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CN112812276A - Preparation method of rosin modified terpene phenol resin - Google Patents

Preparation method of rosin modified terpene phenol resin Download PDF

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Publication number
CN112812276A
CN112812276A CN202110072181.9A CN202110072181A CN112812276A CN 112812276 A CN112812276 A CN 112812276A CN 202110072181 A CN202110072181 A CN 202110072181A CN 112812276 A CN112812276 A CN 112812276A
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Prior art keywords
rosin
phenol resin
modified terpene
terpene phenol
acid
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Inventor
徐媚
卢俊琳
曾丽丽
周浩
张锦龙
冉岳琴
杨毅融
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Xiamen Doingcom Chemical Co ltd
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Xiamen Doingcom Chemical Co ltd
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    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G61/00Macromolecular compounds obtained by reactions forming a carbon-to-carbon link in the main chain of the macromolecule
    • C08G61/02Macromolecular compounds containing only carbon atoms in the main chain of the macromolecule, e.g. polyxylylenes
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G2261/00Macromolecular compounds obtained by reactions forming a carbon-to-carbon link in the main chain of the macromolecule
    • C08G2261/10Definition of the polymer structure
    • C08G2261/12Copolymers
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G2261/00Macromolecular compounds obtained by reactions forming a carbon-to-carbon link in the main chain of the macromolecule
    • C08G2261/10Definition of the polymer structure
    • C08G2261/14Side-groups
    • C08G2261/142Side-chains containing oxygen
    • C08G2261/1422Side-chains containing oxygen containing OH groups
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    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G2261/00Macromolecular compounds obtained by reactions forming a carbon-to-carbon link in the main chain of the macromolecule
    • C08G2261/30Monomer units or repeat units incorporating structural elements in the main chain
    • C08G2261/31Monomer units or repeat units incorporating structural elements in the main chain incorporating aromatic structural elements in the main chain
    • C08G2261/312Non-condensed aromatic systems, e.g. benzene
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G2261/00Macromolecular compounds obtained by reactions forming a carbon-to-carbon link in the main chain of the macromolecule
    • C08G2261/30Monomer units or repeat units incorporating structural elements in the main chain
    • C08G2261/33Monomer units or repeat units incorporating structural elements in the main chain incorporating non-aromatic structural elements in the main chain
    • C08G2261/332Monomer units or repeat units incorporating structural elements in the main chain incorporating non-aromatic structural elements in the main chain containing only carbon atoms
    • C08G2261/3323Monomer units or repeat units incorporating structural elements in the main chain incorporating non-aromatic structural elements in the main chain containing only carbon atoms derived from other monocyclic systems
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G2261/00Macromolecular compounds obtained by reactions forming a carbon-to-carbon link in the main chain of the macromolecule
    • C08G2261/70Post-treatment
    • C08G2261/72Derivatisation
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G2261/00Macromolecular compounds obtained by reactions forming a carbon-to-carbon link in the main chain of the macromolecule
    • C08G2261/70Post-treatment
    • C08G2261/75Reaction of polymer building blocks for the formation of block-copolymers

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  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Phenolic Resins Or Amino Resins (AREA)
  • Adhesives Or Adhesive Processes (AREA)
  • Compositions Of Macromolecular Compounds (AREA)

Abstract

A preparation method of rosin modified terpene phenol resin comprises the following steps: 1) firstly, heating, melting and uniformly mixing phenol and an acidic composite catalyst to obtain a phenol-acidic composite catalyst mixture; heating terpene to 80-150 ℃, then dropwise adding a phenol-acid composite catalyst mixture into the terpene, and stirring; finally adding rosin, heating and refluxing for reaction; 2) after the reaction is finished, adding a neutralizing agent to neutralize the acidic composite catalyst, then continuing heating up and refluxing for reaction, and finally vacuumizing to remove residual phenol, rosin light fraction and terpene oligomer until the test index meets the requirement; 3) cooling, adding an antioxidant, uniformly stirring and discharging to obtain the rosin modified terpene phenol resin. The rosin modified terpene phenol resin is synthesized by adopting the composite protonic acid catalyst under the solvent-free condition, has the characteristics of high temperature resistance, good flexibility and low-temperature tackifying effect, has less sewage and VOC (volatile organic compounds) emission, and is environment-friendly.

Description

Preparation method of rosin modified terpene phenol resin
Technical Field
The invention relates to the field of chemical products, in particular to a preparation method of rosin modified terpene phenol resin.
Background
The terpene-phenol resin is a phenol modified terpene resin and is obtained by copolycondensating terpene and phenol under the condition of a catalyst. Wherein the terpene is unsaturated cyclic C derived from turpentine, sulfate papermaking process and citrus oil10Hydrocarbons, a natural renewable resource. The terpene-phenol resin has good compatibility with various matrix resins, is an excellent tackifying resin of acrylic resin, styrene-butadiene rubber, natural rubber, chloroprene rubber, SIS (styrene-isoprene-styrene block copolymer) and SBS (styrene-butadiene-styrene block copolymer), and can provide ductility and flexibility for manufacturing hot melt adhesives and coatings. The preparation of terpene phenol resin generally adopts Friedel-crafts catalysts such as boron trifluoride and aluminum trichloride and protonic acid catalysts such as sulfuric acid and benzenesulfonic acid; generally, a cold polymerization process is adopted, and benzene solvents such as toluene, xylene and the like are often used in the preparation process. And after the reaction is finished, adding a catalyst neutralizer, washing with water, separating a water layer from an organic layer, distilling the organic layer at a high temperature, and removing the solvent and low molecular weight substances to obtain the tackifying resin. In addition, volatile and toxic organic solvents such as dimethylbenzene are used, which is not beneficial to controlling the VOC content in resin products.
Disclosure of Invention
The invention aims to solve the problems in the prior art and provides a preparation method of rosin modified terpene phenol resin with different ring and ball softening points, the rosin modified terpene phenol resin has the characteristics of high temperature resistance and good low-temperature adhesion, and the preparation method adopts a composite protonic acid catalyst, does not need to use a solvent and neutralize and wash water, does not produce a large amount of waste water, and can reduce environmental pollution.
In order to achieve the purpose, the invention adopts the following technical scheme:
a preparation method of rosin modified terpene phenol resin comprises the following steps:
1) firstly, heating, melting and uniformly mixing phenol and an acidic composite catalyst to obtain a phenol-acidic composite catalyst mixture; heating terpene to 80-150 ℃, then dropwise adding a phenol-acid composite catalyst mixture into the terpene, and stirring; finally adding rosin, heating and refluxing for reaction;
2) after the reaction is finished, adding a neutralizing agent to neutralize the acidic composite catalyst, then continuing heating up and refluxing for reaction, and finally vacuumizing to remove residual phenol, rosin light fraction and terpene oligomer until the test index meets the requirement;
3) cooling, adding an antioxidant, uniformly stirring and discharging to obtain the rosin modified terpene phenol resin.
The acidic composite catalyst comprises organic protonic acid and inorganic protonic acid.
The inorganic protonic acid comprises sulfuric acid, phosphoric acid and hypophosphorous acid; the organic protonic acid comprises benzene sulfonic acid, p-methyl benzene sulfonic acid, methyl sulfonic acid and dodecyl benzene sulfonic acid.
The terpene comprises at least one of alpha-pinene, beta-pinene, limonene, dipentene, carene, terpinolene and camphene.
The rosin comprises at least one of gum rosin, wood rosin and tall oil rosin; the neutralizer comprises magnesium oxide, zinc oxide and calcium oxide.
The weight ratio of the phenol to the terpene is 1.5-0.3; the weight ratio of the rosin to the terpene is 0.6-2.0.
The weight percentage of the acidic composite catalyst and the terpene is 0.1-2%.
In the step 1), the heating and melting temperature is 60-90 ℃; the temperature of the heating reflux is 120-160 ℃, and the time is 5-10 h.
In the step 2), the temperature of the heating reflux is 240-280 ℃, and the time is 4-8 h; in step 3), the temperature is reduced to below 210 ℃, and an antioxidant is added.
The rosin modified terpene phenol resin prepared by the preparation method has a ring-ball softening point of 95-150 ℃, an acid value of 15-50 and a weight average molecular weight of 800-1300.
Rosin is an important natural product in China and is a viable resource. After the terpene-phenol resin is modified by rosin, rosin acid groups are introduced into the terpene-phenol polymer, so that the high temperature resistance, the cohesion and the compatibility of the resin can be improved, and the application of the resin in the fields of adhesives, printing ink and rubber can be widened.
Compared with the prior art, the technical scheme of the invention has the following beneficial effects:
the invention uses rosin in modified terpene phenol resin by chemical method, under the condition of acid composite catalyst, rosin and earlier stage terpene-phenol copolymer are further reacted and polycondensed, after the polycondensation reaction is terminated by neutralizing acid composite catalyst, the temperature is further raised to make terpene-phenol-rosin copolymer produce intermolecular esterification reaction, so that the acid value can be reduced, and the ageing resistance of resin can be raised. The rosin modified terpene phenol resin prepared by the method of the invention introduces abietic acid with a tricyclic condensed ring structure into the terpene phenol resin, increases the rigidity and polarity of the resin, and can improve the adhesive force, cohesive force, heat resistance, aging resistance and low-temperature adhesive property of the adhesive.
The rosin modified terpene phenol resin prepared by the invention has important application in preparing hot melt adhesive. The rosin modified terpene phenol resin has high temperature resistance, good flexibility and low-temperature tackifying effect, the polarity and softening point of the resin can be adjusted according to the using amounts of rosin and phenol, the rosin modified terpene phenol resin has good compatibility with elastomers such as EVA elastomers, natural rubber, chloroprene rubber, SIS rubber and SBS rubber, the rosin modified terpene phenol resin can be used as tackifying resin of an adhesive, and preferably used as pressure-sensitive hot melt adhesive and hot melt adhesive tackifying resin with high temperature resistance, good flexibility and low-temperature tackifying effect, in addition, the polarity and glossiness of the resin can be adjusted by adjusting the weight ratio of phenol to terpene and the weight ratio of rosin to terpene, and the resin is applied to the field of ink.
Detailed Description
In order to make the technical problems, technical solutions and advantageous effects to be solved by the present invention clearer and more obvious, the present invention is further described in detail below with reference to the following embodiments.
The invention relates to a preparation method of rosin modified terpene phenol resin, which comprises the following steps:
1) firstly, heating, melting and uniformly mixing phenol and an acidic composite catalyst at 60-90 ℃ to obtain a phenol-acidic composite catalyst mixture; heating terpene to 80-150 ℃, then dropwise adding a phenol-acid composite catalyst mixture into the terpene, and stirring to synthesize a polycondensation product of phenol and terpene; finally, adding the crushed rosin in batches, heating to 120-160 ℃, and carrying out reflux reaction for 5-10 h to further polymerize the rosin and the terpene phenol polycondensation product;
2) after the reaction is finished, adding a neutralizing agent to neutralize the acidic composite catalyst to prevent decarboxylation and decomposition of the resin at high temperature, and then continuously refluxing for 4-8 h at 240-280 ℃ to perform esterification reaction and reduce the acid value; finally, vacuumizing to remove residual phenol, rosin light fraction and terpene oligomer until the test index meets the requirement; if light-colored resin is needed, a thiophenol decolorant (such as 4, 4' -thiobis (6-tert-butyl-3-methylphenol)) can be added after the acid composite catalyst is neutralized for light-colored treatment;
3) cooling to below 210 ℃, adding an antioxidant, uniformly stirring and discharging to obtain the rosin modified terpene phenol resin.
The terpene is at least one of alpha-pinene, beta-pinene, limonene, dipentene, carene, terpinolene and camphene; in a more preferred embodiment, the terpene is at least one of α -pinene, limonene, dipentene, carene, terpinolene, camphene; in a most preferred embodiment, the terpene is at least one of limonene, dipentene, carene, terpinolene, camphene. The terpene raw materials of the invention all adopt terpene clear oil prepared by the company.
The acidic composite catalyst is composed of at least two of sulfuric acid, phosphoric acid, hypophosphorous acid, benzenesulfonic acid, p-toluenesulfonic acid, methanesulfonic acid and dodecylbenzenesulfonic acid. The acidic composite catalyst is mainly used for catalyzing the condensation polymerization of terpene, phenol and rosin, and improving the reaction efficiency. The catalytic efficiency of sulfuric acid and phosphoric acid is high, but equipment is easy to corrode, rosin decarboxylation is easy to cause, and side reactions are increased; the hypophosphorous acid has medium catalytic efficiency and certain decolorizing effect. Organic protonic acids such as benzenesulfonic acid, p-toluenesulfonic acid and the like have medium catalytic efficiency, but the boiling point of the catalyst is low, and the reaction temperature needs to be controlled to be low, so that the reaction time is long, and the production of light-colored resin is not facilitated. Through a great deal of research, the invention discovers that the use of the catalyst compounded with the organic protonic acid and the inorganic protonic acid can improve the reaction temperature, shorten the reaction time, improve the polycondensation reaction efficiency of the terpene, the phenol and the rosin and obtain the light-colored resin.
The weight ratio of the phenol to the terpene is 1.5-0.3; in a more preferred embodiment, the weight ratio of phenol to terpene is 1.0 to 0.3; in a most preferred embodiment, the weight ratio of phenol to terpene is from 0.8 to 0.4. The amount of phenol directly affects the early polycondensation reaction and the late esterification reaction. As the amount of phenol increases, the softening point increases and the polarity of the resin increases. However, if the amount of phenol is too large, the transparency of the resin is lowered, and the application of the resin in hot melt adhesives is affected.
The weight ratio of the acidic composite catalyst to the terpene is 0.1-2%; in a particularly preferred embodiment, the weight ratio of the acidic composite catalyst to the terpene is from 0.2% to 1.5%. When the dosage of the acidic composite catalyst is less than 0.1%, the catalytic efficiency is low, and the yield of the obtained product is low; with the increase of the dosage of the acidic composite catalyst, the product yield is increased and the softening point is increased; when the dosage of the acidic composite catalyst is more than 2 percent, side reaction is increased, rosin decarboxylation occurs, the resin yield is reduced, and the softening point is reduced.
The rosin is at least one of gum rosin, wood rosin and tall oil rosin. Suitable rosins may be of various origins, gum rosins obtained by distillation of rosin; wood rosin extracted from pine wood chips; tall oil rosin, a by-product of the sulfate papermaking process. The rosin is mainly C20The tricyclic condensed ring monocarboxylic acid (represented by abietic acid and pimaric acid) contains a plurality of double bonds in the molecule, so that under the action of an acidic composite catalyst, rosin can be subjected to polycondensation reaction with a terpene-phenol copolymer at a low temperature, part of rosin can also be directly subjected to alkylation reaction with phenol, and after the acidic composite catalyst is neutralized, the temperature is increased, esterification reaction can be further performed, the acid value is reduced, and the aging resistance of the resin is improved.
The weight ratio of the rosin to the terpene is 0.6-2.0; in a particularly preferred embodiment, the weight ratio of rosin to terpene is from 0.8 to 1.5; the use amount of the rosin is increased, so that the molecular weight of the resin can be increased, and the softening point of the resin can be increased.
The resin prepared by the method has a ring-ball softening point of 95-150 ℃, an acid value of 15-50 and a weight average molecular weight of 800-1300.
Example 1
In an embodiment of the method for preparing rosin modified terpene phenol resin of the present invention, the method of this embodiment comprises the following steps:
(1) 127g of phenol and 0.43g of an acidic composite catalyst (50% of sulfuric acid and 50% of benzenesulfonic acid) were heated, melted and mixed uniformly at 85 ℃ to obtain a phenol-acidic composite catalyst mixture.
(2) 425g of terpene naphtha TO1 (produced by Zhongkun chemical company and mainly comprising dipentene, carene and terpinolene) was put into a four-neck flask and heated TO 90 ℃. The phenol-acid composite catalyst mixture is dripped at the temperature of 90 ℃ for 1 hour, and the stirring is continued for 1 hour after the addition.
(3) 361g of crushed first-class gum rosin is added in batches, the temperature is raised to 120 ℃, and the reflux reaction is carried out for 8 hours.
(4) Adding 0.6g of magnesium oxide serving as a neutralizing agent, stirring for 30min, and neutralizing the acidic composite catalyst.
(5) Heating to 265 ℃ and keeping the temperature for reaction for 4 h. And starting a vacuum pump, and vacuumizing for 3 hours until the test index meets the target requirement.
(6) And cooling to 210 ℃, adding the antioxidants 1010 and 168, uniformly stirring and discharging to obtain the rosin modified terpene phenol resin.
The rosin-modified terpene phenol resin obtained in this example, as measured by the ring and ball method, had a softening point of 98.0 ℃ and an acid value of 35.8mg KOH/g.
Example 2
In an embodiment of the method for preparing rosin modified terpene phenol resin of the present invention, the method of this embodiment comprises the following steps:
(1) 386g of phenol and 2.8g of composite catalyst (50 percent of phosphoric acid, 20 percent of benzenesulfonic acid and 30 percent of dodecylbenzenesulfonic acid) are heated, melted and mixed uniformly at 65 ℃ to obtain a phenol-acid composite catalyst mixture.
(2) 550g of terpene clear oil TO2 (produced by Zhongkun chemical company, and mainly composed of dipentene and terpinolene) was put into a four-neck flask, and the temperature was raised TO 130 ℃. Dripping the mixture of the phenol-acid composite catalyst for 1 hour at the temperature of 130 ℃, and continuing stirring for 1 hour after the addition.
(3) 385g of crushed primary wood rosin is added in batches, the temperature is raised to 140 ℃, and the reflux reaction is carried out for 6 hours.
(4) Adding 4.5g of zinc oxide as a neutralizing agent, stirring for 30min, and neutralizing the acidic composite catalyst.
(5) Heating to 260 ℃ and keeping the temperature for reaction for 6 h. And starting a vacuum pump, and vacuumizing for 4 hours until the test index meets the target requirement.
(6) And cooling to 210 ℃, adding the antioxidants 1010 and 168, uniformly stirring and discharging to obtain the rosin modified terpene phenol resin.
The rosin-modified terpene phenol resin obtained in this example, as measured by the ring and ball method, had a softening point of 127.5 ℃ and an acid value of 46.9mg KOH/g.
Example 3
In an embodiment of the method for preparing rosin modified terpene phenol resin of the present invention, the method of this embodiment comprises the following steps:
(1) 420g of phenol and 6.3g of a composite catalyst (50% of hypophosphorous acid, 30% of benzenesulfonic acid and 20% of methanesulfonic acid) were heated, melted and mixed uniformly at 80 ℃ to obtain a phenol-acidic composite catalyst mixture.
(2) 525g of terpene naphtha TO1 (produced by Zhongkun chemical company, main components of dipentene and terpinolene) was put into a four-neck flask, and the temperature was raised TO 110 ℃. Dripping the phenol-acid composite catalyst mixture for 2 hours at the temperature of 110 ℃, and continuing stirring for 1 hour after the addition is finished.
(3) 367g of crushed first-grade wood rosin is added in batches, the temperature is raised to 130 ℃, and the reflux reaction is carried out for 8 hours.
(4) Adding 8.2g of calcium oxide serving as a neutralizing agent, stirring for 30min, and neutralizing the acidic composite catalyst.
(5) Heating to 270 ℃ and preserving the temperature for reaction for 6 h. And starting a vacuum pump, and vacuumizing for 3 hours until the test index meets the target requirement.
(6) And cooling to 210 ℃, adding the antioxidants 1010 and 168, uniformly stirring and discharging to obtain the rosin modified terpene phenol resin.
The rosin-modified terpene phenol resin obtained in this example, as measured by the ring and ball method, had a softening point of 123.0 ℃ and an acid value of 18.7mg KOH/g.
Example 4
In an embodiment of the method for preparing rosin modified terpene phenol resin of the present invention, the method of this embodiment comprises the following steps:
(1) 384g phenol and 8.7g composite catalyst (50% sulfuric acid, 25% p-toluenesulfonic acid and 25% methanesulfonic acid) were heated, melted and mixed uniformly at 70 ℃ to obtain a phenol-acid composite catalyst mixture.
(2) 480g of terpene naphtha TO2 (produced by Zhongkun chemical company, and the main components of which are dipentene and terpinolene) are added into a four-neck flask, and the temperature is raised TO 130 ℃. Dripping the phenol-acid composite catalyst mixture for 2 hours at the temperature of 130 ℃, and continuing stirring for 1 hour after the addition is finished.
(3) 480g of crushed first-grade gum rosin is added in batches, the temperature is raised to 150 ℃, and the reflux reaction is carried out for 6 hours.
(4) Adding magnesium oxide as neutralizer 12.0g, stirring for 30min, and neutralizing the acidic composite catalyst.
(5) Heating to 275 deg.c and maintaining the temperature for reaction for 5 hr. And starting a vacuum pump, and vacuumizing for 4 hours until the test index meets the target requirement.
(6) And cooling to 210 ℃, adding an antioxidant DTBHQ, uniformly stirring and discharging to obtain the rosin modified terpene phenol resin.
The rosin-modified terpene phenol resin obtained in this example had a softening point of 147.5 ℃ and an acid value of 42.7mg KOH/g, as measured by the ring and ball method.
Example 5
In an embodiment of the method for preparing rosin modified terpene phenol resin of the present invention, the method of this embodiment comprises the following steps:
(1) 306g of phenol and 9.2g of a composite catalyst (50% of phosphoric acid, 20% of p-toluenesulfonic acid and 30% of methanesulfonic acid) were heated, melted and mixed uniformly at 87 ℃ to obtain a phenol-acidic composite catalyst mixture.
(2) 510g of terpene varnish TO2 (manufactured by Zhongkun chemical company, and mainly containing dipentene and terpinolene) was put into a four-neck flask, and the temperature was raised TO 140 ℃. Dripping the phenol-acid composite catalyst mixture for 2 hours at the temperature of 140 ℃, and continuing stirring for 1 hour after the addition is finished.
(3) 357g of crushed tall oil rosin is added in batches, the temperature is raised to 150 ℃, and the reflux reaction is carried out for 6 hours.
(4) Adding 12.8g of magnesium oxide serving as a neutralizing agent, stirring for 30min, and neutralizing the acidic composite catalyst.
(5) Heating to 255 ℃ and keeping the temperature for reaction for 7 h. And starting a vacuum pump, and vacuumizing for 4 hours until the test index meets the target requirement.
(6) And cooling to 210 ℃, adding the antioxidants 1010 and 168, uniformly stirring and discharging to obtain the rosin modified terpene phenol resin.
The rosin-modified terpene phenol resin obtained in this example had a softening point of 113.5 ℃ and an acid value of 21.9mg KOH/g, as measured by the ring and ball method.
Example 6
In an embodiment of the method for preparing rosin modified terpene phenol resin of the present invention, the method of this embodiment comprises the following steps:
(1) 386g of phenol and 5.9g of composite catalyst (30 percent of phosphoric acid, 40 percent of p-toluenesulfonic acid and 30 percent of benzenesulfonic acid) are heated, melted and mixed uniformly at 80 ℃ to obtain a phenol-acid composite catalyst mixture.
(2) 392g of terpene naphtha TO1 (produced by Zhongkun chemical company, main components of dipentene and terpinolene) was put into a four-neck flask, and the temperature was raised TO 120 ℃. Dripping the phenol-acid composite catalyst mixture for 3 hours at the temperature of 120 ℃, and continuing stirring for 1 hour after the addition is finished.
(3) 429g of crushed primary wood rosin is added in batches, the temperature is raised to 150 ℃, and the reflux reaction is carried out for 6 hours.
(4) Adding 8.19g of magnesium oxide serving as a neutralizing agent, stirring for 30min, and neutralizing the acidic composite catalyst.
(5) The temperature is increased to 275 ℃ and the reaction is kept for 6 h. And starting a vacuum pump, and vacuumizing for 3 hours until the test index meets the target requirement.
(6) And cooling to 210 ℃, adding the antioxidants 1010 and 168, uniformly stirring and discharging to obtain the rosin modified terpene phenol resin.
The rosin-modified terpene phenol resin obtained in this example had a softening point of 145.5 ℃ and an acid value of 27.4mg KOH/g, as measured by the ring and ball method.
The rosin modified terpene phenol resin prepared by the invention has important application in preparing hot melt adhesive. The rosin modified terpene phenol resin has high temperature resistance, good flexibility and low-temperature tackifying effect, can adjust the polarity and softening point of the resin according to the dosage of rosin and phenol, has good compatibility with elastomers such as EVA elastomers, SIS and SBS, and can be better used for preparing pressure-sensitive hot melt adhesive and hot melt adhesive.
The invention uses rosin in modified terpene phenol resin by chemical method, under the condition of acid composite catalyst, rosin and earlier stage terpene-phenol copolymer are further reacted and polycondensed, after the polycondensation reaction is terminated by neutralizing acid composite catalyst, the temperature is further raised to make terpene-phenol-rosin copolymer undergo intramolecular esterification reaction, so that the acid value can be reduced, and the ageing resistance of resin can be raised. The rosin modified terpene phenol resin prepared by the method of the invention introduces abietic acid with a tricyclic condensed ring structure into the terpene phenol resin, increases the rigidity and polarity of the resin, and can improve the adhesive force, cohesive force, heat resistance, aging resistance and low-temperature adhesive property of the adhesive.

Claims (10)

1. The preparation method of the rosin modified terpene phenol resin is characterized by comprising the following steps:
1) firstly, heating, melting and uniformly mixing phenol and an acidic composite catalyst to obtain a phenol-acidic composite catalyst mixture; heating terpene to 80-150 ℃, then dropwise adding a phenol-acid composite catalyst mixture into the terpene, and stirring; finally adding rosin, heating and refluxing for reaction;
2) after the reaction is finished, adding a neutralizing agent to neutralize the acidic composite catalyst, then continuing heating up and refluxing for reaction, and finally vacuumizing to remove residual phenol, rosin light fraction and terpene oligomer until the test index meets the requirement;
3) cooling, adding an antioxidant, uniformly stirring and discharging to obtain the rosin modified terpene phenol resin.
2. The method for preparing a rosin-modified terpene phenol resin according to claim 1, wherein the rosin-modified terpene phenol resin comprises: the acidic composite catalyst comprises organic protonic acid and inorganic protonic acid.
3. The method for producing a rosin-modified terpene phenol resin according to claim 2, wherein: the inorganic protonic acid comprises sulfuric acid, phosphoric acid and hypophosphorous acid; the organic protonic acid comprises benzene sulfonic acid, p-methyl benzene sulfonic acid, methyl sulfonic acid and dodecyl benzene sulfonic acid.
4. The method for preparing a rosin-modified terpene phenol resin according to claim 1, wherein the rosin-modified terpene phenol resin comprises: the terpene comprises at least one of alpha-pinene, beta-pinene, limonene, dipentene, carene, terpinolene and camphene.
5. The method for preparing a rosin-modified terpene phenol resin according to claim 1, wherein the rosin-modified terpene phenol resin comprises: the rosin comprises at least one of gum rosin, wood rosin and tall oil rosin; the neutralizer comprises magnesium oxide, zinc oxide and calcium oxide.
6. The method for preparing a rosin-modified terpene phenol resin according to claim 1, wherein the rosin-modified terpene phenol resin comprises: the weight ratio of the phenol to the terpene is 1.5-0.3; the weight ratio of the rosin to the terpene is 0.6-2.0.
7. The method for preparing a rosin-modified terpene phenol resin according to claim 1, wherein the rosin-modified terpene phenol resin comprises: the weight percentage of the acidic composite catalyst and the terpene is 0.1-2%.
8. The method for preparing a rosin-modified terpene phenol resin according to claim 1, wherein the rosin-modified terpene phenol resin comprises: in the step 1), the heating and melting temperature is 60-90 ℃; the temperature of the heating reflux is 120-160 ℃, and the time is 5-10 h.
9. The method for preparing a rosin-modified terpene phenol resin according to claim 1, wherein the rosin-modified terpene phenol resin comprises: in the step 2), the temperature of the heating reflux is 240-280 ℃, and the time is 4-8 h; in step 3), the temperature is reduced to below 210 ℃, and an antioxidant is added.
10. The rosin-modified terpene phenol resin produced by the production method according to any one of claims 1 to 9, characterized in that: the ring-ball softening point of the rosin modified terpene phenol resin is 95-150 ℃, the acid value is 15-50, and the weight average molecular weight is 800-1300.
CN202110072181.9A 2021-01-19 2021-01-19 Preparation method of rosin modified terpene phenol resin Pending CN112812276A (en)

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Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3198760A (en) * 1961-08-15 1965-08-03 Tenneco Chem Polychloroprene stabilized with a phenol-terpene resin and a metal resinate and process for preparation
CN1668717A (en) * 2002-05-13 2005-09-14 阿利桑那化学公司 Phenolic-modified rosin terpene resin
CN104559795A (en) * 2014-12-24 2015-04-29 广西科茂林化有限公司 High-temperature-resistant rosin tackifying resin and preparation method thereof
CN110003446A (en) * 2019-03-20 2019-07-12 江西金安林产实业有限公司 A kind of light color and high softening-point terpene phenol resin and the preparation method and application thereof

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3198760A (en) * 1961-08-15 1965-08-03 Tenneco Chem Polychloroprene stabilized with a phenol-terpene resin and a metal resinate and process for preparation
CN1668717A (en) * 2002-05-13 2005-09-14 阿利桑那化学公司 Phenolic-modified rosin terpene resin
CN104559795A (en) * 2014-12-24 2015-04-29 广西科茂林化有限公司 High-temperature-resistant rosin tackifying resin and preparation method thereof
CN110003446A (en) * 2019-03-20 2019-07-12 江西金安林产实业有限公司 A kind of light color and high softening-point terpene phenol resin and the preparation method and application thereof

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Application publication date: 20210518