Tree extract and method for producing the same

Abstract

To provide a useful tree extract further extracted from refined water, a distillation residue or the like obtained by microwave reduced-pressure steam distillation technique.SOLUTION: A tree extract is obtained by a production method including following steps (a)-(d): (a) heating tree raw material 1 by microwave under reduced pressure for distillation, and separating a distilled tree residue and a distillate; (b) separating an aqueous fraction 7 from the distillate obtained in the step (a); (c) extracting the tree raw material and / or the distilled tree residue with the aqueous fraction obtained in the step (b); and (d), after the extraction treatment in the step (c), removing the extraction residue to obtain an extract.SELECTED DRAWING: Figure 1

Description

Technical Field

[0001] The present invention relates to a tree extract obtained by performing an extraction process using an aqueous fraction of a microwave vacuum distillate of a tree as an extraction solvent and a tree raw material and / or a microwave vacuum distillation residue of a tree as an extraction raw material, and a method for producing the same.

Background Art

[0002] Previously, due to a shortage of successors and a decline in wood prices, mountain forests have not been properly maintained, and their neglect has become a major problem. The maintenance of these mountain forests mainly involves thinning and pruning. However, if the thinned wood and the branches and leaves cut during pruning have no economic value and only incur costs, it is natural that such maintenance will be neglected.

[0003] Therefore, in recent years, attempts have been made to process the wood targeted for thinning and the like into useful resources. For example, after thinning wood is made into chips, it is steamed and used as livestock feed.

[0004] However, the above method requires large equipment for chipping and steaming and is not easily adopted anywhere. In addition, there is no known effective utilization method for the branches and leaves, not to mention the wood itself.

[0005] As a technology for effectively utilizing this wood and branches and leaves, the present applicants have reported that high-value essential oils and essence water can be obtained by a microwave vacuum distillation method in which the xylem and its leaves are distilled under specific apparatuses and conditions (Patent Document 1).

Prior Art Documents

Patent Documents

[0006]

Patent Document 1

Summary of the Invention

Problems to be Solved by the Invention

[0007] The object of the present invention is to obtain even more useful components from purified water, distillation residue, etc., obtained by the above-described microwave reduced-pressure steam distillation technology. [Means for solving the problem]

[0008] As a result of diligent research to solve the above problems, the inventors of the present invention have found that by using the aqueous fraction of the distillate obtained by microwave vacuum distillation of trees as an extraction solvent, and by extracting the tree raw material or its distillation residue, an extract with excellent deodorizing activity and nitrogen oxide removal activity can be obtained, thus completing the present invention.

[0009] In other words, the present invention involves the following steps (a) to (d); (a) A process of heating and distilling tree raw materials using microwaves under reduced pressure, and separating the tree distillation residue from the distillate. (b) A step of separating the aqueous fraction from the distillate obtained in step (a). (c) Extracting tree raw materials and / or tree distillation residues with the aqueous fraction obtained in step (b). (d) A step to obtain an extract by removing the extraction residue after the extraction process in step (c). This is a tree extract characterized by being obtained by a manufacturing method that includes [a specific ingredient / method]. [Effects of the Invention]

[0010] The tree extract of the present invention has excellent deodorizing effects, harmful oxide removal effects such as nitrogen oxides, and antioxidant effects. When used in fragrances, deodorizing components, analgesics, anti-inflammatory topical agents (analgesic tablets, cosmetic creams, soft drinks), antiviral agents, bath additives (foot bath additives), etc., even better effects can be obtained. Furthermore, it exhibits excellent effects when kneaded into or incorporated into garbage bags, trash cans, pillows, futons, carpets, etc. [Brief explanation of the drawing]

[0011] [Figure 1] This is a schematic diagram showing steps (a) and (b) of the present invention. [Figure 2] This is a schematic diagram showing step (c) of the present invention. [Figure 3] This is a schematic diagram showing step (d) of the present invention. [Modes for carrying out the invention]

[0012] The trees used as raw materials for the present invention are not particularly limited, but examples include the genus Chamaecyparis in the family Cupressaceae, the genus Thuja in the family Cupressaceae, the genus Juniper in the family Cupressaceae, the genus Cryptomeria in the family Cupressaceae, the genus Abies in the family Pinaceae, the genus Cedrus in the family Pinaceae, the genus Picea in the family Pinaceae, the genus Larch in the family Pinaceae, the genus Hemlock in the family Myrtaceae, the genus Sciadopitys in the family Sciadopityaceae, the genus Torreya in the family Taxaceae, and the genus Thujopsis in the family Cupressaceae.

[0013] Trees belonging to the genus Chamaecyparis in the family Cupressaceae include Japanese cypress (Hinoki), Taiwanese cypress (Hinoki), Western cypress (Hinoki), Lawson cypress (Hinoki), Chamaecyparis obtusa (Hinoki), Sawara cypress (Hinoki), Peacock cypress (Hinoki), Golden Chamaecyparis obtusa (Hinoki), Water cypress (Hinoki), Thread cypress (Hinoki), Golden cypress (Hinoki), Davallia cypress (Hinoki), Golden Davallia cypress (Hinoki), and Japanese cedar (Hinoki). Trees belonging to the genus Thuja in the family Cupressaceae include Japanese cypress (Hinoki), Japanese cedar (Hinoki), Japanese cedar (Hinoki), Pencil cedar (Hinoki), and Okinawa cedar (Hinoki). Trees belonging to the genus Cryptomeria in the family Cupressaceae include Japanese cedar (Sugi), Japanese cedar (Ashisugi), Japanese cedar (Enkosugi), Japanese cedar (Yoresugi), Golden cedar (Sugi), Japanese cedar (Sekkasugi), and Green cedar (Midorisugi).

[0014] Trees belonging to the genus Abies in the family Pinaceae include fir, Abies firma, Abies veitchii, Abies mariesii, Abies veitchii, Abies veitchii, Abies balsam, Abies sachalinensis, White fir, Abies amavillea, Abies sachalinensis, California red fir, Grand fir, and Noble fir. Trees belonging to the genus Picea in the family Pinaceae include Sakhalin spruce and Spruce. Trees belonging to the genus Pinus in the family Pinaceae include Japanese red pine, Japanese pine, Eastern white pine, and Japanese stone pine. Trees belonging to the genus Larix in the family Pinaceae include Japanese larch. Trees belonging to the genus Hemlock in the family Pinaceae include Hemlock.

[0015] Examples of trees of the genus Eucalyptus of the Myrtaceae family include Eucalyptus, Eucalyptus gunnii, Eucalyptus camaldulensis, Eucalyptus citriodora, etc.

[0016] Examples of trees of the genus Castanopsis of the Fagaceae family include Castanopsis cuspidata, etc.

[0017] Examples of trees of the genus Cryptomeria of the Taxodiaceae family include Cryptomeria japonica, etc.

[0018] Examples of trees of the genus Chamaecyparis of the Cupressaceae family include Chamaecyparis obtusa, Chamaecyparis formosensis, Chamaecyparis pisifera, Chamaecyparis lawsoniana, etc.

[0019] Among the above-mentioned trees, the genera Cryptomeria, Sugi, Abies, Eucalyptus, Castanopsis, and Chamaecyparis are preferred. Since they are widely distributed in Japan and easily available, Cryptomeria japonica, Cryptomeria formosensis, Chamaecyparis obtusa, Cryptomeria fortunei, Sugi of the genus Sugi of the Cupressaceae family, Abies sachalinensis, Abies firma, Eucalyptus of the genus Eucalyptus of the Myrtaceae family, Castanopsis cuspidata of the genus Castanopsis of the Fagaceae family, and Chamaecyparis obtusa of the genus Chamaecyparis of the Cupressaceae family are more preferred. These trees may be combined in multiple species.

[0020] The parts of the above-mentioned trees are not particularly limited, but it is preferable to use the xylem and / or leaves. Heat under reduced pressure with microwaves and distill with the moisture contained in the tree to separate the tree distillation residue, which is a fibrous component from which at least part of the oil and moisture have been removed by distillation, and the distillate. Such an operation is called microwave reduced-pressure steam distillation as a method for obtaining the distillate and reduced-pressure drying as a method for obtaining the fibrous component. These methods can be carried out using, for example, a microwave distillation apparatus equipped with a distillation tank, a microwave heating device, a cooling device, a pump, etc. described in International Publication WO2010 / 098440 pamphlet, etc.

[0021] The present invention will be described below with reference to FIGS. 1 to 3. In the figures, 1 represents the xylem and / or leaves of a tree, 2 represents a distillation tank, 3 represents a microwave heating device, 4 represents a cooling device, 5 represents a pump, 6 represents an oily fraction (essential oil) of the distillate, 7 represents an aqueous fraction (refined water) of the distillate, 8 represents an extraction raw material, and 9 represents an extraction residue, and 10 represents an extract.

[0022] The processes (a) and (b) will be described below with reference to FIG. 1. In the microwave distillation apparatus shown in FIG. 1, the distillation tank 2, the cooling device 4, and the pump 5 are connected in this order. A microwave heating device 3 is installed on the upper surface of the distillation tank 2, and microwaves are radiated therefrom to heat the xylem and / or leaves of the raw material tree placed in the distillation tank 2. An air flow inlet pipe (not shown) is connected to the distillation tank 2. Separately, a distillate outflow pipe is connected to the distillation tank 2 and further connected to the cooling device 4. The air flow inlet pipe introduces a gas of air or an inert gas into the distillation tank 2. The distillate outflow pipe introduces the distillate from the raw material to the cooling device. In the present invention, no additional water is supplied to the raw material during this heating, but it is also possible to supply additional water separately.

[0023] Among the above gases, inert gases, specifically nitrogen, helium, argon, etc. are preferable. As the introduction amount of the gas, for example, the flow rate per minute may be about 0.001 to 0.1 volume times of the distillation tank 2.

[0024] Inside the distillation tank 2, the temperature and pressure can be measured by a temperature sensor and a pressure sensor (both not shown) attached thereto. Further, the temperature and pressure can be adjusted via a heating control device and a pressure control device (both not shown) connected to the distillation tank 2.

[0025] The temperature and pressure at this stage are not particularly limited as long as the raw materials can be heated under reduced pressure, but for example, the pressure is 5 to 95 kPa, preferably 10 to 60 kPa, and the heating temperature is 30 to 90°C, preferably 50 to 70°C. Note that the heating temperature refers to the temperature of the vapor measured in the distillation tank 2. The heating time is not particularly limited, but for example, it is 0.2 to 8 hours, preferably 0.4 to 6 hours.

[0026] The gaseous distillate produced by microwave irradiation of the raw material is introduced into the cooling device 4 through the distillate outlet pipe, where it is converted into a liquid and becomes distillate. Meanwhile, the distillation bed 2 remains with the tree distillation residue, from which the distillate has been removed from the raw material trees, thus separating the distillate from the tree distillation residue.

[0027] This distillate separates into an aqueous fraction and an oily fraction. Therefore, by collecting each fraction according to conventional methods, an oily fraction (essential oil) 6 and an aqueous fraction (purified water) 7 can be obtained.

[0028] Step (c) will be described below with reference to Figure 2. In step (c), the aqueous fraction 7 obtained as described above is used as the extraction solvent, and the tree raw material and / or tree residual extract are used as the extraction material 8 for extraction. The aqueous fraction 7 preferably contains 0.05% by mass or more of organic compounds such as 3-hexen-1-ol, 1-hexanol, maltol, borneol, and bornyl acetate, and preferably contains 0.1% by mass or more. The tree to be used as the extraction material (woody part of the tree and / or leaves, etc., similar to that of step (a)) and / or the tree distillation residue (residue after processing in step (a)) are placed in the distillation tank 2 of a microwave distillation apparatus with the same configuration as in Figure 1, and the aqueous fraction (purified water) 7 is added as the extraction solvent, and extraction is carried out under reduced pressure or atmospheric pressure. The amount of aqueous fraction (purified water) 7 added is not particularly limited, but for example, it is 50% to 1000%, preferably 100% to 500%, relative to the weight of the tree and / or tree distillation residue of the extraction material. Water may be added as an extraction solvent if necessary.

[0029] The temperature and pressure during extraction are not particularly limited, but for example, the pressure is 20 to 110 kPa, preferably 50 to 105 kPa, and the heating temperature is 80 to 120°C, preferably 70 to 100°C. The extraction time is also not particularly limited, but for example, it is 0.2 to 8 hours, preferably 0.4 to 6 hours.

[0030] The following describes step (d) based on Figure 3. In step (d), after the extraction process, the extraction residue 9 is separated and removed to obtain the tree extract 10. Conventional known solid-liquid separation methods can be used to separate the extraction residue 9, for example, by centrifugation, filtration, or by performing the extraction process with the extraction material placed in a mesh beforehand, and then separating the mesh after the extraction process.

[0031] The tree extract 10 obtained as described above can be used, for example, as a fragrance, deodorizing agent, nitrogen oxide remover, anti-allergic substance, sleep inducer, anti-stress substance, plant growth regulator, antiviral agent, etc.

[0032] The tree extract of the present invention contains a relatively large amount of polyphenols, and it is preferable that the total amount of polyphenols measured by the Folin-Ciocalteu method of the ethyl acetate extract, 50% methanol eluate, and 70% acetone eluate prepared from the tree extract by the method described in the examples falls within a predetermined range. Specifically, the total polyphenol content of the ethyl acetate extract is preferably 10-50% by mass, more preferably 20-40% by mass, and even more preferably 25-35% by mass; the total polyphenol content of the 50% methanol eluate is preferably 40-80% by mass, more preferably 50-70% by mass, and even more preferably 55-65% by mass; and the total polyphenol content of the 70% acetone eluate is preferably 45-85% by mass, more preferably 55-75% by mass, and even more preferably 60-70% by mass. It is thought that such polyphenols contribute to the deodorizing and nitrogen oxide removal effects of the tree extract of the present invention. [Examples]

[0033] The present invention will be described in detail below with reference to examples, but the present invention is not limited in any way to these examples.

[0034] Example 1 Preparation of aqueous fraction (purified water): (1) Microwave vacuum distillation Sixty kilograms of fir branches and leaves, representing the woody tissue and / or leaves of the tree, were placed in a distillation tank. The pressure inside the distillation tank was maintained under reduced pressure conditions of 16 kPa, and microwaves were irradiated to achieve a heating temperature (steam temperature) of 60°C. Distillation was carried out for one hour using only the water contained in the fir branches and leaves. The gas produced by this distillation was cooled in a cooling device to obtain 16 kg of aqueous fraction (purified water), 300 g of oily fraction (essential oil), and 43 kg of tree extract residue (fibrous components).

[0035] (2-1) Extraction (atmospheric pressure) 100 g of branches and leaves of fir trees were used as the woody part and / or leaves of the tree, and these, along with 400 g of the aqueous fraction (purified water) obtained in (1), were placed in a glass container measuring 21 cm × 11 cm × 14 cm. The opening was sealed with a silicone lid, and the container was maintained under atmospheric pressure (approximately 101 kPa). Microwaves were irradiated to a heating temperature (steam temperature) of 100°C, and the extraction process was carried out for 1 hour. The liquid in the glass container after extraction was filtered to separate the extraction residue from the extract, yielding 600 g of tree extract (product 1 of the present invention). This tree extract was a brown suspension with viscosity.

[0036] (2-2) Extraction (reduced pressure) process 100g of branches and leaves of fir trees were used as the woody part and / or leaves of the tree, and these, along with 400g of the aqueous fraction (purified water) obtained in (1), were placed in a glass container measuring 21cm × 11cm × 14cm. The opening was sealed with a silicone lid with a stopcock, and the container was maintained under a pressure of approximately 11kPa. Microwaves were irradiated to a heating temperature of 60°C, and extraction was carried out for 0.4 hours. The liquid in the glass container after extraction was filtered to separate the extraction residue from the extract, yielding 200g of tree extract (product 2 of the present invention). This tree extract was a brown suspension with viscosity.

[0037] (Deodorization test) 1 g of tree extracts from products 1 and 2 of the present invention were added to a 110 mm diameter filter paper, placed on a 150 mm diameter glass dish, and sealed in a 10 liter Tedlar bag. 20 ml of NH3 gas was then injected into the bag. The NH3 concentration was measured using a detector tube immediately after injection and after a certain period of time. A comparative sample (comparative sample 1) with deionized water added was also used. The results are shown in Table 1.

[0038] [Table 1]

[0039] It has been confirmed that the tree extracts of products 1 and 2 of this invention have a high deodorizing effect against ammonia.

[0040] (Nitrogen oxide removal test) One g of tree extracts from products 1 and 2 of the present invention were added to a 110 mm diameter filter paper, placed on a 150 mm diameter glass dish, and sealed in a 10 liter Tedlar bag. One liter of NO2 gas was then injected into the bag. The NO2 concentration was measured using a detector tube immediately after injection and after a certain period of time. For comparison, a sample with deionized water added (comparative sample 1) was used. The results are shown in Table 2.

[0041] [Table 2]

[0042] Both the tree extracts of products 1 and 2 of the present invention were found to have a high nitrogen oxide removal effect.

[0043] Example 2 Air conditioner filter: 1000g of the tree extract of product 1 of this invention is placed in a pad and then placed on a breathable cellulose nonwoven fabric (basis weight: 100g / m²). 3 I soaked it in (Futamura Chemical Co., Ltd.) and dried it to create an air conditioner filter.

[0044] Implementation Example 3 Measurement of total polyphenol content:

[0045] 200 g of branches and leaves of fir trees were used as the woody part and / or leaves of the tree. These were placed in a 21 cm × 11 cm × 14 cm glass container along with 800 g of the aqueous fraction (purified water) obtained in Example 1(1). The opening was sealed with a silicone lid with a stopcock, and the container was maintained under a pressure of approximately 10 kPa. Microwaves were irradiated to a heating temperature of 56°C, and extraction was carried out for 0.5 hours. The liquid in the glass container after extraction was filtered, and the extraction residue was further washed four times with 100 ml of distilled water to obtain a tree extract (product 3 of the present invention). This tree extract was a brown suspension with viscosity.

[0046] Experimental method 1) The sample solution was centrifuged (10,000 rpm, 20°C, 1 hour) to separate the water-insoluble and soluble parts, which were then freeze-dried. 2) 15 g of the freeze-dried water-soluble portion was dissolved in 200 mL of water, 467 mL of acetone was added, and the mixture was thoroughly stirred and centrifuged (10,000 rpm, 20°C, 1 h). The mixture was separated into a 70% acetone-insoluble portion and a soluble portion, concentrated under reduced pressure, and freeze-dried. 3) 10 g of the lyophilized portion of the 70% acetone-soluble part was dissolved in 200 mL of water, and liquid-liquid extraction was performed with 150 mL of ethyl acetate (3 times). The ethyl acetate extract was concentrated under reduced pressure and lyophilized (ethyl acetate extract). 4) The ethyl acetate extract was concentrated under reduced pressure and passed through a Sephadex LH-20 column (swelled with water). Elution was performed sequentially with 1 L of water, 1 L of 50% methanol, and 1 L of 70% acetone. Each eluate was concentrated under reduced pressure and freeze-dried to obtain the water eluate, 50% methanol eluate, and 70% acetone eluate, respectively.

[0047] The total polyphenol content of (i) ethyl acetate extract, (ii) 50% methanol eluate, and (iii) 70% acetone eluate obtained above was measured using the Folin-Ciocalteu method and the standard substance Catechin.

[0048] The measured total polyphenol content for each was: (i) The total polyphenol content of the ethyl acetate extract is 33.2% (flavonoids, etc.) (ii) The total amount of polyphenols in the 50% methanol eluate is 60% (e.g., high molecular weight polyphenol glycosides). (iii) The total amount of polyphenols in the 70% acetone eluate is 65% (condensed tannins, etc.). That was the case. These polyphenols are thought to contribute to deodorization and nitrogen oxide removal.

[0049] Implementation Example 4 Garbage bags: (1) Production of masterbatch pellets One kilogram of the spray-dried powder of Product 1 of the present invention and 90 kg of polyethylene pellets (Urtzex® 2022: manufactured by Prime Polymer Co., Ltd.) were mixed in a mixer, fed into an extruder, and extruded. The mixture was then allowed to cool naturally. Next, it was inserted into a pelletizer and cut into pellets (3 mm in diameter, 3 mm in length) to obtain polyethylene masterbatch pellets containing fibrous components. (2) Manufacturing of films and bags Polyethylene pellets (Urtzex® 2022: manufactured by Prime Polymer Co., Ltd.) were mixed with 5% by mass of the masterbatch pellets obtained in (1) above in a ribbon blender. This mixture was then melt-kneaded in an inflation film deposition machine to form a 100 μm thick film, obtaining a polyethylene film (hereinafter simply referred to as "deodorizing film") in the form of a tube. These films were then cut into 30 cm lengths to obtain garbage bags. The deodorizing film was semi-transparent and had a color that resembled a mixture of brown and gold. (3) Deodorizing performance test of garbage bags: A 100mm diameter filter paper was folded into quarters and soaked with 3.0ml of a 250ppm ammonia solution. This filter paper was placed inside the aforementioned bag, and the opening was heat-sealed. This garbage bag was placed inside a 10-liter Tedlar bag, and the ammonia concentration was measured at regular intervals using a detector tube. After 24 hours, the concentration was 0ppm, indicating no ammonia leakage. [Industrial applicability]

[0050] The tree extract of the present invention can be used as a deodorant, a nitrogen oxide remover, and the like. [Explanation of symbols]

[0051] 1. The woody part and / or leaves of a tree 2 distillation tanks 3. Microwave heating device 4 Cooling device 5 pumps 6. Oily fraction (essential oils) 7. Aqueous fraction (purified water) 8 Extraction raw material 9 Extraction residue 10 Tree extract

Claims

1. The following steps (a) to (d); (a) A process of heating the woody part and / or leaves of a tree of the genus Abies in the family Pinaceae with microwaves under reduced pressure and distilling it, and separating the wood distillation residue from the distillate. (b) A step of separating the aqueous fraction from the distillate obtained in step (a). (c) Adding to the tree raw material and / or tree distillation residue an aqueous fraction containing 0.05% by mass or more of an organic compound obtained in step (b) as an extraction solvent in an amount of 100% to 500% relative to the weight of the tree and / or tree distillation residue of the extraction raw material, and performing a heat extraction process. (d) A step in which the extraction residue is removed after the extraction process in step (c) to obtain an extract. A tree extract characterized by being obtained by a manufacturing method that includes the following.

2. The tree extract according to claim 1, wherein the extraction temperature in step (c) is 80 to 120°C.

3. The tree extract according to claim 1 or 2, wherein the pressure in step (a) is 5 to 95 kPa and the heating temperature is 30 to 90°C.

4. The tree extract according to any one of claims 1 to 3, wherein the tree is selected from the group consisting of the genus Chamaecyparis in the family Cupressaceae, the genus Cryptomeria in the family Cupressaceae, the genus Abies in the family Pinaceae, the genus Eucalyptus in the family Myrtaceae, the genus Sciadopitys in the family Sciadopityaceae, and the genus Thujopsis in the family Cupressaceae.

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