Ordered mesoporous copper-rare earth metal-aluminum composite oxide catalyst and application thereof

A technology of rare earth metals and oxides, applied in the field of ordered mesoporous copper-rare earth metal-aluminum composite oxide catalysts and its applications, can solve the problems of complex reaction process, decreased catalytic activity, high requirements, etc., and achieve selectivity and The effect of high yield, close interaction and high specific surface area

Pending Publication Date: 2022-03-04
ZHEJIANG UNIV OF TECH +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Such as high specific surface CeO 2 The supported copper-based catalyst achieved 67% ethanol conversion and up to 30 wt% butanol yield at a reaction temperature of 250 °C, but it required supercritical CO 2 In the medium, the reaction pressure greater than 10MPa has higher requirements on the material of the reaction equipment, the reaction process is more complicated, and the production capacity of butanol per unit volume of the reactor is low, and its industrial application is restricted to a certain extent [Green Chem., 2015 ,17:3018-3025.]
Activated carbon supported Cu-CeO 2 /AC catalyst is used in the reaction of ethanol dehydr

Method used

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  • Ordered mesoporous copper-rare earth metal-aluminum composite oxide catalyst and application thereof
  • Ordered mesoporous copper-rare earth metal-aluminum composite oxide catalyst and application thereof
  • Ordered mesoporous copper-rare earth metal-aluminum composite oxide catalyst and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Example Embodiment

[0034] Example 1

[0035] At room temperature, the 2.0g P123 (EO 20 PO 70 EO 20 ) (0.00035 mol) was dissolved in 40mL of anhydrous ethanol and hydrochloric acid was added 3.2mL 35wt% (0.036mol), 0.286g of salicylic acid (0.0016 mol) of citric acid and 0.2g (0.0010 mol) Stir vigorously, followed by addition of 4.08 g aluminum isopropoxide (0.02mol), 0.0857g copper acetate (0.00047 mol) and lanthanum acetate, 0.1616g (0.00051mol), vigorously stirred for 6h to obtain a uniform mixed solution. The solvent was evaporated at 60 deg.] C for 24h under an air atmosphere and then dried at 65 ℃ 48h. Finally, the resulting dried sample was placed in a muffle furnace, and then calcined at 400 ℃ 4h was heated to at a rate of 1 ℃ / min, and then at a rate of 10 ℃ / min was heated to 700 deg.] C continued firing IH, natural cooling to obtain a catalyst A.

[0036] The above-described catalyst was loaded into a fixed bed reactor, a hydrogen tank connected via closed reaction tube 10, filling N 2 U...

Example Embodiment

[0037] Example 2

[0038] Catalyst B prepared in Example 1, but the amount of copper acetate was added 0.1429g (0.00079mol).

[0039] Reduction reaction of ethanol and a higher alcohol catalyst B prepared in Example 1.

[0040] from figure 2 (A) can be clearly seen after the catalyst ordered mesoporous structure B [Chem Eng J., 2017,303,1583-1592.], And found no discernable Cu nanoparticles. In the element distribution image figure 2 (B), the bright stripes corresponding to Al and O signals, and significant formation of orderly framework, Cu-K and La-L signals are distributed uniformly over the frame material ordered. These results indicate that the active components copper and rare earth metal oxides in the catalyst is highly dispersed, and because of the strong interaction between the copper, lanthanum oxide, and three kinds of stable aluminum.

[0041] image 3 XRD pattern of the catalyst after reaction of B. Before the reaction was almost no clear diffraction peaks on XRD spec...

Example Embodiment

[0043] Example 3

[0044] Preparation of Catalyst C in Example 1, but the amount of copper acetate was added 0.1858g (0.00102mol).

[0045] And higher alcohol reduction reaction of catalyst C prepared in Example 1 in ethanol.

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Abstract

The ordered mesoporous copper-rare earth metal-aluminum composite oxide catalyst disclosed by the invention has a highly ordered mesoporous structure and a relatively high specific surface area, and the copper and rare earth metal oxide and the aluminum oxide carrier are tightly interacted and are highly uniformly dispersed. The highly dispersed Cu active component provides a large amount of ethanol dehydrogenation activity or crotonaldehyde hydrogenation centers, and the highly dispersed rare earth metal oxide and the alumina carrier provide a large amount of acid-base active centers for promoting acetaldehyde aldol condensation, so that efficient conversion from ethanol to higher alcohol is finally realized. And meanwhile, the sintering and growth of the oxides of the Cu and the rare earth metals are limited by mutual doping and strong interaction among the oxides of the Cu, the rare earth metals and the aluminum, so that the catalyst shows excellent stability in 500-hour long-time evaluation.

Description

(1) Technical field [0001] The invention relates to an ordered mesoporous copper-rare earth metal-aluminum composite oxide catalyst (CuO-MO x -Al 2 o 3 ) and its preparation method and application, the catalyst shows excellent catalytic activity, selectivity and stability in the reaction of producing higher alcohols from ethanol, and thus has good industrial application prospects. (2) Background technology [0002] Due to the depletion of fossil resources and the greenhouse effect caused by their use, the development and utilization of renewable biomass fuels has attracted more and more attention. As a renewable biomass fuel, bioethanol is widely used as a gasoline blending component in the United States, Brazil, China and other countries. However, ethanol has problems such as strong hygroscopicity, low energy density, and corrosion of engine cylinders, so it is not an ideal gasoline blending component. Compared with ethanol, n-butanol is insoluble in water, has high ene...

Claims

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Application Information

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IPC IPC(8): B01J23/83B01J35/10C07C29/32C07C31/02
CPCB01J23/83B01J23/002B01J35/1019C07C29/32B01J2523/00B01J2523/17B01J2523/31B01J2523/3706C07C31/02
Inventor 江大好赵豪健胡晓利张继生侯圣国孟华胡皓森许孝良张群峰李小年
Owner ZHEJIANG UNIV OF TECH
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