Quality evaluation method for determining optimal processing technological parameters of bran-stewed ginger

Abstract

The invention discloses a quality evaluation method for determining optimal processing technological parameters of bran-stewed ginger, and belongs to the technical field of traditional Chinese medicine processing and quality control. According to the Box-Behnken central combination design principle, the simmering temperature, the simmering time and the dosage ratio of wheat bran to medicinal materials are selected as three influence factors. Putting ginger slices and wheat bran into a pot according to a certain proportion, heating with slow fire, burying and properly turning until the whole wheat bran is brown, screening out the wheat bran, and cooling to obtain stewed ginger; respectively measuring the contents of 6, 7, 8-gingerol and total gingerol as evaluation indexes, and carrying out a response surface test on the bran-stewed ginger. And carrying out model fitting and variance analysis on the comprehensive scoring result to obtain the optimal processing technological parameters of the wheat bran stewed ginger. According to the invention, the limitations of difficulty in controlling the processing degree, tedious operation and the like of the traditional processing of paper simmering, flour simmering and the like are improved, the simmered products with uniform appearance and color are prepared, and the processing purposes of slow cooking and dryness reduction are realized.

Description

Technical Field

[0001] The present invention belongs to the technical field of traditional Chinese medicine processing and quality control, and specifically relates to a quality evaluation method for establishing the best processing technological parameters of bran-roasted ginger. Background Art

[0002] Ginger is the fresh rhizome of the plant Zingiber officinale Roscoe of the Zingiberaceae family. As a dual-purpose medicine and food, it has a pungent taste and a slightly warm nature, and has the effects of relieving exterior syndrome and dispelling cold, warming the middle-jiao to arrest vomiting, resolving phlegm and relieving cough, and detoxifying fish and crabs. Clinically, it is necessary to select appropriate processed products according to different diseases and patient constitutions. The processed varieties of ginger mainly include dried ginger, stir-fried ginger, roasted ginger, and carbonized ginger, etc., each of which has different medicinal values and application scopes.

[0003] Roasted ginger is one of the processed products of ginger. After roasting, it enhances the effect of warming the middle-jiao to arrest vomiting, and alleviates the pungent and dry nature of ginger. It is applicable to symptoms such as vomiting due to stomach cold and cold pain in the stomach and abdomen, especially suitable for children, the weak, etc. According to the Chinese Pharmacopoeia 2020 Edition, the processing methods of dried ginger, stir-fried ginger, and carbonized ginger are clearly recorded, while there is less record about roasted ginger. The processing methods of roasted ginger include "roasting with straw paper", "roasting with talc powder", and "roasting with wet paper", etc. It is mainly to slice fresh ginger, wrap it with auxiliary materials or media and then heat it until the appearance of the ginger is dark yellow and the inside is yellow. Its processing methods vary significantly in different regions.

[0004] The bran-roasting method, as one of the roasting processing methods, aims to remove some volatile oils and dry components in ginger by heating with wheat bran, thereby reducing its pungency and alleviating its dry nature, and is more applicable to symptoms such as abdominal pain and diarrhea of deficiency-cold type. At present, there are no clear regulations on the key technological parameters such as the roasting time, temperature, and wheat bran amount of roasted ginger.

[0005] In order to solve the problems of the processing technology of ginger roasting and the quality control of volatile components, and ensure the quality and clinical efficacy of the roasted products, the present invention systematically studied the roasting temperature, roasting time, and wheat bran dosage ratio as influencing factors, and the total content of three gingerols and the content of total gingerols as the main pharmacodynamic components as evaluation indexes by using the response surface method, aiming to optimize and determine the best processing technological parameters of roasted ginger. After obtaining stable processing technological parameters, the changes of volatile components before and after roasting were determined by GC-IMS method, providing a basis for controlling the quality of roasted ginger from the perspective of the overall changes of volatile components. Summary of the Invention

[0006] The object of the present invention is to propose a quality evaluation method for establishing the best processing parameters of bran-baked ginger, which can effectively control the temperature of wheat bran, shorten the baking time, reduce the amount of wheat bran used, improve the stability of the processing technology compared with the previous methods, and the appearance color of the baked ginger medicinal materials is uniform after processing. At the same time, the GC-IMS detection technology is used to quickly identify volatile components, so as to evaluate the changes in volatile components before and after bran-baking of ginger and control its quality.

[0007] In order to achieve the above object, the technical solution adopted by the present invention is as follows:

[0008] A quality evaluation method for establishing the best processing parameters of bran-baked ginger, comprising the following steps:

[0009] (1) According to the Box-Behnken central composite design principle, select the baking temperature, baking time, and the ratio of wheat bran to medicinal materials as three influencing factors;

[0010] (2) Put the sliced ginger and wheat bran into the pot in a certain proportion, heat with slow fire, bury and turn appropriately until the whole wheat bran turns dark yellow, sieve off the wheat bran, and let it cool to obtain the baked ginger;

[0011] (3) For the ginger baked with wheat bran, measure the contents of four main pharmacodynamic components: 6-gingerol, 8-gingerol, 10-gingerol, and total gingerol respectively, and conduct a response surface test on the bran-baked ginger using these as evaluation indicators;

[0012] (4) Perform model fitting and variance analysis on the results of the comprehensive score to obtain the best processing parameters for bran-baking ginger;

[0013] (5) Verify the above best bran-baking processing technology.

[0014] As a preferred technical solution of the present invention, in step (1), each factor takes three levels, which are respectively:

[0015] Baking temperature (influence factor A): Select 150 °C, 160 °C, 170 °C;

[0016] Baking time (influence factor B): Select 12 min, 15 min, 18 min;

[0017] Ratio of wheat bran to ginger (influence factor C): Select 1:1, 1.5:1, 2:1.

[0018] As a preferred technical solution of the present invention, the methods for measuring the contents of the four main pharmacodynamic components in step (3) are as follows:

[0019] ① Preparation of mixed reference substance solution: Weigh an appropriate amount of 6-gingerol, 8-gingerol, and 10-gingerol precisely, dissolve them in methanol, and prepare solutions with mass concentrations of 0.03945, 0.00317, and 0.01395 mg / mL respectively;

[0020] ② Preparation of test solution: Cut the processed product into small pieces of approximately the same size, weigh 1 g precisely, place it in a 10 mL test tube, make up the volume to the mark with methanol, tightly stopper and let it stand. Weigh it, ultrasonically treat it for 40 min under the conditions of a power of 100 W and a frequency of 40 Hz. After cooling, dry the outer wall of the test tube, weigh it again, make up the reduced weight with methanol, shake well, filter it through a 0.22 μL filter membrane, and take the subsequent filtrate to obtain the test solution;

[0021] ③ Chromatographic conditions: Waters Acquity HSS C 18 (2.1 mm × 100 mm, 1.8 μm) chromatographic column; The mobile phase is acetonitrile (A) and pure water (B), and the gradient elution program is:

[0022] 0 - 10 min, 3% → 85% A, 97% → 15% B;

[0023] 10 - 15 min, 85% → 100% A, 15% → 0% B;

[0024] 15 - 18 min, 100% → 3% A, 0% → 97% B;

[0025] 18 - 20 min, 3% A, 97% B;

[0026] ④ Determination of total gingerol content: Using ultraviolet spectrophotometry, with 6-gingerol as the reference, measure at a wavelength of 280 nm.

[0027] As a preferred technical solution of the present invention, the following quadratic multiple regression equation is used to calculate the comprehensive score in step (4):

[0028] Y1 = 1.76 + 0.08A + 0.11B + 0.05C - 0.091AB - 0.014AC + 0.012BC - 0.24A 2 - 0.36B 2 - 0.26C 2

[0029] Y2 = 6.81 + 0.23A + 0.19B + 0.091C - 0.20AB - 0.078AC + 0.038BC - 0.53A 2 - 0.37B 2 - 0.40C 2

[0030] The above quadratic multiple regression equation is a model equation obtained by processing data using Design-Expert 13.0 software.

[0031] As a preferred technical solution of the present invention, the optimal processing parameters for bran-roasting ginger in step (4) are: roasting temperature 161.594 °C, roasting time 15.492 min, and the proportion of bran used is 1.549:1; considering the actual operability and the control accuracy of the equipment, the process parameters are adjusted to a roasting temperature of 162 °C, a roasting time of 15.5 min, and the proportion of bran used is 1.5:1.

[0032] As a preferred technical solution of the present invention, the verification of the optimal bran-roasting process in step (5) includes the following steps:

[0033] Take 80 g of ginger, divide it into three equal parts to design three groups of experiments, and process it according to the optimized process above. It is measured that in the three groups of experiments, the total contents of the three components of 6-, 8-, and 10-gingerol are 1.7783 mg / g, 1.7285 mg / g, and 1.7832 mg / g respectively, and the average value is 1.7633 mg / g, which is close to the predicted value of 1.7790 mg / g (RSD is 0.88%); it is measured that the total gingerol contents in the three groups of experiments are 6.8331 mg / g, 6.7585 mg / g, and 6.8656 mg / g respectively, and the average value is 6.8191 mg / g, which is close to the predicted value of 6.8550 mg / g (RSD is 0.52%), indicating that the processing technology is stable and feasible.

[0034] Compared with the prior art, the beneficial effects of the present invention are manifested in:

[0035] 1) First, the present invention improves the roasting process, optimizes the processing parameters of roasted ginger, and then deeply explores the changes in the volatile components of ginger and roasted ginger, providing a basis for the quality control of its processed products.

[0036] 2) The present invention adopts the Box-Behnken central composite design experiment, with the roasting temperature, roasting time, and the proportion of bran used as the investigation factors, screens out the optimal processing technology for bran-roasting ginger, and verifies the optimal bran-roasting process. The present invention improves the limitations of traditional processing methods such as paper-roasting and flour-roasting, which are difficult to control the degree of processing and have cumbersome operations. The bran-roasting method adopted can effectively improve the process defects, improve efficiency, prepare roasted products with uniform appearance and color, and achieve the processing purpose of "slow property and reducing dryness". At the same time, the GC-IMS method established by the present invention for discriminating the volatile components (VOCs) before and after roasting can quickly, intuitively, and comprehensively evaluate the changes in the components before and after bran-roasting of ginger and the quality differences of the processed products. Description of the Drawings

[0037] Figure 1 Appearance of 6 batches of samples before and after baking with bran (FG - raw product, SG - bran - baked product).

[0038] Figure 2 UPLC control charts of three samples (S1 - mixed reference substance, S2 - raw product, and S3 - bran - baked product) (peak 1 corresponds to 6 - gingerol, peak 2 corresponds to 8 - gingerol, and peak 3 corresponds to 10 - gingerol).

[0039] Figure 3 Response surface plot of influencing factors and total content of three gingerols.

[0040] Figure 4 Response surface plot of influencing factors and total gingerol content.

[0041] Figure 5 Fingerprint spectrum of volatile components in the sample.

[0042] Figure 6 OPLS - DA score plot of volatile components in the sample.

[0043] Figure 7 VIP plot of differential markers. Specific implementation manners

[0044] The present invention will be further described in detail below in conjunction with embodiments and drawings.

[0045] First, the present invention proposes a baking - with - bran ginger processing technology. Take ginger slices and wheat bran in a certain proportion and put them into a pot, heat with slow fire, bury and turn appropriately until the whole wheat bran turns dark yellow, sieve off the wheat bran, and let it cool to obtain the product. Secondly, using the Box - Behnken central composite design principle, with the baking temperature, baking time, and ratio of wheat bran to medicinal material dosage as three influencing factors, and the contents of 6 - gingerol, 8 - gingerol, 10 - gingerol and the total gingerol content as evaluation indexes, a response surface experiment on the baking - with - bran ginger processing technology is carried out, so as to screen out the optimal baking - with - bran ginger processing technology, and the optimal technology is verified, and the verification result meets the standard. Finally, in order to identify the volatile components of ginger and baked ginger, 6 batches of ginger from different origins ( Figure 1 as shown) are purchased and baked into baked ginger by the optimal technology, and the volatile components between samples are compared by GC - IMS technology.

[0046] Example 1

[0047] This example provides a quality evaluation method for establishing the processing parameters of baking - with - bran ginger, including the following steps:

[0048] (1) According to the Box-Behnken central composite design principle, the roasting temperature (A), roasting time (B), and ratio of wheat bran dosage (C) were selected as influencing factors, and the total content of three gingerols (Y1) and the content of total gingerols (Y2) were used as evaluation indicators to design a response surface experiment with three factors and three levels (-1, 0, 1).

[0049] The determination methods for the contents of four main pharmacodynamic components are as follows:

[0050] ① Preparation of mixed reference solution: Weigh appropriate amounts of 6-gingerol, 8-gingerol, and 10-gingerol precisely, dissolve them in methanol, and prepare solutions with mass concentrations of 0.03945 mg / mL, 0.00317 mg / mL, and 0.01395 mg / mL respectively;

[0051] ② Preparation of test solution: Cut the processed product into small pieces of approximately the same size, weigh 1 g precisely, place it in a 10 mL test tube, make up the volume to the scale with methanol, tightly stopper and let it stand, weigh it, ultrasonically treat it for 40 min under the conditions of a power of 100 W and a frequency of 40 Hz. After cooling, dry the outer wall of the test tube, weigh it again, make up the reduced weight with methanol, shake well, filter it through a 0.22 μL filter membrane, and take the subsequent filtrate to obtain the test solution;

[0052] ③ Chromatographic conditions: Waters Acquity HSS C 18 (2.1 mm × 100 mm, 1.8 μm) chromatographic column; the mobile phase is acetonitrile (A) and pure water (B), and the gradient elution program is as follows:

[0053] 0 - 10 min, 3% → 85% A, 97% → 15% B;

[0054] 10 - 15 min, 85% → 100% A, 15% → 0% B;

[0055] 15 - 18 min, 100% → 3% A, 0% → 97% B;

[0056] 18 - 20 min, 3% A, 97% B.

[0057] The test results are as Figure 2 shown.

[0058] ④ Determination of total gingerol content: By ultraviolet spectrophotometry, using 6-gingerol as the reference, it was determined at a wavelength of 280 nm.

[0059] Table 1. Orthogonal factor level table

[0060]

[0061] Table 2. Experimental design and results

[0062]

[0063]

[0064] (2) The data was processed using Design-Expert 13.0 software to obtain the quadratic multiple regression equation of the model: Model 1: Y1 = 1.76 + 0.08A + 0.11B + 0.05C - 0.091AB - 0.014AC + 0.012BC - 0.24A 2 -0.36B 2 -0.26C 2 Model 2: Y2 = 6.81 + 0.23A + 0.19B + 0.091C - 0.20AB - 0.078AC + 0.038BC - 0.53A 2 -0.37B 2 -0.40C 2

[0065] As can be seen from Table 3 and Figure 3 it can be known that for Model 1, P < 0.0001, indicating that the model has high significance; the lack-of-fit term P > 0.05, indicating that the model is reliable; the correlation coefficient R 2 = 0.9872, indicating that the experimental values and the predicted values have good fitting. In the results, A, B, and C are significant terms. Among the interaction terms, AB is a significant term, and AC and BC are non-significant terms, indicating that the proportion of wheat bran used has little effect on the total content of the three gingerols, and the order of the influence on the total content of the three gingerols is B roasting time > A roasting temperature > C wheat bran usage ratio.

[0066] As can be seen from Table 4 and Figure 4 it can be known that for Model 2, P < 0.0001, indicating that the model has high significance; the lack-of-fit term P > 0.05, indicating that the model is reliable; the correlation coefficient R 2 = 0.9812, indicating that the experimental values and the predicted values have good fitting. In the results, A, B, and C are significant terms. Among the interaction terms, AB is a significant term, and AC and BC are non-significant terms, indicating that the proportion of wheat bran used has little effect on the total gingerol content, and the order of the influence on the total gingerol content is A roasting temperature > B roasting time > C wheat bran usage ratio.

[0067] According to the Box-Behnken model, the optimal process predicted by the response surface optimization is a roasting temperature of 161.594 °C, a roasting time of 15.492 min, and a wheat bran usage ratio of 1.549:1. Considering the actual operability and the control accuracy of the equipment, the process parameters were adjusted to a roasting temperature of 162 °C, a roasting time of 15.5 min, and a wheat bran usage ratio of 1.5:1.

[0068] Table 3 ANOVA of Model 1

[0069]

[0070] Table 4 Analysis of Variance of Model 2

[0071]

[0072]

[0073] (3) Verification test: Take 80 g of ginger, divide it into three equal parts to design three groups of experiments, process it according to the optimized process above, and measure that the total contents of the three gingerols in the three groups of experiments are 1.7783 mg / g, 1.7285 mg / g, and 1.7832 mg / g respectively, with an average value of 1.7633 mg / g, which is close to the predicted value of 1.7790 mg / g (RSD is 0.88%). It is measured that the total gingerol contents in the three groups of experiments are 6.8331 mg / g, 6.7585 mg / g, and 6.8656 mg / g respectively, with an average value of 6.8191 mg / g, which is close to the predicted value of 6.8550 mg / g (RSD is 0.52%), indicating that the process is stable and feasible.

[0074] Example 2

[0075] This example provides a method for identifying the differences in volatile components of samples before and after roasting, including the following steps:

[0076] (1) Use GC-IMS to detect the volatile components of ginger and roasted ginger to obtain GC-IMS sample difference map data, as shown in Figure 5 , specifically as follows:

[0077] ① Sample preparation

[0078] Accurately weigh 0.5 g of the sample and place it in a 20 mL headspace vial, add 2-octanol as an internal standard, incubate at 80 °C for 15 min and then inject the sample; the samples are divided into two categories, namely 6 batches of ginger from different origins (FG01 - FG06) and the corresponding roasted ginger (SG01 - SG06).

[0079] ② Headspace injection conditions

[0080] Incubation temperature: 80 °C; Incubation time: 15 min; Injection volume: 100 μL; Splitless injection; Incubation rotation speed: 500 r / min; Injection needle temperature: 110 °C.

[0081] ③ GC conditions:

[0082] Column temperature: 60 °C. Carrier gas: High-purity nitrogen (purity ≥ 99.999%). Programmed pressure rise: Initial flow rate of 2.0 mL / min is maintained for 2 min, linearly increased to 10.0 mL / min within 8 min, linearly increased to 100.0 mL / min within 10 min, and then maintained for 30 min to end (chromatographic run time: 50 min). Injection port temperature: 80 °C. Drift gas flow rate: 150.0 mL / min.

[0083] ④ IMS conditions

[0084] Ionization source: Tritium source ( 3 H); Migration tube length: 53 mm; Electric field strength: 500 V / cm; Migration tube temperature: 45 °C; Drift gas: High-purity nitrogen (purity ≥ 99.999%), flow rate: 150.0 mL / min; Positive and negative ion modes: Positive ion. Door opening time: 100 μs, door closing voltage: 90 dgt.

[0085] (2) Using the peak area and peak height in the sample data as variables, perform OPLS-DA analysis on 6 batches of samples of raw ginger and processed ginger using SMICA-P14.1 software, see Figure 6 and screen those with VIP > 1 as differential biomarker components, obtaining 25 differential components. The results are shown in Figure 7 as follows:

[0086] The contents of 2-Heptanone, (+)-limonene, Acetone, 2-Butanone, Acetone, 2-Pentanone-D, isomenthone-M, and isomenthone-D are higher in raw ginger; while after processing with wheat bran, the contents of 2-furaldehyde-D, 1-Hydroxy-2-propanone, 2-furaldehyde-M, 1-(1-methylethyl)-4-methylbenzene, Acetic acid, allyl isothiocyanate-M, citral-D, 2-Methylpyrazine, 5-methyl-2-furancarboxaldehyde-M, 2,3-pentadione, citral-M, Geranyl acetate-M, 3-hydroxy-2-butanone, Ethanol, (E)-2-butenal-D, Propanal-D, allyl isothiocyanate-D, and (E)-2-butenal-M in processed ginger increase.

[0087] The above content is only an example and illustration of the concept of the present invention. Those skilled in the art of this technology can make various modifications, supplements, or use similar methods to replace the specific embodiments described. As long as they do not deviate from the concept of the invention or exceed the scope defined by this claim book, they should all fall within the protection scope of the present invention.

Claims

1. A quality evaluation method for establishing the best processing parameters of bran-fried ginger, characterized in that It includes the following steps: (1) According to the Box-Behnken central composite design principle, select the roasting temperature, roasting time, and the ratio of wheat bran to medicinal materials as three influencing factors; (2) Take ginger slices and wheat bran in a certain proportion and put them into a pot, heat with a slow fire, bury and turn appropriately until the whole wheat bran turns dark yellow, sieve out the wheat bran, and let it cool to obtain roasted ginger; (3) For the ginger roasted with wheat bran, measure the contents of four main pharmacodynamic components: 6-gingerol, 8-gingerol, 10-gingerol, and total gingerol, and conduct a response surface experiment on wheat bran-roasted ginger using these as evaluation indicators; (4) Fit the model and conduct variance analysis on the results of the comprehensive score to obtain the optimal processing parameters for wheat bran-roasted ginger; (5) Verify the above optimal wheat bran roasting process.

2. The quality evaluation method according to claim 1, wherein In step (1), each factor takes three levels, which are respectively: Roasting temperature (influence factor A): Select 150 °C, 160 °C, 170 °C; Roasting time (influence factor B): Select 12 min, 15 min, 18 min; Ratio of wheat bran to ginger (influence factor C): Select 1:1, 1.5:1, 2:

1.

3. The quality evaluation method according to claim 1, wherein The determination methods for the contents of the four main pharmacodynamic components in step (3) are as follows: ① Preparation of the mixed reference substance solution: Weigh appropriate amounts of 6-gingerol, 8-gingerol, and 10-gingerol precisely, dissolve them with methanol, and prepare solutions with mass concentrations of 0.03945, 0.00317, and 0.01395 mg / mL respectively; ② Preparation of the test solution: Cut the processed product into small pieces of approximately the same size, weigh 1 g precisely, place it in a 10 mL test tube, make up the volume to the scale with methanol, tightly stopper and let it stand, weigh it, ultrasonically treat it for 40 min under the conditions of a power of 100 W and a frequency of 40 Hz, after cooling, dry the outer wall of the test tube, weigh it again, make up the reduced weight with methanol, shake well, filter through a 0.22 μL filter membrane, and take the continuous filtrate to obtain the test solution; ③Chromatographic conditions: Waters Acquity HSS C 18 (2.1 mm × 100 mm, 1.8 μm) chromatographic column; the mobile phase was acetonitrile (A) and pure water (B), and the gradient elution program was as follows: 0 - 10 min, 3% → 85% A, 97% → 15% B; 10 - 15 min, 85% → 100% A, 15% → 0% B; 15 - 18 min, 100% → 3% A, 0% → 97% B; 18 - 20 min, 3% A, 97% B; ④ Determination of the total gingerol content: Using ultraviolet spectrophotometry, with 6-gingerol as the reference, measure at a wavelength of 280 nm.

4. The quality evaluation method according to claim 1, characterized in that, In step (4), the following quadratic multiple regression equation is used to calculate the comprehensive score: Y1 = 1.76 + 0.08A + 0.11B + 0.05C - 0.091AB - 0.014AC + 0.012BC - 0.24A 2 - 0.36B 2 - 0.26C 2 Y2 = 6.81 + 0.23A + 0.19B + 0.091C - 0.20AB - 0.078AC + 0.038BC - 0.53A 2 - 0.37B 2 - 0.40C 2 The above quadratic multiple regression equation is a model equation obtained by processing the data using Design-Expert 13.0 software.

5. The quality evaluation method according to claim 1, characterized in that The optimal processing parameters for wheat bran-roasted ginger obtained in step (4) are: roasting temperature 161.594 °C, roasting time 15.492 min, and the ratio of wheat bran dosage 1.549:1; considering the actual operability and the control accuracy of the equipment, the processing parameters are adjusted to roasting temperature 162 °C, roasting time 15.5 min, and the ratio of wheat bran dosage 1.5:

1.

6. The quality evaluation method according to claim 5, characterized in that In step (5), the verification of the optimal wheat bran roasting process includes the following steps: Take 80 g of ginger, divide it into three equal parts to design three groups of experiments, and process it according to the optimized process described above. The total contents of the three gingerols in the three groups of experiments are measured to be 1.7783 mg / g, 1.7285 mg / g, and 1.7832 mg / g respectively, with an average value of 1.7633 mg / g, which is close to the predicted value of 1.7790 mg / g (RSD is 0.88%); the total gingerol contents in the three groups of experiments are measured to be 6.8331 mg / g, 6.7585 mg / g, and 6.8656 mg / g respectively, with an average value of 6.8191 mg / g, which is close to the predicted value of 6.8550 mg / g (RSD is 0.52%), indicating that the processing technology is stable and feasible.

Images