CN115769898A - Zero-valent iron-based hydrogen-rich food enhancer and preparation method and application thereof - Google Patents
Zero-valent iron-based hydrogen-rich food enhancer and preparation method and application thereof Download PDFInfo
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- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 title claims abstract description 117
- 239000001257 hydrogen Substances 0.000 title claims abstract description 117
- 229910052739 hydrogen Inorganic materials 0.000 title claims abstract description 117
- 235000013305 food Nutrition 0.000 title claims abstract description 61
- 239000003623 enhancer Substances 0.000 title claims abstract description 49
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- 238000000034 method Methods 0.000 claims abstract description 11
- 235000015872 dietary supplement Nutrition 0.000 claims description 12
- 239000002270 dispersing agent Substances 0.000 claims description 11
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Abstract
The invention discloses a zero-valent iron-based hydrogen-rich food enhancer and a preparation method and application thereof. The zero-valent iron modified with surface can be used as hydrogen generator to produce oxidation-reduction reaction with gastric juice and convert into Fe easy to be absorbed by human body 2+ And releases hydrogen molecules and has the effect of supplementing iron. Compared with the traditional hydrogen-rich food enhancer, the zero-valent iron hydrogen-rich food enhancer disclosed by the invention is simple in preparation and modification process, low in cost, and has the advantages of good biocompatibility and dispersibility. Importantly, the zero-valent iron hydrogen-rich food enhancer enters an organism in a mild and safe manner, hydrogen molecules are efficiently released in situ, the bioavailability of the hydrogen molecules is effectively improved, and the zero-valent iron hydrogen-rich food enhancer is more easily applied to hydrogen-rich foods in a large scale.
Description
Technical Field
The invention belongs to the technical field of food enhancers, and particularly relates to a zero-valent iron-based hydrogen-rich food enhancer as well as a preparation method and application thereof.
Background
In 2007, professor of Taitian adult male, japan scientists, reported in Nature Medicine (Hydrogen acts as an innovative anatomical antioxidant by selective reduction cytotoxic oxygen radials, nature Medicine,2007,13,688) that Hydrogen molecules can selectively scavenge malignant free radicals, restore human youth, and delay human aging. With the progress of research, hydrogen molecules have been proved to have biological effects of resisting aging, apoptosis and tumor, and the 'hydrogen health' industry has been developed vigorously. At present, the research of 'hydrogen medicine' is in the spotlight, and medical equipment and health care products such as a hydrogen respirator, a hydrogen-rich water cup and the like are developed. However, the application of hydrogen is limited due to its flammable and explosive properties. In addition, the solubility of hydrogen in water is very low (only 1.6ppm at normal temperature and pressure), and the health care effect of drinking hydrogen-rich water is questioned. By developing relevant dissolution techniques (e.g., nano-solubilization techniques), the hydrogen solubility can be increased to about 2.4ppm, but is still very limited. The solubility of hydrogen in water is improved by improving the pressure in the packaging bottle, but high-pressure damage is caused and the application cost is increased.
In recent years, most of the related hydrogen-rich products are prepared by adding elementary calcium, elementary magnesium or elementary calcium-magnesium for compounding,for the in situ generation of hydrogen. For example, CN 109789160A composition for producing hydrogen-rich water and other products uses magnesium metal to react with water-soluble acid to produce dissolved H 2 And magnesium ions to provide a composition of a hydrogen-rich product having an acidic pH; in patent CN 102557227A, an additive of calcium-magnesium hydrogen-rich water and a preparation method thereof, a hydrogen production agent is a calcium simple substance, a magnesium simple substance, a combination of calcium and magnesium simple substances or a calcium-magnesium alloy. However, the methods have the defects of high preparation cost, low hydrogen production reaction efficiency, easy initiation of magnesium poisoning and the like, and are not suitable for the field of food enhancers. Therefore, the development of a mild, safe and efficient hydrogen-rich food enhancer has practical significance for solving the problems of high manufacturing cost, low hydrogen content and the like of the existing hydrogen-rich product.
The zero-valent iron has the advantages of strong reducibility, biocompatibility and the like, and has potential application value in functional foods such as health care products and the like. However, adverse factors such as easy oxidation and easy agglomeration of the nano-sized or micron-sized zero-valent iron limit the application range of the zero-valent iron, and related reports that the zero-valent iron is used as a hydrogen-rich food enhancer do not exist at present.
Disclosure of Invention
In order to overcome the defects of the prior art, the invention aims to provide a hydrogen-rich food enhancer based on zero-valent iron, and a preparation method and application thereof, which can solve the technical problem that zero-valent iron in the prior art cannot be well developed and prepared due to limiting factors.
In order to achieve the purpose, the invention adopts the following technical scheme to realize the purpose:
the invention discloses a zero-valent iron-based hydrogen-rich food enhancer, which is prepared from zero-valent iron and a dispersant coating the zero-valent iron;
wherein the zero-valent iron is nanoscale zero-valent iron or micron-scale zero-valent iron.
Preferably, the dispersing agent adopts dopamine hydrochloride, sodium carboxymethylcellulose, chitosan, starch, pectin, xanthan gum or calcium alginate.
Preferably, the mass ratio of the dispersing agent to the zero-valent iron is (1-3): 4.
the invention also discloses a preparation method of the zero-valent iron-based hydrogen-rich food enhancer, which comprises the following steps: and dispersing zero-valent iron in a dispersing agent by adopting a surface modification method, fully and uniformly mixing, and adjusting the pH value of a reaction system to 6-9 to prepare the hydrogen-rich food enhancer based on the zero-valent iron.
Preferably, the mechanical stirring speed for thorough and uniform mixing is 300 to 600rpm.
The invention also discloses application of the zero-valent iron-based hydrogen-rich food enhancer in preparation of hydrogen-rich food, and the hydrogen-rich food is prepared by adding or not adding an excipient.
Preferably, the excipient is one or more of xylitol, sodium alginate, high fructose corn syrup and potassium sorbate.
Preferably, the hydrogen-rich food is drinking water, beverage, fruit juice, coffee, tea, milk tea, chocolate, soy milk powder, effervescent tablet, milk tablet, cheese, candy, biscuit, cake, bread, pizza, hamburger, chewable tablet or albumen powder.
The invention also discloses application of the zero-valent iron in preparation of the hydrogen-rich food additive.
Preferably, the zero-valent iron is nanoscale zero-valent iron or micron-sized zero-valent iron, and the coated nanoscale zero-valent iron hydrogen-rich food additive or the coated micron-sized zero-valent iron food additive is prepared by adding a dispersing agent by adopting a surface modification method.
Compared with the prior art, the invention has the following beneficial effects:
the zero-valent iron and its modification material (dispersant) are surface modified to obtain green and safe zero-valent iron hydrogen-rich food enhancer, which can be used as hydrogen generator to convert into Fe easy to be absorbed by human body through redox reaction with gastric juice after entering human body 2+ And releases hydrogen molecules and has the effect of supplementing iron. Compared with the traditional hydrogen-rich food enhancer, the zero-valent iron hydrogen-rich food enhancer disclosed by the invention is simple in preparation and modification process, low in cost, and good in biocompatibility and dispersibility; a hydrogen-rich food enhancer, which is mild,The hydrogen-rich food can enter a body in a safe mode, and hydrogen molecules are efficiently released in situ, so that the bioavailability of the hydrogen molecules is effectively improved, and the hydrogen-rich food is easier to apply to a large scale.
Drawings
FIG. 1 is a scanning electron microscope image of dopamine hydrochloride modified zero-valent iron hydrogen-rich dietary supplement of the present invention.
Detailed Description
In order to make the technical solutions of the present invention better understood, the technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the 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. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.
It should be noted that the terms "first," "second," and the like in the description and claims of the present invention and in the drawings described above are used for distinguishing between similar elements and not necessarily for describing a particular sequential or chronological order. It is to be understood that the data so used is interchangeable under appropriate circumstances such that the embodiments of the invention described herein are capable of operation in other sequences than those illustrated or described herein. Furthermore, the terms "comprises," "comprising," and "having," and any variations thereof, are intended to cover a non-exclusive inclusion, such that a process, method, system, article, or apparatus that comprises a list of steps or elements is not necessarily limited to those steps or elements expressly listed, but may include other steps or elements not expressly listed or inherent to such process, method, article, or apparatus.
The invention is described in further detail below with reference to the accompanying drawings:
the zero-valent nano-iron (nZVI) used in the following examples of the invention was purchased from south Gong Fufan metal materials ltd, lot number: 2021062601, zero valent micron iron (mZVI) purchased from south Gong Fufan metal materials ltd, lot number: 2021061201.
example 1
100mg of zero-valent nano-iron (nZVI) and 30mL of Tris-HCl buffer (pH =8.5, 10 mM) were transferred to a three-necked flask, and stirred with a mechanical stirrer after sonication at 300rpm. Adding 75mg dopamine hydrochloride (DA) into the three-neck flask, stirring and reacting for 8h by a mechanical stirrer at room temperature, collecting the product by a high-speed centrifuge (more than 10000 rpm), repeatedly washing by ultrapure water, and carrying out vacuum drying for 4h at 40 ℃ and under the pressure of 0.08MPa to obtain the dopamine hydrochloride modified nZVI zero-valent iron hydrogen-rich food enhancer (DA @ nZVI).
10mg of the zero-valent iron hydrogen-rich food enhancer nZVI prepared in the embodiment is uniformly dispersed in 30mL of gastric acid simulated reaction liquid, and the hydrogen yield is 2.947mg/L by headspace-gas chromatography detection.
A soybean milk powder containing a zero-valent iron hydrogen-rich food enhancer comprises the following components: 2Kg of soybean milk powder with original taste, 40g of xylitol, 0.4g of potassium sorbate and 30mg of zero-valent iron hydrogen-rich food enhancer prepared in the example.
Example 2
Uniformly dispersing 100mg of zero-valent nano iron (nZVI) in 40mL of ultrapure water, uniformly adding 250mg of sodium carboxymethylcellulose (CMC) into a reaction system, and continuously stirring for 1h by using a mechanical stirrer at the rotating speed of 400rpm. Collecting the product with high speed centrifuge (more than 10000 rpm), washing with ultrapure water for several times, and vacuum drying at 45 deg.C under 0.08MPa for 3 hr to obtain sodium carboxymethylcellulose modified nZVI zero-valent iron hydrogen-rich food enhancer (CMC @ nZVI).
10mg of the zero-valent iron hydrogen-rich food enhancer CMC @ nZVI prepared in the example is uniformly dispersed in 30mL of gastric acid simulation reaction liquid, and the hydrogen yield is detected to be 4.012mg/L by headspace-gas chromatography.
A coffee comprising a zero-valent iron hydrogen-rich dietary supplement comprising the following components: 1Kg of coffee powder of 100-200 meshes, 40g of fructose-glucose syrup and 10g of xylitol and 10mg of zero-valent iron hydrogen-rich food enhancer prepared in the example.
Example 3
120mg of chitosan was uniformly dispersed in 30mL of 0.2% glacial acetic acid solution, and mixed with 100mg of nZVI by mechanical stirring for 30min. Then 10mL of glutaraldehyde was added slowly to the reaction and stirring was continued for 4h at 600rpm. Collecting the product with high speed centrifuge (more than 10000 rpm), washing with ultrapure water for several times, and vacuum drying at 55 deg.C under 0.08MPa for 5 hr to obtain chitosan modified nZVI zero-valent iron hydrogen-rich food enhancer (CS @ nZVI).
10mg of the zero-valent iron hydrogen-rich food enhancer CS @ nZVI prepared in the embodiment is uniformly dispersed in 30mL of gastric acid simulation reaction liquid, and the hydrogen yield is detected to be 4.103mg/L by headspace-gas chromatography.
A tea leaf containing a zero-valent iron hydrogen-rich dietary supplement comprises the following components: 0.5Kg of tea powder and 8mg of zero-valent iron hydrogen-rich dietary supplement prepared in this example.
Example 4
2g of zero-valent micron iron (mZVI) is uniformly dispersed in 50mL of ethanol mixed solution (v) Ultrapure water ：v Anhydrous ethanol = 4:1), add slowly 20mL of 0.05g/mL soluble starch solution with magnetic stirring, and continue stirring for 30min. Standing and layering after the reaction is stopped, repeatedly washing the precipitate with ultrapure water, and vacuum-drying at 100 ℃ under the pressure of 0.07MPa for 5 hours to obtain the starch-modified mZVI zero-valent iron hydrogen-rich food enhancer.
10mg of the zero-valent iron hydrogen-rich food enhancer prepared in the embodiment is uniformly dispersed in 30mL of gastric acid simulated reaction liquid, and the hydrogen yield is 3.245mg/L through headspace-gas chromatography detection.
A chewable tablet containing zero-valent iron hydrogen-rich food enhancer comprises the following components: 0.5Kg of xylitol, 5g of chewable tablet and 8mg of zero-valent iron hydrogen-rich dietary supplement prepared in this example.
Example 5
0.1g of zero-valent micron iron (mZVI) is dispersed in 10mL of ultrapure water, 0.2g of pectin is slowly added into the reaction system under the ultrasonic treatment, and the ultrasonic treatment is continued for 30-100 min. Then, in a water bath at the temperature of between 40 and 70 ℃, sequentially dropwise adding 5mL of 0.5mg/mL CaCl into the reaction system 2 The solution, a small amount of sodium dodecyl benzene Sulfonate (SDBC) and anhydrous sodium carbonate are continuously reacted for 3 hours in a water bath. Finally cooling to room temperature, collecting the product by magnetic separation, alternately washing with ultrapure water and ethanol, and vacuum drying at 40 deg.C under 0.07MPa for 5h to obtain pectin modified mZVIZero-valent iron hydrogen-rich food enhancer.
The zero-valent iron hydrogen-rich food enhancer prepared in the example of 10mg is uniformly dispersed in 30mL of gastric acid simulated reaction liquid, and the hydrogen yield is 3.156mg/L by headspace-gas chromatography detection.
A milk tablet containing zero-valent iron hydrogen-rich dietary supplement comprises the following components: 0.5Kg of milk tablet raw material and 8mg of zero-valent iron hydrogen-rich dietary supplement prepared in this example.
Example 6
Dispersing 0.2g of zero-valent micron iron (mZVI) in 80mL of 0.003g/mL xanthan gum solution, sealing and oscillating for 1h at room temperature, collecting precipitate after precipitating for 30min, washing the precipitate for multiple times by ultrapure water, and vacuum drying for 5h at 60 ℃ under the pressure of 0.07MPa to obtain the xanthan gum modified mZVI zero-valent iron hydrogen-rich food enhancer.
The zero-valent iron hydrogen-rich food enhancer prepared in the example of 10mg is uniformly dispersed in 30mL of gastric acid simulated reaction liquid, and the hydrogen yield is 3.156mg/L by headspace-gas chromatography detection.
A biscuit comprising a zero-valent iron hydrogen-rich dietary supplement comprising the following components: 0.5Kg of biscuit raw material, 0.25g of sodium alginate and 8mg of zero-valent iron hydrogen-rich food enhancer prepared in the example.
Example 7
100mg of zero-valent micron iron (mZVI) is uniformly dispersed in 100mL of 2.5mg/mL calcium alginate solution, mechanical stirring is carried out for 0.5h, then 1.0mg/mL CaCl2 solution is slowly added into the system, and the reaction is continued for 0.5h. And (3) magnetically separating, collecting precipitates, washing the precipitates for multiple times by using ultrapure water, and performing vacuum drying for 5 hours at the temperature of 50 ℃ under the pressure of 0.07MPa to obtain the calcium alginate modified mZVI zero-valent iron hydrogen-rich food enhancer.
The zero-valent iron hydrogen-rich food enhancer prepared in the example of 10mg is uniformly dispersed in 30mL of gastric acid simulated reaction liquid, and the hydrogen yield is 3.723mg/L by headspace-gas chromatography detection.
An effervescent tablet containing zero-valent iron hydrogen-rich food enhancer comprises the following components: 0.5Kg of effervescent tablet raw material and 8mg of zero-valent iron hydrogen-rich dietary supplement in example 7.
In conclusion, by surface modificationThe green and safe zero-valent iron is important. After entering human gastric juice, the zero-valent iron is oxidized into Fe by utilizing the acid environment (pH = 0.9-1.8) in the gastric juice 2+ And hydrogen molecules are released in situ, and molecular hydrogen enters the organism for circulation, so that adverse free radicals in the body can be effectively removed, a biological effect is generated, and the formed Fe 2+ Can also be used as iron nutritional agent for supplementing human body. By controlling the introduction amount of zero-valent iron, the concentration of the required hydrogen can be effectively controlled, and the requirements of different hydrogen-rich foods are met, thereby providing a convenient and effective hydrogen-rich food enhancer. The invention discloses an application of a hydrogen-rich food enhancer based on zero-valent iron and modification thereof in food, wherein zero-valent iron and modified iron material thereof are used as a hydrogen generator, and enter human gastric juice to generate redox reaction and convert into Fe easy to be absorbed by human body 2+ And release hydrogen molecules. Compared with the traditional hydrogen-rich food enhancer, the hydrogen-rich food enhancer is simple to prepare and low in cost, can produce hydrogen efficiently in a mild and safe mode after being added into food and taken orally, and effectively improves the bioavailability of hydrogen molecules. The invention widens the preparation strategy of the hydrogen-rich food enhancer and provides a high-efficiency and feasible implementation scheme for the 'hydrogen health' industry.
The above-mentioned contents are only for illustrating the technical idea of the present invention, and the protection scope of the present invention is not limited thereby, and any modification made on the basis of the technical idea of the present invention falls within the protection scope of the claims of the present invention.
Claims (10)
1. A hydrogen-rich food enhancer based on zero-valent iron is characterized in that the hydrogen-rich food enhancer is prepared from zero-valent iron and a dispersant coating the zero-valent iron;
wherein the zero-valent iron is nanoscale zero-valent iron or micron-sized zero-valent iron.
2. The zero-valent iron-based hydrogen-rich dietary supplement of claim 1, wherein the dispersant is dopamine hydrochloride, sodium carboxymethylcellulose, chitosan, starch, pectin, xanthan gum or calcium alginate.
3. The zero-valent iron-based hydrogen-rich dietary supplement of claim 1, wherein the mass ratio of the dispersant to zero-valent iron is (1-3): 4.
4. the method for preparing a zero-valent iron-based hydrogen-rich dietary supplement according to any one of claims 1 to 3, comprising: and dispersing zero-valent iron in the dispersing agent by adopting a surface modification method, fully and uniformly mixing, and adjusting the pH value of the reaction system to 6-9 to prepare the hydrogen-rich food enhancer based on the zero-valent iron.
5. The method according to claim 4, wherein the mechanical stirring speed for sufficient and uniform mixing is 300 to 600rpm.
6. Use of a zero valent iron-based hydrogen-rich food fortifier according to any one of claims 1 to 3 for the preparation of a hydrogen-rich food, wherein the hydrogen-rich food is prepared with or without the addition of excipients.
7. The use of claim 6, wherein the excipient is one or more of xylitol, sodium alginate, high fructose syrup, and potassium sorbate.
8. The use of claim 6, wherein the hydrogen-enriched food is drinking water, a beverage, a fruit juice, coffee, tea, milk tea, chocolate, soymilk powder, an effervescent tablet, a milk tablet, cheese, candy, a biscuit, a cake, bread, pizza, hamburger, a chewable tablet or a protein powder.
9. The application of zero-valent iron in preparing hydrogen-rich food additive.
10. The use of claim 9, wherein the zero-valent iron is nanoscale zero-valent iron or micron-sized zero-valent iron, and the coated nanoscale zero-valent iron hydrogen-rich food additive or the coated micron-sized zero-valent iron food additive is prepared by adding a dispersing agent by a surface modification method.
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