Method for reducing residual heavy metals in pulse-activating particles

Abstract

The invention relates to a method for reducing residual heavy metals in pulse-activating particles. The method comprises the process steps of pretreatment, soaking, washing, adsorption and the like. According to the method, the heavy metal residues of key traditional Chinese medicinal materials including codonopsis pilosula, schisandra chinensis and radix ophiopogonis in the pulse-activating granules are reduced, the removal rate of the heavy metal is 90% or above, the loss rate of effective components is within 2%, the process steps are simple, and the method meets the internal control quality standard of enterprises.

Description

Technical Field

[0001] This invention belongs to the field of traditional Chinese medicine technology, and in particular relates to a method for reducing heavy metal residues in Shengmai granules. Background Technology

[0002] Heavy metal pollution in Chinese medicinal herbs has become a critical issue urgently needing to be addressed in their production. Reports indicate that testing of over 300 commonly used Chinese medicinal herbs nationwide revealed that the heavy metal content of some raw herbs far exceeded the baseline levels set by the World Health Organization and the Food and Agriculture Organization of the United Nations. A survey of 100 types of Chinese medicinal herbs revealed the presence of lead, cadmium, arsenic, mercury, and copper, showing that the vast majority contained some heavy metals, with some exhibiting very high levels. This demonstrates that heavy metal pollution in Chinese medicinal herbs is a serious problem.

[0003] The problem encountered by the company in producing Shengmai granules is as follows: Based on the provisions of the "Green Industry Standard for Foreign Trade of Medicinal Plants and Preparations" (WM / T2-2004), the company has formulated internal control standards for heavy metal residues in Codonopsis pilosula, Schisandra chinensis, and Ophiopogon japonicus in Shengmai granules. To ensure product quality, it is necessary to test for heavy metal residues in Codonopsis pilosula, Schisandra chinensis, and Ophiopogon japonicus. In recent years, the company has found that the heavy metal residues in Codonopsis pilosula, Schisandra chinensis, and Ophiopogon japonicus exceed the standards during the production process. The specific results are shown in the table below.

[0004] Summary of heavy metal residues

[0005] serial number Heavy metal names Standard (≤mg / kg) Maximum metal residue result (mg / kg) Remark 1 Lead (Pb) 5 5.60 2 Cadmium (Cd) 0.3 0.48 3 Arsenic (As) 2 2.15 4 Mercury (Hg) 0.2 0.23 5 Copper (Cu) 20 26.40 6 Total amount of heavy metals 20 34.86

[0006] Currently, the common method for reducing the heavy metal content in Chinese medicinal herbs is...

[0007] (1) Macroporous resin adsorption method. The advantages are that the removal rate of mercury and arsenic in some Chinese medicinal materials is about 60%, with good selectivity, fast adsorption speed and large adsorption capacity; the disadvantages are that the loss rate of effective components in Chinese medicinal materials exceeds 5%, and the adsorption effect is easily affected by the process, requiring high process technology conditions and complicated operation.

[0008] (2) Flocculation method. The advantage is that it can remove about 90% of copper and lead from some Chinese medicinal materials and has a good adsorption effect. However, the adsorption rate of cadmium is relatively small. Moreover, the flocculation method is rarely used in the field of Chinese medicine and no specific process route has been disclosed.

[0009] (3) Supercritical carbon dioxide extraction. The advantages are that the removal rate of copper, lead and arsenic in some Chinese medicinal materials is 55-60%, especially the removal rate of heavy metals in Astragalus membranaceus reaches 85%. It is simple to operate and does not pollute the environment. However, it has certain limitations. It is not easy to select suitable compounding agents and the equipment cost is relatively high.

[0010] (4) Other methods, such as superabsorbent resin method, microbial method, natural zeolite adsorption, ultrasonic method, etc., have many process steps, are complicated to operate, and the loss rate of effective ingredients in Chinese medicinal materials exceeds 5%.

[0011] Therefore, reducing the heavy metal content in traditional Chinese medicine is of utmost urgency. The immediate priority is to adopt effective methods to reduce the heavy metal content in traditional Chinese medicine in order to protect human health and reduce economic losses for enterprises. Summary of the Invention

[0012] The purpose of this invention is to overcome the defects in the prior art and provide a method for reducing heavy metal residues in Codonopsis pilosula, Schisandra chinensis, and Ophiopogon japonicus, with simple process steps and in line with the enterprise's internal quality control standards.

[0013] The technical solution adopted to achieve the above objectives is as follows:

[0014] A method for reducing heavy metal residues in Shengmai granules includes the following steps:

[0015] (1) Preprocessing

[0016] First, the Codonopsis pilosula, Schisandra chinensis and Ophiopogon japonicus in Shengmai Granules are pretreated to remove visible solid impurities;

[0017] Secondly, Codonopsis pilosula, Ophiopogon japonicus, and Schisandra chinensis are mixed and ground into coarse powder;

[0018] (2) Soaking

[0019] Add soaking solution to coarse powder and soak for 100-120 minutes.

[0020] After soaking, solid-liquid separation was performed to obtain liquid ① and coarse powder solid A, respectively.

[0021] (3) Washing

[0022] Add the coarse powder solid to purified water and wash once at room temperature.

[0023] (4) Adsorption

[0024] Add adsorbent to liquid ①, stir for 40-60 minutes, let stand for 120-150 minutes, and then filter to obtain liquid ②;

[0025] (5) Liquid-liquid separation

[0026] Liquid ② was added to an ammonia-ammonium chloride buffer solution, and after phase separation, an upper oil phase and a lower aqueous phase were obtained.

[0027] The oil phase was collected and concentrated under reduced pressure to obtain solid powder B. After being washed with purified water, it was added to the crude solid powder A and mixed.

[0028] (6) Preparation of Shengmai Granules

[0029] The mixed coarse powder solids are used to prepare a paste, granulate, and dry to obtain Shengmai granules.

[0030] In step (1), the mixing ratio is W Codonopsis: W Ophiopogon japonicus: W Schisandra chinensis = 3kg: 2kg: 1kg.

[0031] In step (2), the soaking solution refers to a mixture of butyl acetate, ethanol and purified water, and the mixing ratio is: L butyl acetate: L ethanol: L purified water = 7L: 2L: 1L.

[0032] In step (3), the water washing refers to purified water, and the amount used is W: a mixture of Codonopsis pilosula, Schisandra chinensis, and Ophiopogon japonicus: L of purified water = 1 kg: 15-20 L.

[0033] In step (4), the amount of adsorbent used is:

[0034] Mixture of Codonopsis pilosula, Schisandra chinensis, and Ophiopogon japonicus: Adsorbent = 1 kg : 0.06-0.09 kg.

[0035] In step (4), the adsorbent refers to:

[0036] S1: Weigh polyacrylamide and place it in an enamel-lined reactor. Add isopropyl acetate, start stirring, and after it is fully dissolved, add 4-chloromethylstyrene and 2-tert-butylhydroquinone. Continue stirring, raise the temperature to 55-60℃, and stir the reaction for 300-360 min. After the reaction is complete, concentrate under reduced pressure to remove isopropyl acetate. Wash the solid product once with chloroform, and dry it at 59-61℃ for 60-80 min to obtain a dry solid product.

[0037] Raw material ratio:

[0038] W:L isopropyl acetate = 1kg:8-10L;

[0039] Wpolyacrylamide: W4-chloromethylstyrene = 1 kg : 2.1-2.2 kg

[0040] Wpolyacrylamide: W2-tert-butylhydroquinone = 1 kg : 0.02-0.04 kg

[0041] W:L chloroform = 1kg:4-6L;

[0042] S2: Add isopropyl acetate to the solid product obtained in step S1, stir to dissolve, then add azobisisobutyronitrile, and react under nitrogen protection at 50-60℃ for 10-12 h. After the reaction is complete, concentrate under reduced pressure to remove isopropyl acetate, wash the solid product once with chloroform, and dry at 59-61℃ for 60-80 min to obtain the dry adsorbent;

[0043] Raw material ratio:

[0044] W:L isopropyl acetate = 1kg:8-10L;

[0045] Wpolyacrylamide: Wazobisisobutyronitrile = 1kg: 0.05-0.08kg;

[0046] W:L chloroform = 1kg:4-6L.

[0047] In step (5), the amount of ammonia-ammonium chloride buffer solution used is: L butyl acetate : L ammonia-ammonium chloride buffer solution = 1L : 2-4L.

[0048] In step (5), the amount of purified water used is: W solid powder: L purified water = 1 kg: 4-8 L.

[0049] Technical effects achieved:

[0050] The removal rate of heavy metals lead, cadmium, arsenic, mercury and copper in Shengmai granules exceeded 90%, and the total amount of heavy metals was ≤10mg / kg.

[0051] See the table below for details.

[0052] Summary of heavy metal residues

[0053]

[0054] The loss rate of effective components of the three key Chinese medicinal herbs, namely Codonopsis pilosula, Schisandra chinensis, and Ophiopogon japonicus, in Shengmai Granules is ≤2%.

[0055] The loss of active ingredients is shown in the table below.

[0056] Summary table of effective components of Chinese medicinal herbs

[0057] Detailed Implementation

[0058] The invention is illustrated below with examples. It should be understood that these examples are for illustrative purposes only and not for limiting the invention. The scope and core content of the invention are defined by the claims.

[0059] Heavy metal detection method: derived from "2321 Determination of Lead, Cadmium, Arsenic, Mercury and Copper" in the General Chapter of Part IV of the 2020 Chinese Pharmacopoeia.

[0060] Method for detecting total saponin content in Codonopsis pilosula: derived from the journal "Determination of Total Saponin Content in Codonopsis pilosula from Different Origin Areas in Gansu".

[0061] Method for detecting protocatechuic acid content in Schisandra chinensis: derived from the journal "Determination and Comparison of Protocatechuic Acid Content in Schisandra chinensis Medicinal Materials from the South and North".

[0062] The method for detecting ophiopogonin D content in Ophiopogon japonicus: derived from the journal "Comparative Study of HPLC Fingerprints of Ophiopogon japonicus and Ophiopogon japonicus".

[0063] Example 1

[0064] Weigh out 60kg of Codonopsis pilosula, 40kg of Ophiopogon japonicus, and 20kg of Schisandra chinensis, for a total of 100kg.

[0065] The results of the active ingredient analysis are shown in the table below.

[0066] Summary table of effective components of Chinese medicinal herbs

[0067] Serial Number Product Name Active ingredients Content (mg / g) Remark 1 Codonopsis pilosula Total saponins 46.2 2 Schisandra chinensis Protocatechuic acid 11.8 3 Ophiopogon japonicus Ophiopogon saponin D 25.4

[0068] The results of heavy metal content testing after mixing are shown in the table below.

[0069] Summary of heavy metal residues

[0070] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Remark 1 Lead (Pb) 5 5.54 2 Cadmium (Cd) 0.3 0.45 3 Arsenic (As) 2 2.13 4 Mercury (Hg) 0.2 0.22 5 Copper (Cu) 20 25.9 6 Total amount of heavy metals 20 34.24

[0071] (1) Preprocessing

[0072] First, the Codonopsis pilosula, Schisandra chinensis and Ophiopogon japonicus in Shengmai Granules are pretreated to remove visible solid impurities;

[0073] Secondly, Codonopsis pilosula, Ophiopogon japonicus, and Schisandra chinensis are mixed and ground into coarse powder;

[0074] (2) Soaking

[0075] 1000L of soaking solution was added to the coarse powder, and the soaking time was controlled at 100min. After soaking, solid-liquid separation was performed to obtain 998L of liquid ① and coarse powder solid A.

[0076] (3) Washing

[0077] Add the coarse powder solid to 1500L of purified water and wash once at room temperature;

[0078] (4) Adsorption

[0079] Add 60g of adsorbent to liquid ①, stir for 40min, let stand for 120min, and then filter to obtain liquid ②;

[0080] (5) Liquid-liquid separation

[0081] Liquid ② was added to 1400L of ammonia-ammonium chloride buffer solution, and after phase separation, an upper oil phase and a lower aqueous phase were obtained.

[0082] The oil phase was collected and concentrated under reduced pressure to obtain 12.4 kg of solid powder B. After washing with 49.6 L of purified water, the powder was added to the coarse solid powder A and mixed.

[0083] (6) Preparation of Shengmai Granules

[0084] The mixed coarse powder solids are used to prepare a paste, granulate, and dry to obtain Shengmai granules.

[0085] The results of testing on the heavy metal content and effective components in the mixed coarse powder solid are shown in the table below.

[0086] Summary of heavy metal residues

[0087] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Removal rate (%) Remark 1 Lead (Pb) 5 0.54 90.2 2 Cadmium (Cd) 0.3 0.04 90.4 3 Arsenic (As) 2 0.21 90.1 4 Mercury (Hg) 0.2 0.02 90.3 5 Copper (Cu) 20 2.41 90.7 6 Total amount of heavy metals 20 3.22 90.6

[0088] Summary table of effective components of Chinese medicinal herbs

[0089]

[0090] The data results show that the removal rate of heavy metals exceeded 90%, and the loss rate of effective ingredients was less than 2%.

[0091] Example 2

[0092] Weigh out 60kg of Codonopsis pilosula, 40kg of Ophiopogon japonicus, and 20kg of Schisandra chinensis, for a total of 100kg.

[0093] The results of the active ingredient analysis are shown in the table below.

[0094] Summary table of effective components of Chinese medicinal herbs

[0095] Serial Number Product Name Active ingredients Content (mg / g) Remark 1 Codonopsis pilosula Total saponins 51.2 2 Schisandra chinensis Protocatechuic acid 10.3 3 Ophiopogon japonicus Ophiopogon saponin D 19.7

[0096] The results of heavy metal content testing after mixing are shown in the table below.

[0097] Summary of heavy metal residues

[0098] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Remark 1 Lead (Pb) 5 5.47 2 Cadmium (Cd) 0.3 0.42 3 Arsenic (As) 2 2.14 4 Mercury (Hg) 0.2 0.21 5 Copper (Cu) 20 24.6 6 Total amount of heavy metals 20 32.84

[0099] (1) Preprocessing

[0100] First, the Codonopsis pilosula, Schisandra chinensis and Ophiopogon japonicus in Shengmai Granules are pretreated to remove visible solid impurities;

[0101] Secondly, Codonopsis pilosula, Ophiopogon japonicus, and Schisandra chinensis are mixed and ground into coarse powder;

[0102] (2) Soaking

[0103] 1100L of soaking solution was added to the coarse powder, and the soaking time was controlled at 105min. After soaking, solid-liquid separation was performed to obtain 1098L of liquid ① and coarse powder solid A.

[0104] (3) Washing

[0105] Add the coarse powder solid to 1600L of purified water and wash once at room temperature;

[0106] (4) Adsorption

[0107] Add 70g of adsorbent to liquid ①, stir for 45min, let stand for 130min, and then filter to obtain liquid ②;

[0108] (5) Liquid-liquid separation

[0109] Liquid ② was added to 1925 L of ammonia-ammonium chloride buffer solution, and after phase separation, an upper oil phase and a lower aqueous phase were obtained.

[0110] The oil phase was collected and concentrated under reduced pressure to obtain 16.7 kg of solid powder B. After washing with 83.5 L of purified water, the powder was added to the coarse solid powder A and mixed.

[0111] (6) Preparation of Shengmai Granules

[0112] The mixed coarse powder solids are used to prepare a paste, granulate, and dry to obtain Shengmai granules.

[0113] The results of testing on the heavy metal content and effective components in the mixed coarse powder solid are shown in the table below.

[0114] Summary of heavy metal residues

[0115] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Removal rate (%) Remark 1 Lead (Pb) 5 0.52 90.5 2 Cadmium (Cd) 0.3 0.04 90.7 3 Arsenic (As) 2 0.20 90.6 4 Mercury (Hg) 0.2 0.02 90.5 5 Copper (Cu) 20 2.21 91.0 6 Total amount of heavy metals 20 2.99 90.9

[0116] Summary table of effective components of Chinese medicinal herbs

[0117]

[0118] The data results show that the removal rate of heavy metals exceeded 90%, and the loss rate of effective ingredients was less than 2%.

[0119] Example 3

[0120] Weigh out 60kg of Codonopsis pilosula, 40kg of Ophiopogon japonicus, and 20kg of Schisandra chinensis, for a total of 100kg.

[0121] The results of the active ingredient analysis are shown in the table below.

[0122] Summary table of effective components of Chinese medicinal herbs

[0123] Serial Number Product Name Active ingredients Content (mg / g) Remark 1 Codonopsis pilosula Total saponins 62.3 2 Schisandra chinensis Protocatechuic acid 15.1 3 Ophiopogon japonicus Ophiopogon saponin D 14.7

[0124] The results of heavy metal content testing after mixing are shown in the table below.

[0125] Summary of heavy metal residues

[0126] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Remark 1 Lead (Pb) 5 5.48 2 Cadmium (Cd) 0.3 0.40 3 Arsenic (As) 2 2.09 4 Mercury (Hg) 0.2 0.21 5 Copper (Cu) 20 23.5 6 Total amount of heavy metals 20 31.68

[0127] (1) Preprocessing

[0128] First, the Codonopsis pilosula, Schisandra chinensis and Ophiopogon japonicus in Shengmai Granules are pretreated to remove visible solid impurities;

[0129] Secondly, Codonopsis pilosula, Ophiopogon japonicus, and Schisandra chinensis are mixed and ground into coarse powder;

[0130] (2) Soaking

[0131] 1300L of soaking solution was added to the coarse powder, and the soaking time was controlled at 110min. After soaking, solid-liquid separation was performed to obtain 1297L of liquid ① and coarse powder solid A.

[0132] (3) Washing

[0133] Add the coarse powder solid to 1800L of purified water and wash once with water at room temperature;

[0134] (4) Adsorption

[0135] Add 75g of adsorbent to liquid ①, stir for 50min, let stand for 135min, and then filter to obtain liquid ②;

[0136] (5) Liquid-liquid separation

[0137] Liquid ② was added to 2730L of ammonia-ammonium chloride buffer solution, and after phase separation, an upper oil phase and a lower aqueous phase were obtained.

[0138] The oil phase was collected and concentrated under reduced pressure to obtain 18.2 kg of solid powder B. After washing with 109 L of purified water, the powder was added to the coarse solid powder A and mixed.

[0139] (6) Preparation of Shengmai Granules

[0140] The mixed coarse powder solids are used to prepare a paste, granulate, and dry to obtain Shengmai granules.

[0141] The results of testing on the heavy metal content and effective components in the mixed coarse powder solid are shown in the table below.

[0142] Summary of heavy metal residues

[0143] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Removal rate (%) Remark 1 Lead (Pb) 5 0.50 90.9 2 Cadmium (Cd) 0.3 0.03 91.1 3 Arsenic (As) 2 0.19 90.8 4 Mercury (Hg) 0.2 0.02 90.7 5 Copper (Cu) 20 2.04 91.3 6 Total amount of heavy metals 20 2.78 91.2

[0144] Summary table of effective components of Chinese medicinal herbs

[0145]

[0146] The data results show that the removal rate of heavy metals exceeded 90%, and the loss rate of effective ingredients was less than 2%.

[0147] Example 4

[0148] Weigh out 60kg of Codonopsis pilosula, 40kg of Ophiopogon japonicus, and 20kg of Schisandra chinensis, for a total of 100kg.

[0149] The results of the active ingredient analysis are shown in the table below.

[0150] Summary table of effective components of Chinese medicinal herbs

[0151] Serial Number Product Name Active ingredients Content (mg / g) Remark 1 Codonopsis pilosula Total saponins 55.1 2 Schisandra chinensis Protocatechuic acid 18.4 3 Ophiopogon japonicus Ophiopogon saponin D 10.6

[0152] The results of heavy metal content testing after mixing are shown in the table below.

[0153] Summary of heavy metal residues

[0154] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Remark 1 Lead (Pb) 5 5.41 2 Cadmium (Cd) 0.3 0.44 3 Arsenic (As) 2 2.09 4 Mercury (Hg) 0.2 0.21 5 Copper (Cu) 20 24.33 6 Total amount of heavy metals 20 32.48

[0155] (1) Preprocessing

[0156] First, the Codonopsis pilosula, Schisandra chinensis and Ophiopogon japonicus in Shengmai Granules are pretreated to remove visible solid impurities;

[0157] Secondly, Codonopsis pilosula, Ophiopogon japonicus, and Schisandra chinensis are mixed and ground into coarse powder;

[0158] (2) Soaking

[0159] 1400L of soaking solution was added to the coarse powder, and the soaking time was controlled at 115min. After soaking, solid-liquid separation was performed to obtain 1398L of liquid ① and coarse powder solid A.

[0160] (3) Washing

[0161] Add the coarse powder solid to 1900L of purified water and wash once with water at room temperature;

[0162] (4) Adsorption

[0163] Add 80g of adsorbent to liquid ①, stir for 55min, let stand for 140min, and then filter to obtain liquid ②;

[0164] (5) Liquid-liquid separation

[0165] Liquid ② was added to 3990L of ammonia-ammonium chloride buffer solution, and after phase separation, an upper oil phase and a lower aqueous phase were obtained.

[0166] The oil phase was collected and concentrated under reduced pressure to obtain 19.5 kg of solid powder B. After washing with 136 L of purified water, the powder was added to the coarse solid powder A and mixed.

[0167] (6) Preparation of Shengmai Granules

[0168] The mixed coarse powder solids are used to prepare a paste, granulate, and dry to obtain Shengmai granules.

[0169] The results of testing on the heavy metal content and effective components in the mixed coarse powder solid are shown in the table below.

[0170] Summary of heavy metal residues

[0171] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Removal rate (%) Remark 1 Lead (Pb) 5 0.50 90.7 2 Cadmium (Cd) 0.3 0.04 91.0 3 Arsenic (As) 2 0.20 90.6 4 Mercury (Hg) 0.2 0.02 90.5 5 Copper (Cu) 20 2.14 91.2 6 Total amount of heavy metals 20 2.90 91.1

[0172] Summary table of effective components of Chinese medicinal herbs

[0173]

[0174] The data results show that the removal rate of heavy metals exceeded 90%, and the loss rate of effective ingredients was less than 2%.

[0175] Example 5

[0176] Weigh out 60kg of Codonopsis pilosula, 40kg of Ophiopogon japonicus, and 20kg of Schisandra chinensis, for a total of 100kg.

[0177] The results of the active ingredient analysis are shown in the table below.

[0178] Summary table of effective components of Chinese medicinal herbs

[0179] Serial Number Product Name Active ingredients Content (mg / g) Remark 1 Codonopsis pilosula Total saponins 41.3 2 Schisandra chinensis Protocatechuic acid 11.2 3 Ophiopogon japonicus Ophiopogon saponin D 10.5

[0180] The results of heavy metal content testing after mixing are shown in the table below.

[0181] Summary of heavy metal residues

[0182] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Remark 1 Lead (Pb) 5 5.38 2 Cadmium (Cd) 0.3 0.43 3 Arsenic (As) 2 2.10 4 Mercury (Hg) 0.2 0.21 5 Copper (Cu) 20 23.76 6 Total amount of heavy metals 20 31.88

[0183] (1) Preprocessing

[0184] First, the Codonopsis pilosula, Schisandra chinensis and Ophiopogon japonicus in Shengmai Granules are pretreated to remove visible solid impurities;

[0185] Secondly, Codonopsis pilosula, Ophiopogon japonicus, and Schisandra chinensis are mixed and ground into coarse powder;

[0186] (2) Soaking

[0187] 1500L of soaking solution was added to the coarse powder, and the soaking time was controlled at 120min. After soaking, solid-liquid separation was performed to obtain 1498L of liquid ① and coarse powder solid A.

[0188] (3) Washing

[0189] Add the coarse powder solid to 2000L of purified water and wash once at room temperature;

[0190] (4) Adsorption

[0191] Add 90g of adsorbent to liquid ①, stir for 60min, let stand for 150min, and then filter to obtain liquid ②;

[0192] (5) Liquid-liquid separation

[0193] Liquid ② was added to 4200L of ammonia-ammonium chloride buffer solution, and after phase separation, an upper oil phase and a lower aqueous phase were obtained.

[0194] The oil phase was collected and concentrated under reduced pressure to obtain 19.9 kg of solid powder B. After washing with 159 L of purified water, the powder was added to the coarse solid powder A and mixed.

[0195] (6) Preparation of Shengmai Granules

[0196] The mixed coarse powder solids are used to prepare a paste, granulate, and dry to obtain Shengmai granules.

[0197] The results of testing on the heavy metal content and effective components in the mixed coarse powder solid are shown in the table below.

[0198] Summary of heavy metal residues

[0199] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Removal rate (%) Remark 1 Lead (Pb) 5 0.49 90.8 2 Cadmium (Cd) 0.3 0.04 90.9 3 Arsenic (As) 2 0.20 90.6 4 Mercury (Hg) 0.2 0.02 90.7 5 Copper (Cu) 20 2.14 91.0 6 Total amount of heavy metals 20 2.89 90.9

[0200] Summary table of effective components of Chinese medicinal herbs

[0201]

[0202] The data results show that the removal rate of heavy metals exceeded 90%, and the loss rate of effective ingredients was less than 2%.

[0203] Example 6

[0204] Weigh out 60kg of Codonopsis pilosula, 40kg of Ophiopogon japonicus, and 20kg of Schisandra chinensis, for a total of 100kg.

[0205] The results of the active ingredient analysis are shown in the table below.

[0206] Summary table of effective components of Chinese medicinal herbs

[0207] Serial Number Product Name Active ingredients Content (mg / g) Remark 1 Codonopsis pilosula Total saponins 32.9 2 Schisandra chinensis Protocatechuic acid 14.1 3 Ophiopogon japonicus Ophiopogon saponin D 11.8

[0208] The results of heavy metal content testing after mixing are shown in the table below.

[0209] Summary of heavy metal residues

[0210] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Remark 1 Lead (Pb) 5 5.22 2 Cadmium (Cd) 0.3 0.39 3 Arsenic (As) 2 2.18 4 Mercury (Hg) 0.2 0.22 5 Copper (Cu) 20 24.73 6 Total amount of heavy metals 20 32.74

[0211] (1) Preprocessing

[0212] First, the Codonopsis pilosula, Schisandra chinensis and Ophiopogon japonicus in Shengmai Granules are pretreated to remove visible solid impurities;

[0213] Secondly, Codonopsis pilosula, Ophiopogon japonicus, and Schisandra chinensis are mixed and ground into coarse powder;

[0214] (2) Soaking

[0215] 1200L of soaking solution was added to the coarse powder, and the soaking time was controlled at 103min. After soaking, solid-liquid separation was performed to obtain 1198L of liquid ① and coarse powder solid A.

[0216] (3) Washing

[0217] Add the coarse powder solid to 1950L of purified water and wash once with water at room temperature;

[0218] (4) Adsorption

[0219] Add 68g of adsorbent to liquid ①, stir for 57min, let stand for 122min, and then filter to obtain liquid ②;

[0220] (5) Liquid-liquid separation

[0221] Liquid ② was added to 3000L of ammonia-ammonium chloride buffer solution, and after phase separation, an upper oil phase and a lower aqueous phase were obtained;

[0222] The oil phase was collected and concentrated under reduced pressure to obtain 17.1 kg of solid powder B. After washing with 70 L of purified water, the powder was added to the coarse solid powder A and mixed.

[0223] (6) Preparation of Shengmai Granules

[0224] The mixed coarse powder solids are used to prepare a paste, granulate, and dry to obtain Shengmai granules.

[0225] The results of testing on the heavy metal content and effective components in the mixed coarse powder solid are shown in the table below.

[0226] Summary of heavy metal residues

[0227] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Removal rate (%) Remark 1 Lead (Pb) 5 0.50 90.4 5.22 2 Cadmium (Cd) 0.3 0.04 90.2 0.39 3 Arsenic (As) 2 0.21 90.3 2.18 4 Mercury (Hg) 0.2 0.02 90.2 0.22 5 Copper (Cu) 20 2.35 90.5 24.73 6 Total amount of heavy metals 20 3.12 90.5 32.74

[0228] Summary table of effective components of Chinese medicinal herbs

[0229]

[0230] The data results show that the removal rate of heavy metals exceeded 90%, and the loss rate of effective ingredients was less than 2%.

[0231] Comparative Example 1 (Macroporous Resin Adsorption Method)

[0232] Weigh out 60kg of Codonopsis pilosula, 40kg of Ophiopogon japonicus, and 20kg of Schisandra chinensis, for a total of 100kg.

[0233] The results of the active ingredient analysis are shown in the table below.

[0234] Summary table of effective components of Chinese medicinal herbs

[0235] Serial Number Product Name Active ingredients Content (mg / g) Remark 1 Codonopsis pilosula Total saponins 43.7 2 Schisandra chinensis Protocatechuic acid 12.5 3 Ophiopogon japonicus Ophiopogon saponin D 11.1

[0236] The results of heavy metal content testing after mixing are shown in the table below.

[0237] Summary of heavy metal residues

[0238] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Remark 1 Lead (Pb) 5 5.15 2 Cadmium (Cd) 0.3 0.41 3 Arsenic (As) 2 2.17 4 Mercury (Hg) 0.2 0.21 5 Copper (Cu) 20 25.22 6 Total amount of heavy metals 20 33.16

[0239] (1) Preprocessing

[0240] First, the Codonopsis pilosula, Schisandra chinensis and Ophiopogon japonicus in Shengmai Granules are pretreated to remove visible solid impurities;

[0241] Secondly, Codonopsis pilosula, Ophiopogon japonicus, and Schisandra chinensis are mixed and ground into coarse powder;

[0242] (2) Soaking

[0243] Add 2000L of solvent at a material (kg): solvent (L) ratio of 1:20, soak at 50℃, and then filter to obtain solid Chinese medicinal materials and liquid. Concentrate the liquid under low temperature vacuum conditions to obtain a concentrated extract (20% of the original solution volume) in 90% ethanol solution.

[0244] (3) Washing

[0245] Add 1500L of purified water to the solid Chinese medicinal materials and wash them once.

[0246] (4) Resin pretreatment

[0247] The adsorption resin D401 needs to be pretreated. The pretreatment process is to soak the resin in distilled water, 2% sodium hydroxide and 2% hydrochloric acid for 40, 3 and 5 hours respectively, wash it with water until it is neutral, wash it with anhydrous ethanol until the effluent does not turn white and cloudy when water is added, and finally wash it with distilled water until there is no alcohol in the effluent.

[0248] (5) Adsorption

[0249] The S-8 adsorption resin was packed into a chromatography column, and the extract concentrate was continuously passed through the chromatography column at a certain flow rate. Then, it was eluted with 90% ethanol, the eluent was collected, and mixed with the chromatography solvent.

[0250] (6) Vacuum concentration and spray drying

[0251] The mixed chromatography solution was concentrated under reduced pressure and spray-dried to obtain a solid powder, which was then mixed with solid Chinese medicinal materials. The results of testing showed the heavy metal content and loss of active ingredients, as shown in the table below.

[0252] Summary of heavy metal residues

[0253] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Removal rate (%) Remark 1 Lead (Pb) 5 4.57 11.3 2 Cadmium (Cd) 0.3 0.34 16.4 3 Arsenic (As) 2 0.66 69.7 4 Mercury (Hg) 0.2 0.08 63.4 5 Copper (Cu) 20 19.49 22.7 6 Total amount of heavy metals 20 25.14 24.18

[0254] Summary table of effective components of Chinese medicinal herbs

[0255]

[0256] Data results show that the removal rate of heavy metals by resin adsorption is significantly lower than the technical level described in this patent, and the loss rate of effective components is over 8%.

[0257] Comparative Example 2 (Flocculation Method)

[0258] Weigh out 60kg of Codonopsis pilosula, 40kg of Ophiopogon japonicus, and 20kg of Schisandra chinensis, for a total of 100kg.

[0259] The results of the active ingredient analysis are shown in the table below.

[0260] Summary table of effective components of Chinese medicinal herbs

[0261] Serial Number Product Name Active ingredients Content (mg / g) Remark 1 Codonopsis pilosula Total saponins 38.4 2 Schisandra chinensis Protocatechuic acid 11.3 3 Ophiopogon japonicus Ophiopogon saponin D 10.7

[0262] The results of heavy metal content testing after mixing are shown in the table below.

[0263] Summary of heavy metal residues

[0264] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Remark 1 Lead (Pb) 5 5.54 2 Cadmium (Cd) 0.3 0.45 3 Arsenic (As) 2 2.07 4 Mercury (Hg) 0.2 0.22 5 Copper (Cu) 20 24.8 6 Total amount of heavy metals 20 33.08

[0265] (1) Preprocessing

[0266] First, the Codonopsis pilosula, Schisandra chinensis and Ophiopogon japonicus in Shengmai Granules are pretreated to remove visible solid impurities;

[0267] Secondly, Codonopsis pilosula, Ophiopogon japonicus, and Schisandra chinensis are mixed and ground into coarse powder;

[0268] (2) Extraction

[0269] Add 2300L of purified water at a ratio of material (kg): purified water (L) = 1:23, soak at 50℃, and then filter to obtain solid Chinese medicinal materials and solution.

[0270] (3) Flocculation

[0271] Add 0.82 kg of chitosan flocculant to the solution, stir for 60 min, and then filter to obtain a small amount of solid and solution. (4)

[0273] The solution was spray-dried to obtain a solid powder, which was then mixed with solid Chinese medicinal materials. The results of testing showed the heavy metal content and loss of active ingredients, as shown in the table below.

[0274] Summary of heavy metal residues

[0275] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Removal rate (%) Remark 1 Lead (Pb) 5 0.88 84.1 2 Cadmium (Cd) 0.3 0.09 79.2 3 Arsenic (As) 2 1.75 15.3 4 Mercury (Hg) 0.2 0.19 12.4 5 Copper (Cu) 20 2.25 90.9 6 Total amount of heavy metals 20 5.16 84.4

[0276] Summary table of effective components of Chinese medicinal herbs

[0277]

[0278] Data results show that the removal rate of heavy metals by flocculation adsorption is significantly lower than the technical level described in this patent, and the loss rate of effective components is over 6%.

[0279] Comparative Example 3 (Supercritical Extraction)

[0280] Weigh out 6 kg of Codonopsis pilosula, 4 kg of Ophiopogon japonicus, and 2 kg of Schisandra chinensis, for a total of 10 kg.

[0281] The results of the active ingredient analysis are shown in the table below.

[0282] Summary table of effective components of Chinese medicinal herbs

[0283] Serial Number Product Name Active ingredients Content (mg / g) Remark 1 Codonopsis pilosula Total saponins 32.5 2 Schisandra chinensis Protocatechuic acid 12.9 3 Ophiopogon japonicus Ophiopogon saponin D 9.8

[0284] The results of heavy metal content testing after mixing are shown in the table below.

[0285] Summary of heavy metal residues

[0286] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Remark 1 Lead (Pb) 5 5.34 2 Cadmium (Cd) 0.3 0.39 3 Arsenic (As) 2 2.05 4 Mercury (Hg) 0.2 0.21 5 Copper (Cu) 20 25.0 6 Total amount of heavy metals 20 32.99

[0287] (1) Preprocessing

[0288] First, the Codonopsis pilosula, Schisandra chinensis, and Ophiopogon japonicus in Shengmai Granules are pretreated to remove visible solid impurities; second, the Codonopsis pilosula, Ophiopogon japonicus, and Schisandra chinensis are mixed and pulverized into coarse powder.

[0289] (2) Supercritical extraction

[0290] The process described in the journal "Removal of Heavy Metals from Traditional Chinese Medicine Preparations by Supercritical CO2 Complex Extraction" was adopted. The results of testing, including the heavy metal content and loss of active ingredients, are shown in the table below.

[0291] Summary of heavy metal residues

[0292] serial number Heavy metal names Standard (≤mg / kg) Heavy metal residue results (mg / kg) Removal rate (%) Remark 1 Lead (Pb) 5 2.82 47.2 2 Cadmium (Cd) 0.3 0.34 13.4 3 Arsenic (As) 2 1.24 39.4 4 Mercury (Hg) 0.2 0.15 27.5 5 Copper (Cu) 20 12.58 49.7 6 Total amount of heavy metals 20 17.13 48.1

[0293] Summary table of effective components of Chinese medicinal herbs

[0294]

[0295] Data results show that the removal rate of supercritical fluid extraction is significantly lower than the technical level described in this patent, with a loss rate of about 6% of the effective components.

Claims

1. A method for reducing heavy metal residues in Shengmai granules, comprising the following steps: (1) Pretreatment Firstly, pre-treat the radix codonopsis, schisandra chinensis and ophiopogon japonicus in Shengmai granules to remove visible solid impurities, Secondly, mix and crush the radix codonopsis, ophiopogon japonicus and schisandra chinensis into coarse powder; (2) Soaking Add soaking liquid to the coarse powder, and control the time to be 100-120 min, After soaking, perform solid-liquid separation to obtain liquid ① and coarse powder solid A respectively; (3) Water washing Add purified water to the coarse powder solid, and perform water washing once at room temperature; (4) Adsorption Add adsorbent to the liquid ①, stir for 40-60 min, stand for 120-150 min, and then filter to obtain liquid ②; (5) Liquid-liquid separation Add ammonia chloride buffer solution to the liquid ②, and after phase separation, obtain upper oil phase and lower water phase, Collect the oil phase to perform vacuum concentration to obtain solid powder B, wash with purified water, and then add to the coarse powder solid and mix; (6) Preparation of Shengmai granules Prepare clear paste, granulation and drying from the mixed coarse powder solid to obtain Shengmai granules.

2. The method for reducing heavy metal residues in Shengpi granules according to claim 1, characterized in that In step (1), the mixing ratio is W radix codonopsis: W ophiopogon japonicus: W schisandra chinensis = 3 kg: 2 kg: 1 kg.

3. The method for reducing heavy metal residues in Shengpi granules according to claim 1, characterized in that In step (2), the soaking liquid refers to a mixture of butyl acetate, ethanol and purified water, and the mixing ratio is: L butyl acetate: L ethanol: L purified water = 7 L: 2 L: 1 L; the amount of soaking liquid is: W coarse powder: L soaking liquid = 1 kg: 10-15 L.

4. The method for reducing heavy metal residues in Shengpi granules according to claim 1, characterized in that In step (3), the water washing refers to purified water, and the amount is W radix codonopsis, schisandra chinensis and ophiopogon japonicus mixture: L purified water = 1 kg: 15-20 L.

5. The method for reducing heavy metal residues in Shengpi granules according to claim 1, characterized in that In step (4), the amount of adsorbent is: W radix codonopsis, schisandra chinensis and ophiopogon japonicus mixture: W adsorbent = 1 kg: 0.06-0.09 kg.

6. The method for reducing heavy metal residues in Shengpi granules according to claim 1, characterized in that In step (4), the adsorbent refers to: S1: weigh polyacrylamide into a porcelain reaction kettle, add isopropyl acetate, start stirring, add 4-chloromethylstyrene and 2-tert-butyl hydroquinone after fully dissolving, continue stirring, heat to 55-60℃, and stir for 300-360 min. After the reaction is completed, remove isopropyl acetate by vacuum concentration, wash the solid product with chloroform once, and dry at 59-61℃ for 60-80 min to obtain dry solid product; S2: continue to add isopropyl acetate to the solid product obtained in step S1, stir and dissolve, then add azobisisheptyl nitrile, protect with nitrogen, and react at 50-60℃ for 10-12 h. After the reaction is completed, remove isopropyl acetate by vacuum concentration, wash the solid product with chloroform once, and dry at 59-61℃ for 60-80 min to obtain dry adsorbent.

7. The method for reducing heavy metal residues in Shengpi granules according to claim 6, characterized in that In step S1, the raw material ratio is: W polyacrylamide: L isopropyl acetate = 1 kg: 8-10 L, W polyacrylamide: W 4-chloromethylstyrene = 1 kg: 2.1-2.2 kg, W polyacrylamide: W 2-tert-butyl hydroquinone = 1 kg: 0.02-0.04 kg, W polyacrylamide: L chloroform = 1 kg: 4-6 L.

8. The method for reducing heavy metal residues in Shengpi granules according to claim 6, characterized in that In step S2, the raw material ratio is: W polyacrylamide: L isopropyl acetate = 1 kg: 8-10 L, W polyacrylamide: W azobis diisopropyl cyanide = 1 kg: 0.05-0.08 kg, W polyacrylamide: L chloroform = 1 kg: 4-6 L.

9. The method for reducing heavy metal residues in Shengpi granules according to claim 1, characterized in that In step (5), the amount of the ammonia water-ammonium chloride buffer solution is: L butyl acetate: L ammonia water-ammonium chloride buffer solution = 1 L: 2-4 L.

10. The method for reducing heavy metal residues in Shengpi granules according to claim 1, characterized in that In step (5), the amount of the purified water is: W solid powder B: L purified water = 1 kg: 4-8 L.

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