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Composite cerium-iron-zirconium oxide catalyst, and preparation method and application thereof

A composite oxide and catalyst technology, which can be used in metal/metal oxide/metal hydroxide catalysts, physical/chemical process catalysts, preparation of carbon dioxide or inorganic carbonates, etc. To achieve the effect of easy regeneration and reuse, cheap and easy to obtain raw materials, and little environmental pollution

Active Publication Date: 2018-06-08
SHANXI INST OF COAL CHEM CHINESE ACAD OF SCI
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Metal oxide catalysts mainly use ZrO 2 Mainly, the acid and base groups existing on the surface of zirconia can simultaneously activate methanol and CO 2 , but the acidity and alkalinity of its surface cannot meet the requirements of the reaction, it needs to be modified to improve the catalytic activity

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0019] 1.20mmol Fe(NO 3 ) 3 9H 2 O, 2.76mmol ZrOCl 2 ·8H 2 O, 0.4mmol Ce(NO 3 ) 3 ·6H 2 O was dissolved in 200 mL of ethanol, and 10.00 mmol of citric acid was dissolved in 100 mL of ethanol. Add the ethanol solution of citric acid dropwise to the above salt solution (the volume ratio of the two solutions is 2:1). Stir the mixed solution at room temperature, evaporate the solvent to obtain the xerogel of cerium, iron and zirconium, dry it at 55°C to obtain the catalyst precursor, and finally roast the catalyst precursor at 300°C in the air to obtain 1%Ce-30%Fe-69%Zr solid solution catalyst.

[0020] Raw material methanol and dehydrating agent SiO 2 Added to the batch reactor, filled with CO 2 , under stirring conditions, heating to the temperature required for the reaction to carry out the synthesis reaction, after the reaction, the dehydrating agent and the catalyst are separated from the reaction product to obtain dimethyl carbonate. Methanol and CO 2 The conditi...

Embodiment 2

[0022] 3.30mmolFe(NO 3 ) 3 9H 2 O, 6.40 mmol ZrOCl 2 ·8H 2 O, 0.30 mmol Ce 2 (SO 4 ) 3 ·8H 2 O was dissolved in 100 mL of ethanol, and 40.00 mmol of citric acid was dissolved in 200 mL of ethanol. Add the citric acid ethanol solution dropwise to the above salt solution (the volume ratio of the two solutions is 1:2). Stir the mixed solution at room temperature, evaporate the solvent to obtain a xerogel of cerium, iron and zirconium, and dry it at 70° C. to obtain a catalyst precursor. Finally, the catalyst precursor was calcined at 400°C in air to obtain a 3%Ce-33%Fe-64%Zr solid solution catalyst. Add the raw materials and dehydrating agent into the batch reactor, fill with CO 2 , under stirring conditions, heating to the temperature required for the reaction to carry out the synthesis reaction, after the reaction, the dehydrating agent and the catalyst are separated from the reaction product to obtain dimethyl carbonate. Methanol and CO 2 The conditions for directl...

Embodiment 3

[0024] 16.20mmolFe(NO 3 ) 3 9H 2 O, 26.55mmolZr(NO 3 ) 4 ·5H 2 O, 2.25 mmol Ce 2 (SO 4 ) 3 ·8H 2 O was dissolved in 150 mL of ethanol, and 15.00 mmol of citric acid was dissolved in 150 mL of ethanol. Add the citric acid ethanol solution dropwise to the above salt solution (the volume ratio of the two solutions is 1:1). The mixed solution was stirred at room temperature, the solvent was evaporated to obtain a xerogel of cerium, iron and zirconium, and the catalyst precursor was obtained by drying at 80°C. Finally, the catalyst precursor was calcined at 500°C in air to obtain a 5%Ce-36%Fe-59%Zr solid solution catalyst. Add the raw materials and dehydrating agent into the batch reactor, fill with CO 2 , under stirring conditions, heating to the temperature required for the reaction to carry out the synthesis reaction, after the reaction, the dehydrating agent and the catalyst are separated from the reaction product to obtain dimethyl carbonate. Methanol and CO 2 The...

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PUM

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Abstract

The invention provides a composite cerium-iron-zirconium oxide catalyst. The composite cerium-iron-zirconium oxide catalyst is a solid solution catalyst composed of cerium oxide, iron oxide and zirconium oxide, wherein the molar ratio of Ce to Fe to Zr is (1-30): (30-70): (30-70)%. The composite cerium-iron-zirconium oxide catalyst provided by the invention has the advantages of high catalytic activity, high selectivity, low cost and no pollution.

Description

technical field [0001] The invention relates to a cerium-iron-zirconium composite oxide catalyst and a preparation method, and the catalyst is applied to directly synthesize dimethyl carbonate from carbon dioxide and methanol. Background technique [0002] Dimethyl carbonate (dimethyl carbonate, DMC) is an important environmentally friendly green chemical product, which can be widely used in organic synthesis reactions such as carbonylation, methylation, methoxylation and carbonyl methylation, and can also replace severe Toxic phosgene, methyl chloroformate, dimethyl sulfate, etc. are used as methylating reagents or carbonylating reagents. In addition, DMC has high oxygen content and high octane number, which can greatly increase the oxygen content value of gasoline and can be used as a petroleum additive. DMC is also an excellent green solvent, and has broad application prospects in paints, adhesives, coatings and other fields. DMC has excellent solubility and low viscosi...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J23/83C07C68/04C07C69/96
CPCB01J23/002B01J23/83B01J2523/00C07C68/04B01J2523/3712B01J2523/48B01J2523/842C07C69/96Y02P20/141
Inventor 肖福魁赵宁李爱雪蒲彦锋雒京宣铿王太英杨金海
Owner SHANXI INST OF COAL CHEM CHINESE ACAD OF SCI
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