JPS60166301A - Manufacture of molded article of cellulosic material - Google Patents

Abstract

PURPOSE:To obtain a molded article having excellent characteristics such as water-resistance, and to enable the effective reutilization of cellulosic materials, by adding a polybasic acid anhydride to a cellulosic material, kneading with a compound having plural epoxy groups, and hot-pressing the mixture at a high temperature. CONSTITUTION:(A) An esterified cellulosic material containing carboxyl group and obtained by the addition of a polybasic acid anhydride (preferably phthalic anhydride, etc.) to the hydroxyl group of a cellulosic material is mixed with (B) a compound having >=2 epoxy groups (preferably bisphenol-A epoxy compound), and the mixture is thoroughly kneaded. The objective molded article can be produced by applying a pressure necessary for the plastification of the component A, preferably pressure of >=60kg/cm<2> to the kneaded product at a high temperature, preferably at >=120 deg.C to effect the crosslinking of the material by esterification reaction. EFFECT:Effective to resource saving.

Description

Detailed Description of the Invention The present invention involves adding a compound containing an epoxy group with an IC of 2 or more in the molecule to a carboxyl group-containing esterified cellulose material in which a polybasic acid anhydride is added to the hydroxyl group in the cellulose material. , after sufficiently kneading these materials, a pressure necessary to at least partially plasticize the mixture at high temperature is applied, and crosslinking is performed by an esterification reaction. The present invention relates to a manufacturing method.

Fossil resources such as oil and coal are currently used in large quantities as industrial raw materials, but their reserves are limited and there are concerns about their future prospects. On the other hand, cellulose-based materials have recently attracted attention as renewable resources. A typical cellulosic material is wood, which is used in large quantities as a raw material for building materials and pulp, but there are also small pieces of wood, waste paper, rice straw, wheat straw, rice husk, etc. that are produced by the wood industry. Cellulosic materials such as linters, bagas, and sulphurs are also present in large quantities. Research on how to use them has become active as we enter an age of resource conservation. Among these, wood chips are the most widely used, and are already being used in large quantities as raw materials for particle boards, fiberboards, and the like. However, although some usage methods are being developed for other cellulose-based materials, they have not yet been used as new resources, and most of them are disposed of by incineration or other methods, and there are no effective methods. Development of usage methods is desired.

The present inventors focused on cellulose-based materials, which are in the recycle period and are discarded in large quantities unused, and as a result of intensive study, they developed a method to utilize the reactivity of hydroxyl groups in cellulose-based materials. By crosslinking an esterified cellulose-based material containing carboxyl groups with a polybasic acid anhydride added to the epoxy resin at high temperature by applying pressure necessary to at least partially plasticize the material, the cellulose-based material becomes the main component. They discovered that a molded article with certain excellent properties could be obtained.

BACKGROUND ART Conventionally, the technology of using wood flour as an extender or filler for synthetic resins in cellulose-based materials and the like is well known. In this case, the wood flour is simply physically mixed with the synthetic resin, and it is extremely difficult to disperse it uniformly and finely in the resin, and the molded products obtained from these materials have poor surface smoothness and gloss. Furthermore, there was a decline in hardness and strength, and there was a drawback that it could only be used for specific applications that did not require much beauty or strength.

On the other hand, recently, molded products made from epoxy resins have excellent electrical properties, moisture resistance, chemical resistance, and impact resistance, so they can be used as electrical insulating materials for printed circuit boards, etc., and are also highly durable. Due to its properties, hardness, and dimensional stability, it has come to be used as a material for various industrial products, and has attracted attention as it has been discovered to have many characteristics that are not found in conventionally used phenolic resins, melamine resins, etc. .

Therefore, by using this epoxy resin, which has many characteristics, it is possible to combine cellulose-based materials such as waste paper, rice straw, wheat straw, rice husk, linter, and bagasse, which are discarded in large quantities without being used, with excellent properties. Developing a technology to easily and inexpensively manufacture molded products having the same properties is extremely meaningful from an economical and resource-saving perspective.

In view of the above-mentioned circumstances, the present inventors conducted extensive studies and found that an esterified cellulose material containing a carboxyl group, in which a polybasic acid anhydride is added to the hydroxyl group in the cellulose material, has two or more epoxy groups in the molecule. After adding a compound containing the compound and sufficiently kneading them, a pressure necessary to partially plasticize the kneaded product at high temperature is applied to cause crosslinking, thereby forming a cellulose-based material. It was discovered that a molded article having excellent properties as a main component can be obtained, leading to the present invention.

That is, the present invention adds a compound containing two or more epoxy groups in the molecule to a carboxino group-containing esterified cellulose material in which a polybasic acid anhydride is added to the hydroxyl group in the cellulose material. After sufficiently kneading these, the mixed material is molded by applying pressure necessary to at least partially plasticize it at a high temperature.This allows the carboxyl groups in the esterified cellulose material to form the epoxy compound. Esterification cell a is formed by esterification reaction with epoxy groups.
The present invention provides a method for manufacturing a cellulose-based material molded article, characterized in that a cellulose-based material is cross-linked via the epoxy 7 compound. The molded product obtained by the production method of the present invention is characterized in that the cellulose-based material used as the raw material becomes plasticized in general or at least partially during molding, and exhibits a plastic-like appearance that does not retain the original shape of the cellulose-based material. have. Furthermore, although the molded article is mainly composed of cellulose-based material, it has excellent water resistance, that is, dimensional stability against water, and is also excellent in mechanical strength, hardness, and heat distortion temperature.

On the other hand, the present inventors previously added a polybasic acid anhydride and a compound containing two or more epoxy groups in the molecule to a cellulose-based material, thoroughly mixed these, and then heated the mixture under heat pressure. It has been discovered that by molding, a molded article whose main component is a cellulose material can be obtained. In this hot-press molding method, a part of the hydroxyl groups in the cellulose-based material are bonded to the polybasic acid anhydride through a ring-opening esterification reaction, and the epoxy group is attached to the carboxyl group in the side chain. An addition esterification reaction, ■ an esterification reaction in which anhydride groups and epoxy groups are alternately added to the hydroxyl groups generated by this addition esterification reaction, and ■ an alternating esterification reaction of anhydride groups and epoxy groups occur, resulting in cellulose-based materials. and the cured epoxy resin are chemically bonded together. In this case, the cellulose-based molybdenum is directly chemically bonded to the epoxy compound due to the reaction (■), but at the same time, (■)
Because the reactions of
The degree of this bonding depends on the rate of progress of the reactions of ■, ■, and ■. In addition, in this method, some of the added polybasic acid anhydride sublimes into the atmosphere during the manufacturing process of the molded product, especially when kneading in a kneader or when hot-pressing, causing a problem in the working environment. The problem was that it was not sanitary.

On the other hand, the above-mentioned difficulties are solved in the molding method of the present invention. That is, since active carboxyl groups have already been introduced into the cellulose-based material used, the affinity between the cellulose-based material and the epoxy compound is high, and they can be kneaded effectively. Since there is almost no polybasic acid anhydride in it, the problem of working environment hygiene has been solved. Also,
Since the crosslinking reaction proceeds through the addition esterification reaction between the carboxyl group of the esterified cellulose-based material and the epoxy group, most of the epoxy l in the added epoxy compound forms a direct bond between the cellulose material and the epoxy compound. It has the characteristic of being used in reactions. Therefore, the degree to which the cellulose structure is incorporated into the crosslinked structure through chemical bonding is increased.

The carboxyl group-containing esterified cellulose-based material used in the present invention is produced by reacting a cellulose material with a polybasic acid anhydride and esterifying the hydroxyl groups contained in the cellulose tissue. is chemically introduced. The cellulosic materials used here include waste paper, rice straw, wheat straw, rice husk, linter, bagasse, etc., which are discarded in large quantities without being used, but among these, they are particularly cheap and available in large quantities. Waste paper, rice straw, rice husk, etc. are preferable. There is no particular restriction on the shape of these cellulose-based moieties, but it is preferable to use them in the form of as small pieces as possible.

Polybasic acid anhydrides are polycarboxylic acid anhydrides, specifically maleic anhydride, cono-phosphoric anhydride, phthalic anhydride, tetrahydrophthalic anhydride, hexahydrophthalic anhydride, itaconic anhydride. Examples of the acid include hydrophilic anhydride, tetrabromophthalic anhydride, trimellitic anhydride, pyromellitic anhydride, etc., but maleic anhydride, cono-phosphoric anhydride, and phthalic anhydride are particularly preferred because they are industrially advantageous and inexpensive. . The esterification reaction between a cellulose material and a polybasic acid anhydride may proceed satisfactorily even in the absence of a catalyst, or in order to accelerate the reaction, carbonates, oxides, hydroxides, etc. of alkali metals or alkaline earth metals may be used. Carboxylate salts, amine compounds such as dimethylbenzylamine and triethylamine, and other catalysts such as pyridine, dimethylaniline, and zinc chloride may also be used. Further, the esterification reaction may be carried out in a solvent such as dimethylformamide or dimethylsulfoxide, but in this case, it is necessary to separate the esterified cellulose material from the solvent after the reaction. The present inventors first added a polybasic acid anhydride directly to a cellulose-based material in the absence of a solvent and heated it at a reaction temperature of 60°C or higher, so that the esterification reaction by addition proceeded smoothly and the cellulose material It has been found that polybasic acid anhydrides can be easily added to base materials to obtain carboxyl group-containing esterified cellulose materials with various degrees of esterification. After the reaction, the reaction product is washed and dried to obtain the esterified cellulose material used in the present invention. The addition rate of polybasic acid anhydride to the esterified cellulose material is 5 to 100%, preferably 5 to 70%, based on the cellulose material. In addition, if the amount of unreacted polybasic acid anhydride remaining in the system after the addition reaction is small, the reaction product may be used as it is as the esterified cellulose material used in the present invention without washing after the reaction. Good too. In this case, since the residual amount of polybasic acid anhydride is small, the above-mentioned problems in terms of working environment hygiene due to sublimation are largely eliminated.

Examples of compounds having two or more epoxy groups in the molecule used in the present invention include bisphenol A type epoxy compounds obtained from bisphenol A and epichlorohydrin, novolac type epoxy compounds obtained from phenol resin and epichlorohydrin, and halogenated bisphenols. Halogenated epoxy 7 compound obtained from A and epichlorohydrin, polyalkylene ether type epoxy compound obtained from polyalkylene glycol and epichlorohydrin, polybutadiene type epoxy 7 compound obtained by epoxidizing the double bond part of polybutadiene with peracetic acid etc., and other diisocyanates. Examples include epoxy compounds obtained from Grindor, copolymers of vinyl compounds and glycidyl acrylate or methacrylate, and bisphenol A type epoxy compounds, which are industrially produced in large quantities and available at low cost, are particularly preferred.

The amount of these epoxy compounds used is 0 epoxy groups per equivalent of carboxyl group in the esterified cellulose material.
．． The amount is preferably 3 to 1.2 equivalents, preferably 0.6 to 1.0 equivalents.

In the present invention, first, a compound having two or more epoxy groups in the molecule is mixed into the esterified cellulose material prepared as described above. As the epoxy compound, the above-mentioned bisphenol type epoxy compounds are particularly preferred.

As the molecular weight increases, the crosslinking density of the cured resin phase decreases, so it is usually preferable to have an average molecular weight of about 200 to 2,000. In some cases, a monoepoxy compound such as fer glycidyl ether, styrene oxide, epichlorohydrin, etc. may be added as a diluent to lower the viscosity.

In addition, a solvent that does not have reactivity with the epoxy compound,
For example, an appropriate amount of t l'l', benzene, toluene, xylene, etc. may be added to the esterified cellulose material.

However, in this case, it is necessary to sufficiently remove the solvent after mixing. The crosslinking reaction in the molding of the present invention proceeds satisfactorily without a catalyst, but in order to further stop the reaction, catalysts conventionally used in the curing of epoxy resins with polyhydric carboxylic acids and acid anhydrides, such as metals of carboxylic acids. Salts, tertiary amines, etc. may also be added. In order to further improve the mechanical strength of the cellulosic material molded product obtained, a reinforcing agent such as glass fiber is added, and in order to impart flame resistance, a compound containing nitrogen, such as tetrabromobisphenol A1tetrachlorbisphenol A1hexane, is added. Chlorbenzene etc.
Furthermore, dyes, pigments, etc. may be added at the same time as colorants.

The mixture prepared as described above is further kneaded uniformly using a mixing machine such as a blender, kneader, or mixing roll.The esterified cellulose material used in the present invention is as described above. It has an active carboxyl group and has good affinity for epoxy compounds, and when kneaded with the epoxy compound, the esterified cellulose material and the epoxy compound can be mixed extremely effectively.Therefore, esterified cellulose The mixing ratio of the system material and the epoxy compound can be selected at any desired mixing ratio.

Furthermore, the amount of epoxy compound used can be reduced by using a large amount of esterified cellulose material.

The esterification reaction is then carried out by preheating or placing the mixture in a mold and applying pressure necessary to at least partially plasticize it at elevated temperatures. Crosslinking is carried out for a predetermined period of time.If the molding temperature is too low, the reaction rate will be very slow, so it is better to set the molding temperature to 100°C or higher, preferably 120°C or higher.In addition, the cellulose material is at least partially The pressure necessary for plasticizing is generally preferably 60 H/cm2 or more.

As mentioned above, the cellulose material molded product obtained by the production method of the present invention is crosslinked by an addition esterification reaction between the carboxyl group in the esterified cellulose material and the epoxy group in the epoxy compound. That is, the esterified cellulose material is cross-linked via an epoxy compound, and the cellulose material is generally or at least partially plasticized during molding, so the surface of the molded product is smooth. It has a shiny plastic-like appearance and is very hard, and also has excellent dimensional stability against water and mechanical strength.

As described above, the cellulosic material molded product obtained by the manufacturing method of the present invention is mainly composed of cellulose material, which is discarded in large quantities without being used, and can be manufactured at low cost. Furthermore, since it has excellent properties and excellent workability, it is useful as a building material, an industrial component material, and in many other fields.

Next, the present invention will be specifically explained using examples, but the present invention is not limited thereto. Note that the dried waste paper particles, rice hull powder, and rice straw powder shown below are cellulose-based materials that have been dried to a moisture content of 5% or less. Also, mesh is based on JIS standards, and all parts are by weight.

Reference Example 1 100 parts of dried waste paper pieces (raw material: newspaper), 400 parts of maleic anhydride, and 2 parts of sodium carbonate as a catalyst were added to a reaction vessel, and the mixture was reacted at 120° C. for 3 hours with stirring. After the reaction, the reaction product was taken out, washed with acetone using a Soxhlet extractor, and then washed with water. Thereafter, the material was dried in a hot air dryer and used as the carboxyl group-containing esterified cellulose material used in the present invention. The addition rate of maleic anhydride added to the waste paper particles of the esterified waste paper particles was 29.7% by weight based on the waste paper particles. Further, the monoester content added as a monoester was 22.4% by weight based on the waste paper particles.

Example 1 Micro pieces of esterified waste paper obtained according to Reference Example IVc 10
Diglycidyl ether of bisphenol A (EPOMIKR139 manufactured by Mitsui Petrochemical Epoxy Co., Ltd., epoxy equivalent 180 to 190) (hereinafter referred to as bisphenol A)
It is called diglycidyl ether. ) After adding 33.2 parts of the mixture, the mixture was uniformly kneaded using a mixing roll. Next, the mixed wire was uniformly formed in a mold, and then inserted between hot plates of a press machine to perform hot-press molding. Heat and pressure conditions are immediately after inserting the mold, temperature 180℃, rib 5H/c
Heat on rn2 for 10 minutes.

After pressurizing, further increase the temperature to 180℃ and the pressure to 150kf/c.
The mixture was heated and pressurized for 30 minutes according to the conditions of m2. In addition,
During hot pressurization, degassing was performed every 10 minutes. After hot-press molding, the molded product was taken out of the mold, and a cellulose-based material molded product with excellent properties was obtained, having a thickness of 0.5 tone black, a smooth surface, and a glossy plastic-like appearance. Furthermore, it was observed that the waste paper particles on the surface of this molded article were almost plasticized in appearance.

Reference Example 2 A carboxyl group-containing esterified cellulose material was obtained by reacting, washing, and drying in exactly the same manner as in Reference Example 1 except that cono-phosphoric anhydride was used in place of maleic anhydride in Reference Example 1. The addition rate of phosphoric anhydride added to the waste paper particles of the esterified waste paper particles was 61.8% by weight, based on the waste paper particles. Further, the monoester content added as a monoester was 32.5% by weight on the basis of fine pieces of waste paper.

Example 2 100 pieces of esterified waste paper obtained in Reference Example 2
37. parts of diglycidyl ether of bisphenol A.
After adding 8 parts, the mixture was uniformly kneaded using a mixing roll. Next, the mixed wire was uniformly formed into a molding die, and then the mold was inserted between hot plates of a press machine to perform hot-press molding. Heat and pressure conditions are temperature 200℃ and pressure 1001℃.
Heat 4 parts cm2 for 40 minutes.

Pressurized. In addition, degassing was performed every 10 minutes during hot pressure. After hot-press molding, take out the molded product from the mold and reduce the thickness to 0.5
A cellulose-based material molded product with excellent properties was obtained, which was 1 fl+ black in color, had a smooth, shiny surface, and had a plastic-like appearance. Furthermore, it was observed that the waste paper particles on the surface of this molded article were almost plasticized in appearance.

Reference Example 3 100 parts of dried waste paper particles (raw material - newspaper), 22.8 parts of maleic anhydride, 0 sodium carbonate as a catalyst
．． 5 parts were added to the reaction vessel and reacted at 140° C. for 1 hour with stirring. In this reaction system, the addition rate of maleic anhydride to waste paper particles was 22.8M.

After the reaction, the reaction product was taken out and used as the carboxyl group-containing esterified cellulose material used in the present invention without washing. The addition rate of maleic anhydride added to the waste paper particles of the esterified waste paper particles was 10.6% by weight based on the waste paper particles.

Example 3 To 100 parts of the fine pieces of esterified waste paper obtained in Reference Example, 35 parts of diglyfusyl ether of bisphenol A was added, and the mixture was uniformly kneaded with a mixing roll. Thereafter, the kneaded material was dried in a hot air dryer at 80° C. for about 1 hour, and then uniformly formed into a predetermined mold.

Next, this mold was inserted between the hot plates of a press machine and hot-press molding was performed. The heat and pressure conditions were immediately after inserting the mold, heated and pressurized for 10 minutes at a temperature of 150°C and a pressure of 5kfl/cm2, and then further heated and pressurized at a temperature of 180°C and a pressure of 150 kfl/cm2 for 35 minutes.
Heat and pressurize for minutes.

Note that deaeration was performed at the initial stage of hot pressure. After hot-press molding, the molded product was taken out of the mold to obtain a cellulose-based material molded product with a thickness of 6.4+am, a black color, a smooth surface, and a glossy plastic-like appearance.

Reference Example 4 100 parts of dried waste paper pieces (raw material ISl: newspaper), 23.1 parts of succinic anhydride, and 05 parts of sodium carbonate as a catalyst were added to a reaction vessel and reacted at 140°C for 1 hour with stirring. I forced it. In this reaction system, the addition rate of succinic anhydride to waste paper particles was 23.1% by weight. After the reaction, the reaction product was taken out and used as the carboxyl group-containing esterified cellulose material used in the present invention without washing. The addition rate of co-phosphoric anhydride added to the waste paper particles of the esterified waste paper particles was 17.5% by weight based on the waste paper particles.

Example 4 100 small pieces of esterified waste paper obtained according to Reference Example 4
35. parts of diglycidyl ether of bisphenol A.
3 parts were added and kneaded uniformly using a mixing roll. Thereafter, the mixed material was dried in a hot air dryer at 80° C. for about 1 hour, and then uniformly formed into a predetermined mold. Next, this mold was inserted between the hot plates of a press machine and hot-press molded.

The heat and pressure conditions were immediately after inserting the mold, temperature 1so'c, pressure 5H/
After heating and pressurizing at cm2 for 10 minutes, further increase the temperature to 180
The mixture was heated and pressurized for 50 minutes at a pressure of 150 cm/cm2.

Note that deaeration was performed at the initial stage of hot pressure. After hot-press molding, the molded product was removed from the mold to obtain a cellulose-based material molded product with a thickness of 6.4 cm, black color, smooth surface, and a glossy plastic-like appearance.

Reference Example 5 100 parts of dried waste paper pieces (raw material: newspaper), 293 parts of phthalic anhydride, and 05 parts of sodium carbonate as a solvent were added to a reaction vessel and reacted at 170° C. for 3 hours with stirring. In this reaction system, the addition rate of phthalic anhydride to the waste paper particles was 29.3% by weight. After the reaction,
The reaction product was taken out and used as a carboxyl group-containing esterified cellulose-based detergent used in the present invention without washing. The addition rate of phthalic anhydride added to the esterified waste paper particles was 14.8% by weight based on the waste paper particles.

Example 5 Nisderized waste paper micro g-to obtained in Reference Example 4
In part o, diglycidyl ether of bisphenol A 28
．． 8 parts were added and uniformly kneaded using a mixing roll.

Thereafter, the kneaded material was dried in a hot air dryer at 80° C. for about 1 hour, and then uniformly formed into a predetermined mold. Next, this mold was inserted between the hot plates of a press machine and hot-press molding was performed.

Heat and pressure conditions are immediately after inserting the mold, temperature 150℃, pressure 5cm/c.
After heating and pressurizing at RL for 40 minutes, further heat at 180℃ for 1 part.
, heated for 40 minutes under pressure 15 (jkg/cm2),
Pressurized.

Note that deaeration was performed at the initial stage of hot pressure. After hot-press molding, the molded product was taken out of the mold to obtain a 6.4 m thick black cellulose material molded product with a smooth, glossy surface and a plastic-like appearance.

Reference Example 6 A carboxyl group-containing esterified cellulose material was obtained by reacting in exactly the same manner as in Reference Example 3, except that dried rice hull powder C (particle size 42 mesh or more) was used instead of the waste paper micropieces in Reference Example 3. Ta.

The addition rate of maleic anhydride added to the rice hull powder of this esterified rice hull powder was 8.0% by weight based on the rice hull powder.

Example 6 Reference Example 6r instead of the small pieces of esterified waste paper in Example 3
Hot-press molding was carried out in exactly the same manner as in Example 3 except that the esterified rice hull powder obtained by lc was used, and the thickness was 65 mm.
A cellulose-based material molded product having a dark brown color and a smooth, glossy, plastic-like appearance was obtained.

Reference Example 7 Reference Example 3 except that dried rice straw powder (particle size of 42 mesh or more) is used instead of the tiny pieces of waste paper in Reference Example 3.
A carboxyl group-containing esterified cellulose material was obtained by reacting in exactly the same manner as above.

The addition rate of maleic anhydride added to the rice straw powder of this esterified rice straw powder is 13.
It was 3% by weight.

Example 7 Hot-press molding was carried out in exactly the same manner as in Example 3, except that the esterified rice straw powder obtained in Reference Example 7 was used in place of the esterified waste paper fine pieces of Example 3, and the thickness was 6.5 mm. 7m+
A cellulose-based material molded product was obtained, which was brown in color and had a smooth, glossy, plastic-like appearance.

Comparative Example 1 A gray product with a thickness of 6.5 mm was molded under heat in exactly the same manner as in Example 3, except that untreated dried waste paper particles were used in place of the esterified waste paper particles in Example 3. A cellulose-based material molded article was obtained.

When the surface of the plate-shaped cellulose-based material molded products obtained by the manufacturing method of the present invention obtained in Examples 1 to 7 was observed under a microscope, the shape of the cellulose-based material was hardly seen, and the cellulose-based material was present at least partially. plasticized. Therefore, the surface of the cellulose-based material molded product has a smooth and shiny plastic-like appearance. Examples 3-7
Samples were cut from the cellulose-based two-material molded product obtained in Comparative Example 1 and subjected to physical property tests. The results of this physical property test are shown in Table 1. The physical property test method is AST below.
I followed the MV.

Bending test ASTM-D790-66 Compression test ASTM@D695-69 Impact test ASTM D256-56 Load deflection temperature test ASTM-D648-560 Tsukwell hardness test ASTM-D785-65 Table 1 Examples 3 to 70 based on the results It can be seen that the plate-shaped cellulose-based material molded product manufactured by the manufacturing method of the present invention has excellent physical properties. In particular, it is excellent in compressive strength, hardness 1 degree, water absorption resistance, and dimensional stability due to water absorption. Moreover, the waste paper-based materials of Examples 3 to 5 have particularly excellent bending strength.

Patent applicant: Okura Industries Co., Ltd.

Claims (1)

[Claims] Carboxyl group-containing esterified cellulose material, which is obtained by adding a polybasic acid anhydride to the hydroxyl group in the cellulose material.
Esterification is carried out by adding a compound containing two or more epoxy groups in the molecule and sufficiently mixing them, and then applying pressure necessary to at least partially plasticize the mixed substance at a high temperature. A method for producing a cellulose-based material molded article, characterized by carrying out crosslinking by reaction.