Extraction process and application of Chinese wampee leaf extract

Abstract

The invention relates to the field of extraction, in particular to an extraction process and application of a Chinese wampee leaf extract, and the extraction process of the Chinese wampee leaf extract comprises the following steps: S1, drying Chinese wampee leaves, and crushing to obtain Chinese wampee leaf powder; s2, adding the clausena lansium leaf powder obtained in the step S1 into a solvent for extraction to obtain a mixture; and S3, adding a microwave-assisted absorbent into the mixture obtained in the step S2, carrying out microwave treatment, filtering, washing, collecting filtrate, and drying to obtain the Chinese wampee leaf extract. According to the extraction process, the extraction time can be shortened, and the extraction rate is high.

Description

Technical Field

[0001] The present invention relates to the field of extraction, and specifically relates to an extraction process and application of wampee leaf extract. Background Art

[0002] Wampee leaf is the leaf of Clausena lansium (Lour.) Skeels, a common Chinese herbal medicine, which is mainly distributed in Fujian, Guangxi, Guangdong, Hainan and other places. Wampee leaf contains chemical components such as flavonoids, phenols and amino acids, and can be used to prevent and treat influenza, epidemic cerebrospinal meningitis, malaria, and treat symptoms such as cold and fever. It has good medicinal value. Therefore, the extraction of active ingredients from wampee leaf has gradually become the research focus of those in this field.

[0003] Patent CN104027436A discloses a preparation method of wampee leaf extract. The raw materials are washed, dried, and a low-carbon alcohol is used as the extractant, followed by ultrasonic treatment, concentration, and drying to prepare wampee leaf extract. This invention uses wampee leaf as the raw material and adopts ultrasonic-assisted organic solvent method to extract the active ingredients of wampee leaf. The preparation method of this invention is simple and has a short cycle, making great contributions to food preservation, the development of natural preservatives, and the comprehensive utilization of wampee leaf, but it does not study the improvement of the extraction rate. Patent CN106491503A discloses an extraction method of active ingredients from wampee leaf and its use in preparing skin care cream. Cellulase and compound protease are used to loosen, rupture the plant cell wall, reduce the mass transfer resistance, and accelerate the release of active ingredients such as flavonoids and polyphenols. Weak alkaline small molecule cluster water is used to extract the remaining active ingredients in the paper mulberry residue again, and modern biological engineering technologies such as microfiltration membrane purification of the extract are used to prepare wampee leaf extract, which is rich in antioxidant components such as polyphenols and flavonoids and antibacterial and anti-inflammatory components, and has a high extraction and separation rate, and can be used to prepare skin care cream, but the enzyme cannot be recycled after cell wall breaking, and the cost is relatively high.

[0004] Therefore, there is an urgent need to develop an extraction method with a high extraction rate and the ability to recycle materials. Summary of the Invention

[0005] Aiming at the problems existing in the prior art, the present invention has developed an extraction process of wampee leaf extract with a relatively high extraction rate, and the extraction rate reaches more than 33%.

[0006] In order to achieve the above object, the technical solution adopted by the present invention is as follows:

[0007] The first aspect of the present invention provides an extraction process of wampee leaf extract, comprising the following steps:

[0008] S1. Dry and crush wampee leaves to obtain wampee leaf powder;

[0009] S2. Add the wampee leaf powder obtained in step S1 to a solvent for extraction to obtain a mixture.

[0010] S3. Add a microwave-assisted absorbent to the mixture obtained in step S2 for microwave treatment, filter, wash, collect the filtrate, and dry to obtain the wampee leaf extract.

[0011] In the present invention, by adding a microwave-assisted absorbent and using the microwave-assisted extraction method to extract wampee leaves, the extraction times are effectively reduced, the extraction time is shortened, the extraction rate is improved at the same time, and the microwave-assisted absorbent has a long service life.

[0012] In some embodiments, the solvent is a mixture of 1,4-dioxane and absolute ethanol, and the volume ratio of the two is (0.3 - 0.6):1.

[0013] The preferred extraction solvent of the present invention is a mixture of 1,4-dioxane and absolute ethanol, and further defining the ratio of the two can improve the extraction rate of the wampee leaf extract and effectively reduce the usage amount of volatile toxic reagents. The possible reason is that the specific solvent ratio is closer to the polarity of the active ingredients in wampee leaves, which is beneficial to the precipitation of the active ingredients in wampee leaves.

[0014] In some embodiments, the mass ratio of the wampee leaf powder to the solvent in step S2 is 1:(15 - 25).

[0015] In some embodiments, the extraction temperature in step S2 is 40 - 50 °C, and the extraction time is 1 - 2 h.

[0016] In some embodiments, the preparation method of the microwave-assisted absorbent includes the following steps:

[0017] (1) Immerse carbon nanotubes in a nitric acid solution for 1 - 2 h, wash, and dry to obtain pretreated carbon nanotubes.

[0018] (2) Add the pretreated carbon nanotubes obtained in step (1) and the silane coupling agent KH570 to ethanol, react at 50 - 60 °C for 5 - 6 h, filter, wash, and dry to obtain silane-modified carbon nanotubes.

[0019] (3) Add the silane-modified carbon nanotubes, 2-hydroxy-4-acryloyloxybenzophenone, 1-allyl-3-vinylimidazolium hexafluorophosphate, and initiator obtained in step (2) to ethanol, react at 70 - 80 °C for 1 - 2 h, filter, wash, and dry to obtain the microwave-assisted absorbent.

[0020] Microwave-assisted extraction of active ingredients from plants is a simple, green and efficient method. The applicant improves the extraction efficiency by adding a microwave-assisted absorbent during the microwave extraction process, and can also improve the precipitation of active ingredients. The possible reason is that the silane-modified carbon nanotubes are polymerized with 2-hydroxy-4-acryloyloxy benzophenone and 1-allyl-3-vinylimidazolium hexafluorophosphate, which increases the dispersibility of the carbon nanotubes, enabling them to come into full contact with the wampee leaf powder. Moreover, the added ketone group enhances the interaction with flavonoids in the wampee leaf extract, increasing the precipitation of flavonoids. In addition, the surface of the silane-modified carbon nanotubes after the polymerization reaction has a large number of phenolic hydroxyl groups, which play a certain antioxidant role and can reduce the oxidation of active ingredients in the extract during the microwave treatment. Moreover, the imidazole group and a large number of fluorine atoms increase the hydrogen bond interaction with phenolic and amino acid substances in the extract, further improving the extraction rate and shortening the extraction time. In addition, 1-allyl-3-vinylimidazolium hexafluorophosphate with multiple double bonds is selected for the polymerization reaction to increase the crosslinking degree of the microwave-assisted absorbent, enhancing the stability of the microwave-assisted absorbent and enabling its reuse.

[0021] In some embodiments, the carbon nanotubes are single-walled carbon nanotubes.

[0022] In some embodiments, the mass ratio of the pretreated carbon nanotubes to the silane coupling agent KH570 in step (2) is 1:(0.8 - 1).

[0023] In some embodiments, the mass ratio of the silane-modified carbon nanotubes, 2-hydroxy-4-acryloyloxy benzophenone to 1-allyl-3-vinylimidazolium hexafluorophosphate in step (2) is 1:(0.2 - 0.4):(0.3 - 0.5).

[0024] The present invention specifically selects single-walled carbon nanotubes for pretreatment and defines the mass ratio of the pretreated carbon nanotubes to the silane coupling agent KH570, grafts double bonds on the surface of the pretreated carbon nanotubes, and then polymerizes them with 2-hydroxy-4-acryloyloxy benzophenone and 1-allyl-3-vinylimidazolium hexafluorophosphate, which can effectively improve the dispersibility of single-walled carbon nanotubes and simultaneously increase the extraction rate. The possible reason is that single-walled carbon nanotubes have a single-layer structure, and the surface groups after pretreatment are more active and have stronger reactivity with the silane coupling agent. In addition, by defining the mass ratio of the silane-modified carbon nanotubes, 2-hydroxy-4-acryloyloxy benzophenone to 1-allyl-3-vinylimidazolium hexafluorophosphate, the dispersibility of single-walled carbon nanotubes is improved without reducing the microwave absorption ability of the carbon nanotubes.

[0025] In some embodiments, the addition amount of the microwave-assisted absorbent is 0.7% - 1% of the mass of the wampee leaf powder in step S2.

[0026] In some embodiments, the time of the microwave treatment in step S3 is 40 - 50 s, and the microwave power is 180 - 200 W.

[0027] The second aspect of the present invention provides an application of wampee leaf extract in a disinfectant.

[0028] Compared with the prior art, the present invention has the following beneficial effects:

[0029] (1) By adding a microwave-assisted absorbent during the extraction process of wampee leaves, the present invention effectively reduces the number of extraction times, shortens the extraction time, and simultaneously reduces the loss of active ingredients in the extract, improving the extraction rate, which reaches more than 33%.

[0030] (2) By polymerizing silane-modified carbon nanotubes with 2-hydroxy-4-acryloyloxybenzophenone and 1-allyl-3-vinylimidazolium hexafluorophosphate, the present invention increases the dispersibility of carbon nanotubes, enabling them to fully contact with wampee leaf powder. Moreover, the added ketone group enhances the interaction with flavonoids in the wampee leaf extract, increasing the precipitation of flavonoids. Additionally, the surface of the silane-modified carbon nanotubes after the polymerization reaction has a large number of phenolic hydroxyl groups, which play a certain antioxidant role, capable of reducing the oxidation of active ingredients in the extract during the microwave treatment. Moreover, the imidazole group and a large number of fluorine atoms increase the hydrogen bond interaction with phenolic and amino acid substances in the extract, further improving the extraction rate and shortening the extraction time.

[0031] (3) The present invention selects 1-allyl-3-vinylimidazolium hexafluorophosphate with multiple double bonds for the polymerization reaction to increase the crosslinking degree of the microwave-assisted absorbent, increasing the stability of the microwave-assisted absorbent, enabling it to be reused and reducing the reduction amount of the extraction rate. Specific Embodiments

[0032] The following will illustrate the present invention in conjunction with specific implementation embodiments. It should be noted that the following examples are examples of the present invention, only used to illustrate the present invention, and not to limit the present invention. Other combinations and various improvements within the inventive concept can be made without departing from the main idea or scope of the present invention.

[0033] In the following examples and comparative examples, the compounds and related reagents used are all commercially available. Among them, the single-walled carbon nanotubes with the model CNT100 are purchased from Zhongke Leiming (Beijing) Technology Co., Ltd.

[0034] Preparation Example 1

[0035] A preparation method of microwave-assisted absorbent - 1 includes the following steps:

[0036] (1) Add 20 g of single-walled carbon nanotubes to 200 ml of 75 wt% nitric acid solution, soak for 1.5 h, wash, and dry to obtain pretreated carbon nanotubes;

[0037] (2) Add 10 g of the pretreated carbon nanotubes obtained in step (1) and 9 g of silane coupling agent KH570 to 200 ml of absolute ethanol, react at 55 °C for 5.5 h, filter, wash, and dry to obtain silane-modified carbon nanotubes;

[0038] (3) Add 10 g of the silane-modified carbon nanotubes obtained in step (2), 3 g of 2-hydroxy-4-acryloyloxybenzophenone, 4 g of 1-allyl-3-vinylimidazolium hexafluorophosphate, and 0.02 g of azobisisobutyronitrile to 100 ml of absolute ethanol, react at 75 °C for 1.5 h, filter, wash, and dry to obtain microwave-assisted absorbent-1.

[0039] Preparation Example 2

[0040] A preparation method of microwave-assisted absorbent-2, the specific implementation manner is the same as that of Preparation Example 1, the difference is that the addition amount of silane coupling agent KH570 is 12 g.

[0041] Preparation Example 3

[0042] A preparation method of microwave-assisted absorbent-3, the specific implementation manner is the same as that of Preparation Example 1, the difference is that the addition amount of 2-hydroxy-4-acryloyloxybenzophenone is 6 g.

[0043] Preparation Example 4

[0044] A preparation method of microwave-assisted absorbent-4, the specific implementation manner is the same as that of Preparation Example 1, the difference is that the addition amount of 1-allyl-3-vinylimidazolium hexafluorophosphate is 7 g.

[0045] Example 1

[0046] An extraction process of Clausena lansium leaf extract, comprising the following steps:

[0047] S1. Dry and crush 1000 g of Clausena lansium leaves to obtain Clausena lansium leaf powder;

[0048] S2. Add 200 g of the Clausena lansium leaf powder obtained in step S1 to 4000 g of a solvent for extraction. The solvent is a mixture of 1,4-dioxane and absolute ethanol, and the volume ratio of the two is 0.5:1. The extraction temperature is 45 °C, and the extraction time is 1.5 h to obtain a mixture;

[0049] S3. Add 1.6 g of microwave-assisted absorbent-1 to 4200 g of the mixture obtained in step S2, perform microwave treatment for 45 s, with a microwave power of 190 W, filter, wash, collect the filtrate, and dry to obtain Clausena lansium leaf extract.

[0050] Example 2

[0051] An extraction process of Clausena lansium leaf extract comprises the following steps:

[0052] S1. Dry and crush 1000 g of Clausena lansium leaves to obtain Clausena lansium leaf powder;

[0053] S2. Add 200 g of the Clausena lansium leaf powder obtained in step S1 into 3000 g of a solvent for extraction. The solvent is a mixture of 1,4 - dioxane and absolute ethanol, and the volume ratio of the two is 0.3:1. The extraction temperature is 40 °C, and the extraction time is 2 h to obtain a mixture;

[0054] S3. Add 1.4 g of microwave - assisted absorbent - 1 to 3200 g of the mixture obtained in step S2 for microwave treatment for 40 s. The microwave power is 180 W. Filter, wash, collect the filtrate, and dry to obtain Clausena lansium leaf extract.

[0055] Example 3

[0056] S1. Dry and crush 1000 g of Clausena lansium leaves to obtain Clausena lansium leaf powder;

[0057] S2. Add 200 g of the Clausena lansium leaf powder obtained in step S1 into 5000 g of a solvent for extraction. The solvent is a mixture of 1,4 - dioxane and absolute ethanol, and the volume ratio of the two is 0.6:1. The extraction temperature is 45 °C, and the extraction time is 55 min to obtain a mixture;

[0058] S3. Add 2 g of microwave - assisted absorbent - 1 to 5200 g of the mixture obtained in step S2 for microwave treatment for 50 s. The microwave power is 200 W. Filter, wash, collect the filtrate, and dry to obtain Clausena lansium leaf extract.

[0059] Example 4

[0060] An extraction process of Clausena lansium leaf extract, the specific implementation method is the same as that of Example 1, the difference is that microwave - assisted absorbent - 1 is equally replaced by microwave - assisted absorbent - 2.

[0061] Example 5

[0062] An extraction process of Clausena lansium leaf extract, the specific implementation method is the same as that of Example 1, the difference is that microwave - assisted absorbent - 1 is equally replaced by microwave - assisted absorbent - 3.

[0063] Example 6

[0064] An extraction process of Clausena lansium leaf extract, the specific implementation method is the same as that of Example 1, the difference is that microwave - assisted absorbent - 1 is equally replaced by microwave - assisted absorbent - 4.

[0065] Example 7

[0066] An extraction process of Clausena lansium leaf extract, the specific implementation method is the same as that of Example 1, the difference is that the microwave-assisted absorbent-1 is replaced with single-walled carbon nanotubes in equal amount.

[0067] Comparative Example 1

[0068] An extraction process of Clausena lansium leaf extract, comprising the following steps:

[0069] S1. Dry and crush 1000 g of Clausena lansium leaves to obtain Clausena lansium leaf powder;

[0070] S2. Add 200 g of the Clausena lansium leaf powder obtained in step S1 to 4000 g of a solvent for extraction. The solvent is a mixture of 1,4-dioxane and absolute ethanol, and the volume ratio of the two is 0.5:1. The extraction temperature is 45 °C, and the extraction time is 1.5 h. Filter, wash, collect the filtrate, and dry to obtain Clausena lansium leaf extract.

[0071] Performance Test

[0072] The Clausena lansium leaf extracts obtained by the extraction processes of the above examples and comparative examples were tested as follows:

[0073] Extraction rate: Calculate the extraction rate according to the formula extraction rate = mass of Clausena lansium leaf extract / mass of Clausena lansium leaf powder × 100%.

[0074] The test results are shown in Table 1:

[0075] Table 1

[0076]

[0077]

[0078] From the comparison of the experimental data of Examples 1-3 in Table 1, it can be seen that the extract obtained by the extraction process of the present invention has a higher extraction rate; from the comparison between Example 4 and Example 1, it can be seen that the change in the ratio of pretreated carbon nanotubes to silane coupling agent KH570 results in a decrease in the uniformity of the microwave-assisted absorbent, affecting the dispersion ability and the extraction rate decreases; from the comparison between Examples 5 and 6 and Example 1, it can be seen that the change in the ratio of silane-modified carbon nanotubes, 2-hydroxy-4-acryloyloxybenzophenone and 1-allyl-3-vinylimidazolium hexafluorophosphate may lead to excessive crosslinking degree, affecting the wave absorption rate and the extraction rate decreases; from the comparison between Example 7 and Example 1, it can be seen that directly using carbon nanotubes as the microwave-assisted absorbent has a weak interaction with the active ingredient and the extraction rate decreases; from the comparison between Comparative Example 1 and Example 1, it can be seen that using the ordinary method for extraction results in less precipitation of the active ingredient and a lower extraction rate.

[0079] 2. Recyclability of microwave-assisted extractant

[0080] After circulating the microwave-assisted extractant-1 for 15 times, it was used in Example 1, and the extraction rate was calculated. The extraction rate was 34.9%, indicating that the microwave-assisted extractant has good recyclability and a long service life.

[0081] The above embodiments are only for illustrating the technical concept and characteristics of the present invention, and the purpose is to enable those who are familiar with this technology to understand the content of the present invention and implement it. It should not be used to limit the protection scope of the present invention. Any equivalent changes or modifications made according to the spirit and essence of the present invention should be covered within the protection scope of the present invention.

Claims

1. An extraction process of Clausena lansium leaf extract, characterized in that, It includes the following steps: S1. Dry and crush Clausena lansium leaves to obtain Clausena lansium leaf powder; S2. Add the Clausena lansium leaf powder obtained in step S1 into a solvent for extraction to obtain a mixture; S3. Add a microwave-assisted absorbent into the mixture obtained in step S2 for microwave treatment, filter, wash, collect the filtrate, and dry to obtain the Clausena lansium leaf extract.

2. The extraction process of the wampee leaf extract according to claim 1, wherein, The solvent is a mixture of 1,4-dioxane and absolute ethanol, and the mass ratio of the two is (0.3 - 0.6):

1.

3. The extraction process of the Clausena lansium leaf extract according to claim 1, characterized in that, The mass ratio of the Clausena lansium leaf powder to the solvent in step S2 is 1:(15 - 25).

4. The extraction process of the wampee leaf extract according to claim 1, characterized in that, In step S2, the extraction temperature is 40 - 50°C, and the extraction time is 1 - 2 h.

5. The extraction process of the Clausena lansium leaf extract according to claim 1, characterized in that, The preparation method of the microwave-assisted absorbent includes the following steps: (1) Immerse carbon nanotubes in a nitric acid solution for 1 - 2 h, wash, and dry to obtain pretreated carbon nanotubes; (2) Add the pretreated carbon nanotubes obtained in step (1) and silane coupling agent KH570 into ethanol, react at 50 - 60°C for 5 - 6 h, filter, wash, and dry to obtain silane-modified carbon nanotubes; (3) Add the silane-modified carbon nanotubes, 2-hydroxy-4-acryloyloxybenzophenone, 1-allyl-3-vinylimidazolium hexafluorophosphate, and initiator obtained in step (2) into ethanol, react at 70 - 80°C for 1 - 2 h, filter, wash, and dry to obtain the microwave-assisted absorbent.

6. The extraction process of the wampee leaf extract according to claim 5, characterized in that, In step (2), the mass ratio of the pretreated carbon nanotubes to the silane coupling agent KH570 is 1:(0.8 - 1).

7. The extraction process of the wampee leaf extract according to claim 5, characterized in that, In step (2), the mass ratio of the silane-modified carbon nanotubes, 2-hydroxy-4-acryloyloxybenzophenone, and 1-allyl-3-vinylimidazolium hexafluorophosphate is 1:(0.2 - 0.4):(0.3 - 0.5).

8. The extraction process of the Clausena lansium leaf extract according to claim 1, characterized in that, The addition amount of the microwave-assisted absorbent is 0.7% - 1% of the mass of the Clausena lansium leaf powder in step S2.

9. The extraction process of the Clausena lansium leaf extract according to claim 1, wherein, In step S3, the microwave treatment time is 40 - 50 s, and the microwave power is 180 - 200 W.

10. Application of the Clausena lansium leaf extract obtained by the extraction process of the Clausena lansium leaf extract described in claims 1 - 9 in a disinfectant.

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