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Compound catalyst with palladium and surface-functionalized carbon quantum dots carried by mesoporous carbon microsphere, preparation method and application of compound catalyst

A surface functionalization and composite catalyst technology, which is applied in the preparation of hydroxyl compounds, organic compound/hydride/coordination complex catalysts, and organic compound preparation, can solve the problems of increasing equipment and catalyst costs, low selectivity, and complicated operation and other issues, to achieve the effect of improving selectivity and conversion rate and the rate of selective hydrogenation reaction, accelerating electron transport, and good stability

Active Publication Date: 2019-01-11
ZHEJIANG UNIV OF TECH
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

Although their catalytic activity is relatively high, the selectivity is generally low
Researchers usually add additives (Van Broekhoven E.H.PonecV.Surface chemistry of small particles[J].Surf.Sci.,1985,162(1-3):731-741), change catalyst support (Planex J M. , Coustel N., Brotons V., Kumbhar P.S., Dutartre R., Geneste P., Ajayan P.M. Appication of Carbon Nanotures as Supports in Heterogeneous Catalysis[J], J.Am.Chem.Soc.,1994,116(17):7935 -7936), change the spatial structure of metals (Richard D., Fouilloux P., GallezotP.Structure and selectivity in cinnamaldehyde hydrogenation of new platinumcatalysts on high surface area grapjite[C].Proc.Int.Congr, Catal.9th, Ottawa: Chem.Inst.Of.Canada, 1988 (3): 1074-1081) to solve this problem, but these methods, not only complicated operation, but also increased the cost of equipment and catalyst

Method used

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  • Compound catalyst with palladium and surface-functionalized carbon quantum dots carried by mesoporous carbon microsphere, preparation method and application of compound catalyst
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  • Compound catalyst with palladium and surface-functionalized carbon quantum dots carried by mesoporous carbon microsphere, preparation method and application of compound catalyst

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0034] Take 65ml of deionized water, 25ml of ethanol, 0.2g of F 127, and 1ml of ammonia solution with a mass concentration of 25-28%, and mix and stir for 1 hour until the F 127 is completely dissolved. Then add 3.2g of 3-aminophenol and continue to stir for 0.5h until the 3-aminophenol is completely dissolved. Add 4ml of 37-40% formaldehyde solution slowly, and stir for 24h. Then stop stirring and heat at 100°C for 24h. Then filter and dry at 60°C to obtain brick-red solid powder, namely: polymer microspheres.

[0035] Take 1g of citric acid, 10ml of deionized water, and 0.2g of ethylenediamine, put them in a hydrothermal kettle, and heat them at 200°C for 10 hours, then take out the hydrothermal samples and set the volume to a 100ml volumetric flask to obtain surface functionalization aqueous solution of carbon quantum dots. Afterwards, 50ml of carbon quantum dot aqueous solution was taken out for dialysis, and a dialysis bag of a certain length was first cut and boiled i...

Embodiment 2

[0039] Take 60ml of deionized water, 28ml of ethanol, 0.8g of F 127, and 0.8ml of ammonia solution with a mass concentration of 25-28%, and mix and stir for 0.5h until the F 127 is completely dissolved. Then add 3.5g of 3-aminophenol and continue to stir for 1h until the 3-aminophenol is completely dissolved. Then slowly add 6ml of 37-40% formaldehyde solution and stir for 12h. Then stop stirring and heat at 100°C for 24h. Then filter and dry at 80°C to obtain brick-red solid powder, that is, polymer microspheres.

[0040] Take 5g of citric acid, 15ml of deionized water, 0.05g of urea and 0.05g of ammonia water, put them into a hydrothermal kettle, heat at 190°C for 11 hours, then take out the sample after hydrothermal treatment and dilute it to a 250ml volumetric flask to obtain the surface Functionalized carbon quantum dots in aqueous solution. Afterwards, 50ml of carbon quantum dot aqueous solution was taken out for dialysis, and a dialysis bag with a molecular weight cu...

Embodiment 3

[0044] Take 80ml of deionized water, 26ml of ethanol, 1.5g of F 127, and 0.5ml of ammonia solution with a mass concentration of 25-28%, and mix and stir for 2 hours until the F 127 is completely dissolved. Then add 2.8g of 3-aminophenol and continue to stir for 2h until the 3-aminophenol is completely dissolved. Slowly add 5ml of 37-40% formaldehyde solution and stir for 48h. Then stop stirring, and heat at 100°C for 48h. Then filter and dry at 70°C to obtain a brick-red solid powder, that is, polymer microspheres.

[0045] Take 0.5g of citric acid, 12ml of deionized water, and 0.3g of glycine, put them in a hydrothermal kettle, heat at 180°C for 12h, then take out the hydrothermally heated sample and set the volume to a 250ml volumetric flask to obtain surface functionalized Aqueous solution of carbon quantum dots. Afterwards, 100ml of carbon quantum dot aqueous solution was taken out for dialysis, and a certain length of dialysis bag with a molecular weight cut-off of 700...

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Abstract

The invention discloses a compound catalyst with palladium and surface-functionalized carbon quantum dots carried by mesoporous carbon microsphere, a preparation method and an application thereof. Thecompound catalyst is composed of a mesoporous carbon microsphere carrier and surface-functionalized carbon quantum dots and metal palladium carried by the carrier, wherein dispersing 'snowflakes' areformed on the carrier surface by surface-functionalized carbon quantum dots and metal palladium; a surface-functionalized carbon quantum dot in size of not more than 10nm, which is directly loaded onthe carrier, is served as the center of each 'snowflake'; metal palladium is located by taking each surface-functionalized carbon quantum dot as an anchor and grows in the shape of snowflake around each surface-functionalized carbon quantum dot; the size of each 'snowflake' is within 40nm-100nm; N functional groups are introduced into the carbon quantum dots, so as to form the surface-functionalized carbon quantum dots; N functional groups are one or more of amino, pyridine nitrogen, pyrrolic nitrogen and graphite nitrogen. The invention also provides the application of the catalyst in the reaction of selective catalytic hydrogenation of crotonaldehyde for compounding crotyl alcohol.

Description

(1) Technical field [0001] The invention relates to a composite catalyst of palladium loaded on mesoporous carbon microspheres and surface functionalized carbon quantum dots, a preparation method thereof and an application in the selective catalytic hydrogenation reaction of crotonaldehyde to prepare crotyl alcohol. (2) Technical background [0002] Crotonaldehyde is a representative α,β-unsaturated aldehyde. Hydrogenation of crotonaldehyde can produce a series of products such as butyraldehyde, crotyl alcohol, enol and butanol. Among them, the C=O selective hydrogenation product—crotyl alcohol has wide application value and can be used in the synthesis of spices, medicines and fine chemicals. At present, the commonly used methods for preparing crotyl alcohol include lithium aluminum hydride reduction method, sodium borohydride reduction method and metal catalytic hydrogenation method. However, the first two methods have disadvantages such as high price, difficult product s...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J31/02B01J27/24B01J35/02B01J35/08C07C29/141C07C33/03B01J35/00
CPCC07C29/141B01J27/24B01J31/0254B01J2231/643B01J35/40B01J35/51C07C33/03
Inventor 卢春山朱倩文王昊季豪克周烨彬张雪洁李小年
Owner ZHEJIANG UNIV OF TECH
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