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Catalyst for synthesizing diethyl carbonate by oxidative carbonylation of ethanol and preparation method thereof

A technology for the oxidation of diethyl carbonate and ethanol, which is applied in the preparation of carbon monoxide and oxygen, organic compound/hydride/coordination complex catalysts, physical/chemical process catalysts, etc. It can solve the problems of low catalytic efficiency and easy deactivation , to achieve the effect of good activity, high selectivity and mild conditions

Active Publication Date: 2021-06-08
BEIJING UNIV OF CHEM TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

At present, the catalytic efficiency of industrial catalyst systems is generally low and easily deactivated. It is of great significance to design and prepare catalysts with high activity and high stability.

Method used

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Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0019] Step A: The quantitative relationship between different substances is x TEOS:(1-x)APS:(0.12-1)CTAB:(0.36-2)TMAOH. In this embodiment, 4g of cetyltrimethylammonium bromide was weighed and dissolved in deionized water, and stirred until completely dissolved; then 6g of tetramethylammonium hydroxide was added; 20g of ethyl orthosilicate was then added dropwise, and the stirring continued for a certain period of time. After that, 4g of 3-aminopropyltriethoxysilane was added dropwise, and the resulting suspension was stirred at room temperature, then transferred to a hydrothermal kettle, sealed and placed in an oven at room temperature to 200°C for static aging. After aging, the obtained sample was filtered with a sand core funnel, washed with deionized water until no white foam was produced, washed with absolute ethanol for the last time, and dried in an oven. The obtained white powder was refluxed and stirred in absolute ethanol and repeated 3 times to remove the template ...

Embodiment 2

[0024] Under the completely identical situation of experimental condition and embodiment 1, in the catalyst preparation process CuCl 2 with PdCl 2 The coordination order is adjusted to be with PdCl first 2 CuCl 2 Coordination, the catalyst support remains unchanged, as Schiff base-grafted mesoporous silica ImPy-SiO 2 , the prepared catalyst is recorded as Cu-Pd-ImPy-SiO 2 . Using the same evaluation process as in Example 1, the performance evaluation of the catalyst was carried out on a micro-tubular catalyst evaluation device to obtain 169mg·g -1 h -1 Ethanol space-time conversion rate and 77.5% diethyl carbonate selectivity.

Embodiment 3

[0026] Under the completely identical situation of experimental condition and embodiment 1, the prepared catalyst is carried out 2h pretreatment under the temperature of reaction and pressure under ethanol and (or) CO atmosphere, adopts the evaluation process completely identical with embodiment 1 afterwards , The performance evaluation of the catalyst was carried out on the micro-tubular catalyst evaluation device to obtain 162mg·g -1 h -1 Ethanol space-time conversion and 74.6% diethyl carbonate selectivity.

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PUM

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Abstract

A catalyst for synthesizing diethyl carbonate by oxidative carbonylation of ethanol and a preparation method thereof, belonging to the technical field of alcohol oxidative carbonylation and gas phase synthesis catalytic technology of diethyl carbonate, the catalyst is composed of uniformly distributed Cu ions and Pd ion active centers and a silica carrier. The advantage is that the relative distribution structure of Cu ions and Pd ion centers can be adjusted, and the electronic structures of Cu and Pd centers can be adjusted. The catalyst is used in the oxidative carbonylation process of ethanol, using a miniature fixed-bed reaction device with mild conditions. The catalyst of the invention has high activity and high selectivity to diethyl carbonate. In the steady state, the space-time conversion rate of ethanol is as high as 298 mg·g ‑1 h ‑1 , the selectivity to diethyl carbonate is 85.1%.

Description

technical field [0001] The invention belongs to the technical field of alcohol oxidative carbonylation, and provides a catalyst for synthesizing diethyl carbonate with high selectivity by ethanol oxidative carbonylation, a preparation method and an application. Background technique [0002] As a green chemical, diethyl carbonate (DEC) has important application value in the fields of plastics, medicine, energy, textiles, electronics, etc. The synthesis of diethyl carbonate has received extensive attention in recent years. The industrial production methods of diethyl carbonate include phosgene method, transesterification method, ethyl nitrite carbonylation method, transesterification method, urea alcoholysis method, oxidative carbonylation method, etc. Among them, the oxidative carbonylation of ethanol is a very competitive production route. The raw materials ethanol and CO can be widely derived from biomass conversion, and the production process is green and environmentally f...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J31/22C07C68/01C07C69/96
CPCB01J31/1815B01J31/1633C07C69/96B01J2531/824B01J2531/16C07C68/01
Inventor 何静张亚哲张健安哲宋红艳舒心项顼
Owner BEIJING UNIV OF CHEM TECH
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