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Bioactive hollow nano-fibers and hollow microcapsules for efficiently catalyzing conversion of CO2 into methanol

A nanofiber, biologically active technology, applied in the direction of fiber chemical characteristics, textiles and papermaking, conjugated synthetic polymer artificial filament, etc., can solve the problem of affecting the activity of immobilized multi-enzyme system, low load of multi-enzyme system, increased reaction cost and other issues, to achieve the effect of improving synergy and proximity effect, improving the overall catalytic efficiency, and accelerating the conversion speed

Active Publication Date: 2015-08-05
INST OF PROCESS ENG CHINESE ACAD OF SCI
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AI Technical Summary

Problems solved by technology

However, this immobilization method is complex and cumbersome to operate, and involves a lot of organic solvents, which seriously affects the activity of the immobilized multi-enzyme system, resulting in a low overall catalytic efficiency.
Later, Jiang et al. (ACS Catalysis, 2014, 4, 962-972) used biomimetic mineralization and layer-by-layer self-assembly techniques to synthesize polymer microcapsules. At the same time, the multi-enzyme system formate dehydrogenase, formaldehyde dehydrogenase and ethanol The dehydrogenase is localized and assembled in the microcapsule, and in the case of adding free NADH as the electron donor of the redox reaction, to realize CO 2 Converting to methanol, this method of immobilizing the multi-enzyme system also has complex and cumbersome operations, and also requires template degradation and the introduction of organic solvents, resulting in low loading of the multi-enzyme system and low overall catalytic efficiency
[0008] The above two immobilized multi-enzyme systems can achieve CO 2 The conversion to methanol all uses free NADH as the electron donor of the redox reaction, but due to the high price and poor stability of NADH, the cost of the reaction is further increased. Therefore, Wang et al. (Biotechnology and Bioengineering, 2008, 99, 508-514) used nanoparticles to immobilize the multi-enzyme system and coenzyme NADH respectively, and further introduced glutamate dehydrogenase to realize the regeneration of NADH, which greatly reduced the reaction cost, but due to the loading of nanoparticles The amount is low, and recycling is difficult, which restricts the development of this method to a certain extent.

Method used

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  • Bioactive hollow nano-fibers and hollow microcapsules for efficiently catalyzing conversion of CO2 into methanol
  • Bioactive hollow nano-fibers and hollow microcapsules for efficiently catalyzing conversion of CO2 into methanol
  • Bioactive hollow nano-fibers and hollow microcapsules for efficiently catalyzing conversion of CO2 into methanol

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0045] This example describes a method for CO in solution 2 Catalytic system for conversion to methanol, product detection method.

[0046] The content of each component in the catalytic reaction system is as follows: formate dehydrogenase: 0.5g / L; formaldehyde dehydrogenase: 0.5g / L; alcohol dehydrogenase: 0.5g / L; NADH: 1mmol / L; pH 7.0 Phosphate buffer: 50mM.

[0047] The reaction operation is as follows: First, CO was continuously introduced into 2 mL of phosphate buffer 2 Gas, add the multi-enzyme system of the above concentration, maintain the reactor pressure at 0.3MPa, 150rpm, and react at 37°C for 10 hours. Take out 20L of reaction solution at regular intervals, and use Agilent 7890A gas chromatography to detect the concentration of methanol generated .

Embodiment 2

[0049] This example describes a method for CO in solution 2 A catalytic system for converting to methanol, and a detection method for the product.

[0050] The content of each component in the catalytic reaction system is as follows: formate dehydrogenase: 0.5g / L; formaldehyde dehydrogenase: 0.5g / L; alcohol dehydrogenase: 0.5g / L; glutamate dehydrogenase: 0.5 g / L; NADH: 1 mmol / L; Phosphate buffer at pH 7.0: 50 mM.

[0051] The reaction operation is as follows: First, CO was continuously introduced into 2 mL of phosphate buffer 2 Gas, add the multi-enzyme system of the above concentration, maintain the reactor pressure at 0.3MPa, 150rpm, and react at 37°C for 10 hours. Take out 20μL of the reaction solution at regular intervals, and use Agilent 7890A gas chromatography to detect the concentration of methanol generated. .

Embodiment 3

[0053] This example describes a method for CO in solution 2 A catalytic system for converting to methanol, and a detection method for the product. The content of each component in the catalytic reaction system is as follows: carbonic anhydrase: 0.5g / L; formate dehydrogenase: 0.5g / L; formaldehyde dehydrogenase: 0.5g / L; alcohol dehydrogenase: 0.5g / L ; Glutamate dehydrogenase: 0.5g / L; NADH: 1mmol / L; Phosphate buffer at pH 7.0: 50mM.

[0054] The reaction operation is as follows: First, CO was continuously introduced into 2 mL of phosphate buffer 2 Gas, add the multi-enzyme system of the above concentration, maintain the reactor pressure at 0.3MPa, 150rpm, and react at 37°C for 10 hours. Take out 20L of reaction solution at regular intervals, and use Agilent 7890A gas chromatography to detect the concentration of methanol generated .

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Abstract

The present invention provides bioactive hollow nano-fibers and hollow microcapsules for efficiently catalyzing methanol synthesis through CO2. According to the present invention, a coaxial co-spinning technology is used to embed three enzymes for catalyzing methanol synthesis through CO2 and comprising formic dehydrogenase, formaldehyde dehydrogenase and ethanol dehydrogenase, and coenzyme NADH into the chamber of polyelectrolyte-doped hollow nano-fibers or hollow microcapsules; in order to achieve coenzyme regeneration, an oxidation reduction enzyme R adopting NAD<+> as coenzyme is embedded into the chamber; in order to accelerate a CO2 hydration reaction, carbonic anhydrase is immobilized on the outer surface of the hollow nano-fibers or hollow microcapsules through a layer-by-layer self-assembly technology; the small molecule NADH is bound on the inner wall of the hollow nano-fibers or hollow microcapsules through the electrostatic interaction between the NADH and the polyelectrolyte in the shell layer so as to achieve the recycling; and the polyelectrolyte-doped hollow nano-fiber or hollow microcapsule CO2 conversion catalyst has advantages of simple preparation, high conversion rate, and high stability, and provides wide application prospects in the field of the conversion of CO2 into methanol.

Description

technical field [0001] The invention relates to a highly efficient catalytic CO 2 Bioactive hollow nanofibers and hollow microcapsules for methanol conversion, specifically involving a combination of coaxial co-spinning electrospinning technology and layer-by-layer self-assembly technology principles, which combine CO 2 The multi-enzyme system converted to methanol is embedded in the hollow cavity of hollow nanofibers or hollow microcapsules doped with polyelectrolytes in situ, and carbonic anhydrase is assembled on the outer surface of hollow nanofibers or hollow microcapsules to accelerate CO 2 hydration. Background technique [0002] Atmospheric "greenhouse effect" and global warming will be the biggest environmental problems faced by all mankind in the 21st century. Sea level rise is closely related to major disasters such as land inundation, climate zone shift, hurricane intensification, vegetation migration and species extinction. The gas that plays a major role in ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): D01F1/10D01F8/10D01F8/16D01F8/14C12N11/08C12N11/04C12P7/04
Inventor 张松平姬晓元苏志国
Owner INST OF PROCESS ENG CHINESE ACAD OF SCI
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