CN101461835B - Ultrasonic extraction method of Eucommia flavonoids with multi-frequency combination - Google Patents

Abstract

The invention relates to a method for multi-frequency combination ultrasonic leaching of flavonoids from eucommia, which is characterized in that two or three ultrasonic waves with different frequencies are selected within the range of between 10 and 150 kHz to act on a mixture of eucommia barks and an aqueous ethanol solution; the total intensity of the multi-frequency combination ultrasonic waves I is more than 0 and less than 1 w/cm<2>; the weight ratio of the eucommia barks to the aqueous ethanol solution is 1:4-40; and the leaching time t is more than 0 and less than 70 minutes at a leaching temperature of between 20 and 100 DEG C. The method has the advantages that the leaching effect is better than that of single-frequency ultrasonic leaching; the method has obvious advantages suchas concentration of characteristic components of the eucommia barks, leaching speed, leaching rate and so on; and the method provides a novel path for industrial application of plant component ultrasonic leaching technology.

Description

Ultrasonic extraction method of Eucommia flavonoids with multi-frequency combination

technical field

The invention relates to a method for leaching eucommia flavonoids, in particular to a multi-frequency combined ultrasonic leaching method for eucommia flavonoids.

Background technique

Leaching is one of the key technologies in traditional Chinese medicine, pharmaceuticals, biotechnology, food processing and manufacturing, flavors and fragrances, etc. Its technical level directly affects the economic and technical indicators such as product quality and cost. However, the traditional methods of extracting active ingredients such as solvent extraction, steam distillation, and sublimation have problems of high leaching temperature, long leaching time, changes in the structure and properties of active ingredients, low leaching rate, and leaching. Some inherent defects such as low efficiency.

Ultrasonic waves are mechanical waves with a frequency in the range of 2×10 ^-3 Hz to 10×10 ⁹ Hz. Ultrasound is a kind of elastic wave. Its vibration can not only generate powerful energy, but the energy is continuously absorbed by the medium particle and turned into heat energy during the propagation process of the medium particle, which causes the temperature of the medium particle to rise, and the sound wave enters the plant tissue cells deeper and stays longer. Longer; high-energy ultrasonic waves act on the liquid to be torn into many small cavities, and when these small cavities are closed, an instantaneous pressure of up to several thousand atmospheres can be generated to act on the cavitation of plant tissues; ultrasonic waves use Mechanical effects also produce stirring, dispersion, impact crushing and fatigue damage, which accelerate the change of certain physical, chemical and biological properties of substances; especially can lead to the collapse and rupture of cells such as animals, plants, microorganisms, etc., which is conducive to solvent penetration , and strengthen the release of intracellular components, which is conducive to the dissolution and diffusion of intracellular components; moreover, as long as the appropriate ultrasonic intensity is controlled, it will not cause changes in the structure and properties of chemical components. Ultrasonic leaching can greatly shorten the leaching time and increase the leaching rate, especially for low-temperature leaching of heat-sensitive components, showing special technical advantages.

Because ultrasonic leaching can overcome the shortcomings of traditional leaching techniques, people have a wide range of plants (including roots, stems, leaves, flowers, seed coats, etc.) and some large fungi, algae, etc., including flavonoids, The single-frequency ultrasonic leaching technology of various components such as alkaloids, pigments, polysaccharides, volatile oils, and fats has been extensively studied, and the technical advantages of ultrasonic leaching have been proved. Single-frequency ultrasonic extraction technology has become a fast and simple standard extraction method for measuring the content of active ingredients in Chinese herbal medicines stipulated in the Chinese Pharmacopoeia.

At present, although single-frequency ultrasonic leaching technology has achieved a lot of results in the leaching of active ingredients, it is found that different frequencies of ultrasonic waves have different characteristics. Some frequencies are suitable for breaking solids; The strong vortex disturbance strengthens the mass transfer process by reducing the mass transfer boundary layer at the solid-liquid interface. Therefore, the single-frequency ultrasonic leaching technology cannot be efficiently used to extract the active ingredients in all solids. The optimal ultrasonic frequencies for different solids and different components are quite different, and the ultrasonic power required for single-frequency leaching is relatively large. These defects hinder the industrialization of ultrasonic leaching technology.

Contents of the invention

The purpose of the present invention is to provide a multi-frequency combination ultrasonic leaching method of eucommia flavonoids. Low-frequency ultrasonic waves can cause the collapse and rupture of cells such as animals, plants, and microorganisms, which is beneficial to the solvent penetration and strengthen the release of intracellular components. And high-frequency ultrasound is beneficial to the dissolution and diffusion of intracellular components, and they are used together and played at the same time; thereby obtaining the effective components of plant leaves that cannot be obtained by single-frequency ultrasonic leaching.

To achieve the above object, the present invention takes the following schemes:

In ^this method, two or three ultrasonic waves with different frequencies are selected in the range of 10-150 kHz to act on the mixture of Eucommia ulmoides and ethanol aqueous solution, the total intensity I of multi-frequency combined ultrasonic waves is 0<I<1w/cm The weight ratio is 1:4-40, and the leaching time t is 0<t<70min at the leaching temperature of 20-100°C.

The two ultrasonic waves with different frequencies are selected from any of the following three frequency ranges: 10-40kHz, 20-60kHz, and 50-150kHz. Only one frequency ultrasonic wave is selected in each range as a multi-frequency combination Fundamental frequency ultrasound for ultrasonic leaching.

For the three ultrasonic waves of different frequencies, one ultrasonic wave is selected from the range of 10-40 kHz, another ultrasonic wave of different frequencies is selected within the range of 20-60 kHz, and the third ultrasonic wave of different frequencies is selected within the range of 50-150 kHz, as a multi-frequency Combined ultrasonic leaching with fundamental frequency ultrasound.

The difference frequency of two ultrasonic waves with different frequencies should be in the range of 5~90kHz.

The leaching method may be a multi-frequency composite ultrasonic leaching method, in which two or three different frequency ultrasonic waves acting on the mixture of eucommia ulmoides and ethanol aqueous solution act simultaneously.

The leaching method can also be a multi-frequency alternating ultrasonic leaching method, in which two or three ultrasonic waves of different frequencies act on the mixture of eucommia ulmoides and ethanol solution alternately.

The leaching is a batch operation or a continuous operation.

The weight ratio of Eucommia ulmoides and polar solvents is also called the solid-to-liquid ratio.

In the present invention, the unit of ethanol aqueous solution is volume percent.

The advantages of the present invention are: the result of utilizing the method of the present invention to extract is better than the effect of single-frequency ultrasonic extraction, and the concentration of the characteristic components of Eucommia ulmoides, extraction speed, extraction rate, etc. have greater advantages, for The industrial application of ultrasonic leaching technology of plant components provides a new way.

Detailed ways

The goal of the extraction operation is to extract as many soluble solids in plants, especially the main characteristic components such as flavonoids and pigments as possible. The indicators for evaluating the technical level of the process include the concentration and extraction rate of total flavonoids.

Example 1:

Adopt single-frequency ultrasonic wave intermittently to extract Eucommia ulmoides, use 135kHz, the intensity is the ultrasonic wave of 0.2w/cm ² , leaching 35min with 20% ethanol aqueous solution (volume percentage) at 60 ℃ with the solid-liquid ratio of 1:14, the total flavonoids Concentration 0.91mg/mL. Using single-frequency ultrasound to intermittently extract Eucommia ulmoides, using 28kHz ultrasonic waves with an intensity of 0.8w/ ^cm2 , leaching with 65% ethanol aqueous solution at 60°C for 5 minutes at a solid-to-liquid ratio of 1:24, the extraction rate of total flavonoids is 79.9% %.

Example 2:

If dual-frequency composite ultrasound is used for intermittent leaching of Eucommia, two frequencies of 28kHz and 40kHz are used to act together, with a total intensity of 0.4w/cm ² . Take 15min, the extraction rate of total flavonoids is 67.7%. If dual-frequency composite ultrasound is used for intermittent leaching of Eucommia ulmoides, two frequencies of 50kHz and 135kHz are used to act together, with a total intensity of 0.2w/cm ² . Take 5min, the concentration of total flavonoids is 0.99mg/mL.

Example 3:

If dual-frequency alternating ultrasonic waves are used to leaching Eucommia intermittently, two ultrasonic frequencies of 20kHz and 135kHz are used alternately, with a total intensity of 0.4w/cm ² . After leaching for 35 minutes, the extraction rate of total flavonoids was 77.04%. If dual-frequency alternating ultrasonic waves are used to extract Eucommia intermittently, two ultrasonic frequencies of 20kHz and 28kHz are used alternately, with a total intensity of 0.1w/cm ² . After leaching for 35 minutes, the concentration of total flavonoids was 0.98mg/mL.

Example 4:

If three-frequency compound ultrasonic waves are used for intermittent leaching of Eucommia, three frequencies of 20kHz, 50kHz and 135kHz are used to act together, with a total intensity of 0.3w/cm ² . The aqueous solution was leached for 35 minutes, and the leaching rate of total flavonoids was 91.6%. If three-frequency compound ultrasonic waves are used for intermittent leaching of Eucommia, three frequencies of ultrasonic waves of 20kHz, 50kHz and 135kHz are used to act together, and the ultrasonic intensity is 0.25w/cm ² . After leaching for 15 minutes, the total flavonoid concentration was 1.19mg/ml.

Example 5:

If three-frequency alternating ultrasonic waves are used to intermittently extract Eucommia ulmoides, three frequencies of ultrasonic waves of 20kHz, 50kHz and 135kHz are used alternately, with a total intensity of 0.75w/cm ² . Ethanol aqueous solution leaching for 35min, the extraction rate of total flavonoids was 88.0%. If three-frequency alternating ultrasonic waves are used for intermittent leaching of Eucommia, three frequencies of ultrasonic waves of 20kHz, 50kHz and 135kHz are used alternately, and the ultrasonic intensity is 0.30w/cm ² . ℃ leaching for 35min, the total flavonoid concentration was 1.12mg/ml.

Embodiment 6:

If 25kHz single-frequency ultrasound is used for continuous countercurrent leaching of Eucommia, the total strength is 2400w, and leaching with 70% ethanol aqueous solution for 65min at 40°C with a solid-liquid ratio of 1:29, the concentration of total flavonoids is 0.256mg/ml. And 90kHz single-frequency ultrasonic continuous countercurrent leaching of Eucommia, the total strength is 2400w, leaching with 70% ethanol aqueous solution at 40°C for 65min at a solid-liquid ratio of 1:21, the leaching rate of total flavonoids is 74.9%.

Embodiment 7:

If 25kHz and 50kHz dual-frequency composite ultrasonic continuous countercurrent leaching of Eucommia is adopted, the total strength is 2400w, and the concentration of total flavonoids is 0.274mg/ml when leaching with 70% ethanol water for 55min at 50°C with a solid-liquid ratio of 1:9 . And adopt 50kHz and 90kHz dual-frequency composite ultrasonic continuous countercurrent leaching Eucommia, the total strength is 2400w, with 1: 17 solid-liquid ratio at 50 ℃ with 55% ethanol aqueous solution leaching 27min, the leaching rate of total flavonoids is 57.5% .

Embodiment 8:

If 50/90kHz dual-frequency alternating ultrasonic continuous countercurrent leaching of Eucommia is adopted, the total strength is 2400w, and the concentration of total flavonoids is 0.243mg/ ml. And adopt 25kHz and 90kHz dual-frequency alternating ultrasonic continuous countercurrent leaching Eucommia, the total strength is 1600w, with 1: 25 solid-liquid ratio at 30 ℃ with 70% ethanol aqueous solution leaching 65min, the leaching rate of total flavonoids is 91.8 %.

Embodiment 9:

If 25kHz, 50kHz, 90kHz three-frequency compound ultrasonic continuous countercurrent leaching is used to extract Eucommia ulmoides, the total strength is 2400w, and leaching with 70% ethanol aqueous solution for 65min at 50°C with a solid-liquid ratio of 1:9, the concentration of total flavonoids is 0.341mg /ml. And adopt 25kHz, 50kHz, 90kHz triple-frequency composite ultrasonic continuous countercurrent leaching Eucommia, the total strength is 2400w, with 1:9 solid-liquid ratio at 50 ℃ with 70% ethanol aqueous solution leaching 65min, the leaching rate of total flavonoids 68.3%.

Example 10:

If 25kHz, 50kHz, 90kHz three-frequency alternating ultrasonic continuous countercurrent leaching of Eucommia is used, the total strength is 2400w, and the concentration of total flavonoids is 0.273 mg/ml. And 25kHz, 50kHz, 90kHz three-frequency alternating ultrasonic continuous countercurrent leaching Eucommia, the total strength is 2400w, with 1:9 solid-liquid ratio at 50 ℃ with 70% ethanol aqueous solution leaching 65min, the leaching rate of total flavonoids was 65.9%.

Claims (4)

1. multiplefrequency combined ultrasound leaching method for eucommia bark flavone is characterized in that: select the ultrasound wave of two different frequencies to act on the mixture of the Cortex Eucommiae and ethanol water in 10～150kHz scope, the overall strength I of multi-frequency combined ultrasonic ripple is 0＜I＜1w/cm ², the weight ratio of the Cortex Eucommiae and ethanol water is 1: 4～40, is that 20～100 ℃ of following leaching time t are 0＜t＜70min at leaching temperature; The ultrasound wave of two different frequencies is two scopes of any selection from following three frequency range 10～40kHz, 20～60kHz, 50～150kHz, only select the ultrasound wave of a frequency in each scope, as the fundamental frequency ultrasound wave of multiplefrequency combined ultrasound leaching; Two hyperacoustic difference frequencies of different frequency should be in 5～90kHz scope.

2. multiplefrequency combined ultrasound leaching method for eucommia bark flavone according to claim 1 is characterized in that: described leaching method is a multifrequency composite ultraphonic leaching method, and its different frequency ultrasound wave that acts on the mixture of the Cortex Eucommiae and ethanol water is effect simultaneously.

3. multiplefrequency combined ultrasound leaching method for eucommia bark flavone according to claim 1 is characterized in that: described leaching method is a multifrequency alternation supersonic leaching method, and its different frequency ultrasound wave that acts on the mixture of the Cortex Eucommiae and ethanol water is an alternating action.

4. multiplefrequency combined ultrasound leaching method for eucommia bark flavone according to claim 1 is characterized in that: leach and be intermittently operated or continued operation.