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Lipase-metal palladium nanoparticle composite catalyst as well as preparation method and application thereof

A composite catalyst and nanoparticle technology, applied in catalyst activation/preparation, biochemical equipment and methods, metal/metal oxide/metal hydroxide catalysts, etc., can solve the mismatch of reaction conditions, environmental pollution, and synergistic use Uncommon and other problems to achieve the effect of increasing hydrophobicity

Active Publication Date: 2021-12-14
ZHENGZHOU UNIV +1
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

However, organic solvents are required for catalysis, and harsh conditions such as high temperature and high pressure are easy to cause pollution to the environment.
Although both enzyme catalysts and metal catalysts have high catalytic activity, their synergistic use is uncommon due to the mismatch of their reaction conditions

Method used

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  • Lipase-metal palladium nanoparticle composite catalyst as well as preparation method and application thereof
  • Lipase-metal palladium nanoparticle composite catalyst as well as preparation method and application thereof
  • Lipase-metal palladium nanoparticle composite catalyst as well as preparation method and application thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0060] Example 1: SiO 2 Synthesis of @PDA@Pd catalysts, such as figure 1 shown

[0061] (1) SiO 2 Preparation of @PDA: Weigh 0.5g of SiO 2 In a beaker, add 50mL of Tric-HCl (pH8.5, 10mM) buffer solution, in order to make it evenly dispersed, ultrasonic for 10min, then add 0.5gDA-HCl, shake at 30°C, 2000rpm for 16h; centrifuge at 8000rpm Collect the precipitate for 5 minutes, wash and centrifuge twice with deionized water, disperse the obtained black precipitate in 100 mL of deionized water, and disperse it evenly by ultrasonication for 10 minutes, then divide it into 10 parts, and absorb 10 mL of each part into a centrifuge tube. Each portion was centrifuged to remove the supernatant for later use; one portion was freeze-dried, and its weight was 50.2 mg.

[0062] (2) SiO 2 Preparation of @PDA@Pd:

[0063] Take the SiO prepared above 2 Six parts of @PDA were ultrasonically dispersed in 10mL solutions with pHs of 8, 6, 7, 5, 4, and 3 respectively (the concentration of HC...

Embodiment 2

[0068] Example 2: mSiO 2 Preparation of @PDA@Pd@CALB composite catalyst, such as figure 2 shown

[0069] (1) mSiO 2 Preparation of @PDA@Pd: Weigh SiO prepared under the above optimal conditions 2 @PDA@Pd100mg in a 25mL round bottom flask, add 9mL of toluene, ultrasonic 10min to make it evenly dispersed, then add 1mL of octadecyltrimethoxysilane (TMODS), reflux at 90°C for 15h; centrifuge at 8000rpm Collect the precipitate for 5 min, wash and centrifuge twice with toluene, then wash and centrifuge three times with absolute ethanol, and then dry it in vacuum at 50°C to obtain mSiO 2 @PDA @Pd.

[0070] (2) mSiO 2 Preparation of @PDA@Pd@CALB composite catalyst: Weigh 50mg of mSiO 2 After @PDA@Pd was dispersed with 0.1mL of absolute ethanol, 9.4mL of phosphate (pH7.4, 100mM) buffer was added, ultrasonicated for 10min to disperse evenly, and 0.5mL of enzyme liquid (Novozymes’ CALB, nominal activity 5000LU / g), shaking at 30°C, 200rpm on a shaker for 4h; centrifuging at 8000r...

Embodiment 3

[0072] Example 3: SiO 2 Application of @PDA@Pd catalyst, prepared SiO 2 Dynamic Kinetic Resolution of α-Phenylethylamine by @PDA@Pd and Novozym 435 (Commercial Lipase)

[0073]

[0074] Weigh the SiO prepared in Example 1 2 @PDA@Pd and Novozym 435 each 30mg, 20mg Molecular sieves, 50 mg of anhydrous sodium carbonate in a Schlenk bottle, add 2 mL of toluene, 0.06 mL of the substrate α-phenethylamine, 0.1 mL of ethyl methoxyacetate; fill with H 2 -Ar mixed gas (H 2 accounted for 5%), and maintain a pressure of 0.1Mpa; catalysis at 70 ℃ for 18h. The reaction was detected by gas chromatography.

[0075] Table 1

[0076] Entry catalyst Conversion rates / % ee p / %

[0077] Table 1 is SiO prepared under different pH in embodiment 3 2 @PDA@Pd Catalyst and Novozym 435 (commercial lipase) Dynamic Kinetic Resolution Data of α-Phenylethylamine, Through the Yield and ee p Value comparison, the SiO prepared at pH 4 can be obtained 2 @PDA@Pd pH4 The catalytic e...

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PUM

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Abstract

The invention discloses a lipase-metal palladium nanoparticle composite catalyst as well as a preparation method and application thereof, and the preparation method of the composite catalyst comprises the following steps: coating the surface of silicon dioxide with polydopamine to obtain SiO2@PDA; reducing the palladium precursor by using polydopamine coated on the surface of the silicon dioxide to obtain SiO2@PDA@Pd; then, performing hydrophobic modification on the mSiO2@PDA@Pd to obtain mSiO2@PDA@Pd; and finally, adsorbing the lipase on the surface to obtain the product. The PDA enables the palladium precursor to be adsorbed to the surface of SiO2 (at) PDA and then to be reduced into metal palladium nano particles in situ through nitrogen-containing groups and phenolic hydroxyl groups, wherein the palladium nano particles are uniformly distributed and uniform in particle size; and octadecyltrimethoxysilane is connected with other hydroxyl groups to change the hydrophobicity of the carrier, so that the adsorption of CALB is facilitated, the hydrophobicity provided for the catalyst is beneficial to the dispersion of the catalyst in an organic solvent, and the catalytic ability of the catalyst is further improved.

Description

technical field [0001] The invention belongs to the technical field of nanometer catalysis, and in particular relates to a lipase-metal palladium nanoparticle composite catalyst and its preparation method and application. Background technique [0002] Enzymes, widely present in animals, plants, and microorganisms, are biomacromolecular catalysts that facilitate the transformation of biological and chemical substances in living systems. Enzymes increase reaction efficiency by lowering the activation energy without changing the reaction equilibrium. Under mild conditions (such as room temperature, atmospheric pressure, and physiological pH), enzymes possess ideal catalytic activity, excellent selectivity (stereo, regio, and chemoselectivity), water solubility, and environmental friendliness. Metal catalysts have the advantages of high catalytic efficiency, broad substrates, high stability, and good reusability. However, organic solvents are required for catalysis, and harsh ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): B01J31/06B01J23/44B01J37/16C07B57/00C07C231/02C07C231/20C12N9/20C12N11/089C12N11/14C12P13/02C12P41/00
CPCB01J31/069B01J23/44B01J31/003B01J37/16C07B57/00C07C231/02C07C231/20C12N11/089C12N11/14C12N9/20C12Y301/01003C12P13/02C12P41/007C07B2200/07B01J35/23B01J35/397C07C235/06
Inventor 庄伟应汉杰张文霞刘彤乐欧阳平凯王志许敬亮刘金乐饶远
Owner ZHENGZHOU UNIV
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