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Application of cerium-based catalyst in preparation of dimethyl carbonate by direct conversion of carbon dioxide and methanol

A cerium-based catalyst, dimethyl carbonate technology, applied in the preparation of carbon dioxide or inorganic carbonate, chemical elements of heterogeneous catalysts, catalysts for physical/chemical processes, etc. High specific surface area, excellent mechanical and thermal stability, low pressure drop effect

Active Publication Date: 2021-05-21
DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, dehydrating agents are usually expensive and not environmentally friendly, therefore, it is very worthwhile and desirable to develop a cost-effective, less toxic and dehydrating agent-free production process for the synthesis reaction of dimethyl carbonate in the concept of "green chemistry"

Method used

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  • Application of cerium-based catalyst in preparation of dimethyl carbonate by direct conversion of carbon dioxide and methanol
  • Application of cerium-based catalyst in preparation of dimethyl carbonate by direct conversion of carbon dioxide and methanol
  • Application of cerium-based catalyst in preparation of dimethyl carbonate by direct conversion of carbon dioxide and methanol

Examples

Experimental program
Comparison scheme
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Embodiment 1

[0032] 36 mmoles of analytically pure (NH 4 ) 2 Ce(NO 3 ) 6 with 4 mmol analytically pure Ti(SO 4 ) 2Dissolve in deionized water, introduce the mixed solution into a 1000 ml beaker, dissolve 120 mmol of urea in 200 ml of deionized water and keep stirring. The solution system was heated to 90° C. for 5 hours, filtered and the precipitate was collected. The precipitate was washed with 2000 ml of deionized water and 300 ml of absolute ethanol. Ti 0.1 Ce 0.9 o 2 Particles, Ti 0.1 Ce 0.9 o 2 The X-ray diffraction pattern of figure 1 , see the transmission electron micrograph figure 2 c), see particle size distribution chart figure 2 f). Will get Ti 0.1 Ce 0.9 o 2 The powder was ground with deionized water to obtain a slurry coated on a honeycomb cordierite ceramic carrier (64 cells / cm -2 , hole diameter 10 mm, hole depth 25 mm), the loading of the coating is about 0.5 grams. Finally, the coated catalyst was dried at 80°C for more than 12 hours and calcined in ...

Embodiment 2

[0034] Except that the feeding ratio is changed into 38 millimoles of analytically pure ammonium cerium nitrate and 2 millimoles of analytically pure titanium sulfate, other conditions are the same as in Example 1. Ti 0.05 Ce 0.95 o 2 The X-ray diffraction pattern of figure 1 , see the transmission electron micrograph figure 2 b). After gas chromatograph analysis, the test results are shown in image 3 a), the conversion rate of methanol is 21.6%, and the selectivity of dimethyl carbonate is 80.5%.

Embodiment 3

[0036] Except that the feeding ratio is changed into 34 mmoles of analytically pure ammonium cerium nitrate, and 6 mmoles of analytically pure titanium sulfate, other conditions are the same as in Example 1, Ti 0.15 Ce 0.85 o 2 The X-ray diffraction pattern of figure 1 , see the transmission electron micrograph figure 2 d). After gas chromatograph analysis, the test results are shown in image 3 a), the conversion rate of methanol is 22.1%, and the selectivity of dimethyl carbonate is 76.2%.

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Abstract

The invention provides an application of a cerium-based catalyst in preparation of dimethyl carbonate by direct conversion of carbon dioxide and methanol. The active component of the cerium-based catalyst is M<x>Ce<1-x>O<y> (0 < = x < = 0.2; 1.9 <=y<=2), M is a metal element, and M=Mn, Cu, Ti, Bi, Zr, Fe, Al, Mg and the like. The invention provides a method for applying a cerium-based nano composite catalyst material to a reaction for preparing dimethyl carbonate. The method is simple to operate and has universality. Compared with the existing particle catalyst technology, the catalyst has the advantages of higher specific surface area, lower pressure drop and excellent mechanical stability and thermal stability, and is particularly suitable for continuous reaction operation. Under the condition of not using any dehydrating agent and under the reaction condition of 140 DEG C, the conversion rate of methanol can reach 24.3%, and the selectivity of dimethyl carbonate can reach 78.6%.

Description

technical field [0001] The invention belongs to the technical field of nanometer catalytic materials, and in particular relates to the application of a cerium-based catalyst in the direct conversion of carbon dioxide and methanol into dimethyl carbonate. Background technique [0002] Dimethyl carbonate (DMC) is regarded as an environmentally friendly solvent and reagent because of its low toxicity, high biodegradability and special reactivity. Dimethyl carbonate has proven to be an effective replacement for halogen and sulfate reagents in many important chemical reactions such as carbonation and hydrochlorination. DMC has traditionally been synthesized by methanol phosphation, methanol oxidative carbonation, and esterification, leaving serious environmental concerns. In this regard, the direct synthesis of dimethyl carbonate from the reaction of methanol with carbon dioxide has attracted extensive attention. However, despite the green nature of the reaction, CO 2 The high...

Claims

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Application Information

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IPC IPC(8): B01J23/10B01J23/18B01J35/10C07C68/04C07C69/96
CPCB01J23/10B01J23/18B01J23/002C07C68/04B01J2523/00B01J35/61C07C69/96B01J2523/22B01J2523/31B01J2523/3712B01J2523/41B01J2523/47B01J2523/54Y02P20/141
Inventor 李杲郑凯李志敏
Owner DALIAN INST OF CHEM PHYSICS CHINESE ACAD OF SCI