Environment-friendly filler for preparing aquilaria sinensis and method for preparing aquilaria sinensis

Abstract

The application discloses an environment-friendly filler for preparing agarwood of Aquilaria sinensis and a preparation method of agarwood of Aquilaria sinensis, and comprises the following steps: (1) preparation of agricultural and forestry waste powder; (2) preparation of modified montmorillonite; (3) preparation of modified flake graphite; and (4) preparation of the environment-friendly filler. The environment-friendly filler takes agricultural and forestry waste as a main raw material, realizes comprehensive utilization of resources, restores ecological balance, belongs to an environment-friendly product, utilizes the modified montmorillonite and the modified flake graphite, slows down the smoldering speed of agarwood while ensuring the stability of the smoldering of the agarwood, and the added trifluoropropyl methyl silicone oil can further improve the hydrophobicity of the filler, so that the agarwood cannot absorb moisture and become damp during storage, and the use performance is affected, and the mutual cooperation of the raw materials in the filler effectively solves the problems of little smoke, moisture resistance and combustion efficiency of the agarwood of Aquilaria sinensis.

Description

Technical Field

[0001] This invention belongs to the field of Qinan agarwood production technology, specifically relating to an environmentally friendly filler for preparing Qinan agarwood and a method for preparing Qinan agarwood. Background Technology

[0002] Agarwood is the resinous wood of plants in the genus *Aquilaria* of the family Thymelaeaceae. Domestically produced Qinan agarwood originates from *Aquilaria sinensis*, also in the family Thymelaeaceae. Qinan agarwood is distinguished from ordinary agarwood primarily by its aroma and appearance, and can be categorized into green, purple, black, and yellow varieties based on the color of its surface and cross-section. Qinan is the highest grade and most precious variety of agarwood, highly favored by consumers for its mysterious and elegant fragrance and rich oil content.

[0003] Currently, the main methods for quickly and effectively releasing the aroma of agarwood are combustion and electric heating. Electrically heated agarwood products are heated rather than burned, thus reducing the harmful components produced by the high-temperature combustion and decomposition of traditional agarwood, lowering the levels of harmful components in the main smoke. Furthermore, its applications are more widespread, making electrically heated agarwood products increasingly popular with consumers. However, for combustion-type agarwood products, there is limited research on issues such as reducing smoke and controlling the combustion speed in existing technologies.

[0004] Incense on the market is usually made of wood powder and some added fragrances, medicines, excipients and binders. When using incense, it is usually lit to release fragrant gases or medicines, thereby producing an effect. For example, when mosquito coils commonly found on the market burn, they mainly release tetrafluoroethylene or chlorpyrifos into the air to achieve the effect of repelling mosquitoes.

[0005] Currently, most incense on the market contains chemical adhesives, flame retardants, stone powder, and other additives, which increases the weight of the incense, prevents it from burning completely, and produces a lot of ash. In addition, traditional agarwood incense is exposed to the air for a long time when stored. Its raw materials are mostly made of wood powder that is susceptible to moisture, and the oily components it contains will oxidize, denature, or evaporate and be lost, resulting in mold and mildew. When burning, the fragrance will decrease, or its original efficacy will be lost, or it may even denature and produce harmful substances.

[0006] Chinese Patent Application No. 200910305777.8 discloses a smokeless moxibustion incense and its preparation method. This invention comprises, by weight percentage, 83.2%-85.8% of Artemisia argyi leaves, 2.8%-4% of Nardostachys jatamansi, 1.8%-2% of Angelica dahurica, 1.8%-2% of Asarum heterotropoides, 1.8%-2% of Notopterygium incisum, 1.8%-2% of Aucklandia lappa, 1.8%-2% of Fennel, 1.8%-2% of Clove, and 0.6%-0.8% of sodium alginate. The method involves carbonizing the Artemisia argyi leaves with rice vinegar to obtain carbonized Artemisia argyi granules, which retains the medicinal efficacy of Artemisia argyi while reducing smoke. Chinese patent application number 201911059199.4 discloses an anti-mildew incense and its processing technology, comprising the following raw materials in parts by weight: 20-30 parts sawdust, 50-55 parts woody fragrance residue, 1-2 parts fragrance powder, 2-2.5 parts activated carbon, and 5-8 parts binding powder; wherein the woody fragrance residue is a composition of solid residues remaining after extracting essential oils from star anise, lemongrass, camphor leaves, cinnamon bark, melaleuca, and pine. The addition of activated carbon to the incense in this invention can prevent the incense from becoming difficult to burn due to moisture and mold, improve the structural stability of the incense, extend the shelf life of the incense, and also have the effect of refreshing the mind, while realizing the reuse of waste resources and saving energy.

[0007] While the aforementioned patents can effectively reduce smoke and prevent incense from getting damp and moldy, their functions are relatively limited and cannot meet the requirements of combining less smoke, moisture prevention, and controlled combustion efficiency in incense burning. Summary of the Invention

[0008] To address the shortcomings of existing technologies, the present invention aims to provide an environmentally friendly filler for preparing Qinan agarwood and a method for preparing Qinan agarwood. The addition of this environmentally friendly filler to Qinan agarwood can prevent the agarwood from becoming difficult to burn due to moisture and mold, while also reducing the burning rate and smoke of the agarwood, extending the burning time of the agarwood, and saving energy and protecting the environment.

[0009] To achieve the above objectives, the present invention provides the following technical solution:

[0010] A method for preparing an environmentally friendly filler for agarwood (Kynam) includes the following steps:

[0011] (1) Wash, dry and crush agricultural and forestry waste to 200 mesh, then soak it in sodium hydroxide solution. After soaking, filter, wash and dry to obtain agricultural and forestry waste powder.

[0012] (2) Add montmorillonite to deionized water, then add hexadecyl-3-methylimidazolium chloride, and react at 60-80℃ for 3-5 h. After the reaction is complete, filter, wash and dry, then calcine under nitrogen atmosphere to obtain solid powder. Then add solid powder to anhydrous ethanol, then add potassium permanganate solution and γ-aminopropyltriethoxysilane and stir to react. After the reaction is complete, filter and dry to obtain modified montmorillonite.

[0013] (3) Add flake graphite to hydrogen peroxide solution, soak for 3-5 hours, filter to obtain oxidized flake graphite, then add oxidized flake graphite to deionized water, then add zeolite powder and N-(β-aminoethyl)-γ-aminopropyltrimethoxysilane for heating reaction, filter and dry after reaction to obtain modified flake graphite.

[0014] (4) The agricultural and forestry waste powder obtained above is soaked in an ethanol aqueous solution for 1-2 hours, then modified montmorillonite, modified flake graphite and trifluoropropyl methyl silicone oil are added and reacted at a constant temperature. After the reaction is completed, the mixture is filtered, washed, dried and ground, and passed through a 200-mesh sieve to obtain the environmentally friendly filler.

[0015] Preferably, the agricultural and forestry waste in step (1) is one or more of straw, bark, corn cob, and peanut shell; the mass concentration of the sodium hydroxide solution is 5-10%; the soaking temperature is 50-70℃ and the soaking time is 2-4h.

[0016] Preferably, in step (2), the mass ratio of montmorillonite to hexadecyl-3-methylimidazolium chloride is 50:0.5-1; the calcination temperature is 400-500℃ and the calcination time is 1-3h.

[0017] Preferably, the mass concentration of the potassium permanganate solution in step (2) is 5-8%, and the mass ratio of the solid powder, potassium permanganate solution, and γ-aminopropyltriethoxysilane is 50:40-60:2-3; the temperature of the stirring reaction is 40-50℃, and the reaction time is 1-2h.

[0018] Preferably, the mass concentration of the hydrogen peroxide solution in step (3) is 10%; the mass ratio of the oxidized flake graphite, zeolite powder, and N-(β-aminoethyl)-γ-aminopropyltrimethoxysilane is 50:25-35:1-3.

[0019] Preferably, the heating reaction in step (3) is carried out at a temperature of 70-90°C for 3-5 hours.

[0020] Preferably, the ethanol concentration in the aqueous ethanol solution in step (4) is 50-70%; the mass ratio of the agricultural and forestry waste powder, modified montmorillonite, modified flake graphite, and trifluoropropylmethyl silicone oil is 60:20-30:20-30:1-2; the temperature of the isothermal reaction is 60-70℃, and the reaction time is 3-5h.

[0021] This invention also protects an environmentally friendly filler prepared by the aforementioned preparation method.

[0022] This invention also protects a method for preparing Qinan agarwood using the aforementioned environmentally friendly filler, comprising the following steps:

[0023] S1. Raw material preparation: Wash the agarwood, sandalwood, costus root, rue, angelica, elm, cinnamon, sweet osmanthus, camphor leaves, and atractylodes with water and dry them at 50-70℃ for 5-8 hours.

[0024] S2. Crushing: Crush the dried raw material from step S1 into powder, pass it through a 100-200 mesh sieve and mix it evenly to obtain a mixed powder;

[0025] S3. Making the fragrant mud: After mixing the mixed powder, binder and environmentally friendly filler in step S2 evenly, add water, stir and mix evenly to form a lump of fragrant mud;

[0026] S4. Shaping: Press the fragrant mud from step S3 into shape to obtain the Qinan agarwood blank;

[0027] S5. Air drying: Place the Qinan agarwood blanks from S4 in a dark and dry place at a temperature of 25-30℃ for 6-10 days, while circulating the air with a blower, and control the moisture content at 3-6%.

[0028] S6. Cellaring: After the agarwood blanks in S5 have been air-dried, they are placed in an environment with a temperature of 10-15℃ and a humidity of 15-20% and cellared for 25-30 days to obtain agarwood.

[0029] Preferably, in step S1, the amounts of each raw material by weight are as follows: 15-20 parts of Qinan agarwood, 10-15 parts of sandalwood, 10-15 parts of costus root, 5-10 parts of rue, 3-10 parts of angelica root, 7-10 parts of elm wood, 5-13 parts of cinnamon, 5-12 parts of sweet osmanthus, 3-6 parts of camphor leaves, and 2-7 parts of atractylodes rhizome; the adhesive in step S2 is one or both of gum arabic and konjac gum; the mass ratio of the mixed powder, adhesive, and environmentally friendly filler in step S3 is 60-80:10-15:20-30.

[0030] Compared with the prior art, the present invention has the following beneficial effects:

[0031] (1) The environmentally friendly filler for preparing Qinan agarwood provided by this invention involves alkali treatment of agricultural and forestry waste to activate its numerous hydroxyl and carboxyl groups, which is beneficial for subsequent reactions. Montmorillonite is then modified using hexadecyl-3-methylimidazolium chloride and calcination to increase the interlayer spacing, facilitating the subsequent insertion of potassium permanganate into the interlayer of montmorillonite. On one hand, the lamellar structure of montmorillonite effectively slows down the combustion rate; on the other hand, the added potassium permanganate decomposes to generate oxygen during the combustion of Qinan agarwood, preventing montmorillonite from blocking the smoldering of agarwood and ensuring complete combustion. Furthermore, γ-aminopropyltriethoxysilane increases the active sites on the surface of montmorillonite, which is beneficial for subsequent reactions. Then, [the process continues with...] Flake graphite is oxidized while zeolite powder is added. Zeolite powder slows down the combustion rate of graphite. Furthermore, due to the unique three-dimensional lattice structure of zeolite powder and the presence of various uniformly distributed cavities and channels, it effectively reduces fly ash produced during agarwood combustion. N-(β-aminoethyl)-γ-aminopropyltrimethoxysilane is added to increase the amino groups on the surface of the flake graphite. Then, agricultural and forestry waste powder, modified montmorillonite, and modified flake graphite are reacted. Through the reaction of surface groups, the three are combined in the form of covalent bonds. The addition of siloxane improves the hydrophobicity of the filler and makes the carbon layer structure generated during combustion more dense and stable, effectively preventing the ash from scattering during smoldering agarwood and avoiding pollution to the surrounding environment.

[0032] (2) The environmentally friendly filler for preparing Qinan agarwood provided by the present invention uses agricultural and forestry waste as the main raw material to achieve comprehensive utilization of resources and restore ecological balance. It is an environmentally friendly product. Modified montmorillonite and modified flake graphite are used to slow down the smoldering speed of agarwood while ensuring its smoldering stability. In addition, the manganese salt generated after the decomposition of potassium permanganate loaded on montmorillonite can inhibit the generation of smoke. The added trifluoropropyl methyl silicone oil can further improve the hydrophobicity of the filler, which can ensure that the agarwood will not absorb moisture and become damp during storage, thus affecting its performance. The various raw materials in the filler work together to effectively solve the problems of low smoke, moisture prevention and combustion efficiency of Qinan agarwood.

[0033] (3) The agarwood prepared by this invention has a simple preparation process and can be stored in cellars at a lower temperature for a longer time. This not only helps preserve the agarwood, but also helps retain the aroma of the original powder in the agarwood, resulting in a more mellow aroma in the final agarwood product. The aroma lasts longer, and the ash is not easily dispersed under the action of the filler, which is beneficial to protecting the ecological environment. Detailed Implementation

[0034] The technical solution of the present invention will be clearly and completely described below with reference to the embodiments. Obviously, the described embodiments are only some embodiments of the present invention, and not all embodiments. Based on the embodiments of the present invention, all other embodiments obtained by those of ordinary skill in the art without creative effort are within the scope of protection of the present invention.

[0035] The montmorillonite was purchased from Lingshou County Antai Mining Co., Ltd., with a mesh size of 325; the flake graphite was purchased from Lingshou County Huajing Mica Co., Ltd., with a mesh size of 600; and the zeolite powder was purchased from Chaoyang City Xinhe Zeolite Technology Co., Ltd., with a mesh size of 1500.

[0036] Example 1

[0037] A method for preparing an environmentally friendly filler for agarwood (Kynam) includes the following steps:

[0038] (1) Wash, dry, and crush 100 corn stalks to 200 mesh, then add them to 800 mL of 5% sodium hydroxide solution for soaking at 50°C for 4 hours. After soaking, filter, wash, and dry to obtain corn stalk powder.

[0039] (2) Add 50g of montmorillonite to 500mL of deionized water, then add 0.5g of hexadecyl-3-methylimidazolium chloride, and react at 60℃ for 5h. After the reaction is complete, filter, wash and dry, then calcine under nitrogen atmosphere at 400℃ for 3h to obtain solid powder; then add 50g of solid powder to 400mL of anhydrous ethanol, then add 40g of 8% potassium permanganate solution and 2g of γ-aminopropyltriethoxysilane and stir to react at 40℃ for 2h. After the reaction is complete, filter and dry to obtain modified montmorillonite.

[0040] (3) Add 50g of flake graphite to 500mL of 10% hydrogen peroxide solution and soak for 3h. Filter to obtain oxidized flake graphite. Then add 50g of oxidized flake graphite to 500mL of deionized water. Next, add 25g of zeolite powder and 1g of N-(β-aminoethyl)-γ-aminopropyltrimethoxysilane and heat to react at 70℃ for 5h. After the reaction is completed, filter and dry to obtain modified flake graphite.

[0041] (4) Add 60g of agricultural and forestry waste powder obtained above to 800mL of 50% ethanol aqueous solution and soak for 1h. Then add 20g of modified montmorillonite, 20g of modified flake graphite and 1g of trifluoropropylmethyl silicone oil and carry out constant temperature reaction at 60℃ for 5h. After the reaction is completed, filter, wash, dry and grind, and pass through a 200-mesh sieve to obtain the environmentally friendly filler.

[0042] A method for preparing Qinan agarwood using the above-mentioned environmentally friendly filler includes the following steps:

[0043] S1. Raw material preparation: Wash 20g of Qinan agarwood, 10g of sandalwood, 10g of costus root, 10g of rue, 10g of angelica root, 10g of elm wood, 10g of cinnamon, 10g of sweet osmanthus, 5g of camphor leaves, and 5g of atractylodes with water and dry them at 50℃ for 8 hours.

[0044] S2. Crushing: Crush the dried raw material from step S1 into powder, pass it through a 200-mesh sieve and mix it evenly to obtain a mixed powder;

[0045] S3. Making the fragrant mud: Mix 70g of mixed powder, 10g of gum arabic and 20g of environmentally friendly filler from step S2 evenly, then add 60g of water, stir and mix evenly to form a dough-like fragrant mud.

[0046] S4. Shaping: Press the fragrant mud from step S3 into shape to obtain the Qinan agarwood blank;

[0047] S5. Air drying: Place the Qinan agarwood blanks from S4 in a dark drying place at a temperature of 25℃ for 10 days, while circulating the air with a blower, and control the moisture content at 5%.

[0048] S6. Cellaring: The agarwood blanks of S5, after being air-dried, are placed in an environment with a temperature of 10℃ and a humidity of 15% and cellared for 30 days to obtain agarwood.

[0049] Example 2

[0050] A method for preparing an environmentally friendly filler for agarwood (Kynam) includes the following steps:

[0051] (1) Wash, dry, and pulverize 100g of bark to 200 mesh, then add it to 800mL of 8% sodium hydroxide solution for soaking at 60℃ for 3h. After soaking, filter, wash, and dry to obtain bark powder.

[0052] (2) Add 50g of montmorillonite to 500mL of deionized water, then add 0.8g of hexadecyl-3-methylimidazolium chloride, and react at 70℃ for 4h. After the reaction is complete, filter, wash and dry, then calcine under nitrogen atmosphere at 450℃ for 2h to obtain solid powder; then add 50g of solid powder to 400mL of anhydrous ethanol, then add 50g of 6% potassium permanganate solution and 2.5g of γ-aminopropyltriethoxysilane and stir to react at 45℃ for 2h. After the reaction is complete, filter and dry to obtain modified montmorillonite.

[0053] (3) Add 50g of flake graphite to 500mL of 10% hydrogen peroxide solution and soak for 4h. Filter to obtain oxidized flake graphite. Then add 50g of oxidized flake graphite to 500mL of deionized water. Then add 30g of zeolite powder and 2g of N-(β-aminoethyl)-γ-aminopropyltrimethoxysilane and heat to react. The reaction temperature is 80℃ and the reaction time is 4h. After the reaction is completed, filter and dry to obtain modified flake graphite.

[0054] (4) Add 60g of agricultural and forestry waste powder obtained above to 800mL of 60% ethanol aqueous solution and soak for 1-2h. Then add 25g of modified montmorillonite, 25g of modified flake graphite and 1.5g of trifluoropropylmethyl silicone oil and carry out a constant temperature reaction at 65℃ for 5h. After the reaction is completed, filter, wash, dry and grind, and pass through a 200-mesh sieve to obtain the environmentally friendly filler.

[0055] A method for preparing Qinan agarwood using the above-mentioned environmentally friendly filler includes the following steps:

[0056] S1. Raw material preparation: Wash 20g of Qinan agarwood, 10g of sandalwood, 10g of costus root, 10g of rue, 10g of angelica root, 10g of elm wood, 10g of cinnamon, 10g of sweet osmanthus, 5g of camphor leaves, and 5g of atractylodes with water and dry them at 50℃ for 8 hours.

[0057] S2. Crushing: Crush the dried raw material from step S1 into powder, pass it through a 200-mesh sieve and mix it evenly to obtain a mixed powder;

[0058] S3. Making the fragrant mud: Mix 70g of mixed powder, 10g of gum arabic and 20g of environmentally friendly filler from step S2 evenly, then add 60g of water, stir and mix evenly to form a dough-like fragrant mud.

[0059] S4. Shaping: Press the fragrant mud from step S3 into shape to obtain the Qinan agarwood blank;

[0060] S5. Air drying: Place the Qinan agarwood blanks from S4 in a dark drying place at a temperature of 25℃ for 10 days, while circulating the air with a blower, and control the moisture content at 5%.

[0061] S6. Cellaring: The agarwood blanks of S5, after being air-dried, are placed in an environment with a temperature of 10℃ and a humidity of 15% and cellared for 30 days to obtain agarwood.

[0062] Example 3

[0063] A method for preparing an environmentally friendly filler for agarwood (Kynam) includes the following steps:

[0064] (1) Wash, dry, and crush 100g of corn cob to 200 mesh, then add it to 800mL of 9% sodium hydroxide solution for soaking. The soaking temperature is 65℃ and the soaking time is 3h. After soaking, filter, wash, and dry to obtain corn cob powder.

[0065] (2) Add 50g of montmorillonite to 500mL of deionized water, then add 0.9g of hexadecyl-3-methylimidazolium chloride, and react at 75℃ for 4h. After the reaction is complete, filter, wash and dry, then calcine under nitrogen atmosphere at 450℃ for 2h to obtain solid powder; then add 50g of solid powder to 400mL of anhydrous ethanol, then add 50g of 6% potassium permanganate solution and 2.5g of γ-aminopropyltriethoxysilane and stir to react at 45℃ for 1h. After the reaction is complete, filter and dry to obtain modified montmorillonite.

[0066] (3) Add 50g of flake graphite to 500mL of 10% hydrogen peroxide solution and soak for 4h. Filter to obtain oxidized flake graphite. Then add 50g of oxidized flake graphite to 500mL of deionized water. Next, add 35g of zeolite powder and 2g of N-(β-aminoethyl)-γ-aminopropyltrimethoxysilane and heat to react. The reaction temperature is 85℃ and the reaction time is 4h. After the reaction is completed, filter and dry to obtain modified flake graphite.

[0067] (4) Add 60g of agricultural and forestry waste powder obtained above to 800mL of 60% ethanol aqueous solution and soak for 1-2h. Then add 25g of modified montmorillonite, 30g of modified flake graphite and 1.5g of trifluoropropylmethyl silicone oil and carry out a constant temperature reaction at 65℃ for 4h. After the reaction is completed, filter, wash, dry and grind, and pass through a 200-mesh sieve to obtain the environmentally friendly filler.

[0068] A method for preparing Qinan agarwood using the above-mentioned environmentally friendly filler includes the following steps:

[0069] S1. Raw material preparation: Wash 20g of Qinan agarwood, 15g of sandalwood, 10g of costus root, 5g of rue, 10g of angelica root, 10g of elm wood, 5g of cinnamon, 10g of sweet osmanthus, 5g of camphor leaves, and 5g of atractylodes with water and dry them at 70℃ for 5 hours.

[0070] S2. Crushing: Crush the dried raw material from step S1 into powder, pass it through a 200-mesh sieve and mix it evenly to obtain a mixed powder;

[0071] S3. Making the fragrant mud: Mix 80g of mixed powder, 15g of gum arabic and 30g of environmentally friendly filler from step S2 evenly, then add 90g of water, stir and mix evenly to form a dough-like fragrant mud.

[0072] S4. Shaping: Press the fragrant mud from step S3 into shape to obtain the Qinan agarwood blank;

[0073] S5. Air drying: Place the Qinan agarwood blanks from S4 in a dark drying place at a temperature of 30℃ for 6 days, while circulating the air with a blower, and control the moisture content at 3%.

[0074] S6. Cellaring: The agarwood blanks that have been air-dried in S5 are placed in an environment with a temperature of 15℃ and a humidity of 20% and cellared for 25 days to obtain agarwood.

[0075] Example 4

[0076] A method for preparing an environmentally friendly filler for agarwood (Kynam) includes the following steps:

[0077] (1) Wash, dry, and crush 100g of peanut shells to 200 mesh, then add them to 800mL of 10% sodium hydroxide solution for soaking at 70℃ for 2h. After soaking, filter, wash, and dry to obtain peanut shell powder.

[0078] (2) Add 50g of montmorillonite to 500mL of deionized water, then add 1g of hexadecyl-3-methylimidazolium chloride, and react at 80℃ for 3h. After the reaction is completed, filter, wash and dry, then calcine under nitrogen atmosphere at 500℃ for 1h to obtain solid powder; then add 50g of solid powder to 400mL of anhydrous ethanol, then add 60g of 5% potassium permanganate solution and 3g of γ-aminopropyltriethoxysilane and stir to react at 50℃ for 1h. After the reaction is completed, filter and dry to obtain modified montmorillonite.

[0079] (3) Add 50g of flake graphite to 500mL of 10% hydrogen peroxide solution and soak for 5h. Filter to obtain oxidized flake graphite. Then add 50g of oxidized flake graphite to 500mL of deionized water. Next, add 35g of zeolite powder and 3g of N-(β-aminoethyl)-γ-aminopropyltrimethoxysilane and heat to react. The reaction temperature is 90℃ and the reaction time is 3h. After the reaction is completed, filter and dry to obtain modified flake graphite.

[0080] (4) The 60g of agricultural and forestry waste powder obtained above was added to 800mL of 70% ethanol aqueous solution and soaked for 2h. Then, 30g of modified montmorillonite, 30g of modified flake graphite and 2g of trifluoropropylmethyl silicone oil were added and reacted at a constant temperature of 70℃ for 3h. After the reaction was completed, the mixture was filtered, washed, dried and ground and passed through a 200-mesh sieve to obtain the environmentally friendly filler.

[0081] A method for preparing Qinan agarwood using the above-mentioned environmentally friendly filler includes the following steps:

[0082] S1. Raw material preparation: Wash 20g of Qinan agarwood, 15g of sandalwood, 10g of costus root, 5g of rue, 10g of angelica root, 10g of elm wood, 5g of cinnamon, 10g of sweet osmanthus, 5g of camphor leaves, and 5g of atractylodes with water and dry them at 70℃ for 5 hours.

[0083] S2. Crushing: Crush the dried raw material from step S1 into powder, pass it through a 200-mesh sieve and mix it evenly to obtain a mixed powder;

[0084] S3. Making the fragrant mud: Mix 80g of mixed powder, 15g of gum arabic and 30g of environmentally friendly filler from step S2 evenly, then add 90g of water, stir and mix evenly to form a dough-like fragrant mud.

[0085] S4. Shaping: Press the fragrant mud from step S3 into shape to obtain the Qinan agarwood blank;

[0086] S5. Air drying: Place the Qinan agarwood blanks from S4 in a dark drying place at a temperature of 30℃ for 6 days, while circulating the air with a blower, and control the moisture content at 3%.

[0087] S6. Cellaring: The agarwood blanks that have been air-dried in S5 are placed in an environment with a temperature of 15℃ and a humidity of 20% and cellared for 25 days to obtain agarwood.

[0088] Comparative Example 1

[0089] A method for preparing an environmentally friendly filler for agarwood (Kynam) includes the following steps:

[0090] (1) Wash, dry, and crush 100 corn stalks to 200 mesh, then add 800 mL of 5% sodium hydroxide solution for soaking at 50°C for 4 hours. After soaking, filter, wash, and dry to obtain straw powder.

[0091] (2) Add 50g of flake graphite to 500mL of 10% hydrogen peroxide solution and soak for 3h. Filter to obtain oxidized flake graphite. Then add 50g of oxidized flake graphite to 500mL of deionized water. Next, add 25g of zeolite powder and 1g of N-(β-aminoethyl)-γ-aminopropyltrimethoxysilane and heat to react at 70℃ for 5h. After the reaction is completed, filter and dry to obtain modified flake graphite.

[0092] (3) Add 60g of agricultural and forestry waste powder obtained above to 800mL of 50% ethanol aqueous solution and soak for 1h. Then add 15g of montmorillonite, 40g of 8% potassium permanganate solution, 20g of modified flake graphite and 1g of trifluoropropylmethyl silicone oil and carry out a constant temperature reaction at 60℃ for 5h. After the reaction is completed, filter, wash, dry and grind, and pass through a 200-mesh sieve to obtain the environmentally friendly filler.

[0093] A method for preparing Qinan agarwood using the above-mentioned environmentally friendly filler includes the following steps:

[0094] S1. Raw material preparation: Wash 20g of Qinan agarwood, 10g of sandalwood, 10g of costus root, 10g of rue, 10g of angelica root, 10g of elm wood, 10g of cinnamon, 10g of sweet osmanthus, 5g of camphor leaves, and 5g of atractylodes with water and dry them at 50℃ for 8 hours.

[0095] S2. Crushing: Crush the dried raw material from step S1 into powder, pass it through a 200-mesh sieve and mix it evenly to obtain a mixed powder;

[0096] S3. Making the fragrant mud: Mix 70g of mixed powder, 10g of gum arabic and 20g of environmentally friendly filler from step S2 evenly, then add 60g of water, stir and mix evenly to form a dough-like fragrant mud.

[0097] S4. Shaping: Press the fragrant mud from step S3 into shape to obtain the Qinan agarwood blank;

[0098] S5. Air drying: Place the Qinan agarwood blanks from S4 in a dark drying place at a temperature of 25℃ for 10 days, while circulating the air with a blower, and control the moisture content at 5%.

[0099] S6. Cellaring: The agarwood blanks of S5, after being air-dried, are placed in an environment with a temperature of 10℃ and a humidity of 15% and cellared for 30 days to obtain agarwood.

[0100] Comparative Example 2

[0101] A method for preparing an environmentally friendly filler for agarwood (Kynam) includes the following steps:

[0102] (1) Wash, dry, and crush 100 corn stalks to 200 mesh, then add 800 mL of 5% sodium hydroxide solution for soaking at 50°C for 4 hours. After soaking, filter, wash, and dry to obtain straw powder.

[0103] (2) Add 50g of montmorillonite to 500mL of deionized water, then add 0.5g of hexadecyl-3-methylimidazolium chloride, and react at 60℃ for 5h. After the reaction is complete, filter, wash and dry, then calcine under nitrogen atmosphere at 400℃ for 3h to obtain solid powder; then add 50g of solid powder to 400mL of anhydrous ethanol, then add 40g of 8% potassium permanganate solution and 2g of γ-aminopropyltriethoxysilane and stir to react at 40℃ for 2h. After the reaction is complete, filter and dry to obtain modified montmorillonite.

[0104] (3) Add 60g of agricultural and forestry waste powder obtained above to 800mL of 50% ethanol aqueous solution and soak for 1h. Then add 20g of modified montmorillonite, 15g of flake graphite, 5g of zeolite powder and 1g of trifluoropropylmethyl silicone oil and carry out a constant temperature reaction at 60℃ for 5h. After the reaction is completed, filter, wash, dry and grind, and pass through a 200-mesh sieve to obtain the environmentally friendly filler.

[0105] A method for preparing Qinan agarwood using the above-mentioned environmentally friendly filler includes the following steps:

[0106] S1. Raw material preparation: Wash 20g of Qinan agarwood, 10g of sandalwood, 10g of costus root, 10g of rue, 10g of angelica root, 10g of elm wood, 10g of cinnamon, 10g of sweet osmanthus, 5g of camphor leaves, and 5g of atractylodes with water and dry them at 50℃ for 8 hours.

[0107] S2. Crushing: Crush the dried raw material from step S1 into powder, pass it through a 200-mesh sieve and mix it evenly to obtain a mixed powder;

[0108] S3. Making the fragrant mud: Mix 70g of mixed powder, 10g of gum arabic and 20g of environmentally friendly filler from step S2 evenly, then add 60g of water, stir and mix evenly to form a dough-like fragrant mud.

[0109] S4. Shaping: Press the fragrant mud from step S3 into shape to obtain the Qinan agarwood blank;

[0110] S5. Air drying: Place the Qinan agarwood blanks from S4 in a dark drying place at a temperature of 25℃ for 10 days, while circulating the air with a blower, and control the moisture content at 5%.

[0111] S6. Cellaring: The agarwood blanks of S5, after being air-dried, are placed in an environment with a temperature of 10℃ and a humidity of 15% and cellared for 30 days to obtain agarwood.

[0112] Comparative Example 3

[0113] A method for preparing an environmentally friendly filler for agarwood (Kynam) includes the following steps:

[0114] (1) Wash, dry, and crush 100 corn stalks to 200 mesh, then add 800 mL of 5% sodium hydroxide solution for soaking at 50°C for 4 hours. After soaking, filter, wash, and dry to obtain straw powder.

[0115] (2) Add 60g of agricultural and forestry waste powder obtained above to 800mL of 50% ethanol aqueous solution and soak for 1h. Then add 15g of montmorillonite, 15g of flake graphite, 40g of 8% potassium permanganate solution, 5g of zeolite powder and 1g of trifluoropropylmethyl silicone oil and carry out a constant temperature reaction at 60℃ for 5h. After the reaction is completed, filter, wash, dry and grind, and pass through a 200-mesh sieve to obtain the environmentally friendly filler.

[0116] A method for preparing Qinan agarwood using the above-mentioned environmentally friendly filler includes the following steps:

[0117] S1. Raw material preparation: Wash 20g of Qinan agarwood, 10g of sandalwood, 10g of costus root, 10g of rue, 10g of angelica root, 10g of elm wood, 10g of cinnamon, 10g of sweet osmanthus, 5g of camphor leaves, and 5g of atractylodes with water and dry them at 50℃ for 8 hours.

[0118] S2. Crushing: Crush the dried raw material from step S1 into powder, pass it through a 200-mesh sieve and mix it evenly to obtain a mixed powder;

[0119] S3. Making the fragrant mud: Mix 70g of mixed powder, 10g of gum arabic and 20g of environmentally friendly filler from step S2 evenly, then add 60g of water, stir and mix evenly to form a dough-like fragrant mud.

[0120] S4. Shaping: Press the fragrant mud from step S3 into shape to obtain the Qinan agarwood blank;

[0121] S5. Air drying: Place the Qinan agarwood blanks from S4 in a dark drying place at a temperature of 25℃ for 10 days, while circulating the air with a blower, and control the moisture content at 5%.

[0122] S6. Cellaring: The agarwood blanks of S5, after being air-dried, are placed in an environment with a temperature of 10℃ and a humidity of 15% and cellared for 30 days to obtain agarwood.

[0123] The agarwood prepared in Examples 1-4 and Comparative Examples 1-3 was tested. The agarwood was incense sticks with a length of 280 mm and a diameter of 5 mm. The burning time and burning pattern of the products were tested. The moisture resistance test was conducted by placing the agarwood in a constant temperature and humidity chamber for 45 days to test its water absorption rate. The test conditions were: temperature 25±1℃ and humidity 95±2%. Afterwards, the sample was taken out and the surface moisture was absorbed with filter paper. Then it was placed in an environment with a temperature of 25±1℃ and humidity of 50±2% for 20 minutes to test its water absorption rate.

[0124] Water absorption rate calculation:

[0125] Where m0 represents the mass of Qinan agarwood before testing; and m1 represents the mass of Qinan agarwood after adjustment.

[0126] The test results are shown in Table 1 below:

[0127] Table 1

[0128] Example 1 65 Black, thread-like particles; minimal ash and smoke. 6.04 Example 2 62 Black, thread-like particles; minimal ash and smoke. 5.86 Example 3 66 Black, thread-like particles; minimal ash and smoke. 5.74 Example 4 68 Black, thread-like particles; minimal ash and smoke. 5.97 Comparative Example 1 51 Black, thread-like structure; little ash; high smoke content. 11.82 Comparative Example 2 47 Black linear pattern, high ash content, low smoke 12.59 Comparative Example 3 39 Black powder, large amount of ash, and a lot of smoke. 18.47

[0129] As shown in Table 1, the Qinan agarwood prepared by this invention has a longer burning time, produces less smoke during combustion, and the ash is linear and not easily dispersed. It also has good moisture resistance, low water absorption rate under humid conditions, and good storage performance, thus improving the quality of Qinan agarwood.

[0130] Although embodiments of the invention have been shown and described, it will be understood by those skilled in the art that various changes, modifications, substitutions and alterations can be made to these embodiments without departing from the principles and spirit of the invention, the scope of which is defined by the appended claims and their equivalents.

Claims

1. A method for preparing an environmentally friendly filler for preparing Qinan agarwood, characterized in that, Includes the following steps: (1) Wash, dry and crush agricultural and forestry waste to 200 mesh, then soak it in sodium hydroxide solution. After soaking, filter, wash and dry to obtain agricultural and forestry waste powder; (2) Add montmorillonite to deionized water, then add hexadecyl-3-methylimidazolium chloride, and react at 60-80℃ for 3-5 h. After the reaction is complete, filter, wash and dry, then calcine under nitrogen atmosphere to obtain solid powder. Then add solid powder to anhydrous ethanol, then add potassium permanganate solution and γ-aminopropyltriethoxysilane and stir to react. After the reaction is complete, filter and dry to obtain modified montmorillonite. (3) Add flake graphite to hydrogen peroxide solution and soak for 3-5 hours. Filter to obtain oxidized flake graphite. Then add oxidized flake graphite to deionized water, followed by zeolite powder and N-(β-aminoethyl)-γ-aminopropyltrimethoxysilane for heating reaction. After the reaction is completed, filter and dry to obtain modified flake graphite. (4) Add agricultural and forestry waste powder to an ethanol aqueous solution and soak for 1-2 hours. Then add modified montmorillonite, modified flake graphite and trifluoropropyl methyl silicone oil and carry out a constant temperature reaction. After the reaction is completed, filter, wash, dry and grind, and pass through a 200-mesh sieve to obtain the environmentally friendly filler.

2. The preparation method according to claim 1, characterized in that, The agricultural and forestry waste mentioned in step (1) is one or more of straw, bark, corn cob, and peanut shell; the mass concentration of the sodium hydroxide solution is 5-10%; the soaking temperature is 50-70℃ and the soaking time is 2-4h.

3. The preparation method according to claim 1, characterized in that, In step (2), the mass ratio of montmorillonite to hexadecyl-3-methylimidazolium chloride is 50:0.5-1; the calcination temperature is 400-500℃ and the calcination time is 1-3h.

4. The preparation method according to claim 1, characterized in that, In step (2), the mass concentration of the potassium permanganate solution is 5-8%, and the mass ratio of the solid powder, potassium permanganate solution, and γ-aminopropyltriethoxysilane is 50:40-60:2-3; the temperature of the stirring reaction is 40-50℃, and the reaction time is 1-2h.

5. The preparation method according to claim 1, characterized in that, The mass concentration of the hydrogen peroxide solution in step (3) is 10%; the mass ratio of the oxidized flake graphite, zeolite powder, and N-(β-aminoethyl)-γ-aminopropyltrimethoxysilane is 50:25-35:1-3.

6. The preparation method according to claim 1, characterized in that, The heating reaction in step (3) is carried out at a temperature of 70-90℃ for 3-5 hours.

7. The preparation method according to claim 1, characterized in that, In step (4), the ethanol aqueous solution contains 50-70% ethanol by mass; the mass ratio of the agricultural and forestry waste powder, modified montmorillonite, modified flake graphite, and trifluoropropylmethyl silicone oil is 60:20-30:20-30:1-2; the constant temperature reaction is 60-70℃ and the reaction time is 3-5h.

8. An environmentally friendly filler prepared by the preparation method according to any one of claims 1-7.

9. A method for preparing Qinan agarwood using the environmentally friendly filler as described in claim 8, characterized in that, Includes the following steps: S1. Raw material preparation: Wash the agarwood, sandalwood, costus root, rue, angelica, elm, cinnamon, sweet osmanthus, camphor leaves, and atractylodes with water and dry them at 50-70℃ for 5-8 hours. S2. Crushing: Crush the dried raw material from step S1 into powder, pass it through a 100-200 mesh sieve and mix it evenly to obtain a mixed powder; S3. Making the fragrant mud: After mixing the mixed powder, binder and environmentally friendly filler from step S2 evenly, add water, stir and mix evenly to form a lump of fragrant mud; S4. Shaping: Press the fragrant mud from step S3 into shape to obtain the Qinan agarwood blank; S5. Air drying: Place the Qinan agarwood blanks from S4 in a dark and dry place at a temperature of 25-30℃ for 6-10 days, while circulating the air with a blower, and control the moisture content at 3-6%. S6. Cellaring: After the agarwood blanks in S5 have been air-dried, they are placed in an environment with a temperature of 10-15℃ and a humidity of 15-20% and cellared for 25-30 days to obtain agarwood.

10. The method for preparing Qinan agarwood according to claim 9, characterized in that, In step S1, the amounts of each raw material by weight are as follows: 15-20 parts of Qinan agarwood, 10-15 parts of sandalwood, 10-15 parts of costus root, 5-10 parts of rue, 3-10 parts of angelica root, 7-10 parts of elm wood, 5-13 parts of cinnamon, 5-12 parts of sweet osmanthus, 3-6 parts of camphor leaves, and 2-7 parts of atractylodes rhizome; the adhesive mentioned in step S3 is one or two of gum arabic and konjac gum, and the mass ratio of the mixed powder, adhesive, and environmentally friendly filler is 60-80:10-15:20-30.