CN116496757A - Modified oil tea cake-based adhesive and preparation method and application thereof - Google Patents

Modified oil tea cake-based adhesive and preparation method and application thereof Download PDF

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Publication number
CN116496757A
CN116496757A CN202310449546.4A CN202310449546A CN116496757A CN 116496757 A CN116496757 A CN 116496757A CN 202310449546 A CN202310449546 A CN 202310449546A CN 116496757 A CN116496757 A CN 116496757A
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China
Prior art keywords
oil tea
tea cake
based adhesive
parts
modified oil
Prior art date
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Pending
Application number
CN202310449546.4A
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Chinese (zh)
Inventor
吴红
肖志红
李力
王勇
李昌珠
李培旺
张爱华
刘旭东
彭邵锋
吉悦娜
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Hunan Academy of Forestry
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Hunan Academy of Forestry
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Publication date
Application filed by Hunan Academy of Forestry filed Critical Hunan Academy of Forestry
Priority to CN202310449546.4A priority Critical patent/CN116496757A/en
Publication of CN116496757A publication Critical patent/CN116496757A/en
Pending legal-status Critical Current

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    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J189/00—Adhesives based on proteins; Adhesives based on derivatives thereof
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B27—WORKING OR PRESERVING WOOD OR SIMILAR MATERIAL; NAILING OR STAPLING MACHINES IN GENERAL
    • B27N—MANUFACTURE BY DRY PROCESSES OF ARTICLES, WITH OR WITHOUT ORGANIC BINDING AGENTS, MADE FROM PARTICLES OR FIBRES CONSISTING OF WOOD OR OTHER LIGNOCELLULOSIC OR LIKE ORGANIC MATERIAL
    • B27N3/00—Manufacture of substantially flat articles, e.g. boards, from particles or fibres
    • B27N3/002—Manufacture of substantially flat articles, e.g. boards, from particles or fibres characterised by the type of binder
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B27—WORKING OR PRESERVING WOOD OR SIMILAR MATERIAL; NAILING OR STAPLING MACHINES IN GENERAL
    • B27N—MANUFACTURE BY DRY PROCESSES OF ARTICLES, WITH OR WITHOUT ORGANIC BINDING AGENTS, MADE FROM PARTICLES OR FIBRES CONSISTING OF WOOD OR OTHER LIGNOCELLULOSIC OR LIKE ORGANIC MATERIAL
    • B27N3/00—Manufacture of substantially flat articles, e.g. boards, from particles or fibres
    • B27N3/08—Moulding or pressing
    • B27N3/10—Moulding of mats
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J11/00—Features of adhesives not provided for in group C09J9/00, e.g. additives
    • C09J11/02—Non-macromolecular additives
    • C09J11/04—Non-macromolecular additives inorganic
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J11/00—Features of adhesives not provided for in group C09J9/00, e.g. additives
    • C09J11/02—Non-macromolecular additives
    • C09J11/06—Non-macromolecular additives organic
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J129/00—Adhesives based on homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by an alcohol, ether, aldehydo, ketonic, acetal, or ketal radical; Adhesives based on hydrolysed polymers of esters of unsaturated alcohols with saturated carboxylic acids; Adhesives based on derivatives of such polymers
    • C09J129/02—Homopolymers or copolymers of unsaturated alcohols
    • C09J129/04—Polyvinyl alcohol; Partially hydrolysed homopolymers or copolymers of esters of unsaturated alcohols with saturated carboxylic acids
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
    • C08K3/00—Use of inorganic substances as compounding ingredients
    • C08K3/38—Boron-containing compounds
    • C08K2003/387—Borates
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02W—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO WASTEWATER TREATMENT OR WASTE MANAGEMENT
    • Y02W30/00—Technologies for solid waste management
    • Y02W30/50—Reuse, recycling or recovery technologies
    • Y02W30/91—Use of waste materials as fillers for mortars or concrete

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  • Chemical & Material Sciences (AREA)
  • Organic Chemistry (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Manufacturing & Machinery (AREA)
  • Wood Science & Technology (AREA)
  • Forests & Forestry (AREA)
  • Inorganic Chemistry (AREA)
  • Adhesives Or Adhesive Processes (AREA)

Abstract

The invention discloses a modified oil tea cake based adhesive, and a preparation method and application thereof, wherein the preparation raw materials of the modified oil tea cake based adhesive comprise: borax, pyrogallol, polyvinyl alcohol, oil tea cake protein and triglycidyl amine. The invention provides a modified oil tea cake-based adhesive which can realize the enhancement of the flame retardant property and the mechanical property of a plate.

Description

Modified oil tea cake-based adhesive and preparation method and application thereof
Technical Field
The invention belongs to a tea-oil cake protein-based adhesive, and particularly relates to a modified tea-oil cake protein-based adhesive, and a preparation method and application thereof.
Background
Along with the collapse of wood resources, people increasingly replace solid wood furniture with artificial board furniture, so that the consumption of adhesive is also increasing. The research and application of the adhesive are a new science for a long time, at present, the adhesive for the artificial board is mainly made of 'trialdehyde glue', but the 'trialdehyde glue' is mainly made of formaldehyde, urea, melamine, phenol and the like, and toxic and harmful substances such as formaldehyde, phenol and the like can be released in the production, transportation and use processes. Along with the gradual enhancement of environmental awareness of people, the search for a novel natural environment-friendly adhesive to replace 'triacid adhesive' becomes a necessary trend. The biomass adhesive mainly comprises a protein adhesive, a starch adhesive, a lignin adhesive, a pyrolysis bio-oil adhesive and modified products thereof. The oil tea cake is used as a byproduct in the oil tea processing industry and mainly contains substances such as protein, polysaccharide, tea saponin, cellulose, tannin and the like. In the traditional process, the oil tea cake is generally used for extracting tea saponin and polysaccharides, but the production process is complex and the cost is high, so that the large-scale industrial application is not realized at present. The oil tea cake can also be used as an organic fertilizer, but because the oil tea cake contains tea saponin, the tea saponin is a hemolytic toxin, and can dissolve red blood cells of aquatic animals, and serious toxicity is generated on fishes, loaches, snails, clams and the like, so that the oil tea cake needs to be detoxified if the oil tea cake is used as the organic fertilizer. The wood adhesive prepared from the oil tea cake not only can effectively improve the utilization rate of the oil tea cake, but also is beneficial to improving the added value of the whole oil tea processing industry chain. As an environment-friendly adhesive, the oil tea cake adhesive has no formaldehyde release problem in the production and product application stages. Meanwhile, the oil tea cake is taken as a renewable resource, and the large-scale application of the oil tea cake has great promotion effect on reducing the petrochemical resource dependence and has important practical significance on the development of the wood industry. The prior art discloses an aldehyde-free oil tea cake protein-based wood adhesive and a preparation and use method thereof. The formaldehyde-free protein-based wood adhesive comprises water, oil tea cake protein, a modifier, a cross-linking agent, a curing agent, a filler and an additive; the components are prepared from the following components in parts by mass: 100 parts of water, 20-40 parts of oil tea cake protein, 0.1-5 parts of modifier, 20-40 parts of cross-linking agent, 2-20 parts of curing agent, 1-5 parts of filler and 0-3 parts of additive. And (3) dissolving the oil tea cake protein, and performing a crosslinking reaction and a curing reaction to form a finished product. The adhesive has poor water resistance and low bonding strength, meanwhile, a large amount of impurities exist in the oil tea cake protein, the protein can be obtained by further separation, in addition, the adhesive can realize a flame retardant effect by adding a flame retardant, and the preparation method is complex.
In conclusion, the development of a preparation method and application of the modified oil tea cake-based adhesive, which can effectively improve the physical and mechanical properties and flame retardant properties of the rapid material, is urgent.
Disclosure of Invention
The present invention aims to solve at least one of the technical problems existing in the prior art. Therefore, the invention provides the modified oil tea cake based adhesive which does not need formaldehyde addition and has good mechanical property and flame retardant property.
According to an embodiment of the first aspect of the invention, the preparation raw materials of the modified oil tea cake based adhesive comprise: borax, pyrogallol, polyvinyl alcohol, oil tea cake protein and triglycidyl amine.
The reaction principle of the invention is as follows:
the preparation method comprises the steps of obtaining a prepolymer with boric acid ester bonds, hydrogen bonds and pi-pi bond stacks for linking by utilizing polyvinyl alcohol, borax and pyrogallol to react, wherein the prepolymer is a soft segment crosslinked network taking the polyvinyl alcohol as a main body; active groups (amino, carboxyl, hydroxyl, sulfhydryl and the like) on the oil tea cake protein react with triglycidyl amine to form a hard segment part of a crosslinked network.
The modified oil tea cake-based adhesive curing reaction mainly comprises the following steps:
(1) In the curing reaction process, the prepolymer can be subjected to curing reaction to form a soft segment three-dimensional network structure taking a boric acid ester bond as a main body;
(2) The triglycidyl amine is polymerized through epoxy ring opening, and a polymerization reaction is carried out through active groups on the oil-tea camellia cake protein macromolecules to form a hard segment three-dimensional network structure taking the oil-tea camellia cake protein macromolecules as a main body;
(3) The formation process of the double-crosslinked network structure comprises the following steps: the hydroxyl in the oil tea cake protein can also replace part of polyvinyl alcohol and borax to form boric acid ester bond, hydrogen bond and pi-pi bond stack for linking, so that the formed crosslinked network soft chain segment and hard chain segment are combined, the oil tea cake protein has a stable double-crosslinked network structure, the gluing performance of the adhesive is enhanced, and the cured adhesive has certain self-repairing performance and flame retardant performance.
According to some embodiments of the present invention, the preparation raw materials of the modified oil tea cake based adhesive include, in parts by weight: 5-8 parts of borax, 10-13 parts of pyrogallol, 6-18 parts of polyvinyl alcohol, 12-15 parts of oil tea cake protein and 0.5-10 parts of triglycidyl amine.
According to some embodiments of the invention, the weight ratio of the polyvinyl alcohol to the triglycidyl amine is 3:2.
In the invention, the addition of the polyvinyl alcohol and the addition of the triglycidyl amine are key factors for influencing the difference of the performance of the whole adhesive. The addition of too high or too low amounts of both components adversely affects the overall properties. The excessive addition of the polyvinyl alcohol can influence the sufficient reaction of boric acid and pyrogallol with the polyvinyl alcohol due to steric hindrance, and the too low addition can lead to too high proportion of the boric acid and the pyrogallol and too high residual unreacted substances, thereby influencing the subsequent reaction to be smoothly carried out. The excessive content of triglycidyl amine can lead to the main polymerization reaction of triglycidyl amine and the reaction between triglycidyl amine and protein in the reaction process of the hard segment, so that the consumption of reactive groups on a macromolecular chain of the protein is excessive, the polymerization reaction of oil-tea cake protein molecules and modifier soft segments is influenced, and the hard segment cannot be effectively formed due to the excessively low triglycidyl amine.
According to some embodiments of the present invention, the preparation raw materials of the modified oil tea cake based adhesive further include: and (3) a solvent.
According to some embodiments of the invention, the solvent comprises at least one of dimethyl sulfoxide and N, N-dimethylformamide.
According to an embodiment of the second aspect of the present invention, a preparation method of a modified oil tea cake-based adhesive is provided, including:
s1: mixing the borax plate, the pyrogallol and the polyvinyl alcohol to obtain a mixture A;
s2: and mixing the oil tea cake protein and the triglycidyl amine to obtain a mixture B, and then mixing the mixture B with the mixture A.
According to some embodiments of the invention, in step S1, the temperature of the reaction is 90-100 ℃.
According to some embodiments of the invention, in step S1, the reaction time is 1-2 h.
According to some embodiments of the invention, in step S2, the temperature of the reaction is 90-100 ℃.
According to some embodiments of the invention, in step S2, the reaction time is 1-2 h.
According to an embodiment of the third aspect of the invention, an artificial board is provided, wherein the preparation raw materials of the artificial board comprise a modified oil tea cake-based adhesive.
According to some embodiments of the invention, the artificial board comprises a multi-layer board and a particle board.
According to some embodiments of the invention, the method of making the multilayer board includes applying the adhesive to the multilayer board and then hot pressing.
According to some embodiments of the invention, the hot pressing temperature is 110-120 ℃.
According to some embodiments of the invention, in the method for producing a multilayer board, the hot pressing pressure is 1-2 MPa.
According to some embodiments of the invention, in the method for manufacturing the multilayer board, the hot pressing time is 5-10 min.
According to some embodiments of the invention, the sizing amount is 180-230 g/m in the preparation method of the multilayer board 2 。
According to some embodiments of the invention, the method of making the particle board comprises applying the adhesive to a multilayer board and then hot pressing.
According to some embodiments of the invention, the temperature of the hot pressing is 110-120 ℃.
According to some embodiments of the invention, the hot pressing pressure is 1-2 MPa.
According to some embodiments of the invention, in the method for manufacturing the multilayer board, the hot pressing time is 25-40 min.
Detailed Description
Example 1
The embodiment discloses a preparation method of a hybridized double-crosslinked modified oil tea cake-based adhesive, which comprises the following specific steps:
(1) 12 parts of PVA are dissolved in water, the temperature is kept at 95 ℃ for reflux, boric acid, pyrogallol and DMSO (5 parts, 10 parts and 8 parts respectively) are added for continuous reaction for 1-2 hours, and the mixture is cooled to room temperature to obtain the modifier A.
(2) 15 parts of oil tea cake protein is dissolved in water, and then 5 parts of TGA is added, and the mixture is uniformly mixed and stirred. Then adding 10 parts of modifier A, and reacting for 1h at 90 ℃ to obtain the double-crosslinking modified oil tea cake-based adhesive.
Example 2
The embodiment discloses a preparation method of a hybridized double-crosslinked modified oil tea cake-based adhesive, which comprises the following specific steps:
(1) 18 parts of PVA is dissolved in water, the temperature is kept at 95 ℃ for reflux, boric acid, pyrogallol and DMSO (5 parts, 10 parts and 8 parts respectively) are added for continuous reaction for 1-2 hours, and the mixture is cooled to room temperature to obtain the modifier A.
(2) 15 parts of oil tea cake protein is dissolved in water, and then 5 parts of TGA is added, and the mixture is uniformly mixed and stirred. And then adding 10 parts of modifier A to obtain the double-crosslinking modified oil tea cake-based adhesive.
Example 3
The embodiment discloses a preparation method of a hybridized double-crosslinked modified oil tea cake-based adhesive, which comprises the following specific steps:
(1) 6 parts of PVA is dissolved in water, the temperature is kept at 95 ℃ for reflux, boric acid, pyrogallol and DMSO (5 parts, 10 parts and 8 parts respectively) are added for continuous reaction for 1-2 hours, and the mixture is cooled to room temperature to obtain the modifier A.
(2) 15 parts of oil tea cake protein is dissolved in water, and then 5 parts of TGA is added, and the mixture is uniformly mixed and stirred. Then adding 10 parts of modifier A, and reacting for 1h at 90 ℃ to obtain the double-crosslinking modified oil tea cake-based adhesive.
Example 4
The embodiment discloses a preparation method of a hybridized double-crosslinked modified oil tea cake-based adhesive, which comprises the following specific steps:
(1) 12 parts of PVA are dissolved in water, the temperature is kept at 95 ℃ for reflux, boric acid, pyrogallol and DMSO (5 parts, 10 parts and 8 parts respectively) are added for continuous reaction for 1-2 hours, and the mixture is cooled to room temperature to obtain the modifier A.
(2) 15 parts of oil tea cake protein is dissolved in water, 10 parts of TGA is added, and the mixture is uniformly mixed and stirred. Then adding 10 parts of modifier A, and reacting for 1h at 90 ℃ to obtain the double-crosslinking modified oil tea cake-based adhesive.
Example 5
The embodiment discloses a preparation method of a hybridized double-crosslinked modified oil tea cake-based adhesive, which comprises the following specific steps:
(1) 12 parts of PVA are dissolved in water, the temperature is kept at 95 ℃ for reflux, boric acid, pyrogallol and DMSO (5 parts, 10 parts and 8 parts respectively) are added for continuous reaction for 1-2 hours, and the mixture is cooled to room temperature to obtain the modifier A.
(2) 15 parts of oil tea cake protein is dissolved in water, then 0.5 part of TGA is added, and the mixture is uniformly mixed and stirred. Then adding 10 parts of modifier A, and reacting for 1h at 90 ℃ to obtain the double-crosslinking modified oil tea cake-based adhesive.
Comparative example 1
The comparative example discloses a preparation method of a double-crosslinking modified oil-tea camellia cake-based adhesive, and the comparative example is different from example 1 in that borax, pyrogallol and polyvinyl alcohol are not included, and the rest conditions are the same.
Comparative example 2
The comparative example discloses a preparation method of a double-crosslinking modified oil-tea camellia cake-based adhesive, and the comparative example is different from example 1 in that oil-tea camellia cake protein and triglycidyl amine are not included, and the rest conditions are the same.
Test example 1
The test example tests the performances of the double-crosslinking modified oil-tea camellia cake protein-based adhesives obtained in examples 1 to 5 and comparative examples 1 to 2, and three-layer plywood is prepared by hot pressing (the glue applying amount is 180-220g/m < 2 > (double-sided), the hot pressing time is 6min and the hot pressing pressure is 1.2 MPa) with eucalyptus veneers. The test results are shown in table 1:
the test results are shown in table 1:
table 1 performance test in plywood
Comparative example 1 and the composition excluding borax, pyrogallol and polyvinyl alcohol are the same as the rest of the conditions and examples, comparative example 2 does not include oil tea cake protein and triglycidyl amine, and the rest of the conditions and examples are the same, so that the decrease of the strength and the water resistance of the adhesive caused by double cross-linking cannot be realized, and sufficient strength, water resistance and repairability can be formed only by fully forming a double cross-linked network of two components.
Test example 2
The test examples the results of the performance tests of the examples and comparative examples in poplar particle board (P6 type wood shaving board, thickness > 6-13 mm) are shown in Table 2:
TABLE 2 Performance test of adhesives in Poplar particle Board (P6 type particle board, thickness > 6-13 mm)
Comparative example 1 and the composition excluding borax, pyrogallol and polyvinyl alcohol were the same as in the examples, comparative example 2 did not include oil tea cake protein and triglycidyl amine, and the composition alone did not provide sufficient strength and water resistance. Only two are mixed and fully reacted to form a double-crosslinked network, so that high strength and water resistance can be realized.
The embodiments of the present invention have been described in detail, but the present invention is not limited to the above embodiments, and various changes can be made without departing from the spirit of the present invention within the knowledge of those skilled in the art.

Claims (10)

1. The modified oil tea cake based adhesive is characterized by comprising the following preparation raw materials: borax, pyrogallol, polyvinyl alcohol, oil tea cake protein and triglycidyl amine.
2. The modified oil tea cake based adhesive of claim 1, wherein the preparation raw materials of the modified oil tea cake based adhesive comprise, in parts by weight: 5-8 parts of borax, 10-13 parts of pyrogallol, 6-18 parts of polyvinyl alcohol, 12-15 parts of oil tea cake protein and 0.5-10 parts of triglycidyl amine.
3. The modified oil tea cake based adhesive of claim 1, wherein the weight ratio of polyvinyl alcohol to triglycidyl amine is 3:2.
4. The modified oil tea cake based adhesive of claim 1, wherein the preparation raw materials of the modified oil tea cake based adhesive further comprise: a solvent; preferably, the solvent includes at least one of dimethyl sulfoxide and N, N-dimethylformamide.
5. A method for preparing the modified oil tea cake based adhesive as claimed in any one of claims 1 to 4, comprising:
s1: mixing the borax, the pyrogallol and the polyvinyl alcohol to obtain a mixture A;
s2: and mixing the oil tea cake protein and the triglycidyl amine to obtain a mixture B, and then mixing the mixture B with the mixture A.
6. The method according to claim 5, wherein the temperature at which the borax plate, the pyrogallol and the polyvinyl alcohol are mixed is 90 to 100 ℃.
7. The method according to claim 5, wherein the mixing time is 1 to 2 hours.
8. An artificial board, characterized in that the preparation raw materials of the artificial board comprise the modified oil tea cake-based adhesive as claimed in any one of claims 1 to 4.
9. The artificial board according to claim 8, wherein the artificial board comprises a multi-layer board or a particle board.
10. The artificial board according to claim 9, wherein the manufacturing method of the artificial board comprises hot pressing.
CN202310449546.4A 2023-04-24 2023-04-24 Modified oil tea cake-based adhesive and preparation method and application thereof Pending CN116496757A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
CN202310449546.4A CN116496757A (en) 2023-04-24 2023-04-24 Modified oil tea cake-based adhesive and preparation method and application thereof

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
CN202310449546.4A CN116496757A (en) 2023-04-24 2023-04-24 Modified oil tea cake-based adhesive and preparation method and application thereof

Publications (1)

Publication Number Publication Date
CN116496757A true CN116496757A (en) 2023-07-28

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Country Status (1)

Country Link
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