KR20130013686A - A method of extrating curcumin from tumeric using supercritical fluid extraction - Google Patents

Abstract

PURPOSE: A method for extracting curcumin derived from Curcumae Rhizoma by supercritical extraction is provided to obtain curcumin with high efficiency from Curcumae Rhizoma. CONSTITUTION: A method for extracting curcumin derived from Curcumae Rhizoma comprises: a step of drying Curcumae Rhizoma with hot air; a step of pulverizing the dried Curcumae Rhizoma to have a particle size of 0.5-2 mm; and a step of extracting the pulverized Curcumae Rhizoma using supercritical carbon dioxide at 40-60 deg. C and 150-350 bar. The method for extracting curcumin additionally comprises a step of concentrating the extract.

Description

A method of extrating curcumin from tumeric using supercritical fluid extraction}

The present invention relates to a turmeric-derived curcumin extraction method using supercritical extraction, and more particularly, after the hot air is dried with hot air, the turmeric dry matter is pulverized to a particle size of 0.5 to 2 mm, followed by a temperature of 40 to 60 ° C. and 150 to A method of extracting large amounts of curcumin from turmeric by supercritical extraction with supercritical carbon dioxide under a pressure of 350 bar.

Turmeric is a perennial herbaceous herbaceous plant native to tropical Asia belonging to the Ginger family. Roots are thick and strong, with bulging ends, forming a long egg-shaped tube root. Tubers are ovate, lateral, rhizomes are columnar, and yellow in cross section.

Curcumin contains 1 ~ 3% of curcumin, 1 ~ 5% of essential oils, and 30 ~ 40% of starch. Curcumin is the main ingredient of yellow cattle. In addition, it contains various ingredients such as ρ- methydollrucabinole, tumerone, azulene, kampfa flavonoids, and plant fiber.

Curcumin, a major component of turmeric, has a strong antioxidant function and structurally belongs to phenolic antioxidants. Recently, as the anti-cancer effect is revealed, the attention of the scientific community has been focused. It has been shown that curcumin can block the expression of a major protein associated with esophageal cancer by inhibiting NF-kappaB, which helps cancer cells continue to grow. Curcumin has also been shown to induce tumor cell death in many other cancers, including skin cancer. It prevents the accumulation of brain cell destroying protein, which causes not only cancer, but also Alzheimer's disease, delays the progression of the disease, and inhibits the expression of inflammatory protein 'interleukin 8'. In addition, various functions have been reported, such as preventing blood from being nourished by effectively preventing new blood vessels from being formed at concentrations that are not toxic to other cells, that is, without cytotoxicity, and inducing cancer cells to die.

Curcumin extraction from conventional turmeric has been mostly carried out by hot water extraction or solvent extraction. The conventional extraction method made in this way has a problem in that residual waste and an organic solvent remain after extraction. In addition, there is a disadvantage that the extraction efficiency of curcumin is low.

Under this background, the inventors have crushed the turmeric dry to a particle size of 0.5 mm to 2 mm after hot air drying the turmeric and then at a temperature of 40 to 60 ° C. and a pressure of 150 to 350 bar, in particular a particle size of 0.5 mm, Supercritical extraction with supercritical carbon dioxide at a temperature of 60 ° C. and a pressure of 350 bar confirms that curcumin can be extracted, particularly from turmeric, with high efficiency.

It is an object of the present invention to provide a turmeric-derived curcumin extraction method using supercritical extraction.

In order to solve the above problems, the present invention provides a turmeric-derived curcumin extraction method comprising the following steps.

1) hot air drying turmeric;

2) grinding the turmeric dry matter to a particle size of 0.5 to 2 mm; And

3) supercritical extraction of the turmeric powder with supercritical carbon dioxide at a temperature of 40 to 60 ℃ and a pressure of 150 to 350 bar.

Preferably, the turmeric-derived curcumin extraction method of the present invention further comprises the step of concentrating the extract after step 3 (step 4).

Preferably, the turmeric-derived curcumin extraction method of the present invention further comprises the step of separating and purifying curcumin from the concentrate after step 4 (step 5).

Step 1 is a step of drying the turmeric with hot air, and drying the turmeric with hot air as a pretreatment for increasing the extraction efficiency of the turmeric.

The terms used in the present invention, turmeric (Turmeric) "is keokyu equine that (Curcuma sp.) Means the tuberous root of the plant belonging to the keokyu equine (Curcuma sp.) Plants has come turmeric (Curcuma belonging to wenyujin , YH Chen et C. Ling, Curcuma longa Linne, Curcuma longa Salisb.), Purple Curcuma zedoaria), Guangxi ahchul (based turmeric) (Curcuma kwansiensis , SG Lee et CF Liang), Curcuma aeruginosa , Curcuma phaeocaulis Val. (Ginger and Zingiberaceae)] or Curcuma dometica domestica ), but are not necessarily limited thereto.

The term 'hot air drying' used in the present invention means a drying method of drying with hot air of room temperature or more. The hot air drying temperature is preferably in the temperature range of 40 to 50 ℃.

In the present invention, the hot air drying may be performed for several days, preferably 1 to 5 days. The hot air drying time may be appropriately adjusted according to the moisture content of turmeric.

In step 2, the turmeric dry matter is pulverized to a particle size of 0.5 to 2 mm, and the turmeric dry matter is pulverized to a predetermined size as a pretreatment for increasing extraction efficiency of turmeric.

The milling is preferably milled into particles having a size of 0.5 (milled) to 2 mm (milled). If the particle size during the grinding is outside the above range, there is a disadvantage in that the extraction efficiency of turmeric falls. Particularly, in the particle size of less than 0.5 mm, the extraction efficiency decreases due to the pressure load during supercritical extraction. In the particle size larger than 2 mm, the curcumin contained in the particles is difficult to extract to the outside by the supercritical fluid. There is a drawback of poor extraction efficiency.

In particular, in the present invention, the grinding is more preferably pulverized into particles having a size of 0.5 to 1 mm. Most preferably, it is fine to pulverize into particles having a size of 0.5 mm. This is because under the same temperature and pressure conditions, the curcumin extraction efficiency is rather high, although the extraction yield of turmeric extract is rather low when the turmeric dry matter is pulverized to the above particle size range than the medium grinding to larger particle size than 1 mm. to be.

In this regard, in Examples 8 and 11 of the present invention, the supercritical extraction conditions were set to the same temperature and pressure as 60 ° C. and 250 bar, respectively, and only the grain size of turmeric dry matter was changed to 2 mm and 0.5 mm, respectively. As a result of performing the critical extraction, as shown in Table 2, the extraction yield of turmeric extract was 8.0% and 7.0%, respectively, which was rather high in Example 8 which was pulverized to a particle size of 2 mm, but the extraction efficiency of curcumin, The content of curcumin contained in the turmeric extract can be seen to be significantly higher in Example 11, which was pulverized to a particle size of 0.5 mm as shown in Table 3. This can be seen that the same tendency also in Examples 9 and 12 with the temperature and pressure set to 60 ℃ and 350 bar as the supercritical extraction conditions, the particle size significantly affects the curcumin extraction efficiency It can be seen that it is an important influence factor.

Step 3 is a step of supercritical extraction of the turmeric powder with supercritical carbon dioxide at a temperature of 40 to 60 ℃ and a pressure of 150 to 350 bar, supercritical extraction of pretreatment turmeric under a certain extraction conditions curcumin derived Extracting step.

The supercritical extraction of step 3 is particularly preferably performed at a temperature of 60 ° C. and a pressure of 250 to 350 bar in terms of curcumin extraction efficiency.

In this regard, in the embodiment of the present invention, using fine grinding (0.5 mm) or medium grinding (2 mm) turmeric powder obtained in step 2), the temperature is adjusted to 40, 50 and 60 ℃ under supercritical extraction conditions , By adjusting the pressure to 150, 250 and 350 bar at each temperature condition to obtain a turmeric-derived supercritical extract under each extraction condition and to investigate the content of curcumin in each extract. As a result, it was found that the curcumin content in the turmeric supercritical extract obtained at 60 ° C. and 350 bar was the highest in the case of unpulverized turmeric powder, and the extract condition was 60 ° C. and 250 bar in the case of medium-pulverized turmeric powder. Curcumin content in the turmeric supercritical extract obtained in was confirmed that the highest. In particular, the curcumin content in the turmeric supercritical extract obtained at 60 ° C. and 350 bar extraction conditions using pulverized turmeric powder was used in the turmeric supercritical extract obtained at 60 ° C. and 250 bar extraction conditions using medium grinding turmeric powder. 1.7 times higher than the curcumin content was confirmed (Table 3). Thus, it can be seen that the extraction temperature is suitable for curcumin extraction efficiency regardless of other influence factors, and the extraction pressure is appropriately selected according to the particle size of turmeric powder.

The supercritical extraction of step 3 may be performed using an additional cosolvent. The use of additional cosolvents is preferred in terms of extraction efficiency.

The cosolvent may be used in a volume of 1 to 10% by volume in the mixture with the entire supercritical fluid, and preferably in an amount of 4% by volume in terms of extraction efficiency.

Cosolvents that can be used include ethanol.

In step 4, the extract is concentrated, and the extract is concentrated to remove moisture in the turmeric extract obtained by the extraction.

The concentration can be carried out using conventional thickeners known in the art.

Step 5 is a step of separating and purifying curcumin from the concentrate, and separating and purifying curcumin in the concentrate of the turmeric extract obtained by concentration.

Separation and purification of the curcumin can be carried out using conventional methods known in the art.

Curcumin-derived curcumin extraction method of the present invention by using a supercritical fluid extraction method was almost no residual solvent, the HPLC analysis results showed that the content of curcumin is extracted higher than the existing hot water extraction and solvent extraction.

The present invention is the hot air drying of turmeric to pulverize the turmeric dry to a particle size of 0.5 to 2 mm and then under a temperature of 40 to 60 ℃ and a pressure of 150 to 350 bar, in particular a particle size of 0.5 mm, a temperature of 60 ℃ and Supercritical extraction with supercritical carbon dioxide under a pressure of 350 bar has the effect of providing a high efficiency extraction of curcumin, particularly from turmeric.

1 is a photograph showing the appearance of turmeric used for supercritical extraction. At this time, a is the state of turmeric raw material before pretreatment, b is the state of turmeric powder after medium grinding, and c is the state of turmeric powder after medium grinding supercritical extraction. d is the appearance of turmeric powder after pulverization, e is the appearance of turmeric powder after supercritical extraction at 60 ℃, 350 bar after pulverization.
Figure 2 is the HPLC analysis results measured at 280 nm for turmeric hydrothermal extract.
Figure 3 is the HPLC analysis results measured at 430 nm for turmeric hydrothermal extract.
Figure 4 is the HPLC analysis results measured at 280 nm for the turmeric supercritical extract obtained by supercritical extraction at 60 ℃, 350 bar after pulverization to 0.5 mm.
Figure 5 is the HPLC analysis results measured at 430 nm for the turmeric supercritical extract obtained by supercritical extraction at 60 ℃, 350 bar after pulverization to 0.5 mm.
Figure 6 is a graph showing the curcumin content change measured in the UV 280 nm region for each turmeric extract obtained by varying the extraction conditions of temperature and pressure and pretreatment conditions of particle size. In FIG. 6, milling means pulverizing to a particle size of 2 mm, and fine grinding means pulverizing to a particle size of 0.5 mm.
7 is a graph showing the curcumin content change measured in the UV 430 nm region for each turmeric extract obtained by varying the extraction conditions of temperature and pressure and pretreatment conditions of particle size. In FIG. 7, milling means pulverizing to a particle size of 2 mm, and fine grinding means pulverizing to a particle size of 0.5 mm.
FIG. 8 shows UV when supercritical extraction is performed at 60 ° C. after fine grinding or milling to 2 mm to determine the effect of particle size on curcumin extraction efficiency. It is a graph showing the curcumin content change measured in the 280 nm region. In FIG. 8, milling means pulverizing to a particle size of 2 mm, and fine grinding means pulverizing to a particle size of 0.5 mm.
FIG. 9 is a case of supercritical extraction by varying the pressure at 60 ° C. after fine grinding or milling at 2 mm, respectively, to determine the effect of particle size on curcumin extraction efficiency. It is a graph showing the curcumin content change measured in the 430 nm region. In FIG. 9, milling means pulverizing to a particle size of 2 mm, and fine grinding means crushing to a particle size of 0.5 mm.

Hereinafter, the present invention will be described in more detail with reference to Examples. These embodiments are only for describing the present invention more specifically, and the scope of the present invention is not limited by these examples.

Example  1-12: Turmeric Supercritical  extraction

Jindo turmeric was hot-air dried at 50 ° C. for 3 days and then pretreated by using a grinder to finely grind to a particle size of 0.5 mm or to a heavy particle size of 2 mm.

The supercritical extraction device (ISA-SCFE-) under each extraction condition by adjusting the temperature to 40, 50 and 60 ℃ as the supercritical extraction conditions, and the pressure to 150, 250 and 350 bar at each temperature condition as shown in Table 1 below. 0050-0100-080-re, Ilshin Autoclave, South Korea), and the pretreated turmeric powder having the particle size as shown in Table 1 below was injected in an amount of 200 g and supercritical extraction was performed for 90 minutes for each turmeric sample. Was carried out. The flow rate of the supercritical extraction was 75 ml per minute, and 4 vol% (3 ml) of ethanol (alcohol) was used as a cosolvent with supercritical carbon dioxide.

Example No. Temperature (℃) Pressure (bar) Particle size (mm) One 40 150 2 2 40 250 2 3 40 350 2 4 50 150 2 5 50 250 2 6 50 350 2 7 60 150 2 8 60 250 2 9 60 350 2 10 60 150 0.5 11 60 250 0.5 12 60 350 0.5

When the supercritical extraction was completed, the extraction tank was recovered by lowering the pressure of the extraction tank of the supercritical extraction device to release the supercritical fluid. The recovered extract was concentrated using a concentrator.

Figure 1 shows the appearance of turmeric used for supercritical extraction. At this time, a is the state of turmeric raw material before pretreatment, b is the state of turmeric powder after medium grinding, and c was the state of turmeric powder after medium grinding supercritical extraction. d is the appearance of turmeric powder after pulverization, e was the appearance of turmeric powder after supercritical extraction at 60 ℃, 350 bar after pulverization.

Experimental Example  1: according to the temperature and pressure extraction conditions Extraction yield  Research

The extraction yield of turmeric extract obtained in Examples 1 to 9 was investigated, and the results are shown in Table 2 below.

Example No. Injection sample volume (g) Sample amount after extraction (g) Weight loss (g) Extraction yield (%) Example 1 200 190 10 5.0 Example 2 200 192 8 4.0 Example 3 200 189 11 5.5 Example 4 200 186 14 7.0 Example 5 200 185 15 7.5 Example 6 200 185 15 7.5 Example 7 200 186 14 7.0 Example 8 200 184 16 8.0 Example 9 200 184 16 8.0 Example 10 200 187 13 6.5 Example 11 200 186 14 7.0 Example 12 200 186 14 7.0

As can be seen in Table 2, the extraction yield is about 4 ~ 8% extraction depending on the pressure, it can be seen that the extraction efficiency is high when the temperature and pressure is high.

In addition, it can be seen that as the particle size of turmeric powder decreases, the extraction yield of turmeric extract is somewhat smaller at the same extraction temperature and extraction pressure.

Experimental Example  2: Turmeric Supercritical  Extract ingredient investigation

The components were investigated by performing HPLC analysis on the turmeric supercritical extract of Example 12, which was obtained by the extraction of 0.5 mm fine grinding pretreatment and extraction conditions of 60 ° C. and 350 bar among the turmeric supercritical extracts of Examples 1 to 12. .

On the other hand, turmeric hot water extract was used as a control for comparing the curcumin content. The turmeric hot water extract was obtained by drying hot air at Jindosan turmeric for 3 days at 50 ° C., pulverizing it to a size of 0.5 mm using a grinder, and extracting it with hot water at 100 ° C. for 90 minutes, and then concentrating.

HPLC analysis was carried out using UFLC (Prominece UFLCXR, Shimadzu, Japan) equipped with a Shim-pack VP-ODS (250L × 4.6) column with 1 μL injection volume and 2% acetic acid (Merck, Germany) as mobile phase. ) And acetonitrile (JT Baker, USA) were used in a concentration gradient (acetonitrile content: 45% to 100% by weight) and eluted at a flow rate of 1.2 mL / min for 45 minutes. The temperature of the oven was 40 ° C., and the eluted material was detected using a PDA (SPD-M20A, UV: 190 nm-800 nm, Shimadzu Corp, Japan) as a detector. Curcumin purchased from Sigma was used as a standard.

HPLC analysis results for each turmeric extract are shown in FIGS. 2 to 5.

It can be seen from Figures 2 to 5 that the curcumin content in the turmeric extract extracted with the supercritical fluid of Example 12 was 84 times higher at 430 nm compared to the hydrothermal extract of the control.

Experimental Example  3: Turmeric Supercritical  Extract Curcumin  Content investigation

HPLC analysis was performed on the turmeric supercritical extracts obtained in Examples 1 to 12 to investigate the amount of curcumin contained in each extract.

HPLC analysis was carried out using UFLC (Prominece UFLCXR, Shimadzu, Japan) equipped with a Shim-pack VP-ODS (250L × 4.6) column with 1 μL injection volume and 2% acetic acid (Merck, Germany) as mobile phase. ) And acetonitrile (JT Baker, USA) were used in a concentration gradient (acetonitrile content: 45% to 100% by weight) and eluted at a flow rate of 1.2 mL / min for 45 minutes. The temperature of the oven was 40 ° C., and the eluted material was detected using a PDA (UV: 280, 430 nm) as a detector. Curcumin purchased from Sigma was used as a standard. Each analysis was performed twice, and the results are expressed as average values.

The HPLC analysis results are shown in Table 3 below.

Example No. Curcumin content (ppm) measured at 280 nm Curcumin content (ppm) measured at 430 nm One 163.978 515.181 2 225.551 213.538 3 497.567 482.498 4 242.704 226.314 5 412.185 394.407 6 412.257 393.756 7 393.529 370.946 8 902.259 866.149 9 375.787 349.989 10 218.034 180.155 11 1249.713 1167.116 12 1545.740 1426.876

Meanwhile, the curcumin content changes measured in the UV 280 nm and 430 nm regions, respectively, are shown in FIGS. 6 and 7, respectively.

As a result, it was confirmed that curcumin content was the highest in the turmeric supercritical extract obtained under the pretreatment conditions of 0.5 mm particle size and the extraction conditions of 60 ° C. and 350 bar in Example 12, whereby the extraction conditions resulted in the extraction of curcumin derived from turmeric. It was found that the most suitable for.

In particular, the curcumin content was significantly changed according to the change of pressure and particle size at 60 ℃ extraction conditions, and it was confirmed that the pressure and particle size control greatly influenced the curcumin extraction efficiency. It was found to be an influencing factor.

In addition, the changes in the curcumin content according to the particle size change in the extraction conditions of 60 ℃, 350 bar the same temperature and pressure are shown in Figures 8 and 9.

As a result, the curcumin content significantly changes according to the particle size of the turmeric dried material at the same temperature and pressure, indicating that the particle size is an important influence factor that greatly affects the curcumin extraction efficiency.

Claims (7)

Turmeric-derived curcumin extraction method comprising the following steps:
Hot air drying the turmeric (step 1);
Grinding the turmeric dry matter to a particle size of 0.5 to 2 mm (step 2); And
Supercritical extraction of the turmeric powder with supercritical carbon dioxide at a temperature of 40 to 60 ° C. and a pressure of 150 to 350 bar (step 3).
The turmeric-derived curcumin extraction method according to claim 1, wherein the grinding of step 2 is pulverized to a size of 0.5 to 1 mm.
The method of claim 1, wherein the supercritical extraction of step 3 is carried out at a temperature of 60 ℃ and pressure of 250 to 350 bar.
The method of claim 1, wherein the supercritical extraction of step 3 is performed by further using ethanol as a cosolvent.
The method of claim 1, further comprising concentrating the extract after step 3, turmeric-derived curcumin extraction method.
According to claim 1, wherein step 1 is carried out at 40 to 50 ℃, turmeric-derived curcumin extraction method.
According to claim 1, wherein Step 1 is carried out for 1 to 5 days, turmeric-derived curcumin extraction method.

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