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A method for preparing methanol by catalytic reduction of carbon dioxide with cheap metal complexes

A metal complex, carbon dioxide technology, applied in the preparation of hydroxyl compounds, the preparation of organic compounds, organic compounds/hydrides/coordination complex catalysts, etc. problems, to achieve high conversion rate, high economic applicability, and good catalytic effect.

Active Publication Date: 2021-03-26
DALIAN UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Using borane (HBCat, HBpin, 9-BBN, BH 3 ·THF、BH 3 ·SMe 2 ) or silane as a hydrogen source can reduce the difficulty of the reaction, but borane and silane are expensive and borane is unstable in the air, which is not conducive to the reaction operation

Method used

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  • A method for preparing methanol by catalytic reduction of carbon dioxide with cheap metal complexes
  • A method for preparing methanol by catalytic reduction of carbon dioxide with cheap metal complexes
  • A method for preparing methanol by catalytic reduction of carbon dioxide with cheap metal complexes

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0036] Under normal pressure carbon dioxide gas atmosphere, add 0.0036g (0.02mmol) o-phenanthroline and 0.0038g (0.02mmol) CuI into the reaction tube, add 1mL tetrahydrofuran and stir for 2min, then add 0.2270g (6mmol) sodium borohydride, 9mL of tetrahydrofuran was heated in a water bath to keep the temperature of the reaction system constant at 25°C. After 12h of reaction, 1mL of 4mol / L hydrochloric acid was added dropwise to the reaction system and stirred for 2h to stop the reaction. The yield of methanol was 6%.

Embodiment 2

[0038] Under normal pressure carbon dioxide gas atmosphere, add 0.0031g (0.02mmol) bipyrimidine and 0.0038g (0.02mmol) CuI into the reaction tube, add 1mL tetrahydrofuran and stir for 2min, then add 0.2270g (6mmol) sodium borohydride and 9mL tetrahydrofuran , heated in a water bath to keep the temperature of the reaction system constant at 25° C. After 12 hours of reaction, 1 mL of 4 mol / L hydrochloric acid was added dropwise to the reaction system and stirred for 2 hours to stop the reaction. The yield of methanol was 35%.

Embodiment 3

[0040]Under normal pressure carbon dioxide gas atmosphere, add 0.0072g (0.04mmol) imidazole and 0.0038g (0.02mmol) CuI into the reaction tube, add 1mL tetrahydrofuran and stir for 2min, then add 0.2270g (6mmol) sodium borohydride and 9mL tetrahydrofuran, Heating in a water bath kept the temperature of the reaction system constant at 25° C. After 12 hours of reaction, 1 mL of 4 mol / L hydrochloric acid was added dropwise to the reaction system and stirred for 2 hours to stop the reaction. The yield of methanol was 16%.

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Abstract

The invention provides a method for preparing methyl alcohol by catalytically reducing cheap metal complex, and belongs to the technical field of energy and catalysis. The method is characterized in that cheap metal salt is separately coordinated with nitrogen-containing monodentate ligand, NN bidentate ligand or NNN tridentate ligand to generate complex in situ; and under low-temperature normal pressure, carbon dioxide is catalyzed to reduce with sodium borohydride to generate methyl alcohol. The method has the advantages that the adopted metal salt, the nitrogen-containing monodentate ligand, NN bidentate ligand or NNN tridentate ligand are cheap and easily available, and are relatively low in cost. Sodium borohydride is stable in air, and is convenient to operate. The reaction conditions are gentle, and the methyl alcohol yield is relatively higher.

Description

technical field [0001] The invention belongs to the field of energy and catalysis technology, and relates to a method for preparing methanol by catalytic reduction of carbon dioxide with a cheap metal complex, which is a method of using nitrogen-containing monodentate ligands, NN bidentate ligands or NNN tridentate ligands and cheap metal salts The complex is generated in situ, and sodium borohydride is used as a hydrogen source to catalyze the reduction of carbon dioxide to generate methanol. Background technique [0002] Methanol is a basic organic raw material widely used in chemical and chemical fields such as synthetic pesticides, pharmaceuticals, plastics, and synthetic fibers. At the same time, methanol is also an important clean fuel. When methanol is fully burned, only carbon dioxide and water are produced, and no toxic and harmful gases such as sulfur dioxide and nitrogen oxides are released. Methanol is liquid at room temperature. Compared with other clean fuels s...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): C07C29/154C07C31/04B01J31/22C07D213/40
CPCB01J31/1805B01J31/1815B01J31/183B01J2231/625B01J2531/0213B01J2531/16C07C29/154C07D213/40C07C31/04Y02P20/52
Inventor 王万辉邱立春王群慧包明
Owner DALIAN UNIV OF TECH