additives, the conversion of methanol was 15%, the selectivity for DMC methanol 36.8%. Add appropriate amount of glycerol, the methanol conversion rate reached 27.5% of DMC 92.1% methanol selectivity. XRD, SEM, TEM characterization results show that: the polyhydroxy compound additives add, can effectively improve the dispersion of metal active component. Precursor of the active component of the catalyst performance. The CuCl 2 , CuO, Cu 2 (OH) 2 CO 3 and other prepared as a precursor catalyst , methanol carbonylation DMC synthesis reaction performance results show that the CuO, Cu 2 (OH) of 2 CO 3 as the active component Preparation of the catalyst having a higher catalytic activity, when the Cu 2 (OH) of 2 CO 3 as an active ingredient, the methanol conversion rate can be up to 32% and the selectivity is also about 90%. 4 different activated carbon treatment for methanol oxidation carbonylation-synthesis of DMC catalyst performance. The results show that to to 0.5M nitric deal with the preparation of activated carbon for the best performance of the catalyst, methanol highest conversion rate exceeds 30%, stable conversion rate reached 25%, while having a higher selectivity. The characterization results showed that the nitric acid treatment can significantly improve the carbon surface concentration of oxygen-containing groups, so that the metal active component easily dispersed. With the increase in the concentration of nitric acid, the unstable carbon molecules of the carbon surface of a high concentration of nitric acid oxidation, so that some of the carbon surface an oxygen-containing Group is destroyed, thereby reducing the activity of the catalyst.

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CLC: > Industrial Technology > Chemical Industry > Synthetic resins and plastics industry > Polycondensation resin and plastic > Polyester resins and plastic materials > Unsaturated polyester
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