CN112588280A - Preparation method of mesoporous alumina photocatalytic material with long afterglow property and application of mesoporous alumina photocatalytic material in biosynthesis - Google Patents
Preparation method of mesoporous alumina photocatalytic material with long afterglow property and application of mesoporous alumina photocatalytic material in biosynthesis Download PDFInfo
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- B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
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Abstract
The invention relates to the technical field of photocatalysis, in particular to a preparation method of a mesoporous alumina photocatalytic material with long afterglow property and application of the mesoporous alumina photocatalytic material in biosynthesis, which comprises the following steps: taking the block copolymer as a template, an alcoholic solution as a solvent and an aluminum-containing complex as a precursor, and carrying out hydrolysis reaction under an acidic condition; drying the reacted solution at 40-70 ℃ to remove the solvent; calcining the dried product in the step at the temperature of 300-500 ℃ to remove the block copolymer, and grinding the calcined product to obtain the mesoporous alumina photocatalytic material with the long afterglow property. The invention firstly provides the method for improving the biosynthesis efficiency of metabolic pathways such as mevalonic acid by utilizing defect-mediated long-life photogenerated electrons. The life of the photo-generated electrons of the mesoporous alumina photocatalytic material with the long afterglow property is prolonged to 165.4ms, and the yield of a target product can be improved when the mesoporous alumina photocatalytic material is applied to biosynthesis of terpenoid compounds.
Description
Technical Field
The invention relates to the technical field of photocatalysis, in particular to a preparation method of a mesoporous alumina photocatalytic material with long afterglow property and application of the mesoporous alumina photocatalytic material in biosynthesis.
Background
Biosynthesis is a novel green and environment-friendly synthesis technology which takes microorganisms as carriers and reforms microbial metabolic pathways through a gene editing means to produce high value-added chemicals by using cheap raw materials, and is considered to be one of the most promising synthesis technologies in the future. The formoxyl metabolic pathway is a microbial basic metabolic pathway widely used for biosynthesis, and the production of clinical medicines such as artemisinin and paclitaxel and fuels such as farnesene is realized based on the formoxyl pathway. The nature of metabolism is a series of redox processes, and substances with reducing activity such as NADH, NADPH and the like are necessary in the metabolic pathway of mevalonate and the like. A large amount of reduction active substances are necessary conditions for realizing the high-efficiency synthesis of high value-added chemicals. However, microorganisms are generally unicellular organisms, and have simple structures, require little nutrition and energy for growth and reproduction, and have weak metabolic activity inherent to microorganisms. The production of reductively active substances in the weak metabolic activity of microorganisms is limited, resulting in generally low yields of high value-added chemical biosynthesis. The shortage of the reduction active substances becomes an important factor for limiting the improvement of the biosynthesis pathway efficiency of mevalonic acid and the like, and the supply of the reduction active substances for microorganisms has important significance for improving the biosynthesis efficiency of the pathway of mevalonic acid and the like.
The microorganism can receive electrons from the outside through pili and the like to produce NADPH, NADH and other reducing active substances. Therefore, providing exogenous electrons to the microorganisms is expected to increase the amount of reducing active substances in the microorganisms, thereby increasing the biosynthesis efficiency of metabolic pathways such as mevalonate. Semiconductor materials are capable of generating free electrons under light conditions, which can be transferred to microorganisms as biosynthetic exogenous electrons. However, free electrons generated by the semiconductor material need to migrate from the interior of the material to the surface and further across the "material-biological" interface before being received by the microorganisms, which requires that the free electrons have a sufficiently long lifetime to complete the migration and traversal process. The defects are formed by irregular arrangement of atoms in the crystal, stabilize free electrons and prevent the free electrons from being combined with holes, so that the defects can prolong the service life of the free electrons in the semiconductor material. Therefore, the defect-rich semiconductor material can be used for providing long-life free electrons for microorganisms and improving the biosynthesis efficiency of metabolic pathways such as mevalonate.
Disclosure of Invention
One of the purposes of the invention is to provide a preparation method of the mesoporous alumina photocatalytic material with long afterglow property, which has simple operation, rich raw material sources and low price.
The invention also aims to provide the application of the mesoporous alumina photocatalytic material with long afterglow property in biosynthesis.
The scheme adopted by the invention for realizing one of the purposes is as follows: a preparation method of a mesoporous alumina photocatalytic material with long afterglow property comprises the following steps:
(1) taking the block copolymer as a template, an alcoholic solution as a solvent and an aluminum-containing complex as a precursor, and carrying out hydrolysis reaction under an acidic condition;
(2) drying the solution reacted in the step (1) at 40-70 ℃ to remove the solvent;
(3) and (3) calcining the dried product in the step (2) at the temperature of 300-500 ℃ to remove the block copolymer, and grinding the calcined product to obtain the mesoporous alumina photocatalytic material with the long afterglow property.
Preferably, in the step (1), the template is any one of P123, F127 and Pluronic F68.
Preferably, in the step (1), the solvent is any one of ethanol, propanol and isopropanol.
Preferably, in the step (1), the precursor is any one of aluminum isopropoxide, aluminum acetylacetonate, aluminum phthalocyanine chloride, aluminium triethyl trichloride, and aluminum hydroxy bis (2-ethylhexanoate).
Preferably, in the step (1), the mass ratio of the template, the solvent and the precursor is 1: (10-30):(1-3).
Preferably, in the step (3), the heating rate is 1-5 ℃ for min–1。
The second scheme adopted by the invention for achieving the purpose is as follows: the application of the mesoporous alumina photocatalytic material with long afterglow property prepared by the preparation method is to apply the mesoporous alumina photocatalytic material to biosynthesis of terpenoid compounds in a mevalonic acid pathway.
Preferably, the terpenoid is at least one of farnesene, paclitaxel, artemisinin, lycopene and carotenoid.
Preferably, the specific application method is as follows: the mesoporous alumina photocatalytic material with long afterglow property is added in the biosynthesis of mevalonic acid pathway, and the biosynthesis is carried out under the illumination condition of 300-450 nm.
The application of the invention takes mevalonic acid approach to synthesize aviation fuel oil farnesene as a model, proves that the defect can prolong the electron life, the defect-mediated long-life photogenerated electrons can improve the efficiency of electron transfer to bacteria, and the reduction of HMG-CoA to generate mevalonic acid is accelerated, so that the synthesis efficiency of farnesene can be improved by 2.02 times to the maximum.
The invention prepares the mesoporous alumina photocatalytic material with long afterglow property. The aperture of the porous material is about 4-10nm, the specific surface area of the material is increased by the porous material, and the number of surface defects is increased. Due to the influence of surface defects, the service life of the material photo-generated electrons is prolonged to 165.4ms, and the synthesis efficiency is improved by 2.02 times when the material is applied to the biosynthesis of farnesene.
The invention has the following advantages and beneficial effects:
the photocatalyst used in the preparation method has rich raw material sources, low price and stability; the preparation method is simple to operate, the prepared photocatalytic material can be applied to biosynthesis of terpenoid compounds in a mevalonic acid pathway, and in addition, defect-mediated electron transfer provided by the application is expected to provide a research basis in the field of material-microorganism research.
The invention firstly provides the method for improving the biosynthesis efficiency of metabolic pathways such as mevalonic acid by utilizing defect-mediated long-life photogenerated electrons. The preparation method of the invention realizes the regulation and control of the aperture of the material by simply using the block copolymer as a template, thereby optimizing the defect property of the material. The material prepared by the method has more surface defects, and the defects can capture photogenerated electrons, so that the material prepared by the method has longer photogenerated electron life, and the yield of a target product can be improved when the material is applied to biosynthesis of terpenoid compounds.
The invention prepares the mesoporous alumina photocatalytic material with long afterglow property. The aperture of the porous material is about 4-10nm, the specific surface area of the material is increased by the porous material, and the number of surface defects is increased. Due to the influence of surface defects, the photoproduction electron life of the material is prolonged to 165.4ms, the yield of a target product can be improved when the material is applied to biosynthesis of terpenoid, and the synthesis efficiency is improved by 2.02 times when the material is applied to biosynthesis of farnesene.
Drawings
FIG. 1 is a transmission electron microscope image of a mesoporous alumina photocatalytic material prepared in example 1 of the present invention;
FIG. 2 is a graph showing a comparison of the production of farnesene biosynthesis under different conditions in example 4 of the present invention.
Detailed Description
The following examples are provided to further illustrate the present invention for better understanding, but the present invention is not limited to the following examples.
Example 1: preparation of mesoporous alumina photocatalytic material with long afterglow property
The preparation method in this example is as follows: 20mL of absolute ethanol was added to a 50mL beaker, and 1g P123 template was added and mixed well. Stirring is carried out under a magnetic stirrer, and 1.4mL of concentrated nitric acid is added dropwise while stirring. 2.046g of aluminum isopropoxide is weighed, and the weighed aluminum isopropoxide is slowly added while stirring. A layer of plastic PE film is covered on the beaker to prevent water from evaporating in the stirring process. And stirring the mixed solution at room temperature for 5 hours, putting the stirred solution into an oven at 60 ℃, and drying for 48 hours. And after 48 hours, putting the obtained solid into a muffle furnace for calcining, and removing the template agent. Setting the heating rate to be 1 ℃/min, calcining for 4h at the temperature of 400 ℃, and grinding the calcined solid to obtain the mesoporous alumina photocatalytic material with long afterglow property.
FIG. 1 is a TEM image of the mesoporous alumina photocatalytic material prepared in this example, and it can be seen that the mesoporous alumina prepared in the present invention has a regular porous structure, and the pore diameter is about 4-8 nm.
Example 2: preparation of mesoporous alumina photocatalytic material with long afterglow property
The preparation method in this example is as follows: 12.5mL of propanol was added to a 50mL beaker, and 1g F127 template was added and mixed well. Stirring is carried out under a magnetic stirrer, and 1.4mL of concentrated nitric acid is added dropwise while stirring. 1.33g of aluminum phthalocyanine chloride was weighed, and the weighed aluminum phthalocyanine chloride was slowly added thereto with stirring. A layer of plastic PE film is covered on the beaker to prevent water from evaporating in the stirring process. And stirring the mixed solution at room temperature for 5h, putting the solution into an oven at 40 ℃ after stirring, and drying for 48 h. And after 48 hours, putting the obtained solid into a muffle furnace for calcining, and removing the template agent. Setting the heating rate to be 2 ℃/min, calcining for 4h at the temperature of 300 ℃, and grinding the calcined solid.
Example 3: preparation of mesoporous alumina photocatalytic material with long afterglow property
The preparation method in this example is as follows: 38mL of absolute ethanol was added to a 50mL beaker, 1g of Pluronic F68 template was added and mixed well. Stirring is carried out under a magnetic stirrer, and 1.4mL of concentrated nitric acid is added dropwise while stirring. 3g of aluminum acetylacetonate was weighed and the weighed aluminum acetylacetonate was slowly added under stirring. A layer of plastic PE film is covered on the beaker to prevent water from evaporating in the stirring process. And stirring the mixed solution at room temperature for 5h, putting the stirred solution into an oven at 70 ℃, and drying for 48 h. And after 48 hours, putting the obtained solid into a muffle furnace for calcining, and removing the template agent. Setting the heating rate to be 5 ℃/min, calcining for 4h at 500 ℃, and grinding the calcined solid.
Example 4: mesoporous alumina photocatalytic material with long afterglow property as photocatalyst for biosynthesis
E.coli monoclonal antibody of farnesene was picked and cultured overnight at 37 ℃ in 20mL of LB medium. 50mL of 2TY medium was placed in a 250mL Erlenmeyer flask and sterilized. 0.5mL of a culture broth of the cultured bacteria was taken in a conical flask containing the culture medium, and 2% glycerol, 50. mu.g/mL of kanamycin, 100. mu.g/mL of ampicillin and 34. mu.g/mL of chloramphenicol were added, followed by culture in a 30-degree shaker. When the OD600 was between 0.6 and 0.8, the inducer IPTG was added so that its final concentration was 0.1 uM. The culture was continued, and when OD600 was 1, 10mL of n-decane was added, and at the same time, 25mg of mesoporous aluminum was added, and irradiation was performed with blue light having a wavelength of about 400 nm. After further incubation in a 30 degree shaker for 48 hours, the supernatant product was extracted and analyzed. Several sets of parallel tests were set under different conditions, namely a reference set without any treatment, a comparative set 1 with only light irradiation, and a comparative set 2 with only photocatalytic material.
FIG. 2 is a comparison graph of the yield of farnesene biosynthesis under different conditions obtained in this example, and it can be seen from the graph that the mesoporous alumina photocatalytic material prepared by the present invention can significantly improve the yield of farnesene biosynthesis under blue light excitation.
While the foregoing is directed to the preferred embodiment of the present invention, other and further embodiments of the invention may be devised without departing from the basic scope thereof, and the scope thereof is determined by the claims that follow.
Claims (9)
1. A preparation method of a mesoporous alumina photocatalytic material with long afterglow property is characterized by comprising the following steps:
(1) taking the block copolymer as a template, an alcoholic solution as a solvent and an aluminum-containing complex as a precursor, and carrying out hydrolysis reaction under an acidic condition;
(2) drying the solution reacted in the step (1) at 40-70 ℃ to remove the solvent;
(3) and (3) calcining the dried product in the step (2) at the temperature of 300-500 ℃ to remove the block copolymer, and grinding the calcined product to obtain the mesoporous alumina photocatalytic material with the long afterglow property.
2. The method for preparing the mesoporous alumina photocatalytic material with long afterglow property as claimed in claim 1, wherein: in the step (1), the template is any one of P123, F127 and Pluronic F68.
3. The method for preparing the mesoporous alumina photocatalytic material with long afterglow property as claimed in claim 1, wherein: in the step (1), the solvent is any one of ethanol, propanol and isopropanol.
4. The method for preparing the mesoporous alumina photocatalytic material with long afterglow property as claimed in claim 1, wherein: in the step (1), the precursor is any one of aluminum isopropoxide, aluminum acetylacetonate, aluminum phthalocyanine chloride, aluminium trichloride triethylcomplex and aluminum hydroxy bis (2-ethylhexanoate).
5. The method for preparing the mesoporous alumina photocatalytic material with long afterglow property as claimed in claim 1, wherein: in the step (1), the mass ratio of the template, the solvent and the precursor is 1: (10-30):(1-3).
6. The method for preparing the mesoporous alumina photocatalytic material with long afterglow property as claimed in claim 1, wherein: in the step (3), the heating rate is 1-5 ℃ for min–1。
7. Use of a mesoporous alumina photocatalytic material with long afterglow properties prepared by the preparation method according to any one of claims 1 to 6, characterized in that: the mesoporous alumina photocatalytic material is applied to biosynthesis of terpenoid compounds in a mevalonic acid pathway.
8. Use of a mesoporous alumina photocatalytic material with long afterglow properties according to claim 7, characterized in that: the terpenoid is at least one of farnesene, paclitaxel, artemisinin, lycopene and carotenoid.
9. Use of a mesoporous alumina photocatalytic material with long afterglow properties according to claim 7, characterized in that: the specific application method comprises the following steps: the mesoporous alumina photocatalytic material with long afterglow property is added in the biosynthesis of mevalonic acid pathway, and the biosynthesis is carried out under the illumination condition of 300-450 nm.
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| DE19954769A1 (en) * | 1999-11-15 | 2001-05-17 | Remmers Bauchemie Gmbh | Microcapsules with a silicone wall containing a solid adsorbent loaded with an adsorptive substance used as a latent heat storage medium e.g. in fireproof linings or thermal insulation for buildings |
| JP2007077199A (en) * | 2005-09-12 | 2007-03-29 | Tokyo Institute Of Technology | Water vapor sorption-desorption heat-accumulation material and method for producing the same |
| CN101948150A (en) * | 2010-09-10 | 2011-01-19 | 中国科学院化学研究所 | Method for purifying water |
| US8796188B2 (en) * | 2009-11-17 | 2014-08-05 | Baker Hughes Incorporated | Light-weight proppant from heat-treated pumice |
| US9663734B2 (en) * | 2011-04-02 | 2017-05-30 | Bcr Science Pllc | Solutions of allotropes of carbon and methods of making and using the same |
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Patent Citations (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| DE19954769A1 (en) * | 1999-11-15 | 2001-05-17 | Remmers Bauchemie Gmbh | Microcapsules with a silicone wall containing a solid adsorbent loaded with an adsorptive substance used as a latent heat storage medium e.g. in fireproof linings or thermal insulation for buildings |
| JP2007077199A (en) * | 2005-09-12 | 2007-03-29 | Tokyo Institute Of Technology | Water vapor sorption-desorption heat-accumulation material and method for producing the same |
| US8796188B2 (en) * | 2009-11-17 | 2014-08-05 | Baker Hughes Incorporated | Light-weight proppant from heat-treated pumice |
| CN101948150A (en) * | 2010-09-10 | 2011-01-19 | 中国科学院化学研究所 | Method for purifying water |
| US9663734B2 (en) * | 2011-04-02 | 2017-05-30 | Bcr Science Pllc | Solutions of allotropes of carbon and methods of making and using the same |
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