LU506034B1 - Enzyme catalyst preparation method for enzyme biofuel cell - Google Patents
Enzyme catalyst preparation method for enzyme biofuel cell Download PDFInfo
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- LU506034B1 LU506034B1 LU506034A LU506034A LU506034B1 LU 506034 B1 LU506034 B1 LU 506034B1 LU 506034 A LU506034 A LU 506034A LU 506034 A LU506034 A LU 506034A LU 506034 B1 LU506034 B1 LU 506034B1
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- Prior art keywords
- enzyme
- graphene oxide
- catalyst preparation
- enzyme catalyst
- biofuel cell
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- 102000004190 Enzymes Human genes 0.000 title claims abstract description 74
- 108090000790 Enzymes Proteins 0.000 title claims abstract description 74
- 239000003054 catalyst Substances 0.000 title claims abstract description 48
- 238000002360 preparation method Methods 0.000 title claims abstract description 32
- 239000002551 biofuel Substances 0.000 title claims abstract description 26
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 claims abstract description 18
- 238000003756 stirring Methods 0.000 claims abstract description 18
- 239000008367 deionised water Substances 0.000 claims abstract description 15
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 13
- 229910021389 graphene Inorganic materials 0.000 claims abstract description 13
- 239000000203 mixture Substances 0.000 claims abstract description 12
- 229940071125 manganese acetate Drugs 0.000 claims abstract description 11
- UOGMEBQRZBEZQT-UHFFFAOYSA-L manganese(2+);diacetate Chemical compound [Mn+2].CC([O-])=O.CC([O-])=O UOGMEBQRZBEZQT-UHFFFAOYSA-L 0.000 claims abstract description 11
- 238000001132 ultrasonic dispersion Methods 0.000 claims abstract description 11
- 238000006243 chemical reaction Methods 0.000 claims abstract description 10
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 claims abstract description 7
- -1 carboxyl group-activated graphene oxide powder Chemical class 0.000 claims abstract description 6
- 239000006185 dispersion Substances 0.000 claims abstract description 6
- FDRCDNZGSXJAFP-UHFFFAOYSA-M sodium chloroacetate Chemical compound [Na+].[O-]C(=O)CCl FDRCDNZGSXJAFP-UHFFFAOYSA-M 0.000 claims abstract description 6
- 239000000243 solution Substances 0.000 claims description 20
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 claims description 15
- 239000002244 precipitate Substances 0.000 claims description 15
- 238000001291 vacuum drying Methods 0.000 claims description 15
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 10
- 238000004321 preservation Methods 0.000 claims description 10
- SXRSQZLOMIGNAQ-UHFFFAOYSA-N Glutaraldehyde Chemical compound O=CCCCC=O SXRSQZLOMIGNAQ-UHFFFAOYSA-N 0.000 claims description 5
- 230000007935 neutral effect Effects 0.000 claims description 5
- 238000009210 therapy by ultrasound Methods 0.000 claims description 5
- 239000007864 aqueous solution Substances 0.000 claims description 4
- 238000003763 carbonization Methods 0.000 claims description 2
- 230000003068 static effect Effects 0.000 claims description 2
- 238000006386 neutralization reaction Methods 0.000 claims 1
- 230000000694 effects Effects 0.000 abstract description 9
- 230000003197 catalytic effect Effects 0.000 abstract description 3
- 230000002195 synergetic effect Effects 0.000 abstract description 2
- 238000006555 catalytic reaction Methods 0.000 abstract 1
- 230000003472 neutralizing effect Effects 0.000 abstract 1
- 238000000034 method Methods 0.000 description 8
- 239000000446 fuel Substances 0.000 description 7
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 230000002255 enzymatic effect Effects 0.000 description 2
- 238000002474 experimental method Methods 0.000 description 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 2
- 230000004888 barrier function Effects 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 238000010586 diagram Methods 0.000 description 1
- 239000003792 electrolyte Substances 0.000 description 1
- 239000007943 implant Substances 0.000 description 1
- 238000009776 industrial production Methods 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 239000011664 nicotinic acid Substances 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 239000010970 precious metal Substances 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 238000011160 research Methods 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C01—INORGANIC CHEMISTRY
- C01B—NON-METALLIC ELEMENTS; COMPOUNDS THEREOF; METALLOIDS OR COMPOUNDS THEREOF NOT COVERED BY SUBCLASS C01C
- C01B32/00—Carbon; Compounds thereof
- C01B32/15—Nano-sized carbon materials
- C01B32/182—Graphene
- C01B32/198—Graphene oxide
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M4/00—Electrodes
- H01M4/86—Inert electrodes with catalytic activity, e.g. for fuel cells
- H01M4/90—Selection of catalytic material
- H01M4/9008—Organic or organo-metallic compounds
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
- H01M8/00—Fuel cells; Manufacture thereof
- H01M8/16—Biochemical fuel cells, i.e. cells in which microorganisms function as catalysts
Landscapes
- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Electrochemistry (AREA)
- General Chemical & Material Sciences (AREA)
- Life Sciences & Earth Sciences (AREA)
- Organic Chemistry (AREA)
- Microbiology (AREA)
- Manufacturing & Machinery (AREA)
- Sustainable Development (AREA)
- Sustainable Energy (AREA)
- Nanotechnology (AREA)
- Inorganic Chemistry (AREA)
- Biochemistry (AREA)
- Catalysts (AREA)
- Enzymes And Modification Thereof (AREA)
Abstract
The present invention discloses an enzyme catalyst preparation method for enzyme biofuel cell, comprising the steps of S1, taking graphene oxide GO aqueous dispersion, adding NaOH and sodium chloroacetate, and ultrasonic reaction in a water bath; neutralising it with dilute HCl, and then adding manganese acetate solution by stirring and ultrasonic dispersion treatment, and The mixture was prepared, S2, and to S1 in the mixture was washed with deionised water, and then freeze-dried to obtain the surface carboxyl group-activated graphene oxide powder. By using graphene as an enzyme immobilisation carrier, the enzyme catalytic efficacy can be enhanced through synergistic catalysis, and the enzyme catalyst produced has high activity and stability.
Description
ENZYME CATALYST PREPARATION METHOD FOR ENZYME BIOFUEL CELL 0506034
The present invention relates to the technical field of enzyme biofuel cell, specifically an enzyme catalyst preparation method for enzyme biofuel cell.
An enzyme biofuel cell is a special type of fuel cell that uses enzymes as catalysts to oxidise its fuel rather than precious metals. Enzyme biofuel cells, although currently limited to research facilities, are widely acclaimed for their relatively inexpensive components and fuels as well as potential power source for bionic implants.
Enzymatic biofuel cells work on the same principle as all fuel cells: a catalyst is used to separate the electrons from the parent molecule and force them through a wire that bypasses an electrolyte barrier in order to generate an electric current. What makes enzymatic biofuel cells different from more traditional fuel cells is the catalyst they use and the fuel they accept. Most fuel cells use metals such as platinum and nickel as catalysts, whereas enzyme biofuel cells use enzymes from living cells, and enzyme catalysts prepared in the prior art for enzyme biofuel cells are generally active and unstable, and the process is complex and costly to use, and therefore the present invention proposes an enzyme catalyst preparation method for enzyme biofuel cell to solve the above mentioned problems.
For the deficiencies of the prior art, the present invention provides an enzyme catalyst preparation method for enzyme biofuel cell, which solves the above mentioned problems of the background art.
In order to achieve the above purpose, the present invention is realised by the following technical solution: an enzyme catalyst preparation method for enzyme biofuel cell, specifically comprising the following steps:
S1, stirring and ultrasonic treatment: take a certain amount of graphene oxide GO aqueous dispersion, add an appropriate amount of NaOH and sodium chloroacetate, and ultrasonicate the reaction in a water bath for a certain period of time; neutralise it with dilute HCI, and then add manganese acetate solution through the reactor after stirring and processing in ultrasonic dispersion, and then leave it to make a mixture;
S2, the preparation of graphene oxide: the mixture in step S1 is then washed with deionised 906034 water to neutral, and then freeze-dried to obtain the surface carboxyl group activated graphene oxide powder.
S3, vacuum drying: the graphene oxide powder in step S2 is subjected to vacuum drying treatment through a vacuum dryer;
S4, airtight preservation: airtight preservation of the dried graphene oxide powder by means of a sealed bag;
SS, enzyme catalyst preparation: then add graphene oxide powder to Tris-HCI buffer, ultrasonic dispersion for a certain period of time, add a certain volume of 50% glutaraldehyde solution to the above solution, stirring at room temperature for 30 min, the resulting precipitate was washed with deionised water, ethanol, and then the precipitate separated to dry, the resulting precipitate was washed with deionised water at 500-600°C The enzyme catalyst was produced after carbonisation under the condition.
Further, said standing in said step S1 is standing at 10 to 20°C for 24h.
Further, said stirring in said step S1 is reacted for 12+2h using a microwave reactor heated to 260+£30°C.
Further, the concentration of dilute HCL in said step S1 was 0.1-0.2 mol/L.
Further, the frequency of ultrasonic dispersion in said step S5 is 2000 KHz.
Further, the temperature of the vacuum drying treatment in said step S3 is 100°C and the treatment time is 1-2h.
Further, the concentration of the aqueous manganese acetate solution in said step S1 is 0.3-0.6 mol/L.
BENEFICIAL EFFECTS
The present invention provides an enzyme catalyst preparation method for enzyme biofuel cell. with the following beneficial effects compared with the prior art:
The enzyme catalyst preparation method for enzyme biofuel cell can enhance the enzyme catalytic efficacy by using graphene as an enzyme immobilisation carrier through synergistic catalytic effect, and the enzyme catalyst produced has high activity and stability, and the process is simple, the use cost is low, and industrial production is utilised.
FIG. 1 is a flow chart of the preparation process of the enzyme catalyst of the present invention: > 00%
FIG. 2 shows a chart comparing the market enzyme catalyst of the present invention with the embodiments;
FIG. 3 shows a table diagram comparing Examples 1-3 of the present invention.
The technical solutions in the embodiments of the present invention will be described clearly and completely in the following in conjunction with the accompanying drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention and not all of the embodiments. Based on the embodiments in the present invention, all other embodiments obtained by a person of ordinary skill in the art without making creative labour fall within the scope of protection of the present invention.
Referring to FIG. 1, the present invention provides a technical solution:
Example 1
An enzyme catalyst preparation method for enzyme biofuel cell, specifically comprising the following steps:
S1, stirring and ultrasonic treatment: take a certain amount of 100 ml of graphene oxide GO aqueous dispersion, add 5 g of NaOH and 5 g of sodium chloroacetate, and ultrasonicate the reaction for a certain period of time in a water bath; neutralise the reaction with dilute HCI, and then add manganese acetate solution by stirring and treating it through a reactor before ultrasonically dispersing it, and then leave it to stand for 24h at 10°C to make the mixture;
S2, graphene oxide preparation: the mixture in step S1 is then washed with deionised water to neutral, and then freeze-dried to obtain the surface carboxyl group activated graphene oxide powder.
S3, vacuum drying: the graphene oxide powder in step S2 is subjected to vacuum drying treatment at a temperature of 100°C for 1h through a vacuum dryer;
S4, airtight preservation: airtight preservation of the dried graphene oxide powder through a sealed bag;
S5, enzyme catalyst preparation: then graphene oxide powder was added to Tris-HCI buffer 0.07 mol/L, pH 7.0), ultrasonically dispersed for 30 min, a certain volume of 50% glutaraldehyde solution was added to the above solution, and stirred for 30 min at room temperature, and the 206034 resulting precipitate was washed with deionised water and ethanol, and then the separated precipitate was dried, and the resulting precipitate was washed with deionised water carbonised at 500°C to produce the enzyme catalyst.
Step S1 in the case of stirring using a microwave reactor was heated to 260 + 30 °C under the reaction of 12 + 2h.
The concentration of dilute HCL in step S1 was 0.1 mol/L.
The frequency of ultrasonic dispersion in Step S5 was 2000 KHz.
The temperature of the vacuum drying treatment in Step S3 was 100°C, and the treatment time was 1 h. The concentration of manganese acetate aqueous solution in Step S1 was 0.3 mol/L.
Example 2
An enzyme catalyst preparation method for enzyme biofuel cell, specifically comprising the following steps:
S1, stirring and ultrasonic treatment: take a certain amount of 100 ml of graphene oxide GO aqueous dispersion, add 5 g of NaOH and 5 g of sodium chloroacetate, and ultrasonicate the reaction for a certain period of time in a water bath; neutralise it with dilute HCI, and then add manganese acetate solution through the reactor after stirring and treatment in the ultrasonic dispersion, and then the mixture was made by static standing for 24 h at 15 °C;
S2, graphene oxide preparation: the mixture in step S1 is then washed with deionised water to neutral, and then freeze-dried to obtain the surface carboxyl group activated graphene oxide powder.
S3, vacuum drying: the graphene oxide powder in step S2 is subjected to vacuum drying treatment for 1.5h at a temperature of 100°C by a vacuum dryer;
S4, airtight preservation: airtight preservation of the dried graphene oxide powder through a sealed bag;
S5, enzyme catalyst preparation: then graphene oxide powder was added to Tris-HCI buffer 0.07 mol/L, pH 7.0), ultrasonically dispersed for 30 min, a certain volume of 50% glutaraldehyde solution was added to the above solution, and stirred for 30 min at room temperature, and the resulting precipitate was washed with deionised water and ethanol, and then the precipitate isolated was dried, and the resulting precipitate was washed with deionised water carbonised at
550°C to produce the enzyme catalyst. 0506034
Step S1 in the case of stirring using a microwave reactor was heated to 260 + 30 °C under the reaction of 12 + 2h.
The concentration of dilute HCL in step S1 was 0.15 mol/L. 5 The frequency of ultrasonic dispersion in Step SS was 2000 KHz.
The temperature of the vacuum drying treatment in Step S3 was 100°C, and the treatment time was 1.5 h. The concentration of manganese acetate aqueous solution in Step S1 was 0.45 mol/L.
Example 3
An enzyme catalyst preparation method for enzyme biofuel cell, specifically comprising the following steps:
S1, stirring and ultrasonic treatment: take a certain amount of 100 ml of graphene oxide GO aqueous dispersion, add 5 g of NaOH and 5 g of sodium chloroacetate, and ultrasonicate the reaction for a certain period of time in a water bath; neutralise it with dilute HCI, and then add the manganese acetate solution through the reactor with stirring and treatment before ultrasonically dispersing it, and then leave it to stand for 24h at 20°C to make the mixture;
S2, graphene oxide preparation: the mixture in step S1 is then washed with deionised water to neutral, and then freeze-dried to obtain the surface carboxyl group activated graphene oxide powder.
S3, vacuum drying: the graphene oxide powder in step S2 is subjected to vacuum drying treatment at a temperature of 100°C for 2h through a vacuum dryer;
S4, airtight preservation: airtight preservation of the dried graphene oxide powder through a sealed bag;
S5, enzyme catalyst preparation: then graphene oxide powder was added to Tris-HCI buffer 0.07 mol/L, pH 7.0), ultrasonically dispersed for 30 min, a certain volume of 50% glutaraldehyde solution was added to the above solution, and stirred for 30 min at room temperature, and the resulting precipitate was washed with deionised water and ethanol, and then the precipitate isolated was dried, and the resulting precipitate was washed with deionised water carbonised at 600°C to produce the enzyme catalyst.
Step S1 in the case of stirring using a microwave reactor was heated to 260 + 30 °C under the reaction of 12 + 2h.
The concentration of dilute HCL in step S1 was 0.2 mol/L. 0506036
The frequency of ultrasonic dispersion in Step S5 was 2000 KHz.
The temperature of vacuum drying treatment in Step S3 was 100°C, and the treatment time was 2 h. The concentration of manganese acetate aqueous solution in Step S1 was 0.6 mol/L.
Comparison experiment
An enzyme catalyst manufacturer, respectively, selected the enzyme catalyst of the preparation process in Examples 1-3 and the market enzyme catalyst for activity and stability comparison experiments, as can be seen from Fig. 2, the enzyme catalyst of the preparation process in
Examples 1-3 has an activity of 0.94, a stability of 0.85, and the market enzyme catalyst has an activity of 0.80, a stability of 0.6, which shows that the enzyme catalyst of the invention is much better than the market enzyme catalyst activity and stability. Far better than the market enzyme catalyst activity and stability, as can be seen from Figure 3, the enzyme catalyst prepared in
Example 2 has the highest enzyme catalyst activity and stability, and is the preferred solution; the remaining two are available.
Meanwhile, the contents not described in detail in this specification belong to the prior art known to the technicians in the field.
It is to be noted that in this paper, relationship terms such as first and second are used only to distinguish one entity or operation from another, and do not necessarily require or imply that any such actual relationship or order exists between these entities or operations. Further, the terms "including", "comprising", or any other variant thereof, are intended to cover non-exclusive inclusion, such that a process, method, article, or apparatus comprising a set of elements includes not only those elements, but also other elements not expressly listed, or other elements that are not expressly listed for the purpose of such a process, method, article or apparatus. elements, or also includes elements that are inherent to such process, method, article, or apparatus.
Although embodiments of the present invention have been shown and described, it will be appreciated by those of ordinary skill in the art that a variety of changes, modifications, substitutions, and variations may be made to these embodiments without departing from the principle and spirit of the present invention, and that the scope of the present invention is limited by the appended claims and their equivalents.
Claims (7)
1. Enzyme catalyst preparation method for enzyme biofuel cell, characterised in that: it specifically includes the following steps: SI, stirring ultrasonic treatment: take a certain amount of graphene oxide GO aqueous dispersion, add an appropriate amount of NaOH and sodium chloroacetate, water bath ultrasonic reaction for a certain period of time; neutralisation with dilute HCI, and then add manganese acetate solution through the reactor after stirring treatment in the ultrasonic dispersion, and then static to produce the mixture; S2, graphene oxide preparation: the mixture in step S1 is then washed with deionised water to neutral, and then freeze-dried to obtain the surface carboxyl group activated graphene oxide powder; S3, vacuum drying: the graphene oxide powder in step S2 is subjected to vacuum drying treatment through a vacuum dryer; S4, airtight preservation: airtight preservation of the dried graphene oxide powder by means of a sealed bag; SS, enzyme catalyst preparation: then add graphene oxide powder to Tris-HCI buffer, ultrasonic dispersion for a certain period of time, add a certain volume of 50% glutaraldehyde solution to the above solution, stirring at room temperature for 30 min, the resulting precipitate was washed with deionised water, ethanol, and then the precipitate separated to dry, the resulting precipitate was washed with deionised water at 500-600°C The enzyme catalyst was produced after carbonisation under conditions.
2. Enzyme catalyst preparation method for enzyme biofuel cell according to claim 1, characterised in that: said standing in said step S1 is standing at 10~20°C for 24h.
3. Enzyme catalyst preparation method for enzyme biofuel cell according to claim 1, characterised in that: said stirring in said step S1 is reacted for 12+2h using a microwave reactor heated to 260+30°C.
4. Enzyme catalyst preparation method for enzyme biofuel cell according to claim 1, characterised in that: the concentration of dilute HCL in said step S1 is 0.1-0.2 mol/L.
5. Enzyme catalyst preparation method for enzyme biofuel cell according to claim 1,
characterised in that the frequency of ultrasonic dispersion in said step S5 is 2000 KHz. 0506034
6. Enzyme catalyst preparation method for enzyme biofuel cell according to claim 1, characterised in that the temperature of the vacuum drying treatment in said step S3 is 100°C and the treatment time is 1-2h.
7. Enzyme catalyst preparation method for enzyme biofuel cell according to claim 1, characterised in that the concentration of manganese acetate aqueous solution in said step S1 is
0.3-0.6 mol/L.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| LU506034A LU506034B1 (en) | 2024-01-05 | 2024-01-05 | Enzyme catalyst preparation method for enzyme biofuel cell |
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| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| LU506034A LU506034B1 (en) | 2024-01-05 | 2024-01-05 | Enzyme catalyst preparation method for enzyme biofuel cell |
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| Publication Number | Publication Date |
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| LU506034B1 true LU506034B1 (en) | 2024-07-05 |
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| LU506034A LU506034B1 (en) | 2024-01-05 | 2024-01-05 | Enzyme catalyst preparation method for enzyme biofuel cell |
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- 2024-01-05 LU LU506034A patent/LU506034B1/en active IP Right Grant
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