CN102746704A - Ultrasonic extracting process for gardenia yellow pigment and optimized method of response surface methodology used therein - Google Patents

Ultrasonic extracting process for gardenia yellow pigment and optimized method of response surface methodology used therein Download PDF

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CN102746704A
CN102746704A CN2012102051210A CN201210205121A CN102746704A CN 102746704 A CN102746704 A CN 102746704A CN 2012102051210 A CN2012102051210 A CN 2012102051210A CN 201210205121 A CN201210205121 A CN 201210205121A CN 102746704 A CN102746704 A CN 102746704A
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gardenia yellow
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陈绍瑗
吕贞儿
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Zhejiang University ZJU
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Abstract

The invention discloses an ultrasonic extracting process for gardenia yellow pigment. The process comprises the steps of mixing gardenia fruit powder and an ethanol-water solution having a volume concentration of 71-73% with the ratio of the solution to the powder (V/m) being 23-24 mL : 1 g; extracting for 1.1-1.2 hours with ultrasonic at a temperature of 51-52 DEG C twice, wherein the ultrasonic frequency is 27 kHz-31 kHz; and mixing the obtained extracting solutions of the gardenia yellow pigment. The invention also discloses an optimized method of response surface methodology used in the extracting process for the gardenia yellow pigment. The optimized method sets four variables of the volume concentration of ethanol in the ethanol water solution, the liquor-to-material ratio of the gardenia fruit powder and the ethanol water solution, extracting temperature and extracting time, and performs an optimization by using a design expert soft according to a Box-Behnken design principle. By adopting the extracting process for the gardenia yellow pigment, an extraction rate of the gardenia yellow pigment is improved.

Description

Gardenia Yellow ultrasonic extracting process and used response surface method optimized method
Technical field
The present invention relates to a kind of optimization method of Gardenia Yellow ultrasonic extraction condition, particularly relate to the method for utilizing Response Surface Method to optimize the Gardenia Yellow extraction conditions.
Background technology
Gardenia Yellow is from cape jasmine fruit, to extract the yellow pigment that obtains; Be the rare water-soluble carotenoid class pigment of a kind of nature, belong to natural pigment, good stability, strong coloring force; Reducing resistance, anti-mikrobe property are good; Fast light, heat-resisting, color is constant basically in pH value 4-11 scope, and is stable to metals ion; Dying effective to starch, protein.In April, 2012; Health ministry is intended 38 kinds of foodstuff additive of cancellation, comprises tea yellow pigment, tea green pigment, Pasania cuspidata palm fibre, citrus is yellow, black currant is red, Fruit of Cherokee Rose, palm fibre fall, and certain herbaceous plants with big flowers is red, Mi Menghuang, mulberry fruit is red, sea-buckthorn is yellow, wild jujube look, acorn cup palm fibre, Chlorophyll Cu sylvite, maize, algae indigo plant (light, seawater), red, the red 17 kinds of natural pigments of Lonicera caerulea of Testa arachidis hypogaeae.Gardenia Yellow is that China's regulation allows to use, and the natural pigment in plan is cancelled scope is not that the domestic and international market demand accounts for deputy natural pigment.2011, the cultivated area of Zhejiang Anji County water cape jasmine reached 15000 mu, reached the whole nation second.Gardenia Yellow is the main products of Zhejiang Anji County water cape jasmine deep processing.
Cape jasmine, another name Yellow Fructus Gardeniae, mountain Cape jasmine, white toad are the fruits of madder wort cape jasmine.The fruit of cape jasmine is a traditional Chinese medicine, and the l that belongs to Ministry of Health's promulgation criticizes the medicine-food two-purpose resource, has effects such as the liver of protecting, cholagogic, step-down, calmness, hemostasis, detumescence, is usually used in treating diseases such as icterohepatitis, sprain and contusion, hypertension, mellitus at tcm clinical practice.Gardenia Yellow belongs to natural pigment, and its staple is a Crocin, and 440 nm places have maximum absorption band at wavelength, contain numerous oxy radicals, and a little less than the lipotropy, wetting ability is strong, and the solubleness in sherwood oil is little, and the solubleness in alcohol and methyl alcohol is big.
Gardenia Yellow contains hydrophilic radical, and is soluble in water, can use water extraction.But water extraction production pigment purity is low, and visual appearance is poor, is difficult to make with extra care, unfavorable industrialized production.The many infiltration with ethanol of traditional extraction technique extracted, and the cycle is long, and temperature is high, and the liquid material is unfavorable for suitability for industrialized production than big.
The process for extracting of present existing Gardenia Yellow is: the cape jasmine fruit powder with the liquid material ratio of aqueous ethanolic solution is: 40-50ml/g, and alcohol concn is: 80%, extracting temperature is 60 ℃, soaking into extraction time is 3-5 hour, extracts 2 ~ 3 times.Recording extraction yield is 80-91%, and yield is 5-7%, and the look valency is 10-50, and the OD value is 0.7-1.2.
Summary of the invention
The technical problem that the present invention will solve provides a kind of Gardenia Yellow extraction process of using the Response Surface Method optimization method to be obtained; The present invention is optimized these factors that influence the Gardenia Yellow extraction yield of alcohol concn, extraction time, extraction temperature and solid-liquid ratio; Thereby improve the extraction yield of Gardenia Yellow; Promote food safety, improved the natural pigment resource utilization ratio.
In order to solve the problems of the technologies described above; The present invention provides a kind of Gardenia Yellow extraction process; Cape jasmine fruit powder and volumetric concentration are 71 ~ 73% aqueous ethanolic solution according to the liquid material of 23 ~ 24ml aqueous ethanolic solution/g cape jasmine fruit powder than mixing; Supersound extraction is 1.1 ~ 1.2 hours under 51 ~ 52 ℃ temperature, and extraction time is 2 times, merges the Gardenia Yellow extracting solution of 2 gained; Ultrasonic frequency is 27kHz~31kHz hertz (for example being the 30kHz hertz).
Behind above-mentioned Gardenia Yellow extracting solution rotary evaporation recovery solvent, can obtain the Gardenia Yellow raw product.
For the ease of detecting, with 1g cape jasmine fruit powder according to the method described above the Gardenia Yellow extracting solution constant volume (with the aqueous ethanolic solution of same concentration) after the merging of gained to 60ml, behind the redilution 100 times (volume ratio is with aqueous ethanolic solution of same concentration); Record: extraction yield is 93.73%, and yield is 10.2%, and the look valency is 70, and the OD value is 0.69.
The remarks explanation:
Said fixing volume (being constant volume) is to do unitized the processing, and is relatively convenient; Absorbancy could arrive below 1 after diluting 100 times.
Above-mentioned cape jasmine fruit powder is meant: be dried to water ratio≤8% (weight content), pulverize, cross the cape jasmine fruit of 100 mesh sieves.
Improvement as Gardenia Yellow extraction process of the present invention: the aqueous ethanolic solution of cape jasmine fruit powder and volumetric concentration 72% according to the liquid material of 23.5ml aqueous ethanolic solution/g cape jasmine fruit powder than mixing; Supersound extraction is 1.19 hours under 51.7 ℃ temperature, and extraction time is 2 times.
The present invention also provides a kind of response surface method to optimize the method for Gardenia Yellow extraction process simultaneously, and 4 variablees are set: alcoholic acid volumetric concentration in the aqueous ethanolic solution, and the cape jasmine fruit powder compares, extracts temperature and extraction time with the liquid material of aqueous ethanolic solution; Utilize design expert software to be optimized according to Box-Behnken principle of design.
The present invention provides a scientific basis for the Gardenia Yellow suitability for industrialized production.The application principle of ultrasound assisted extraction technique is to utilize cavitation effect of ultrasonic waves to quicken the stripping of effective ingredients in plant; Hyperacoustic in addition second-order effect; Like mechanical vibration, emulsification, spread, smash, chemical effect etc. can quicken also that desire extracts that the diffusion of composition discharges and fully and solvent, be beneficial to and extract fully.Response surface analysis method (RSM) is according to the regression relation between several variablees and the one or more dependent variable, obtains extraction conditions and the regression relation that extracts the result through regression analysis, thereby tries to achieve a kind of mathematical method of optimum extraction process.
The present invention provides a kind of optimization method that extracts Gardenia Yellow, and alcohol concn, extraction time, extraction temperature and the solid-liquid ratio influence factor to the Gardenia Yellow extraction yield is optimized, and the optimum optimizing condition that obtains is an alcohol concn: 72%; Temperature is 51.7 ° of C, and extraction time is 1.19 hours, and liquid material ratio is 23.5 o'clock; Extract 2 times, Gardenia Yellow extraction rate reached to 93.73%, yield are 10.2%; The look valency is 70, and the OD value is 0.69.
Concrete technical scheme of the present invention is following:
The present invention is a kind of method that application responds surface analysis method is optimized the Gardenia Yellow extraction process.With 27 groups of minimum experiment (Orthogonal Method 4 4The group experiment) the Gardenia Yellow extraction conditions being carried out alcohol concn, extraction time, extraction temperature and liquid material is optimized than 4 factors that these influence the Gardenia Yellow extraction yield; Obtain best extraction optimal conditions; Obtain the optimum extraction rate, improved extraction efficiency, promoted food safety; Improve the natural pigment resource utilization ratio, practical significance with suitability for industrialized production.
The present invention just can optimize the extraction process of Gardenia Yellow rationally and effectively only through a spot of experiment, and is simple and feasible.
The present invention has very high use value applicable to the optimum problem of technology in the suitability for industrialized production Gardenia Yellow.
The present invention has following advantage and efficient:
Application responds surface analysis method is optimized a kind of method of Gardenia Yellow ultrasonic extracting process.Only just can be optimized the Gardenia Yellow extraction process through 27 groups of experiments.
When extraction conditions is that alcohol concn is 72%, temperature is 51.7 ° of C, and extraction time is 1.19 hours, and liquid material ratio is 23.5 o'clock, extracts 2 times, and the extraction yield of Gardenia Yellow can reach 93.73%, and yield reaches 10.2%, and the look valency reaches 70, and the OD value reaches 0.69.The present invention has reduced the extraction temperature, has practiced thrift the energy; Shorten extraction time, improved production efficiency; Promote food safety, improved the utilization ratio of natural pigment resource.
In sum; It is the response surface analysis method that Box-Behnken (BBD) center combination that the present invention adopts designs a model; With four changed factors,, compare with Orthogonal Method only with three levels; Just can obtain a result with a spot of experimental group, and resulting top condition is not the value set but within the scope that imposes a condition.Through taking the response surface method to analyze the optimal conditions that Gardenia Yellow extracts,, obtain the best optimization condition through alcohol concn, extraction time, extraction temperature and the solid-liquid ratio influence factor to the Gardenia Yellow extraction yield is optimized.
Description of drawings
Do further explain below in conjunction with the accompanying drawing specific embodiments of the invention.
Do further explain below in conjunction with the accompanying drawing specific embodiments of the invention.
Fig. 1 is that extraction factor is three-dimensional to the response surface of Gardenia Yellow extraction yield influence, X-Y scheme;
(a) last figure is extracting solution material ratio and the response surface three-dimensional plot of extraction temperature to the influence of Gardenia Yellow extraction yield,
Figure below is extracting solution material ratio and the response surface X-Y scheme of extraction temperature to the influence of Gardenia Yellow extraction yield;
(b) last figure is the response surface three-dimensional plot that solid-liquid ratio and extraction time the Gardenia Yellow extraction yield is influenced,
Figure below is liquid material ratio and the response surface X-Y scheme of extraction time to the influence of Gardenia Yellow extraction yield;
(c) last figure is the response surface three-dimensional plot that solid-liquid ratio and alcohol concn influence the Gardenia Yellow extraction yield,
Figure below is liquid material ratio and the response surface X-Y scheme of alcohol concn to the influence of Gardenia Yellow extraction yield;
(d) last figure is the response surface three-dimensional plot that extraction temperature and extraction time the Gardenia Yellow extraction yield is influenced,
Figure below is for extracting temperature and the extraction time response surface X-Y scheme to the influence of Gardenia Yellow extraction yield;
(e) last figure is the response surface three-dimensional plot that extraction temperature and alcohol concn influence the Gardenia Yellow extraction yield,
Figure below is for extracting temperature and the alcohol concn response surface X-Y scheme to the influence of Gardenia Yellow extraction yield;
(f) last figure is the response surface three-dimensional plot that extraction time and alcohol concn influence the Gardenia Yellow extraction yield,
Figure below is the response surface X-Y scheme that extraction time and alcohol concn influence the Gardenia Yellow extraction yield;
Fig. 2 is that the liquid material is than the figure that influences that changes the Gardenia Yellow extraction yield;
Fig. 3 extracts the influence figure of temperature variation to the Gardenia Yellow extraction yield;
Fig. 4 is that extraction time is than the figure that influences that changes the Gardenia Yellow extraction yield;
Fig. 5 is that alcohol concn is than the figure that influences that changes the Gardenia Yellow extraction yield.
Embodiment
Embodiment 1, response surface method are optimized the method for Gardenia Yellow extraction process:
One, sample is prepared
Cape jasmine fruit is dried to water ratio≤8% (weight content), pulverizes, cross 100 mesh sieves, the cape jasmine fruit powder of gained is as sample.
Weigh sample thief 1.00g in the balance; Add certain density aqueous ethanolic solution by material ratio, under differing temps, carry out UW (frequency of 30kHz) by the regular hour and extract 2 times, the solution after the extraction filters; Merge clear liquid; To 60ml, dilute 100 times (aqueous ethanolic solutions of this concentration) with solvent (aqueous ethanolic solution of this concentration) constant volume then, adopt i.e. (1% solution of the said method of GB7912--87 Gardenia Yellow national standard; 440 nm, the 1mL cuvette) on 751 G spectrophotometers, measure absorbancy.Calculate the Gardenia Yellow extraction yield.
Extraction yield=(A*V)/(A Always* V Always)
Under optimum extraction conditions, the cape jasmine fruit powder of classification ultrasonic extraction 1.00g until extracting liquid colourless, merges each extracting solution then and obtains TV (V Always) and total absorbance (A Always).A representes the 400nm absorbancy of mensuration under this extraction conditions, and V representes the volume after the extracting solution dilution.
Two, experimental design and statistical study
1, experiment of single factor
Change alcohol concn, extraction temperature, extraction time, material ratio carry out experiment of single factor, adopt the said method of GB7912--87 Gardenia Yellow national standard on 751 G spectrophotometers, to measure absorbancy (1% solution, 440 nm, 1mL cuvette), calculate extraction yield.Each processing repeats for three times.
2, response surface method optimization design
According to the single factor experiment result; Choose the significant alcohol concn of Gardenia Yellow extraction yield influence, extraction time, extraction temperature, these four factors of material ratio; Utilize design expert software according to Box-Behnken principle of design contrived experiment; Choose the extraction temperature, the experimentize setting of factor and level of extraction time and material ratio is set the result and is seen table 1.
Table 1 empirical factor and level set
Figure BDA0000178760131
Is independent variable(s) with extraction temperature (A), extraction time (B), liquid material than (C) and alcohol concn (D), is response value (y) with the extraction yield, and testing program and result see table 2.Test point 1-24 is the factorial point, and 25-27 is zero points.Data are seen table 2.
Table 2 Box-Behnken test design and result
Experiment numbers A B C D y
1 1 0 0 1 18.15
2 -1 -1 0 0 42.84
3 0 1 -1 0 58.08
4 1 -1 0 0 72.64
5 1 0 0 -1 82.03
6 -1 0 -1 0 48.29
7 0 -1 0 -1 47.53
8 0 1 1 0 65.64
9 0 0 -1 1 14.13
10 1 0 1 0 83.57
11 0 0 1 1 41.00
12 0 -1 1 0 71.18
13 0 -1 -1 0 42.54
14 0 1 0 -1 82.93
15 0 0 1 -1 71.61
16 -1 0 0 -1 55.04
17 0 -1 0 1 24.25
18 0 0 -1 -1 56.86
19 1 1 0 0 67.30
20 -1 1 0 0 70.33
21 -1 0 1 0 69.81
22 -1 0 0 1 19.06
23 0 1 0 1 35.01
24 1 0 -1 0 53.76
25 0 0 0 0 86.01
26 0 0 0 0 85.72
27 0 0 0 0 86.21
3, the foundation of model and statistical study
Carry out multiple regression analysis according to the gained data, the polynary quadratic regression equation between variable that meets with a response (alcohol concn, extraction temperature, extraction time and liquid material ratio) and the response value (extraction yield).
Extraction yield=85.98+6.01*A+6.53*B+10.76*C-20.37D-11.54*A 2-11.86*B 2-12.33*C 2-28.44*D 2-8.21*AB+2.07*AC-6.97*AD-5.27*BC-6.16*BD+3.03*CD
Linear relationship significance between each factor and the response value judges that by the check of F value the P value is more little, and then the significance of explanatory variable is high more.Can know that by analysis of variance table (table 3) linear relationship between its dependent variable and all independent variable(s) is (R significantly 2=0.9715), the level of signification of model is less than 0.0001, so this regression variance model is extremely significant.
The The results of analysis of variance of table 3 experimental data
Figure BDA0000178760132
4, test result analysis and optimization
Utilize Design Expert software according to the regression equation analysis of drawing, obtain the response surface and the isogram thereof of regression equation, as shown in Figure 1.
Learn that according to model analysis the extraction of Gardenia Yellow is optimized processing parameter and is: alcohol concn 72%, extract temperature 51.7 C carries extraction time 1.19h, liquid material than 23.5.With this understanding, the extraction yield predictor 93.73% of Gardenia Yellow.
Experiment 1, a kind of Gardenia Yellow process for extracting comprise the steps:
Cape jasmine fruit is dried to water ratio≤8% (weight content), pulverizes, cross 100 mesh sieves; Get the cape jasmine fruit powder.Above-mentioned cape jasmine fruit powder 1g is mixed (promptly with the aqueous ethanolic solution of the volumetric concentration 72% of 23.5 mL; The liquid material is than 23.5); UW under 51.7 ℃ temperature (frequency of 30kHz) extracted 1.19 hours; Extraction time is 2 (that is alternative 1g cape jasmine fruit powder of residue of gained after, usefulness is extracted first; Repeat the said extracted process); The Gardenia Yellow extracting solution that merges 2 gained.
The Gardenia Yellow extracting solution of gained after the above-mentioned merging is settled to 60ml (aqueous ethanolic solution with volumetric concentration 72% carries out constant volume) with volumetric flask; After diluting 100 times (aqueous ethanolic solution with volumetric concentration 72% dilutes); Adopt the said method of GB7912--87 Gardenia Yellow national standard on 751 G spectrophotometers, to measure extraction yield (1% solution, 440nm, 1mL cuvette); Recording extraction yield is 93.73%; Rotary evaporation obtains 0.102g Gardenia Yellow raw product after reclaiming solvent, and promptly under this technology, the Gardenia Yellow yield is 10.2%.Recording the look valency is 70, and the OD value is 0.69.
Look valency=Af/100m,
A representes the absorbancy of wavelength 400nm, and f representes extension rate, and m representes sample mass in the test fluid.
OD=A 440/A 280
A 440Be illustrated in the absorbancy under the wavelength 440nm, A 280Be illustrated in the absorbancy under the wavelength 280nm.
Experiment 2, extracting solution material are than the influence that changes Gardenia Yellow solution extraction yield
Extracting temperature is 50 ℃, and alcohol concn 80% under the condition of extraction time 1h, is set at 10-50:1 with liquid material ratio, 5 changing values; All the other are with experiment 1.The result is as shown in Figure 2.
When liquid material ratio was 20:1, extraction yield was 84.06%, and along with liquid material ratio increases, the solution extraction yield maintains one than stable status.
Test 3, extract the influence of temperature variation Gardenia Yellow solution extraction yield:
Be set at 1 hour in extraction time, the liquid material under the condition of alcohol concn 80%, is set at 30-70 ℃ five changing values with extracting temperature than 20:1; All the other are with experiment 1.The result is as shown in Figure 3.
When the extraction temperature was 50 ℃, extraction yield was 84.36%, and along with the increase of temperature, the solution extraction yield maintains one than stable status.
Experiment 4, extraction time change the influence to Gardenia Yellow solution extraction yield:
Be set at 20:1 at liquid material ratio, extract 50 ℃ of temperature, under the condition of alcohol concn 80%, will be set at five changing values under the 0.5-2.5h condition extraction time; All the other are with experiment 1.The result is as shown in Figure 4.
When extraction time was 1h, extraction yield was 84.44%, and along with the increase of time, the solution extraction yield maintains one than stable status.
Experiment 5, alcohol concn change the influence to Gardenia Yellow solution extraction yield:
Be set at 20:1 at liquid material ratio, extract 50 ℃ of temperature, under the condition of extraction time 1h, alcohol concn is set at five changing values under the 20-100% condition; All the other are with experiment 1.The result is as shown in Figure 5.
When alcohol concn was 80%, extraction yield was 85.27%, and along with the increase of alcohol concn, the solution extraction yield reduces on the contrary.
Experiment 6, make the liquid material ratio of cape jasmine fruit powder and the aqueous ethanolic solution of volumetric concentration 80% into 50, extract temperature and change 70 ℃ into, extraction time changes 2.5 hours into, and all the other are with experiment 1.The pigment extraction yield is 92.28%.
At last, it is also to be noted that what more than enumerate only is several specific embodiments of the present invention.Obviously, the invention is not restricted to above embodiment, many distortion can also be arranged.All distortion that those of ordinary skill in the art can directly derive or associate from content disclosed by the invention all should be thought protection scope of the present invention.

Claims (3)

1. Gardenia Yellow extraction process; It is characterized in that: cape jasmine fruit powder and volumetric concentration are 71 ~ 73% aqueous ethanolic solution according to the liquid material of 23 ~ 24ml aqueous ethanolic solution/g cape jasmine fruit powder than mixing; Supersound extraction is 1.1 ~ 1.2 hours under 51 ~ 52 ℃ temperature, and extraction time is 2 times; The Gardenia Yellow extracting solution that merges 2 gained; Said ultrasonic frequency is 27kHz~31kHz hertz.
2. Gardenia Yellow extraction process according to claim 1; It is characterized in that: said cape jasmine fruit powder and volumetric concentration are 72% aqueous ethanolic solution according to the liquid material of 23.5ml aqueous ethanolic solution/g cape jasmine fruit powder than mixing; Supersound extraction is 1.19 hours under 51.7 ℃ temperature, and extraction time is 2 times.
3. a response surface method is optimized the method for Gardenia Yellow extraction process, it is characterized in that: following 4 variablees are set: alcoholic acid volumetric concentration in the aqueous ethanolic solution, the liquid material of cape jasmine fruit powder and aqueous ethanolic solution than, extract temperature and extraction time; Utilize design expert software to be optimized according to Box-Behnken principle of design.
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CN104672948A (en) * 2015-02-15 2015-06-03 广西壮族自治区林业科学研究院 Method for optimally extracting lithocarpus polysachyus rehd brow pigment with response surface process
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CN103083939A (en) * 2013-02-18 2013-05-08 浙江桐庐百草园中药材开发有限公司 Method for extracting borneol camphor tree leaf crude extract and applied response surface methodology
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CN103589433A (en) * 2013-11-15 2014-02-19 嘉兴职业技术学院 Method for extracting antioxidant components of solidago canadensis L. by response surface method
CN104672948A (en) * 2015-02-15 2015-06-03 广西壮族自治区林业科学研究院 Method for optimally extracting lithocarpus polysachyus rehd brow pigment with response surface process
CN105712847A (en) * 2015-10-17 2016-06-29 浙江大学 Process for extracting effective components of fig leaves and response surface optimization method used by process
CN112341504A (en) * 2015-12-21 2021-02-09 河北科技师范学院 Method for optimizing conditions for extracting tannin from grape seeds by organic solvent extraction method
CN109370283A (en) * 2018-09-26 2019-02-22 张惠柳 A kind of child drawing yellow uitramarine and preparation method thereof
CN112251044A (en) * 2020-11-13 2021-01-22 安顺职业技术学院 Response surface method optimized hotbed chives pigment extraction process and application thereof
CN112251044B (en) * 2020-11-13 2021-11-16 安顺职业技术学院 Response surface method optimized hotbed chives pigment extraction process and application thereof

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Application publication date: 20121024