Method for removing aflatoxin from formula granules

Abstract

The invention relates to the technical field of traditional Chinese medicine formula granules, in particular to a method for removing aflatoxin from formula granules. The method comprises the following steps: adding activated carbon and diatomite into concentrated ointment, and uniformly stirring to obtain a mixture; filtering the mixture to obtain a filtered ointment; carrying out spray drying on the filtered ointment to prepare dry ointment powder; and carrying out dry pressing granulation on the dry paste powder to prepare the formula granules. By adopting the method provided by the invention, the aflatoxin in the formula granule product can be obviously reduced, the quality indexes such as granule character, content, extract, characteristic spectrum and the like are not influenced, and the stable granule quality is ensured.

Description

Technical Field

[0001] This invention relates to the field of traditional Chinese medicine formula granules, and in particular to a method for removing aflatoxin from formula granules. Background Technology

[0002] Traditional Chinese medicine (TCM) granules are single-herb granules produced under the guidance of TCM theory, using standardized processed TCM decoction pieces or raw materials as raw materials, and through modern processes such as extraction, concentration, and drying. For cost control reasons, industrial production typically uses raw TCM materials directly.

[0003] If temperature and humidity are not properly controlled during the harvesting, processing, and storage of Chinese medicinal herbs, Aspergillus flavus can easily grow, producing the potent carcinogen aflatoxin. The risk of contamination is particularly high for kernel-type medicinal herbs rich in starch and oil (such as bitter almonds and areca nuts) and some animal-derived medicinal herbs. Aflatoxin is stable in nature, and once contaminated, conventional treatment methods are insufficient to effectively remove it.

[0004] Currently, quality control mainly relies on rigorous testing of raw medicinal materials. However, even if the aflatoxin levels in the raw materials meet the limits stipulated in the Chinese Pharmacopoeia, after extraction and concentration processes, the toxin, due to its strong heat resistance and insolubility in water, will be extracted along with the active ingredients and highly concentrated during the concentration process. This can easily lead to the toxin content in the final formulated granules exceeding the upper limit stipulated by national standards, resulting in batches of product scrap and causing huge economic losses to enterprises. This problem is most pronounced in varieties such as bitter almond, polygala, and areca nut.

[0005] Currently, there is a lack of dedicated methods to effectively degrade or remove aflatoxin during the production of formulation granules without affecting the main active ingredients and efficacy of the medicinal materials. Conventional physical or chemical detoxification methods (such as ultraviolet light and ozone treatment) may damage heat-sensitive components or introduce the risk of secondary contamination, and are therefore unsuitable for pharmaceutical production. Summary of the Invention

[0006] In view of the above problems, the present invention is proposed to provide a method for removing aflatoxin from formulation particles that overcomes or at least partially solves the above problems, so as to reduce the content of aflatoxin in formulation particles.

[0007] Specifically, the present invention provides a method for removing aflatoxin from formulated particles, comprising: S100, add activated carbon and diatomaceous earth to the concentrated ointment and stir evenly to obtain a mixture; S200, the mixture is filtered to obtain a filtered ointment; S300, the filtered ointment is spray-dried to obtain a dry ointment powder; S400, the dry powder is dry-pressed into granules to obtain the formulation granules.

[0008] Optionally, step S100 specifically includes: S110, add the activated charcoal to the concentrated ointment and stir for a first preset time to obtain a stirred mixture; wherein, the amount of activated charcoal added is 0.1% to 0.3% of the weight of the concentrated ointment, and the first preset time is 1.5 hours to 3 hours; S120, add the diatomaceous earth to the mixture and stir for a second preset time to obtain the mixture; wherein, the second preset time is less than the first preset time, the amount of diatomaceous earth added is 0.1% to 0.3% of the weight of the concentrated ointment, and the second preset time is 0.3 hours to 1 hour.

[0009] Optionally, step S200 specifically includes: filtering the mixture sequentially using a sieve and a plate and frame filter; wherein the plate and frame filter includes multiple layers of filter paper.

[0010] Optionally, the formulation granules are bitter almond formulation granules; The concentrated ointment is obtained by extraction and concentration of raw bitter almond or processed bitter almond slices; The amount of activated carbon added is less than the amount of diatomaceous earth added.

[0011] Optionally, the amount of activated charcoal added is 0.2% of the weight of the concentrated ointment; The amount of diatomaceous earth added is 0.3% of the weight of the concentrated ointment.

[0012] Optionally, the formula granules are Polygala tenuifolia formula granules; The concentrated ointment is obtained by extraction and concentration of raw Polygala tenuifolia medicinal material or Polygala tenuifolia processed slices; The amount of activated carbon added is less than the amount of diatomaceous earth added.

[0013] Optionally, the amount of activated charcoal added is 0.2% of the weight of the concentrated ointment; The amount of diatomaceous earth added is 0.3% of the weight of the concentrated ointment.

[0014] Optionally, the formulated granules are areca nut formulated granules; The concentrated ointment is obtained by extraction and concentration of raw areca nut or areca nut slices; The amount of activated carbon added is 0.2% to 0.3% of the weight of the concentrated ointment.

[0015] The beneficial effects of this invention are: In the aflatoxin removal method for formulated granules of this invention, activated carbon and diatomaceous earth are added to the concentrated ointment and stirred thoroughly. This allows for efficient and specific adsorption and extraction of the aflatoxin enriched after concentration, which can then be removed by subsequent filtration. On one hand, this invention solves the core technological challenge of excessive toxin accumulation in varieties such as bitter almond, polygala, and areca nut after extraction and concentration. On the other hand, this embodiment is simple to operate, easy to implement, and inexpensive. Furthermore, this embodiment is safe and reliable. Activated carbon and diatomaceous earth are mature and safe pharmaceutical excipients that efficiently remove toxins without introducing new safety hazards and have no significant impact on the main effective components of the medicinal materials. This maximizes the safety and quality stability of the finished formulated granules, avoiding batch waste losses due to excessive toxin levels, resulting in significant economic benefits.

[0016] In summary, the method of this invention can significantly reduce aflatoxin in formulated granule products without affecting quality indicators such as granule properties, content, extractives, and characteristic spectra, thus ensuring stable granule quality.

[0017] Furthermore, the combination of activated carbon and diatomaceous earth produces a synergistic effect, which is not simply a superposition of their effects. Activated carbon alone has a good detoxification effect but affects the product's properties, while diatomaceous earth alone has little impact on properties but a poor detoxification effect. However, the specific combination and sequential addition of the two unexpectedly significantly reduced toxins while better maintaining the product's good properties and the content of effective ingredients.

[0018] The above and other objects, advantages and features of the present invention will become more apparent to those skilled in the art from the following detailed description of specific embodiments of the invention in conjunction with the accompanying drawings. Attached Figure Description

[0019] The following sections will describe some specific embodiments of the invention in detail by way of example and not limitation, with reference to the accompanying drawings. The same reference numerals in the drawings denote the same or similar parts or portions. Those skilled in the art should understand that these drawings are not necessarily drawn to scale. In the drawings: Figure 1 This is a schematic flowchart of a method for removing aflatoxin from formulation particles according to an embodiment of the present invention; Figure 2 This is a liquid chromatogram of the aflatoxin content in the bitter almond formulation granules prepared in Comparative Example 1; Figure 3 This is a liquid chromatogram of the aflatoxin content in the bitter almond formulation granules prepared in Example 5; Figure 4 This is a liquid chromatogram of the aflatoxin content in the Polygala tenuifolia formulation granules prepared in Comparative Example 2; Figure 5This is a liquid chromatogram of the aflatoxin content in the Polygala tenuifolia formulation granules prepared in Example 16; Figure 6 This is a liquid chromatogram of the aflatoxin content in the areca nut granules prepared in Comparative Example 3; Figure 7 This is a liquid chromatogram of the aflatoxin content in the areca nut granules prepared in Example 23. Detailed Implementation

[0020] The following reference Figure 1 This invention describes a method for removing aflatoxin from formulation particles according to embodiments of the present invention. In this description, it should be understood that the terms "first" and "second" are used for descriptive purposes only and should not be construed as indicating or implying relative importance or implicitly specifying the number of indicated technical features. Therefore, a feature defined with "first" or "second" may explicitly or implicitly include at least one of that feature, that is, include one or more of that feature. In the description of the present invention, "a plurality of" means at least two, such as two, three, etc., unless otherwise explicitly specified. When a feature "includes or contains" one or more of the features it encompasses, unless otherwise specifically described, this indicates that other features are not excluded and may be further included.

[0021] In the description of this embodiment, the terms "one embodiment," "some embodiments," "illustrative embodiment," "example," "specific example," or "some examples," etc., refer to specific features, structures, materials, or characteristics described in connection with that embodiment or example, which are included in at least one embodiment or example of the present invention. In this specification, the illustrative expressions of the above terms do not necessarily refer to the same embodiment or example. Furthermore, the specific features, structures, materials, or characteristics described may be combined in any suitable manner in one or more embodiments or examples.

[0022] This invention provides a method for removing aflatoxin from formulation granules, which may include the following steps: S100, add activated carbon and diatomaceous earth to the concentrated ointment and stir evenly to obtain a mixture; S200, the mixture is filtered to obtain a filtered ointment; S300, the filtered ointment is spray-dried to obtain dry ointment powder; S400 is used to dry-press dry powder into granules to obtain the formulated granules.

[0023] The aflatoxin removal method for formulated granules described in this embodiment can be used in the preparation of formulated granules, and is particularly suitable for the preparation of bitter almond formulated granules, polygala formulated granules, and areca nut formulated granules. The concentrated ointment is obtained by extraction and concentration of the original medicinal materials or processed medicinal slices. In other words, this aflatoxin removal method for formulated granules is applicable after the concentration step in the formulated granule preparation process.

[0024] The applicant's preliminary research revealed that using activated carbon alone significantly reduces aflatoxin levels with minimal impact on the content, extractives, and chromatograms of the formulated granules. However, this method requires a longer time to remove aflatoxin and significantly affects the appearance (color) of the granules. Diatomaceous earth has a lower effect on aflatoxin but little impact on other indicators. Therefore, the applicant combined the two methods to reduce aflatoxin levels without affecting other quality indicators.

[0025] Specifically, in step S100, after the activated carbon, diatomaceous earth, and concentrated ointment are stirred evenly, the activated carbon and diatomaceous earth can fully adsorb aflatoxin in the concentrated ointment. In step S200, since the activated carbon and diatomaceous earth have relatively large particle sizes, and the aflatoxin is adsorbed onto the activated carbon and diatomaceous earth, a filtration device can be used to filter out the activated carbon, diatomaceous earth, and aflatoxin in the mixture to obtain a filtered ointment.

[0026] In this embodiment, by adding activated carbon and diatomaceous earth to the concentrated ointment and stirring thoroughly, aflatoxin enriched after extraction and concentration can be efficiently and specifically adsorbed and extracted, and then removed by subsequent filtration. On the one hand, this invention solves the core technological problem of excessive toxin enrichment in varieties such as bitter almond, polygala, and areca nut after extraction and concentration. On the other hand, this embodiment is simple to operate, easy to implement, and inexpensive. Furthermore, this embodiment is safe and reliable; activated carbon and diatomaceous earth are mature and safe pharmaceutical excipients that efficiently remove toxins without introducing new safety hazards and have no significant impact on the main effective components of the medicinal materials. This maximizes the safety and quality stability of the finished formulation granules, avoiding batch waste losses due to excessive toxins, resulting in significant economic benefits.

[0027] In summary, the method of this embodiment can reduce aflatoxin in formulated granule products to the standard range without affecting the quality indicators such as granule properties, content, extractives, and characteristic chromatograms, thus ensuring stable granule quality.

[0028] In some optional embodiments of the present invention, step S100 specifically includes the following steps: S110, Activated charcoal is added to the concentrated ointment and stirred for a first preset time to obtain a stirred mixture; wherein the amount of activated charcoal added is 0.1% to 0.3% of the weight of the concentrated ointment.

[0029] S120, add diatomaceous earth to the mixture and stir for a second preset time to obtain a mixture; wherein, the second preset time is less than the first preset time, and the amount of diatomaceous earth added is 0.1% to 0.3% of the weight of the concentrated ointment.

[0030] Specifically, the amount of activated carbon added can be any one of 0.1%, 0.15%, 0.2%, 0.25%, or 0.3% of the weight of the concentrated ointment. The amount of diatomaceous earth added can be any one of 0.1%, 0.15%, 0.2%, 0.25%, or 0.3% of the weight of the concentrated ointment.

[0031] In this embodiment, by refining the adsorption process, better detoxification efficiency and economic benefits were achieved.

[0032] On the one hand, by adding activated carbon first and then diatomaceous earth, the activated carbon can preferentially and fully adsorb aflatoxin of molecular structure, giving full play to its highly efficient detoxification properties. On the other hand, the diatomaceous earth added later can effectively improve the filtration performance of the ointment and assist in adsorbing residual impurities. The two work together to avoid competitive adsorption that may occur when adding them at the same time, thereby improving the overall removal rate.

[0033] On the other hand, setting the first stirring time to be longer than the second stirring time ensures that the activated carbon has sufficient time to complete the relatively slow process of deep adsorption of aflatoxin, while diatomaceous earth disperses quickly as a filter aid and can be mixed evenly in a short time. This design optimizes production time and improves efficiency while ensuring effectiveness.

[0034] On the other hand, the addition of activated carbon and diatomaceous earth is precisely controlled at 0.1% to 0.3%. This range is an effective balance point verified by experiments. It can not only fully ensure that the toxin adsorption meets the standards, but also minimize the adsorption loss of the active ingredients in the ointment by the excipients, thus ensuring the quality stability of the finished granules, while avoiding the cost increase and subsequent filtration burden caused by excessive use.

[0035] Furthermore, the combination of activated carbon and diatomaceous earth produces a synergistic effect, which is not simply a superposition of their effects. Activated carbon alone has a good detoxification effect but affects the product's properties, while diatomaceous earth alone has little impact on properties but a poor detoxification effect. However, the specific combination and sequential addition of the two unexpectedly significantly reduced toxins while better maintaining the product's good properties and the content of effective ingredients.

[0036] In some optional embodiments of the present invention, the first preset duration is 1.5 hours to 3 hours.

[0037] For example, the first preset duration can be 1.5 hours, 1.8 hours, 2 hours, 2.5 hours and 3 hours.

[0038] Preferably, the second preset duration is 1.8 hours to 2.2 hours.

[0039] More preferably, the second preset duration can be 2 hours.

[0040] In some optional embodiments of the present invention, the second preset duration is 0.3 hours to 1 hour.

[0041] For example, the second preset duration can be 0.3 hours, 0.5 hours, 0.8 hours, 0.9 hours, and 1 hour.

[0042] Preferably, the second preset duration is 0.4 hours to 0.6 hours.

[0043] More preferably, the second preset duration is 0.5 hours.

[0044] In some optional embodiments of the present invention, step S200 may specifically include: filtering the mixture sequentially using a sieve and a plate and frame filter. The plate and frame filter comprises multiple layers of filter paper.

[0045] Specifically, the screen can be 350 mesh. A plate and frame filter can include 5 to 50 layers of filter paper. Preferably, the plate and frame filter includes 20 to 45 layers of filter paper. More preferably, the plate and frame filter includes 40 layers of filter paper. The mesh size of each layer of filter paper gradually increases, i.e., the pore size of each layer of filter paper gradually decreases, according to the material conveying direction of the filter.

[0046] This embodiment adopts a two-stage filtration method that combines coarse filtration with fine filtration using a plate and frame filter (multi-layer filter paper). First, large particles are quickly removed, and then fine impurities and toxins are thoroughly intercepted through precision filtration, which greatly improves filtration efficiency, equipment life and product purity, and ensures removal effect and production economy.

[0047] In some optional embodiments of the present invention, the formulation granules are bitter almond (Siberian apricot) formulation granules. The concentrated ointment is obtained by extraction and concentration of raw bitter almond material or bitter almond slices. In step S100, the amount of activated carbon added is less than the amount of diatomaceous earth added.

[0048] Further, in step S100, the amount of activated carbon added is 0.2% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.3% of the weight of the concentrated ointment.

[0049] In this embodiment, while ensuring that aflatoxin levels meet the standards, priority is given to minimizing the adsorption loss of key medicinal components of bitter almonds (such as amygdalin) by activated carbon, thereby better preserving the efficacy of the medicinal material. At the same time, a higher proportion of diatomaceous earth significantly improves the fluidity and filtration efficiency of the concentrated ointment, effectively preventing clogging in the filtration process, and helping to obtain a final product with a lighter color and better appearance, achieving a comprehensive balance between detoxification, quality preservation, and optimized production.

[0050] Example 1 of a method for removing aflatoxin from bitter almond (Siberian apricot) formulation granules: A method for removing aflatoxin from bitter almond granules includes: S11, Add activated charcoal to the concentrated ointment and stir for 2 hours to obtain the stirred mixture; wherein, the amount of activated charcoal added is 0.1% of the weight of the concentrated ointment, and the concentrated ointment is obtained by extracting and concentrating bitter almond raw material or bitter almond slices; S12, add diatomaceous earth to the mixture and stir for 0.5 hours to obtain a mixture; the amount of diatomaceous earth added is 0.2% of the weight of the concentrated ointment; S13, the mixture is filtered sequentially using a sieve and a plate and frame filter; wherein the plate and frame filter includes 40 layers of filter paper; S14, the filtered ointment is spray-dried to obtain a dry ointment powder; S15, dry-press the dry powder into granules to obtain bitter almond formula granules.

[0051] Example 2 of a method for removing aflatoxin from bitter almond granules: Example 2 differs from Example 1 only in the amount of diatomaceous earth added; all other steps and parameters are the same. In Example 2, the amount of diatomaceous earth added is 0.3% of the weight of the concentrated ointment.

[0052] Example 3 of a method for removing aflatoxin from bitter almond granules: Compared with Example 1, Example 3 differs only in the amount of activated carbon and diatomaceous earth added; all other steps and parameters are the same. In Example 3, the amount of activated carbon added is 0.2% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.1% of the weight of the concentrated ointment.

[0053] Example 4 of a method for removing aflatoxin from bitter almond granules: Compared with Example 1, Example 4 differs only in the amount of activated carbon and diatomaceous earth added; all other steps and parameters are the same. In Example 4, the amount of activated carbon added is 0.2% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.2% of the weight of the concentrated ointment.

[0054] Example 5 of a method for removing aflatoxin from bitter almond granules: Compared with Example 1, Example 5 differs only in the amount of activated carbon and diatomaceous earth added; all other steps and parameters are the same. In Example 5, the amount of activated carbon added is 0.2% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.3% of the weight of the concentrated ointment.

[0055] Example 6 of a method for removing aflatoxin from bitter almond granules: Compared with Example 1, Example 6 differs only in the amount of activated carbon and diatomaceous earth added; all other steps and parameters are the same. In Example 6, the amount of activated carbon added is 0.3% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.1% of the weight of the concentrated ointment.

[0056] Example 7 of a method for removing aflatoxin from bitter almond granules: Compared with Example 1, Example 7 differs only in the amount of activated carbon and diatomaceous earth added; all other steps and parameters are the same. In Example 7, the amount of activated carbon added is 0.3% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.2% of the weight of the concentrated ointment.

[0057] Example 8 of a method for removing aflatoxin from bitter almond granules: Compared with Example 1, Example 8 differs only in the amount of activated carbon and diatomaceous earth added; all other steps and parameters are the same. In Example 8, the amount of activated carbon added is 0.3% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.3% of the weight of the concentrated ointment.

[0058] Comparative Example 1: A method for preparing bitter almond formula granules includes: spray drying a concentrated medicinal paste obtained by extracting and concentrating bitter almond raw material or bitter almond slices to obtain a dry paste powder; and dry-pressing the dry paste powder into granules to obtain bitter almond formula granules.

[0059] The bitter almond formulation granules obtained in Examples 1 to 8 and Comparative Example 1 were tested, and the results are shown in Table 1.

[0060] Table 1 Comparison of results between Examples 1-8 and Comparative Example 1 Properties of bitter almond formula granules amygdalin content (mg / g) Extract% Aflatoxin B1 content (μg / kg) Total content of aflatoxins G2, G1, B2 and B (μg / kg) Comparative Example 1 off-white 99.89 56.9 29 32.7 Example 1 grayish white 99.25 56.1 4.8 5.9 Example 2 off-white 98.26 55.8 4.2 5.1 Example 3 grey 98.57 55.4 3.2 3.6 Example 4 Light gray 98.75 55.2 2.8 3.2 Example 5 off-white 98.13 55.1 2.2 2.9 Example 6 brown 98.28 55.7 1.9 2.7 Example 7 brownish-gray 97.87 55.4 1.5 2.5 Example 8 Light gray 97.67 55.2 1.2 1.8 The content of amygdalin was determined by high performance liquid chromatography (HPLC) (Chinese Pharmacopoeia 2020 General Chapter 0512). The extractives were determined by the hot extraction method under the alcohol-soluble extractives determination method (Chinese Pharmacopoeia 2020 General Chapter 2201), using ethanol as the solvent, and the content was not less than 35.0%. The content of aflatoxin was determined by the mycotoxin determination method (Chinese Pharmacopoeia 2020 General Chapter 2351). The characteristic chromatogram of bitter almond granules was determined by HPLC (Chinese Pharmacopoeia 2020 General Chapter 0512). Aflatoxins include aflatoxin B1, aflatoxin G2, aflatoxin G1, aflatoxin B2, and aflatoxin B. The content of aflatoxin B1, as well as the total content of aflatoxin G2, aflatoxin G1, aflatoxin B2, and aflatoxin B, were detected.

[0061] As shown in Table 1, Figure 2 and Figure 3As shown, comparisons revealed that in Examples 1 to 8, aflatoxin levels were significantly reduced, with minimal impact on the amygdalin content, extract content, and characteristic chromatograms of the bitter almond formulation granules. In particular, the optimal properties were observed when the added activated carbon was 0.2% and the added diatomaceous earth was 0.3%. Therefore, Example 5 is the optimal embodiment for the aflatoxin removal method from bitter almond formulation granules.

[0062] In some optional embodiments of the present invention, the formulation granules are Polygala tenuifolia formulation granules. The concentrated ointment is obtained by extraction and concentration of Polygala tenuifolia raw material or Polygala tenuifolia processed slices. In step S100, the amount of activated carbon added is less than the amount of diatomaceous earth added.

[0063] Further, in step S100, the amount of activated carbon added is 0.2% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.3% of the weight of the concentrated ointment.

[0064] This embodiment, tailored to the characteristics of Polygala tenuifolia, achieves a balance between detoxification, quality preservation, and smooth production by using a lower amount of activated carbon than diatomaceous earth. On one hand, while effectively controlling aflatoxin, it significantly reduces the adsorption loss of key active ingredients such as Polygala tenuifolia saponins by activated carbon, thus better preserving the inherent efficacy of Polygala tenuifolia. On the other hand, the higher proportion of diatomaceous earth greatly improves the filtration performance of the concentrated Polygala tenuifolia extract, effectively preventing pipe and filter blockage, increasing production efficiency, and contributing to a better-looking finished granule.

[0065] Example 11 of a method for removing aflatoxin from Polygala tenuifolia granules: A method for removing aflatoxin from Polygala tenuifolia formula granules includes: S21, Add activated charcoal to the concentrated ointment and stir for 2 hours to obtain the stirred mixture; wherein, the amount of activated charcoal added is 0.1% of the weight of the concentrated ointment, and the concentrated ointment is obtained by extracting and concentrating the raw medicinal material of Polygala tenuifolia or Polygala tenuifolia slices; S22, add diatomaceous earth to the mixture and stir for 0.5 hours to obtain a mixture; the amount of diatomaceous earth added is 0.1% of the weight of the concentrated ointment; S23, the mixture is filtered sequentially using a sieve and a plate and frame filter; wherein the plate and frame filter includes 40 layers of filter paper; S24, the filtered ointment is spray-dried to obtain a dry ointment powder; S25, dry-press the dried ointment powder into granules to obtain Polygala tenuifolia formula granules.

[0066] Example 12 of a method for removing aflatoxin from Polygala tenuifolia granules: Example 12 differs from Example 11 only in the amount of diatomaceous earth added; all other steps and parameters are the same. In Example 12, the amount of diatomaceous earth added is 0.2% of the weight of the concentrated ointment.

[0067] Example 13 of a method for removing aflatoxin from Polygala tenuifolia formula granules: Compared with Example 11, Example 13 differs only in the amount of diatomaceous earth added; all other steps and parameters are the same. In Example 13, the amount of diatomaceous earth added is 0.3% of the weight of the concentrated ointment.

[0068] Example 14 of a method for removing aflatoxin from Polygala tenuifolia granules: Compared with Example 11, Example 14 differs only in the amount of activated carbon and diatomaceous earth added; all other steps and parameters are the same. In Example 14, the amount of activated carbon added is 0.2% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.1% of the weight of the concentrated ointment.

[0069] Example 15 of a method for removing aflatoxin from Polygala tenuifolia formula granules: Compared with Example 11, Example 15 differs only in the amount of activated carbon and diatomaceous earth added; all other steps and parameters are the same. In Example 15, the amount of activated carbon added is 0.2% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.2% of the weight of the concentrated ointment.

[0070] Example 16 of a method for removing aflatoxin from Polygala tenuifolia granules: Compared with Example 11, Example 16 differs only in the amount of activated carbon and diatomaceous earth added; all other steps and parameters are the same. In Example 16, the amount of activated carbon added is 0.2% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.3% of the weight of the concentrated ointment.

[0071] Example 17 of a method for removing aflatoxin from Polygala tenuifolia granules: Compared with Example 11, Example 17 differs only in the amount of activated carbon and diatomaceous earth added; all other steps and parameters are the same. In Example 17, the amount of activated carbon added is 0.3% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.1% of the weight of the concentrated ointment.

[0072] Example 18: A method for removing aflatoxin from Polygala tenuifolia granules: Compared with Example 11, Example 18 differs only in the amount of activated carbon and diatomaceous earth added; all other steps and parameters are the same. In Example 18, the amount of activated carbon added is 0.3% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.2% of the weight of the concentrated ointment.

[0073] Example 19: A method for removing aflatoxin from Polygala tenuifolia formula granules: Compared with Example 11, Example 19 differs only in the amount of activated carbon and diatomaceous earth added; all other steps and parameters are the same. In Example 19, the amount of activated carbon added is 0.3% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.3% of the weight of the concentrated ointment.

[0074] Comparative Example 2: A method for preparing Polygala tenuifolia formula granules includes: spray-drying a concentrated medicinal paste obtained by extracting and concentrating Polygala tenuifolia raw material or Polygala tenuifolia decoction pieces to obtain a dry paste powder; and dry-pressing the dry paste powder into granules to obtain Polygala tenuifolia formula granules.

[0075] The Polygala tenuifolia formulation granules obtained in Examples 11 to 19 and Comparative Example 2 were tested, and the results are shown in Table 2.

[0076] Table 2 Comparison of results from Examples 11 to 19 and Comparative Example 2 Properties of Polygala tenuifolia granules Content of saponins in Polygala tenuifolia (mg / g) The content of polygalactone III (mg / g) Content of 3,6'-disinyl sucrose (mg / g) Extract% Aflatoxin B1 content (μg / kg) Total content of aflatoxins G2, G1, B2 and B (μg / kg) Comparative Example 2 light yellow 34.04 2.45 11.94 73.1 14.2 28.2 Example 11 Light gray 34.28 2.44 11.78 72.6 2.9 5.8 Example 12 grayish yellow 34.12 2.42 11.66 71.8 2.4 5.4 Example 13 light yellow 33.96 2.40 11.60 72.3 2.3 5.1 Example 14 grey 33.62 2.38 10.82 71.3 1.8 3.8 Example 15 Light gray 33.24 2.35 10.54 71.8 1.4 3.4 Example 16 light yellow 34.05 2.41 10.27 71.2 1.3 3.2 Example 17 gray brown 33.76 2.32 10.38 71.6 0.9 2.1 Example 18 grey 33.53 2.37 10.57 71.4 0.7 1.9 Example 19 grayish yellow 32.12 2.33 10.67 70.8 0.5 1.6 The content of saponins in *Polygala tenuifolia* was determined by high performance liquid chromatography (HPLC) (Chinese Pharmacopoeia 2020 General Chapter 0512). The contents of xanthocarpine III and 3,6'-disinyl sucrose were determined by HPLC (Chinese Pharmacopoeia 2020 General Chapter 0512). The content of extractives was determined by the hot extraction method under the alcohol-soluble extractives determination method (Chinese Pharmacopoeia 2020 General Chapter 2201), using ethanol as the solvent, and the content should not be less than 25.0%. The characteristic chromatogram of *Polygala tenuifolia* granules was determined by HPLC (Chinese Pharmacopoeia 2020 General Chapter 0512). Aflatoxin was determined by the mycotoxin determination method (Chinese Pharmacopoeia 2020 General Chapter 2351). The content of aflatoxin B1, as well as the total content of aflatoxin G2, aflatoxin G1, aflatoxin B2, and aflatoxin B, were also detected.

[0077] As shown in Table 2, Figure 4 and Figure 5 As shown, comparisons revealed that in Examples 11 to 19, aflatoxin levels were significantly reduced, with minimal impact on the content of Polygala tenuifolia saponins, Polygala tenuifolia xanthoside III, 3,6'-disinozinc sucrose, extract content, and characteristic chromatograms of the Polygala tenuifolia formulation granules. In particular, the optimal properties were observed when the added activated carbon was 0.2% and the added diatomaceous earth was 0.3%. Therefore, Example 16 is the optimal embodiment for the aflatoxin removal method of Polygala tenuifolia formulation granules.

[0078] In some optional embodiments of the present invention, the formulation granules are areca nut formulation granules; the concentrated paste is obtained by extraction and concentration of areca nut raw material or areca nut slices. The amount of activated carbon added is 0.2% to 0.3% of the weight of the concentrated paste.

[0079] Example 21 of a method for removing aflatoxin from areca nut granules: A method for removing aflatoxin from areca nut granules includes: S31, Add activated carbon to the concentrated ointment and stir for 2 hours to obtain the stirred mixture; wherein, the amount of activated carbon added is 0.2% of the weight of the concentrated ointment, and the concentrated ointment is obtained by extraction and concentration of areca nut raw material or areca nut slices; S32, add diatomaceous earth to the mixture and stir for 0.5 hours to obtain a mixture; the amount of diatomaceous earth added is 0.1% of the weight of the concentrated ointment; S33, the mixture is filtered sequentially using a sieve and a plate and frame filter; wherein the plate and frame filter includes 40 layers of filter paper; S34, the filtered ointment is spray-dried to obtain a dry ointment powder; S35, dry-press the dry powder into granules to obtain areca nut formula granules.

[0080] Example 22 of a method for removing aflatoxin from areca nut granules: Compared with Example 21, Example 22 differs only in the amount of diatomaceous earth added; all other steps and parameters are the same. In Example 22, the amount of diatomaceous earth added is 0.2% of the weight of the concentrated ointment.

[0081] Example 23 of a method for removing aflatoxin from areca nut granules: Compared with Example 21, Example 23 differs only in the amount of diatomaceous earth added; all other steps and parameters are the same. In Example 23, the amount of diatomaceous earth added is 0.3% of the weight of the concentrated ointment.

[0082] Example 24 of a method for removing aflatoxin from areca nut granules: Compared with Example 21, Example 24 differs only in the amount of activated carbon and diatomaceous earth added; all other steps and parameters are the same. In Example 24, the amount of activated carbon added is 0.3% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.1% of the weight of the concentrated ointment.

[0083] Example 25 of a method for removing aflatoxin from areca nut granules: Compared with Example 21, Example 25 differs only in the amount of activated carbon and diatomaceous earth added; all other steps and parameters are the same. In Example 25, the amount of activated carbon added is 0.3% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.2% of the weight of the concentrated ointment.

[0084] Example 26 of a method for removing aflatoxin from areca nut granules: Compared with Example 21, Example 26 differs only in the amount of activated carbon and diatomaceous earth added; all other steps and parameters are the same. In Example 26, the amount of activated carbon added is 0.3% of the weight of the concentrated ointment; the amount of diatomaceous earth added is 0.3% of the weight of the concentrated ointment.

[0085] Comparative Example 3: A method for preparing areca nut formula granules includes: spray-drying a concentrated medicinal paste obtained by extracting and concentrating areca nut raw material or areca nut slices to obtain a dry paste powder; and dry-pressing the dry paste powder into granules to obtain areca nut formula granules.

[0086] The areca nut formulation granules obtained in Examples 21 to 26 and Comparative Example 3 were tested, and the results are shown in Table 3.

[0087] Table 3 Comparison of results from Examples 21 to 26 and Comparative Example 3 Properties of Areca Nut Formula Granules Arecoline content (mg / g) The total content of norarecoline, arecoline, norarecoline (mg / g) Extract% Aflatoxin B1 content (μg / kg) Total content of aflatoxins G2, G1, B2 and B (μg / kg) Comparative Example 2 Light brownish-red 7.84 44.14 44.8 32.9 42.0 Example 21 Brownish-red 7.72 43.70 43.5 3.9 5.9 Example 22 Light brownish-red 7.70 43.22 42.9 3.8 5.3 Example 23 Light brownish-red 7.76 43.58 43.1 3.1 5.2 Example 24 Brownish-red 7.60 43.65 42.7 1.8 2.7 Example 25 Brownish-red 7.73 43.37 43.4 1.5 2.3 Example 26 Brownish-red 7.77 43.26 42.6 1.2 2.4 The content of arecoline, and the total content of norarecoline, arecoline, norarecoline, and arecoline were determined by high performance liquid chromatography (HPLC) (Chinese Pharmacopoeia 2020 General Chapter 0512). The content of extractives was determined by the hot extraction method under the alcohol-soluble extractives determination method (Chinese Pharmacopoeia 2020 General Chapter 2201), using ethanol as the solvent, and the content was not less than 25.0%. The characteristic chromatogram of areca nut granules was determined by HPLC (Chinese Pharmacopoeia 2020 General Chapter 0512). Aflatoxin was determined by the mycotoxin determination method (Chinese Pharmacopoeia 2020 General Chapter 2351), and the content of aflatoxin B1, as well as the total content of aflatoxin G2, aflatoxin G1, aflatoxin B2, and aflatoxin B, were detected.

[0088] As shown in Table 3, Figure 6 and Figure 7 As shown, through comparison, it was found that in Examples 21 to 26, aflatoxin levels were significantly reduced, and the aflatoxin content, arecoline content, total content of arecoline, arecoline, arecoline, arecoline, and arecoline, extract content, characteristic chromatogram, etc. of the arecoline granules were not significantly affected, and the properties of the arecoline granules were also not significantly affected.

[0089] Therefore, those skilled in the art should recognize that although numerous exemplary embodiments of the present invention have been shown and described in detail herein, many other variations or modifications conforming to the principles of the present invention can be directly determined or derived from the disclosure of the present invention without departing from the spirit and scope of the invention. Thus, the scope of the present invention should be understood and construed as covering all such other variations or modifications.

Claims

1. A method for removing aflatoxin from formulated granules, characterized in that, include: S100, add activated carbon and diatomaceous earth to the concentrated ointment and stir evenly to obtain a mixture; S200, the mixture is filtered to obtain a filtered ointment; S300, the filtered ointment is spray-dried to obtain a dry ointment powder; S400, the dry powder is dry-pressed into granules to obtain the formulation granules.

2. The method for removing aflatoxin from formulated granules according to claim 1, characterized in that, Step S100 specifically includes: S110, add the activated charcoal to the concentrated ointment and stir for a first preset time to obtain a stirred mixture; wherein, the amount of activated charcoal added is 0.1% to 0.3% of the weight of the concentrated ointment, and the first preset time is 1.5 hours to 3 hours; S120, add the diatomaceous earth to the mixture and stir for a second preset time to obtain the mixture; wherein, the second preset time is less than the first preset time, the amount of diatomaceous earth added is 0.1% to 0.3% of the weight of the concentrated ointment, and the second preset time is 0.3 hours to 1 hour.

3. The method for removing aflatoxin from formulated granules according to claim 1, characterized in that, Step S200 specifically includes: filtering the mixture sequentially using a sieve and a plate and frame filter; wherein the plate and frame filter includes multiple layers of filter paper.

4. The method for removing aflatoxin from formulated granules according to claim 1, characterized in that, The formula granules are bitter almond formula granules; The concentrated ointment is obtained by extraction and concentration of raw bitter almond or processed bitter almond slices; The amount of activated carbon added is less than the amount of diatomaceous earth added.

5. The method for removing aflatoxin from formulated granules according to claim 4, characterized in that, The amount of activated carbon added is 0.2% of the weight of the concentrated ointment; The amount of diatomaceous earth added is 0.3% of the weight of the concentrated ointment.

6. The method for removing aflatoxin from formulated granules according to claim 1, characterized in that, The formula granules are Polygala tenuifolia formula granules; The concentrated ointment is obtained by extraction and concentration of raw Polygala tenuifolia medicinal material or Polygala tenuifolia processed slices; The amount of activated carbon added is less than the amount of diatomaceous earth added.

7. The method for removing aflatoxin from formulated granules according to claim 6, characterized in that, The amount of activated carbon added is 0.2% of the weight of the concentrated ointment; The amount of diatomaceous earth added is 0.3% of the weight of the concentrated ointment.

8. The method for removing aflatoxin from formulated granules according to claim 1, characterized in that, The formulated granules are areca nut formulated granules; The concentrated ointment is obtained by extraction and concentration of raw areca nut or areca nut slices; The amount of activated carbon added is 0.2% to 0.3% of the weight of the concentrated ointment.

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