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A polymer-enzyme-metal composite nanocatalyst and its controllable synthesis method

A nano-catalyst and metal composite technology, applied in chemical instruments and methods, organic compound/hydride/coordination complex catalysts, physical/chemical process catalysts, etc., can solve the problem of uncontrollable synthesis and uneven distribution of metal nanoparticles , It is difficult to prevent the aggregation and growth of metal particles, so as to reduce the reaction mass transfer resistance, improve the compatibility and catalytic efficiency, and achieve good stability.

Active Publication Date: 2019-11-08
TSINGHUA UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

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Problems solved by technology

In this method, since only natural lipase is used as a template, it is difficult to prevent the aggregation and growth of metal particles, metal nanoparticles agglomerate during the growth process, and the distribution of metal nanoparticles is not uniform, so the diameter of the metal particles in the aggregate The distribution is 1.5-6.8nm, and the metal-enzyme bifunctional catalyst containing metal nanoparticles with extremely small particle size cannot be controlled and synthesized

Method used

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  • A polymer-enzyme-metal composite nanocatalyst and its controllable synthesis method
  • A polymer-enzyme-metal composite nanocatalyst and its controllable synthesis method
  • A polymer-enzyme-metal composite nanocatalyst and its controllable synthesis method

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Embodiment 1

[0061] Preparation of polymer-lipase-palladium composite nanocatalyst

[0062] Enzyme is Candida antarctica lipase B (enzyme activity is 9U / mg) is 10 parts by weight, polymer compound The weight is 60 parts, the activator Dess-Martin oxidizing agent is 10 parts by weight, and the reducing agent sodium cyanoborohydride is 5 parts by weight.

[0063] Step (1): the above ratio and Dess-Martin oxidant dissolved in dichloromethane, where, The mass fraction in dichloromethane is 1.5%, and the oxidation reaction is carried out at room temperature for 24 hours to oxidize the terminal hydroxyl group to an aldehyde group, and then add cold ether to precipitate to obtain an aldylated polymer compound, which is vacuum-dried;

[0064] Step (2): Dissolve the aldylated polymer compound and lipase obtained in step (1) in 10 mM disodium hydrogen phosphate-sodium dihydrogen phosphate buffer solution with a pH value of 7, and carry out coupling of aldehyde groups and amino groups at room te...

Embodiment 2

[0069] Preparation of polymer-lipase-silver composite nanocatalyst

[0070] The enzymes are Candida antarctica lipase B (enzyme activity: 9U / mg) and Candida rugosa lipase (enzyme activity: 700-1,000U / mg), 5 parts and 5 parts by weight, polymer compound and 60 parts and 40 parts by weight, the activator manganese dioxide oxidizing agent is 50 parts by weight, and the reducing agent sodium cyanoborohydride is 10 parts by weight.

[0071] Step (1): the above ratio and and Dess-Martin oxidant dissolved in chloroform, wherein, and The mass fraction in chloroform is 5%, and the oxidation reaction is carried out at room temperature for 16 hours to oxidize the terminal hydroxyl group into an aldehyde group, and then add a mixed solution of cold ether and petroleum ether to precipitate to obtain an aldylated polymer compound, and dry it in vacuum;

[0072] Step (2): Dissolve the aldylated polymer compound obtained in step (1), Candida antarctica lipase B and Candida rugosa l...

Embodiment 3

[0077] Preparation of polymer-lipase-gold composite nanocatalyst

[0078] Enzyme is Thermomyces lanuginosus lipase (enzyme activity is 100,000-180,000U / g) is 10 parts by weight, polymer compound It is 5 parts by weight, the activator pyridinium chlorochromate oxidant is 5 parts by weight, and the reducing agent sodium borohydride is 5 parts by weight.

[0079] Step (1): the above ratio and pyridinium chlorochromate oxidizing agent are dissolved in the mixed solution of dichloromethane and chloroform, wherein, The mass fraction in dichloromethane and chloroform is 1%, and the oxidation reaction is carried out at room temperature for 10 hours to oxidize the terminal hydroxyl group into an aldehyde group, and then add cold petroleum ether for precipitation to obtain an aldylated polymer compound, which is vacuum-dried;

[0080] Step (2): dissolving the aldylated polymer compound obtained in step (1) and Thermomyces lanuginosus lipase in 50mM disodium hydrogen phosphate-sodiu...

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Abstract

The invention belongs to the field of catalysts and discloses a polymer-enzyme-metal composite nanocatalyst and a controllable synthesis method thereof. The catalyst is prepared from polymer compounds, enzymes, and metal salts. It is a metal nanoparticle composite catalyst limited to a polymer-enzyme conjugate. Its preparation steps include the construction of a polymer-enzyme conjugate and metal ions. In-situ reduction of the two parts within a single polymer-enzyme conjugate can effectively control the size of metal particles during the synthesis process, prevent aggregation, and achieve controllable preparation of highly active extremely small metal nanoparticles. At the same time, the catalyst can be used in aqueous solutions and The formation of nanoscale dispersion in conventional organic solvents is beneficial to maintaining its enzyme catalytic activity and metal catalyst activity during the reaction process. At the same time, the catalyst has temperature response characteristics in common organic solvents and can be separated by simple centrifugation at low temperatures. Reuse multiple times.

Description

technical field [0001] The invention belongs to the field of catalyst preparation, and in particular relates to a polymer-enzyme-metal composite nano catalyst and a controllable synthesis method thereof. Background technique [0002] The chemical-biological coupling catalytic process that couples heterogeneous catalysis and enzyme catalysis has great application potential in biomedicine production and chemical green manufacturing industry. The "one-pot" multi-step series or cascade chemical-biological reaction catalyzed by the bifunctional chemical-biological composite catalyst can avoid the separation and purification steps of reaction intermediate products, and has the advantages of economy, environmental protection and high efficiency. However, the reaction conditions of enzyme-catalyzed processes and noble metal heterogeneous catalyzed processes do not match in most cases, and the respective reaction conditions will lead to the inactivation of the other catalyst, thus se...

Claims

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Application Information

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Patent Type & Authority Patents(China)
IPC IPC(8): B01J31/28B01J35/02B01J35/00
CPCB01J31/28B01J35/393B01J35/40
Inventor 戈钧黎晓阳
Owner TSINGHUA UNIV