WO2023074842A1 - パルプ繊維含有樹脂ペレットの製造方法および成形体の製造方法 - Google Patents

パルプ繊維含有樹脂ペレットの製造方法および成形体の製造方法 Download PDF

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Publication number
WO2023074842A1
WO2023074842A1 PCT/JP2022/040342 JP2022040342W WO2023074842A1 WO 2023074842 A1 WO2023074842 A1 WO 2023074842A1 JP 2022040342 W JP2022040342 W JP 2022040342W WO 2023074842 A1 WO2023074842 A1 WO 2023074842A1
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WIPO (PCT)
Prior art keywords
fiber
pulp
fiber assembly
containing resin
producing
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Ceased
Application number
PCT/JP2022/040342
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English (en)
French (fr)
Japanese (ja)
Inventor
圭一 梶田
靖章 中山
拓也 磯貝
速雄 伏見
実央 山中
利奈 宍戸
みづき 酒井
敬子 奥田
剛之 白尾
彩樹子 山口
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Oji Holdings Corp
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Oji Holdings Corp
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Publication date
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Priority to JP2023556665A priority Critical patent/JPWO2023074842A1/ja
Publication of WO2023074842A1 publication Critical patent/WO2023074842A1/ja
Anticipated expiration legal-status Critical
Ceased legal-status Critical Current

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29B—PREPARATION OR PRETREATMENT OF THE MATERIAL TO BE SHAPED; MAKING GRANULES OR PREFORMS; RECOVERY OF PLASTICS OR OTHER CONSTITUENTS OF WASTE MATERIAL CONTAINING PLASTICS
    • B29B9/00—Making granules
    • B29B9/02—Making granules by dividing preformed material
    • B29B9/04—Making granules by dividing preformed material in the form of plates or sheets
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B5/00—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts
    • B32B5/02—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by structural features of a fibrous or filamentary layer
    • 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
    • B27N3/04—Manufacture of substantially flat articles, e.g. boards, from particles or fibres from fibres
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29B—PREPARATION OR PRETREATMENT OF THE MATERIAL TO BE SHAPED; MAKING GRANULES OR PREFORMS; RECOVERY OF PLASTICS OR OTHER CONSTITUENTS OF WASTE MATERIAL CONTAINING PLASTICS
    • B29B9/00—Making granules
    • B29B9/02—Making granules by dividing preformed material
    • B29B9/06—Making granules by dividing preformed material in the form of filamentary material, e.g. combined with extrusion
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29B—PREPARATION OR PRETREATMENT OF THE MATERIAL TO BE SHAPED; MAKING GRANULES OR PREFORMS; RECOVERY OF PLASTICS OR OTHER CONSTITUENTS OF WASTE MATERIAL CONTAINING PLASTICS
    • B29B9/00—Making granules
    • B29B9/12—Making granules characterised by structure or composition
    • B29B9/14—Making granules characterised by structure or composition fibre-reinforced
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C70/00—Shaping composites, i.e. plastics material comprising reinforcements, fillers or preformed parts, e.g. inserts
    • B29C70/04—Shaping composites, i.e. plastics material comprising reinforcements, fillers or preformed parts, e.g. inserts comprising reinforcements only, e.g. self-reinforcing plastics
    • B29C70/06—Fibrous reinforcements only
    • B—PERFORMING OPERATIONS; TRANSPORTING
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    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B5/00—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts
    • B32B5/22—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed
    • B32B5/24—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed one layer being a fibrous or filamentary layer
    • B32B5/26—Layered products characterised by the non- homogeneity or physical structure, i.e. comprising a fibrous, filamentary, particulate or foam layer; Layered products characterised by having a layer differing constitutionally or physically in different parts characterised by the presence of two or more layers which are next to each other and are fibrous, filamentary, formed of particles or foamed one layer being a fibrous or filamentary layer another layer next to it also being fibrous or filamentary
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    • B32B9/06—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising such particular substance as the main or only constituent of a layer, which is next to another layer of the same or of a different material of paper or cardboard
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    • D04H1/42—Non-woven fabrics formed wholly or mainly of staple fibres or like relatively short fibres from fleeces or layers composed of fibres without existing or potential cohesive properties characterised by the use of certain kinds of fibres insofar as this use has no preponderant influence on the consolidation of the fleece
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    • D04H1/732—Non-woven fabrics formed wholly or mainly of staple fibres or like relatively short fibres characterised by the method of forming fleeces or layers, e.g. reorientation of fibres the fibres being randomly arranged by fluid current, e.g. air-lay
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
    • B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
    • B29C43/00—Compression moulding, i.e. applying external pressure to flow the moulding material; Apparatus therefor
    • B29C43/02—Compression moulding, i.e. applying external pressure to flow the moulding material; Apparatus therefor of articles of definite length, i.e. discrete articles
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    • B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
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    • B32B2307/7375—Linear, e.g. length, distance or width
    • B32B2307/7376—Thickness

Definitions

  • the present invention relates to a method for producing pulp fiber-containing resin pellets, and a method for producing molded articles using the obtained pulp fiber-containing resin pellets.
  • Fiber-reinforced plastic moldings molded from non-woven fabrics (also called sheets for fiber-reinforced plastic moldings) containing reinforcing fibers such as carbon fibers and glass fibers have already been used in various fields such as sports and leisure goods, aircraft materials, and electronic equipment parts. used in the field.
  • Thermosetting resins and thermoplastic resins are used as matrix resins in fiber-reinforced plastic molded articles.
  • fiber-reinforced plastic molded articles using thermoplastic resins have been developed.
  • Carbon fiber, glass fiber, aramid fiber, etc. are used as reinforcing fibers. Such reinforcing fibers serve to increase the strength of the fiber-reinforced plastic molding. When disposing of such molded products, they are disposed of in landfills or incinerated. However, there is a problem that the load applied to the incinerator or the like is large during incineration.
  • Patent Documents 1 to 3 a molded article is obtained by making paper from a slurry containing pulp fibers and a thermoplastic resin, and subjecting the molded paper-making intermediate product to heat-press molding.
  • Patent Document 3 proposes forming pellets from a slurry containing pulp fibers and a thermoplastic resin and injection molding the pellets to produce a molded product.
  • Patent Documents 1 to 3 use pulp fibers as reinforcing fibers, they have good biodegradability and can reduce the environmental load during incineration. However, the dispersibility of the pulp fibers in the resin is not sufficient, and although the rigidity and strength against bending are improved, there is a problem that the impact resistance is not improved.
  • An object of the present invention is to provide a method for producing pulp fiber-containing resin pellets that yields moldings that are excellent in rigidity and strength against bending, as well as in impact resistance.
  • a further object of the present invention is to provide a method for producing a molded article using the pulp fiber-containing resin pellets.
  • the present inventors have developed pulp fiber-containing pellets having a step of producing a fiber aggregate containing pulp fibers and resin A by dry papermaking, and a step of compressing the fiber aggregate to produce a fiber aggregate sheet.
  • the inventors have found that the molded article obtained from the pulp fiber-containing pellets obtained by the production method has excellent bending rigidity and strength, and further has improved impact resistance, leading to the completion of the present invention.
  • ⁇ 1> A method for producing pulp fiber-containing resin pellets comprising the following steps 1, 2, and 3-1 in this order, or comprising steps 1, 2, and 3-2 in this order: .
  • Step 1 A fiber assembly manufacturing step of manufacturing a fiber assembly containing pulp fibers and resin A by dry papermaking.
  • Process 2 A fiber assembly sheet manufacturing step of compressing the fiber assembly to manufacture a fiber assembly sheet.
  • Step 3-1 Pulp fiber-containing resin pellet production step of melt-kneading the fiber assembly sheet to produce pellets
  • Step 3-2 Pulp fiber-containing resin pellet production step of cutting the fiber assembly sheet
  • T The method for producing pulp fiber-containing resin pellets according to ⁇ 1>, wherein the resin A contains resin fibers.
  • ⁇ 3> The method for producing a pulp fiber-containing resin pellet according to ⁇ 1> or ⁇ 2>, wherein the pulp fiber content in the pulp fiber-containing resin pellet is 10% by mass or more and 90% by mass or less.
  • T is the tensile strength of the fiber assembly sheet in the first direction
  • Y is the tensile strength in the second direction perpendicular to the first direction
  • T/Y is 0.5 or more.
  • ⁇ 5> The method for producing pulp fiber-containing resin pellets according to any one of ⁇ 1> to ⁇ 4>, wherein in step 3-1, an elastomer is further blended and melt-kneaded.
  • ⁇ 6> Any one of ⁇ 1> to ⁇ 5>, wherein in step 2, the bulk specific gravity of the fiber assembly sheet subjected to step 3-1 is 0.10 g/mL or more and 0.60 g/mL or less.
  • ⁇ 7> Any one of ⁇ 1> to ⁇ 4>, wherein in step 2, the bulk specific gravity of the fiber assembly sheet subjected to step 3-2 is 0.3 g/mL or more and 1.5 g/mL or less.
  • a method for producing a molded product comprising: producing pulp fiber-containing resin pellets by the method according to any one of ⁇ 1> to ⁇ 7>; and molding the pulp fiber-containing resin pellets.
  • the molding step is a step of injection molding a pulp fiber-containing resin pellet.
  • ⁇ 10> The method for producing a molded article according to ⁇ 8> or ⁇ 9>, wherein the obtained molded article has a density of 0.8 g/cm 3 or more and 1.5 g/cm 3 or less.
  • ⁇ 11> The method for producing a molded article according to any one of ⁇ 8> to ⁇ 10>, wherein the obtained molded article has a thickness of 2 mm or more.
  • ⁇ 12> The method for producing a molded article according to any one of ⁇ 8> to ⁇ 11>, wherein the obtained molded article has a flexural modulus of 1.5 GPa or more measured according to JIS K 7171:2016. .
  • ⁇ 13> The method for producing the molded article according to any one of ⁇ 8> to ⁇ 12>, wherein the Charpy impact strength measured according to JIS K 7111-1:2012 is 2.0 kJ/m 2 or more. .
  • a method for producing pulp fiber-containing resin pellets that yields moldings that are excellent in rigidity and strength against bending, as well as excellent impact resistance. Furthermore, according to the present invention, there is provided a method for producing a molded article using the pulp fiber-containing resin pellets.
  • FIG. 1 is a schematic diagram showing a web forming apparatus used in a manufacturing method for manufacturing a fiber assembly for molding according to this embodiment.
  • the method for producing pulp fiber-containing resin pellets includes the following steps 1, 2, and 3-1 in this order, or step 1, step 2 , and step 3-2 in this order.
  • Step 1 A fiber assembly manufacturing step of manufacturing a fiber assembly containing pulp fibers and resin A by dry papermaking.
  • Process 2 A fiber assembly sheet manufacturing step of compressing the fiber assembly to manufacture a fiber assembly sheet.
  • Step 3-1 Pulp fiber-containing resin pellet production step of melt-kneading the fiber assembly sheet to produce pellets
  • Step 3-2 Pulp fiber-containing resin pellet production step of cutting the fiber assembly sheet
  • step 1 by producing a fiber assembly containing pulp fibers and resin A by dry papermaking, the pulp fibers and resin A are uniformly dispersed, and a highly isotropic fiber assembly is obtained. Further, in step 2, the fiber assembly sheet obtained in step 1 is compressed to produce a fiber assembly sheet, and the fiber assembly sheet in which uniform dispersion and isotropy in the fiber assembly are maintained. is obtained. When the obtained fiber assembly sheet is melt-kneaded to produce pellets as in step 3-1, pulp fibers and resin A are uniformly dispersed in the fiber assembly sheet in advance.
  • pellets with excellent dispersibility of pulp fibers can be obtained.
  • the dispersed state of the pulp fibers in the fiber assembly sheet is maintained as it is, and the pellets with excellent dispersibility of the pulp fibers are obtained. can get.
  • pellets having excellent dispersibility of pulp fibers can be obtained, and the molded article produced from the pellets can be bent. It is considered to have excellent rigidity and strength against and also excellent impact resistance.
  • Step 1 is a fiber assembly production step for producing a fiber assembly containing pulp fibers and resin A by dry papermaking.
  • the pulp fiber applicable to the method for producing pulp fiber-containing resin pellets of the present embodiment is not particularly limited in its production method, type, and the like.
  • chemical pulps such as hardwood and/or softwood kraft pulps, mechanical pulps such as SGP, RGP, BCTMP and CTMP, waste paper pulps such as deinked pulps, and kenaf, jute, bagasse, bamboo, straw, hemp, etc. of non-wood pulp.
  • Chlorine-free pulp such as ECF pulp and TCF pulp can also be used.
  • kraft pulp fibers especially softwood kraft pulp fibers (NBKP) having a long fiber length, are preferably used because the obtained moldings are superior in rigidity and strength against bending and impact resistance.
  • NNKP softwood kraft pulp fibers
  • the average fiber length of the pulp fibers is preferably 0.1 mm or more, more preferably 0, from the viewpoint of improving the rigidity and strength against bending of the resulting molded product and impact resistance, and from the viewpoint of easiness in manufacturing the fiber aggregate.
  • the average fiber length of pulp fibers is measured by the method described in Examples.
  • the average fiber width of the pulp fibers is preferably 1 ⁇ m or more, more preferably 5 ⁇ m or more, from the viewpoint of improving the rigidity and strength against bending of the resulting molded article and the impact resistance, and from the viewpoint of the ease of manufacturing the fiber aggregate. It is more preferably 10 ⁇ m or more, still more preferably 15 ⁇ m or more, and preferably 150 ⁇ m or less, more preferably 100 ⁇ m or less, even more preferably 80 ⁇ m or less, and even more preferably 50 ⁇ m or less.
  • the average fiber width of pulp fibers is measured by the method described in Examples.
  • the pulp fibers can be in the form of defibrated dry pulp, for example.
  • the pulp fibers are preferably unbeaten pulp fibers from the viewpoint of improving the impact resistance of the resulting molded article. In order for the molded article to exhibit impact resistance, it is necessary that the pulp fibers are appropriately pulled out from the resin when an impact is applied. .
  • the fine fiber ratio of the pulp fibers is preferably 50% or less, more preferably 30% or less, and still more preferably 20% or less from the above-mentioned viewpoint, and the lower limit is not particularly limited. The fine fiber ratio of pulp fibers is measured by the method described in Examples.
  • the content of pulp fibers in the fiber assembly and the fiber assembly sheet is preferably 10% by mass or more from the viewpoint of obtaining a molded article having excellent bending rigidity and strength and impact resistance, and is easy to manufacture. More preferably 15% by mass or more, still more preferably 20% by mass or more, and even more preferably 25% by mass or more from the viewpoint of biomass conversion, and even more preferably 50% by mass or more, particularly preferably 50% by mass or more. is 55% by mass or more. From the viewpoint of obtaining a molded article, the content is preferably 90% by mass or less, more preferably 85% by mass or less, and even more preferably 75% by mass or less.
  • the content of the pulp fiber in the pulp fiber-containing resin pellet is preferably 10% by mass or more from the viewpoint of obtaining a molded article having excellent rigidity and strength against bending and impact resistance, and from the viewpoint of productivity and ease of manufacture. Therefore, it is more preferably 15% by mass or more, still more preferably 20% by mass or more, and from the viewpoint of the degree of biomass conversion, it is even more preferably 50% by mass or more, and particularly preferably 55% by mass or more. From the viewpoint of obtaining a molded article, the content is preferably 90% by mass or less, more preferably 85% by mass or less, and even more preferably 75% by mass or less.
  • resin A components include polyolefin, polyvinyl chloride, polystyrene, ABS, acrylonitrile-styrene, polyester, acrylic resin, polyamide, polyacetal, polycarbonate, polybutylene succinate and polylactic acid.
  • the exemplified resins may be used.
  • any of fibers, powders, granules and pellets can be used.
  • the resin A is preferably a fiber or powder, more preferably a fiber, from the viewpoint of papermaking easiness in step 1. That is, the resin A preferably contains resin fibers or resin powder, more preferably resin fibers, and even more preferably resin fibers.
  • fibers of resin A include polyolefin fibers, polyvinyl chloride fibers, polyester fibers, acrylic fibers, polyamide fibers, polycarbonate fibers and polylactic acid fibers.
  • Components of Resin A powders, granules, and pellets include polyolefins, polyvinyl chloride, polyesters, acrylics, polyamides, polycarbonates, polylactic acid, polystyrene, ABS (acrylonitrile-butadiene-styrene), acrylonitrile-styrene, polyacetal, and polybutylene.
  • a preferred example is succinate.
  • the resin A powder is preferably exemplified by polystyrene powder, ABS powder, acrylonitrile-styrene powder, polyacetal powder and polybutylene succinate powder.
  • the polyolefin include the same specific examples of polyolefin in the polyolefin fiber shown below.
  • resin A polyolefin fibers are preferable.
  • resin A can be used 1 type or in combination of 2 or more types.
  • the resin A two kinds of polylactic acid fiber and polybutylene succinate powder may be used in combination.
  • the polyolefin constituting the polyolefin fiber is not particularly limited, and polyolefin (unmodified polyolefin) and modified polyolefin are exemplified.
  • the melting point of the polyolefin constituting the polyolefin fiber is preferably 200° C. or less, more preferably 195° C. or less, still more preferably 180° C. or less, from the viewpoint of ease of molding and suppression of deterioration of the pulp fiber, and It is preferably 80° C. or higher, more preferably 90° C. or higher, and still more preferably 100° C. or higher.
  • polyolefins examples include polyethylene, polypropylene, and ethylene-propylene copolymers (also referred to as propylene-ethylene copolymers), with polyethylene and polypropylene being preferred.
  • methods for modifying the polyolefin include acid modification, chlorination, and the like, and among these, acid modification is preferred from the viewpoint of improving affinity with pulp fibers.
  • the acid-modifying component used for acid-modifying the acid-modified polyolefin is preferably an unsaturated carboxylic acid component.
  • the unsaturated carboxylic acid component is a component derived from an unsaturated carboxylic acid and its acid anhydride.
  • unsaturated carboxylic acids include acrylic acid, methacrylic acid, maleic acid, maleic anhydride, itaconic acid, itaconic anhydride, fumaric acid and crotonic acid.
  • the unsaturated carboxylic acid component is preferably at least one selected from acrylic acid, methacrylic acid, maleic acid and maleic anhydride, and at least one selected from maleic acid and maleic anhydride. is particularly preferred.
  • Polyolefins modified with at least one of maleic acid and maleic anhydride are also referred to as maleic acid-modified polyolefins.
  • maleic acid-modified polyolefin is preferable, and maleic acid-modified polyethylene and maleic acid-modified polypropylene are more preferable. At least a part of the acid-modified polyolefin should be acid-modified.
  • Polyolefins include polyethylene, polypropylene, at least partially maleic acid-modified polyethylene and at least partially maleic acid-modified polypropylene, At least one selected from the group consisting of ethylene-propylene copolymers is particularly preferred. From the viewpoint of improving the rigidity and strength against bending of the molded article obtained, it is preferable to contain an acid-modified polyolefin as the polyolefin. It is more preferable to contain at least one polypropylene modified with maleic acid, and it is further preferable to contain at least a portion of polyethylene modified with maleic acid.
  • polyolefin fibers may be used singly or in combination of two or more.
  • the polyolefin fiber may be a composite fiber composed of two or more polyolefins, and examples thereof include split fibers, sea-island fibers, core-sheath fibers, and laminated fibers.
  • a core-sheath fiber is preferable from the viewpoint of obtaining a molded article having excellent properties.
  • a fiber having a concentric cross-sectional structure or an eccentric cross-sectional structure is used, but a fiber having a concentric cross-sectional structure is preferable. It is preferable to use fibers having a concentric cross-sectional structure because a more uniform fiber aggregate can be obtained.
  • the fiber length of the polyolefin fibers is preferably 0.1 mm or more, more preferably 1.0 mm or more, and still more preferably 2.0 mm or more, from the viewpoint of obtaining a uniform fiber assembly and from the viewpoint of ease of manufacturing the fiber assembly. It is more preferably 3.0 mm or more, and preferably 50 mm or less, more preferably 20 mm or less, still more preferably 10 mm or less.
  • the fiber length of polyolefin fibers is measured by the method described in Examples.
  • the fiber diameter of the polyolefin fibers is preferably 0.1 ⁇ m or more, more preferably 1 ⁇ m or more, and still more preferably 10 ⁇ m or more, from the viewpoint of obtaining a uniform fiber assembly and from the viewpoint of ease of manufacturing the fiber assembly, and It is preferably 100 ⁇ m or less, more preferably 80 ⁇ m or less, and even more preferably 50 ⁇ m or less.
  • the fiber diameter of polyolefin fibers is measured by the method described in Examples.
  • the fineness of the polyolefin fibers is preferably 0.01 dtex or more, more preferably 0.1 dtex or more, still more preferably 1 dtex or more, from the viewpoint of obtaining a uniform fiber assembly and facilitating the production of the fiber assembly, and , preferably 100 dtex or less, more preferably 50 dtex or less, still more preferably 10 dtex or less.
  • the content of the polyolefin fiber in the fiber assembly is preferably 90% by mass or less from the viewpoint of obtaining a molded article having excellent bending rigidity and strength and impact resistance. From the viewpoints of easiness of production and productivity, it is more preferably 70% by mass or less, more preferably 55% by mass or less, and from the viewpoint of the degree of biomass conversion, even more preferably 50% by mass or less, particularly preferably 45% by mass or less. is. From the viewpoint of obtaining a molded article, the content is preferably 10% by mass or more, more preferably 15% by mass or more, and even more preferably 25% by mass or more. In addition, when using two or more types of polyolefin fibers, the above content means the total content of the polyolefin fibers.
  • the preferred fiber length, fiber diameter, fineness and content of the said fiber are the same as the preferred fiber length, fiber diameter, fineness and content of the polyolefin fiber.
  • the preferred content of the powder, granules, or pellets is the same as the preferred content of the polyolefin fibers.
  • the particle size of the powder, granules, or pellets is not particularly limited.
  • the fiber assembly may contain other components in addition to the pulp fibers and polyolefin fibers described above.
  • Other components include elastomers and binder components, which will be described later.
  • the content of the binder component is preferably 0.1% by mass or more and 45% by mass or less, more preferably 0.3% by mass or more and 30% by mass or less, relative to the total mass of the fiber assembly. It is more preferably 0.4% by mass or more and 20% by mass or less, and even more preferably 0.5% by mass or more and 10% by mass or less.
  • Binder components include various starches, casein, sodium alginate, hydroxyethyl cellulose, carboxymethyl cellulose, acrylic resins, styrene-(meth)acrylic acid ester copolymer resins, urethane resins, polyvinyl alcohol (PVA) resins, various starches, and cellulose derivatives.
  • the fiber assembly may further contain fillers and papermaking chemicals.
  • fillers include kaolin, calcined kaolin, calcium carbonate, calcium sulfate, barium sulfate, titanium dioxide, talc, zinc oxide, alumina, magnesium carbonate, magnesium oxide, silica, white carbon, bentonite, zeolite, sericite and smectite.
  • mineral pigments and organic pigments such as polystyrene-based resins, urea-based resins, melamine-based resins, acrylic-based resins and vinylidene chloride-based resins.
  • Paper manufacturing chemicals include paper strength agents, retention aids, drainage improvers, dyes, fluorescent whitening agents, pH adjusters, antifoaming agents, pitch control agents, slime control agents, and the like.
  • Paper strength agents include polyacrylamide and the like.
  • a wet strength agent can also be used in combination, and examples thereof include polyamide resins, melamine-formaldehyde resins, urea-formaldehyde resins, polyamide-polyamine-epichlorohydrin resins and polyethyleneimine resins.
  • the content of the other components excluding pulp fibers and polyolefin fibers is preferably 0.1% by mass or more and 45% by mass or less, more preferably 0.1% by mass or more and 45% by mass or less, based on the total mass of the fiber assembly. 3% by mass or more and 30% by mass or less, more preferably 0.4% by mass or more and 20% by mass or less, and even more preferably 0.5% by mass or more and 10% by mass or less.
  • pulp fibers and resin A are manufactured by dry papermaking.
  • the manufacturing process of the fiber assembly preferably includes a process of mixing pulp fibers and polyolefin fibers in the air and depositing them. That is, the fiber assembly of this embodiment is preferably a dry nonwoven fabric.
  • an air-laid web is produced by blowing an air stream containing raw materials such as polyolefin fibers and pulp fibers uniformly mixed in an air stream onto a mesh-like endless belt equipped with a suction box on the lower side.
  • the airlaid method is a method including a step of mixing pulp fibers and polyolefin fibers in the air and depositing them.
  • the above operation may be repeated multiple times as necessary.
  • the web formed by the above method is made into a sheet by the fiber bonding process shown below.
  • the fiber bonding step for example, there is a method such as a needle punch method in which a needle is passed through the web surface in a vertical direction to entangle polyolefin fibers or pulp fibers with each other to form a sheet.
  • a bonding step is preferably used in combination with a web forming method by a carding method.
  • the heat-sealing adhesive blended in the dry method web is fused by heating to bond the raw material fibers (thermal bonding method), and the adhesive is applied to the obtained dry method web.
  • a process (chemical bond method) in which the raw material fibers are bonded together using a thermal bond method or a method in which the thermal bond method and the chemical bond method are combined (multi-bond method) can be employed.
  • the thermal bonding method it is preferable to heat at a temperature 20°C or more higher than the melting point of the heat-fusible adhesive.
  • the heat treatment include hot air treatment and heat pressure treatment at low pressure after hot air treatment.
  • the heat-sealable adhesive may be the polyolefin fiber or binder component described above.
  • heat-fusible resin particles such as polyethylene, polypropylene, polyester low-melting-point polyethylene terephthalate, low-melting-point polyamide, low-melting-point polylactic acid, and polybutylene succinate are used.
  • Fibrous heat-fusible adhesives include polyesters such as low-melting polyethylene terephthalate, low-melting polylactic acid, polybutylene succinate (PBS), and polyethylene terephthalate (PET), low-melting polyamides, acrylic resins, vinyl acetate ( PVAc) resins are used.
  • polyesters such as low-melting polyethylene terephthalate, low-melting polylactic acid, polybutylene succinate (PBS), and polyethylene terephthalate (PET), low-melting polyamides, acrylic resins, vinyl acetate ( PVAc) resins are used.
  • PBS polybutylene succinate
  • PET polyethylene terephthalate
  • PVAc vinyl acetate
  • the heat-fusible synthetic fiber a heat-fusible composite synthetic fiber having a core-sheath structure obtained by combining two kinds of resins having different melting points and melting only on the surface of the fiber is also preferably used. can.
  • a heat-fusible conjugate synthetic fiber having a core-sheath structure has a structure in which a sheath made of a resin with a low melting point is formed on the outer periphery of a core made of a resin with a high melting point.
  • a sheath made of a resin with a low melting point is formed on the outer periphery of a core made of a resin with a high melting point.
  • two resins having different melting points are combined (PET/PET composite fiber, PE/PET composite fiber, PP/PET composite fiber, PE/PP composite fiber, PVAc/PET composite resin).
  • a binder component to fix the fibers together.
  • the binder component can be appropriately selected as necessary.
  • solution-type binders such as starch, casein, sodium alginate, hydroxyethyl cellulose, carboxymethyl cellulose sodium salt, polyvinyl alcohol (PVA), and sodium polyacrylate, Polyacrylic acid ester, acrylic styrene copolymer, polyvinyl acetate, ethylene vinyl acetate copolymer, acrylonitrile butadiene copolymer, methyl methacrylate butadiene copolymer, urea-melamine resin, styrene-butadiene copolymer resin, etc.
  • an emulsion type binder etc.
  • various forms such as fibers, powder, granules, solutions, emulsions, etc. can be used, and two or more types can be used in combination.
  • each fiber constituting the fiber assembly is randomly oriented three-dimensionally in the longitudinal direction, width direction and thickness direction. Therefore, in the present embodiment, the tensile strength in the first direction and the tensile strength in the second direction of the fiber assembly have approximately the same values. That is, in the present embodiment, a fiber aggregate having excellent isotropy in the planar direction can be obtained.
  • a laminated sheet may be manufactured by laminating an arbitrary sheet that does not impede moldability on the fiber assembly.
  • arbitrary sheets can be laminated on the surface of the fiber assembly or between sheets when the fiber assembly is laminated.
  • Sheets such as tissues and nonwoven fabrics can be used as arbitrary sheets to be laminated. These optional sheets are laminated for the purpose of improving surface properties, improving interlaminar strength, and imparting other functions.
  • Step 2 is a fiber assembly sheet manufacturing step of compressing the fiber assembly obtained in step 1 to manufacture a fiber assembly sheet.
  • a sheet-like fiber assembly (fiber assembly sheet) is obtained.
  • the above compression may be performed at the same time as the heat treatment, or may be performed after the heat treatment.
  • Compression of the fiber aggregate can be obtained by pressurizing the fiber aggregate with a roll press.
  • heating may be performed at the same time as a heating and pressurizing treatment.
  • the density of the obtained fiber assembly sheet can be arbitrarily controlled by applying pressure with a metal roll or a resin roll in the roll press treatment.
  • a fiber assembly sheet having an arbitrary density can be obtained by setting an arbitrary number of rolls for roll-pressing at an arbitrary temperature and clearance, and heating and pressurizing the sheet. It may be passed through multiple rolls and compressed to the desired density.
  • Compression of the fiber assembly can also be obtained by pressure treatment using a hot press.
  • the density of the fiber assembly sheet obtained by pressurizing the fiber assembly sheet cut out to an appropriate size or the fiber assembly sheet subjected to the roll press treatment by an autoclave method or a mold press method can be set arbitrarily. can be controlled to By heating to a temperature of 100° C. or higher and applying a pressure of 2 MPa or higher, a fiber assembly sheet having a higher density than the pressure treatment by a roll press can be obtained.
  • a preliminary pressing step may be performed, and after preliminary pressing is performed at a lower pressure under the desired heating conditions, the pressure is increased, and hot pressing is performed. It is also preferable to perform a pressure treatment with.
  • the pressure treatment process by hot press may be a stamping molding method.
  • the stamping molding method is a method in which a fiber assembly is heated in advance, the polyolefin is melted and softened, placed inside a mold, the mold is closed and clamped, and then pressure is cooled.
  • a heating device such as a far-infrared heater, a heating plate, a high-temperature oven, or a dielectric heating can be used for heating.
  • the pressure treatment step by hot press may be a vacuum forming method.
  • the vacuum forming method by creating a vacuum between the fiber assembly and the mold, it is possible to improve the adhesion between the fiber assembly and the mold and improve moldability.
  • Vacuum forming is preferably performed in the mold clamping step of the stamping molding method described above. Specifically, the fiber assembly is heated, the polyolefin is melted and softened, placed inside a mold, and then the mold is closed and clamped, and vacuum forming is performed. In vacuum forming, vacuum suction is performed from the mold side.
  • the forming pressure in the vacuum forming is usually 1.0 kg/cm 2 or less, and the forming is performed for about 0.1 seconds or more and 60 seconds or less.
  • the pressure treatment step by hot pressing may be a pressure molding method.
  • compressed air is blown onto the fiber assembly to bring it into close contact with the mold, thereby enhancing the adhesion between the fiber assembly and the mold.
  • Pneumatic molding is preferably performed in the clamping step of the stamping molding method described above. Specifically, the fiber assembly is heated, the polyolefin is melted and softened, placed in a mold, and then compressed air is blown from the fiber assembly side to perform molding. Compression molding is often performed with compressed air pressure of 3 kg/cm 2 or more and 8 kg/cm 2 or less, and it is preferable to perform molding for 0.1 seconds or more and 60 seconds or more.
  • Compression of the fiber assembly can also be obtained by supercalendering.
  • the fiber assembly is formed by passing it between heated rollers while applying a nip pressure.
  • the heating temperature of the roller used is preferably 10° C. or higher, more preferably 20° C. or higher, and still more preferably 30° C. or higher than the melting point of the polyolefin fiber.
  • the temperature is preferably 100° C. or lower, more preferably 90° C. or lower, and even more preferably 80° C. or lower than the melting point.
  • the nip pressure is preferably 100 kg/cm or more, more preferably 150 kg/cm or more, still more preferably 200 kg/cm or more, and is preferably 450 kg/cm or less, more preferably 400 kg/cm or less, still more preferably 350 kg/cm or less.
  • the number of nip stages is preferably 1 or more, more preferably 3 or more, still more preferably 5 or more, and preferably 20 or less, more preferably 18 or less, still more preferably 16 or less.
  • T/Y is It is preferably 0.5 or more and 1.5 or less.
  • T/Y is preferably 0.60 or more, more preferably 0.70 or more, still more preferably 0.80 or more, still more preferably 0.85 or more, and preferably 1.45 or less, more preferably is 1.40 or less, more preferably 1.35 or less.
  • the first direction of the fiber assembly sheet is any one direction in the planar direction of the fiber assembly sheet. However, when the fibers contained in the fiber assembly sheet are oriented in one of the planar directions, the oriented direction is defined as the first direction. Further, when the flow direction in the dry papermaking process of the fiber assembly is known, the flow direction is defined as the first direction. When the flow direction in the manufacturing process of the fiber assembly is known, the flow direction in the manufacturing process is referred to as the first direction (MD direction), and the flow direction in the obtained fiber assembly and fiber assembly sheet is referred to as the T-th direction. Sometimes.
  • the second direction of the fiber assembly is one direction in the planar direction of the fiber assembly and is a direction orthogonal to the first direction.
  • the direction perpendicular to the flow direction in the manufacturing process is called the second direction (CD direction), and the obtained fiber assembly and the fiber assembly sheet are the second direction.
  • the direction of is sometimes referred to as the Y-th direction.
  • the tensile strength of the fiber assembly sheet in the first direction and the second direction is measured according to JIS P 8113:2006.
  • the tensile strength in each direction is a value obtained by measuring a strip of 15 ⁇ 0.1 mm ⁇ 180 ⁇ 1 mm at a speed of 20 ⁇ 5 mm / min using a Tensilon manufactured by A&D Co., Ltd. as a tensile tester. be.
  • the fiber assembly sheet of the present embodiment is obtained by mixing at least pulp fibers and resin A (preferably polyolefin fibers), followed by dry papermaking, and is in the form of a sheet. It is a sheet obtained by pressing a cotton-like fiber aggregate after dry papermaking (hereinafter also referred to as a cotton-like fiber aggregate), and may have various bulk specific gravities (densities).
  • the bulk specific gravity of the fiber assembly to be subjected to step 3-1 is the easiness of compression in step 2, the easiness of melt-kneading in step 3-1, the easiness of cutting when cutting to supply to the melt-kneader, etc.
  • the bulk specific gravity of the fiber assembly sheet to be subjected to step 3-2 is preferably 0.3 g/mL or more, more preferably 0.4 g/mL or more, from the viewpoint of using the pulp fiber-containing resin pellets for subsequent molding. More preferably 0.5 g/mL or more, and from the viewpoint of ease of production and cutting, preferably 1.5 g/mL or less, more preferably 1.4 g/mL or less, and still more preferably 1.3 g /mL or less.
  • the bulk specific gravity of the fiber assembly sheet is measured by the method described in Examples.
  • Step 3-1 is a step of producing pulp fiber-containing resin pellets by melt-kneading the fiber assembly sheet obtained in step 2 to produce pellets. From the viewpoint of facilitating the supply to the melt-kneader, it is preferable that the fiber aggregate sheet is cut, crushed, or the like before being introduced into the melt-kneader before melt-kneading.
  • the cutting machine is not particularly limited, and examples thereof include shredders.
  • the size after cutting, crushing, etc. is not particularly limited as long as it can be supplied to the melt-kneader.
  • the method for producing pellets is not particularly limited, and may be provided by supplying a fiber assembly sheet and melt-kneading, and is not particularly limited.
  • devices used for melt-kneading include a single-screw extruder, a twin-screw extruder, a kneader, a Banbury mixer, a mixing roll mill, an open roll mill, and a goulash mixer.
  • a method of extruding into a strand and cooling and solidifying to obtain pulp fiber-containing resin pellets (2) A method of obtaining pulp fiber-containing resin pellets by cooling and solidifying the melt-kneaded product as it is or after stretching it into a sheet, and crushing it with a crusher; (3) A method of extruding into a rod or cylinder and cooling to obtain pulp fiber-containing resin pellets; (4) A method of extruding from a T-die to obtain a sheet-like or film-like pulp fiber-containing resin, followed by cutting or crushing to obtain pulp fiber-containing resin pellets; , a method of obtaining pulp fiber-containing resin pellets by cutting with a rotary blade in air or water, etc. are exemplified.
  • the size of the pellets obtained in step 3-1 is not particularly limited, it is preferably 1 to 10 mm from the viewpoint of ease of injection into an injection molding machine.
  • the melt-kneading temperature is not particularly limited, but the barrel is adjusted so that the temperature of the melt-kneaded product (the temperature of the actually obtained kneaded product, the resin temperature) is at least 5°C higher than the melting point of the polyolefin. It is preferable to adjust the set temperature, more preferably a temperature higher than 10 ° C., more preferably a temperature higher than 15 ° C., and from the viewpoint of deterioration of pulp fibers, relative to the melting point of polyolefin
  • the temperature is preferably 100° C. or more, more preferably 90° C. or less, and even more preferably 80° C. or less.
  • the temperature of the melt-kneaded product becomes higher than the melt-kneading temperature (barrel set temperature) due to shear heat generated during melt-kneading. That is, it varies depending on various conditions during melt-kneading, such as melt-kneading temperature (barrel set temperature), discharge speed, number of revolutions, and screw design of the melt-kneader.
  • the temperature of the melt-kneaded material is about 20 to 40° C. higher than the melt-kneading temperature (barrel setting temperature), so the melt-kneading temperature (barrel setting temperature) is higher than the preferred temperature of the melt-kneading material. ) is about 20 to 40°C lower.
  • melt-kneading Various conditions at the time of melt-kneading, such as discharge speed and number of revolutions, may be adjusted according to known techniques.
  • the screw design is set so that the kneading force is as weak as possible.
  • the pulp fibers and the resin A are uniformly dispersed in the fiber assembly sheet in advance, and even if melt-kneading is performed without applying a high shearing force, the dispersed state of the pulp fibers in the fiber assembly sheet remains as it is. This is because pellets with excellent pulp fiber dispersibility can be obtained.
  • R type kneading parts are mainly used for kneading parts, and the number of L type and N type kneading parts is preferably equal to or less than the number of R type kneading parts, It is more preferable that the number of kneading parts is less than the number of R-type kneading parts.
  • the R-type kneading parts may be used without using the L-type or N-type kneading parts.
  • the number of kneading parts is preferably 5 or less, more preferably 3 or less, out of 10 parts of the whole screw.
  • the melt-kneading is performed using only the cut chips of the fiber assembly sheet, only one kneading part may be used.
  • a resin component may be further blended and melt-kneaded together with the fiber assembly sheet. Resins and elastomers described below are preferred.
  • step 3-1 blending at least one selected from the resin A and the elastomer is preferable because a molded article having more excellent impact resistance can be obtained. That is, the obtained pulp fiber-containing resin pellets contain the components blended in step 3-1 in addition to the components derived from the fiber assembly sheet.
  • the elastomer that may be blended in step 3-1 refers to a polymer compound that exhibits elastic deformation, and is a substance that softens and exhibits fluidity when heated and returns to a rubbery state when cooled. Point.
  • an elastomer has a structure composed of two polymers, a hard segment and a soft segment. Therefore, at room temperature, the hard segments aggregate to form a quasi-crosslinked state and exhibit rubber-like physical properties. Depending on the combination of hard segment polymer and soft segment polymer, it is classified into polystyrene, olefin/alkene, polyester, polyvinyl chloride, polyurethane, polyamide, polyacrylic elastomer, silicone, polyimide, etc. be. Moreover, even within the same system, the properties differ depending on the ratio of the hard segment to the soft segment and the molecular weight.
  • polystyrene there is one that uses styrene for the hard segment and butadiene for the soft segment.
  • the amount of styrene is large, the hardness will be high, and the compatibility with polystyrene and polyphenylene ether will be improved.
  • the molecular weight is high, the temperature characteristics and mechanical properties are improved, and when the molecular weight is low, the workability and transparency are improved.
  • the Tuftec series manufactured by Asahi Kasei Corporation is exemplified.
  • olefin/alkene elastomers examples include TAFMER series manufactured by Mitsui Chemicals, Inc. Among these, polystyrene-based elastomers and olefin/alkene-based elastomers are preferred from the viewpoint of impact resistance and the like.
  • elastomers include various elastomers described in paragraphs 0043 to 0065 of Retable 2020/080328.
  • the method of adding the elastomer is not particularly limited, and it is preferable to supply and melt-knead the elastomer together with the fiber assembly sheet when the fiber assembly sheet is melt-kneaded.
  • the content of the elastomer is preferably 55% by mass or less, more preferably 55% by mass or less, based on the total mass of resin A and the elastomer, from the viewpoint of excellent bending rigidity and strength. is 50% by mass or less, more preferably 45% by mass or less, more preferably 40% by mass or less, and even more preferably 35% by mass or less.
  • the content of the elastomer is preferably 5% by mass or more, more preferably 8% by mass or more, based on the total mass of resin A and the elastomer, from the viewpoint of improving impact resistance. , more preferably 10% by mass or more, still more preferably 12% by mass or more, and particularly preferably 15% by mass or more.
  • Step 3-2 is a step of producing pulp fiber-containing resin pellets by cutting the fiber assembly sheet obtained in step 2.
  • cutting machines used in step 3-2 include rotary cutters, crushers, grinders, electric saws, chain saws, and laser cutters.
  • the thickness of the pellet after cutting is preferably 1 mm or more and 10 mm or less, and the length and width are preferably 1 mm or more and 10 mm or less.
  • the thickness of the pellet after cutting is the thickness of the fiber assembly sheet obtained in step 2.
  • the shape of the pulp fiber-containing resin pellets of the present embodiment is not particularly limited, and may be spherical, spheroidal, oblate spherical, rod-like, plate-like, block-like, or any shape similar thereto.
  • the pulp fiber-containing resin pellets of the present embodiment are suitably used as resin pellets for various moldings.
  • the method for producing a molded article according to the present embodiment includes a step of producing the pulp fiber-containing resin pellets described above and a step of molding the pulp fiber-containing resin pellets.
  • Various molding methods are employed in the molding process, for example, injection molding (e.g. injection compression molding (press injection, hot flow stamping molding, gas injection compression molding), gas injection molding, and ultra-high speed injection molding).
  • injection molding e.g. injection compression molding (press injection, hot flow stamping molding, gas injection compression molding), gas injection molding, and ultra-high speed injection molding.
  • various extrusion molding cold runner method or hot runner method
  • compression (press) molding e.g., insert molding, in-mold coating molding, heat insulation molding, rapid heating and cooling molding
  • various profile extrusion molding such as two-color molding and sandwich molding
  • various extrusion molding methods are suitable for molding sheets, films, fibers, and the like.
  • a blowing method, a calendering method, a casting method, or the like can also be used to form a sheet or film.
  • a specific stretching operation may be applied.
  • a plurality of molding steps may be combined, or a plurality of steps may be carried out simultaneously to form one step.
  • the pulp fiber-containing resin pellets may be formed into a sheet and hot-press molded to obtain a molded body, or the pulp fiber-containing resin pellets may be formed into a sheet and supercalendered to obtain a molded body.
  • the material after forming into a sheet, the material may be formed by vacuum forming, pressure forming, or the like.
  • injection molding is preferably exemplified.
  • the injection molding step includes, for example, melt-kneading the fiber assembly using a known injection molding machine, and injecting the melted mixture into a mold. to mold.
  • a known kneader may be used for melt-kneading, and examples thereof include a single-screw kneader and a twin-screw kneader.
  • Examples of known injection molding machines include screw type injection molding machines, screw pre-plastic injection molding machines, plunger pre-plastic injection molding machines, and plunger-type injection molding machines.
  • drive systems include hydraulic, electric, and hydraulic-electric hybrid systems.
  • the temperature conditions for injection molding are appropriately determined according to the type of resin contained in the pellets, and the cylinder temperature of the injection molding machine is preferably set to a temperature 0 to 100° C. higher than the flow start temperature of the resin to be used.
  • the temperature of the mold may be appropriately selected from the viewpoint of the cooling rate and productivity of the resin used.
  • room temperature eg, 23°C
  • Other injection conditions such as screw rotation speed, back pressure, injection speed, holding pressure, holding pressure time, etc., may be appropriately adjusted.
  • the pulp fiber-containing resin pellets of the present embodiment may contain other resins such as elastomers by adding other resins such as elastomers and melt-kneading them in step 3-1.
  • other resins, various additives, master batches containing various additives, and the like may be added in the manufacturing process of the molded body.
  • additives include additives that are commonly used in resin compositions. Examples of such additives include stabilizers, ultraviolet absorbers, plasticizers, flame retardants, flame retardant aids, antistatic agents, surfactants, colorants, lubricants, release agents and the like.
  • stabilizers include hindered phenols, hydroquinones, phosphites and substituted products thereof.
  • UV absorbers examples include resorcinol, salicylate, benzotriazole, and benzophenone.
  • Colorants include materials including dyes such as nitrosine, and pigments such as cadmium sulfide, phthalocyanine, carbon black, and the like.
  • lubricants include fatty acids such as stearic acid and montanic acid, amides thereof, esters thereof, half esters thereof with polyhydric alcohols, stearyl alcohol, stearamide, and polyethylene wax.
  • the density of the molded product obtained is preferably 0.5 g/cm 3 or more, more preferably 0.8 g/cm 3 or more, still more preferably 0.95 g/cm 3 or more, and even more preferably 1 0 g/cm 3 or more.
  • the density of the molded body is preferably 3.0 g/cm 3 or less, more preferably 1.5 g/cm 3 or less, still more preferably 1.2 g/cm 3 or less.
  • the thickness of the molded body is not particularly limited, but is 0.5 mm or more, more preferably 1 mm or more, still more preferably 2 mm or more, and is preferably 200 mm or less, more preferably 100 mm or less, further preferably 50 mm or less. More preferably 20 mm or less, particularly preferably 10 mm or less. By setting the thickness of the molded body to 2 mm or more, the molded body can be suitably used in applications requiring impact resistance.
  • the molded article of the present embodiment preferably has a high flexural modulus, and the molded article having a high flexural modulus is preferable because the molded article has excellent bending rigidity.
  • the flexural modulus of the molded article is preferably 1.5 GPa or more, more preferably 2.0 GPa or more, still more preferably 2.5 GPa or more, still more preferably 2.8 GPa or more, and even more preferably 3.0 GPa or more. .
  • the upper limit is not particularly limited, it is preferably 10 GPa or less from the viewpoint of ease of manufacture.
  • the flexural modulus of the molded article is measured according to JIS K 7171:2016.
  • the molded article of the present embodiment preferably has high bending strength, and it is preferable that the molded article has high bending strength because the molded article has excellent rigidity.
  • the bending strength of the compact is preferably 20 MPa or higher, more preferably 30 MPa or higher, and still more preferably 35 MPa or higher.
  • the upper limit is not particularly limited, it is preferably 100 MPa or less from the viewpoint of ease of production.
  • the bending strength of the molded article is measured according to JIS K 7171:2016.
  • the molded article of the present embodiment preferably has a high Charpy impact strength. It is more preferably 8.0 kJ/m 2 or more, still more preferably 10.0 kJ/m 2 or more, and even more preferably 12 kJ/m 2 or more. Although the upper limit is not particularly limited, it is preferably 100 kJ/m 2 or less from the viewpoint of ease of manufacture.
  • Charpy impact strength means that it is excellent in impact resistance, so that a numerical value is large.
  • the Charpy impact strength is measured according to JIS K 7111-1:2012, and more specifically by the method described in Examples.
  • the molded article obtained by the method for manufacturing the molded article of the present embodiment includes electrical and electronic equipment, OA equipment, home appliances, civil engineering, automobiles, aircraft parts, structural parts and housings, containers (e.g., food containers, drug packaging containers, cosmetic packaging containers, medical equipment packaging containers), furniture, daily necessities, medical tools, and the like.
  • containers e.g., food containers, drug packaging containers, cosmetic packaging containers, medical equipment packaging containers
  • furniture daily necessities, medical tools, and the like.
  • impact resistance such as civil engineering and construction, parts of automobiles or aircraft, structural parts, and housings.
  • Example 1 ⁇ Production of fiber assembly> NBKP was defibrated using a swirl-type jet stream defibrator to obtain defibrated dry pulp.
  • the processing wind speed in the defibrator was 45 m/min, and the flow was turbulent with a baffle provided in the apparatus.
  • the obtained defibrated dry pulp had an average fiber length of 2.38 mm, an average fiber width of 34.3 ⁇ m, and a fine fiber ratio of 11.4%.
  • the obtained defibrated dry pulp, polypropylene fiber (melting point 160 ° C., fineness 6.6 dtex, fiber length 5 mm, fiber diameter 30 ⁇ m, also called PP fiber), and polyethylene / polypropylene composite core-sheath fiber (core melting point 160 °C, sheath melting point 110 °C, fineness 1.7 dtex, fiber length 5 mm, fiber diameter 15 ⁇ m, core diameter 10.6 ⁇ m, core mass/sheath mass 1/1, also referred to as "PE/PP composite fiber") were uniformly mixed with an air flow at a ratio (mass ratio) of 50/35/15 to obtain a fiber mixture.
  • Example 1 an airlaid web was formed from the fiber mixture.
  • the first carrier sheet 41 was let out by the first carrier sheet supplying means 40 onto the air-permeable endless belt 20 mounted on the conveyor 10 and running.
  • a tissue (basis weight: 14 g/m 2 ) was used as the first carrier sheet 41 .
  • the “basis weight” was measured in accordance with “Paper and paperboard—Method for measuring basis weight” described in JIS P8124:2011.
  • the fiber mixture was dropped and accumulated on the first carrier sheet 41 from the fiber mixture supplying means 30 together with an air flow to obtain a cotton-like fiber aggregate.
  • the fiber mixture was supplied so that the set basis weight of the airlaid web portion was 400 g/m 2 .
  • a second carrier sheet 51 was laminated on the cotton-like fiber assembly on the first carrier sheet 41 by a second carrier sheet supplying means 50 to obtain an airlaid web-containing laminated sheet.
  • a tissue (basis weight: 14 g/m 2 ) was used as the second carrier sheet 51 . That is, in Example 1, the same sheet was used for the first carrier sheet 41 and the second carrier sheet 51 .
  • the air-laid web-containing laminated sheet thus obtained was passed through a box-type drier of a hot air circulation conveyor oven system and subjected to hot air treatment at a temperature of 140°C. After that, the density was adjusted by roll pressing so that the bulk specific gravity was 0.3 g / mL, and without separating the first carrier sheet and the second carrier sheet, fibers with a basis weight of 438.9 g / m 2 An aggregate bulky sheet was obtained.
  • the fiber assembly bulky sheet had a T/Y of 0.88, a bulk specific gravity of 0.33 g/mL, and a thickness of 1.33 mm.
  • the fiber assembly sheet was cut with a shredder (AFS100M, manufactured by Iris Ohyama Co., Ltd.) to obtain press-cut chips of about 4 mm ⁇ 13 mm.
  • the press-cut chips are kneaded with a twin-screw kneading extruder (manufactured by Ikegai Co., Ltd., PCM46) at a kneading temperature of 145° C. (resin temperature: 170 to 180° C.), a barrel setting temperature of 145° C., a rotation speed of 56 rpm, and a discharge amount of 0.9 kg. / hour.
  • the screw used for kneading is divided into 10 parts, and only the 8th part counted from the raw material inlet side uses R type kneading parts consisting of 6 parts, and the rest are all composed of feed screws.
  • a type A1 multi-purpose test piece specified in JIS K 7139:2009 was injection molded under the conditions of a molding temperature of 190 ° C., a mold temperature of 40 ° C., and an injection speed of 100 mm / sec to obtain a pulp fiber-containing molded product. rice field.
  • the density of the pulp fiber-containing compact was 1.03 g/cm 3 .
  • Example 2 In ⁇ Production of fiber assembly> of Example 1, the fiber mixture was changed to a ratio (mass ratio) of 60/25/15 to obtain a fiber assembly sheet, and the output of the twin-screw kneading extruder was 1.2 kg.
  • a molded body containing pulp fibers was obtained in the same manner as in Example 1, except that the time was changed to /.
  • the fiber assembly sheet had a T/Y of 0.90, a basis weight of 394.8 g/m 2 , a bulk specific gravity of 0.28 g/mL, and a thickness of 1.41 mm. Further, the density of the pulp fiber-containing compact was 1.09 g/cm 3 .
  • Example 3 In ⁇ Fabrication of fiber assembly> of Example 2, maleic anhydride-modified polyethylene/polypropylene composite core-sheath fiber (core melting point 160°C, sheath melting point 100°C, fineness 1) was used instead of polyethylene/polypropylene composite core-sheath fiber.
  • Pulp was produced in the same manner as in Example 2 except that the density was adjusted to 0.2 g / mL, a fiber assembly sheet was obtained, and the discharge rate of the twin-screw kneading extruder was 1.0 kg / hour. A fiber-containing molding was obtained.
  • the fiber assembly sheet had a T/Y of 1.08, a basis weight of 403.2 g/m 2 , a bulk specific gravity of 0.18 g/mL, and a thickness of 2.24 mm. Further, the density of the pulp fiber-containing compact was 1.14 g/cm 3 .
  • Example 4 In ⁇ Production of fiber assembly> of Example 1, the fiber mixture was changed to a ratio (mass ratio) of 70/15/15, and the density was adjusted by roll pressing so that the bulk specific gravity was 0.4 g / mL.
  • a molded body containing pulp fibers was obtained in the same manner as in Example 1, except that a bulky fiber assembly sheet was obtained.
  • the fiber assembly sheet had a T/Y of 0.87, a basis weight of 412.0 g/m 2 , a bulk specific gravity of 0.40 g/mL, and a thickness of 1.03 mm. Further, the density of the pulp fiber-containing compact was 1.14 g/cm 3 .
  • core melting point 160°C, sheath melting point 100°C, fineness 1 .7 dtex, fiber length 3 mm, fiber diameter 15 ⁇ m, core diameter 10.6 ⁇ m, core mass / sheath mass 1/1, also called “MAPE / PP composite
  • the fiber assembly sheet had a T/Y of 1.15, a basis weight of 399.5 g/m 2 , a bulk specific gravity of 0.47 g/mL, and a thickness of 0.85 mm. Further, the density of the pulp fiber-containing compact was 1.19 g/cm 3 .
  • Example 6 Press-cut chips were obtained in the same manner as in Example 2.
  • a propylene/ethylene copolymer (SunAllomer PM472W, SunAllomer Co., Ltd.) as resin A was mixed as shown in Table 1 using a twin-screw kneading extruder (PCM46, Ikegai Co., Ltd.). ), and was melt-kneaded and dispersed at a kneading temperature of 160° C. (resin temperature: 190 to 200° C.) and a discharge rate of 7.2 kg/hour.
  • PCM46 twin-screw kneading extruder
  • Example 6 20 parts by mass of a propylene/ethylene copolymer was added to 100 parts by mass of press-cut chips.
  • the screw used for kneading was the same as in Example 1, except that one of the six R-type kneading parts closest to the outlet was changed to an L-type kneading part.
  • a molded body containing pulp fibers was obtained in the same manner as in Example 1, except that the molding temperature was 180°C.
  • the density of the pulp fiber molding was 1.08 g/cm 3 .
  • Example 7 pulp was prepared in the same manner as in Example 6 except that the formulation was as shown in Table 1, the kneading temperature was 190 ° C. (resin temperature: 200 to 210 ° C.), and the discharge amount was 12 kg / hour. A fiber-containing molding was obtained.
  • the fiber mixture was obtained by uniformly mixing the fibrillated dry pulp, the polypropylene fiber, and the PE/PP composite fiber at a ratio (mass ratio) of 60/25/15 with an air flow. .
  • 100 parts by mass of a propylene/ethylene copolymer was added to 100 parts by mass of press-cut chips.
  • the density of the pulp-containing compact was 1.00 g/cm 3 .
  • Example 8 Press-cut chips were obtained in the same manner as in Example 1, except that the ratio (mass ratio) of the fiber mixture was changed to 30/55/15.
  • the fiber assembly sheet before obtaining the press-cut chips had a T/Y of 0.88, a basis weight of 449.5 g/m 2 , a bulk specific gravity of 0.29 g/mL, and a thickness of 1.55 mm.
  • the press cut chips and the elastomer (Tuftec H1062, manufactured by Asahi Kasei Corporation) were supplied so that the formulation was as shown in Table 1, and the discharge amount was changed to 9.9 kg / hour, and the molding temperature was changed to 170 ° C.
  • a molded body containing pulp fibers was obtained in the same manner as in Example 6 except for the above.
  • 15 parts by mass of elastomer was added to 85 parts by mass of press-cut chips.
  • the density of the pulp fiber molding was 1.00 g/cm 3 .
  • Example 9 A molded article containing pulp fibers was obtained in the same manner as in Example 8, except that the elastomer was changed to TAFUMER DF810 (manufactured by Mitsui Chemicals, Inc.). The density of the pulp-containing compact was 1.00 g/cm 3 .
  • Example 10 A molded body containing pulp fibers was obtained in the same manner as in Example 8, except that the elastomer was changed to Toughmer DF940 (manufactured by Mitsui Chemicals, Inc.). The density of the pulp-containing compact was 1.00 g/cm 3 .
  • Example 11 A molded product containing pulp fibers was obtained in the same manner as in Example 8, except that the elastomer was changed to Toughmer DF9200 (manufactured by Mitsui Chemicals, Inc.). The density of the pulp-containing compact was 1.00 g/cm 3 .
  • Example 12 A molded article containing pulp fibers was obtained in the same manner as in Example 8, except that the elastomer was changed to Toughmer DF610 (manufactured by Mitsui Chemicals, Inc.). The density of the pulp-containing compact was 1.00 g/cm 3 .
  • Example 13 Press-cut chips were obtained in the same manner as in Example 2.
  • a propylene/ethylene copolymer (SunAllomer PM472W, manufactured by SunAllomer Co., Ltd.) and an elastomer (Tuftec H1062, manufactured by Asahi Kasei Co., Ltd.) were used as resin A so that the formulation was as shown in Table 1.
  • a pulp fiber-containing compact in the same manner as in Example 8, except that the discharge amount was changed to 20.2 kg/hour.
  • 43 parts by mass of propylene-ethylene copolymer and 15 parts by mass of elastomer were added to 42 parts by mass of press-cut chips.
  • the density of the pulp-containing compact was 0.97 g/cm 3 .
  • Example 14 ⁇ Production of fiber assembly sheet>
  • the density was adjusted so that the bulk specific gravity was 0.06 g/mL by roll pressing, and the first carrier sheet and the second carrier sheet were separated in the same manner as in Example 1.
  • a bulky fiber assembly sheet having a basis weight of 451 g/m 2 was obtained.
  • the fiber assembly bulky sheet had a T/Y of 1.12, a bulk specific gravity of 0.055 g/mL, and a thickness of 8.2 mm.
  • the bulky fiber assembly sheet was cut into a size of 20 cm ⁇ 20 cm to obtain 5 cut pieces. The obtained cut pieces were piled up to produce a five-layer laminated structure.
  • the laminated structure was placed in a stainless steel mold having an opening of 20 cm x 20 cm and a depth of 2 mm.
  • the mold was set in a hot press, pre-pressed at a temperature of 180° C. and a pressure of 1.5 MPa for 5 minutes, and further pressurized to 10 MPa for 15 minutes. After that, it was cooled while maintaining 10 MPa to obtain a fiber assembly sheet.
  • the density of the fiber assembly sheet was 1.12 g/cm 3 .
  • the fiber assembly sheet had a tensile strength (T) in the first direction of 37.0 MPa, a tensile strength (Y) in the second direction of 33.0 MPa, and T/Y was 1.12.
  • EVOH fiber (trade name Name: S030, melting point: 170° C., fiber thickness: about 9 ⁇ m, fiber length: 5 mm, manufactured by Kuraray Co., Ltd.) was added and dispersed by stirring to obtain a 0.5% EVOH fiber dispersion.
  • the fiber assembly sheet had a T/Y of 2.69, a basis weight of 130 g/m 2 , a bulk specific gravity of 0.52 g/mL, and a thickness of 0.25 mm.
  • the resulting dense fiber assembly sheet was cut with a shredder (AFS100M, manufactured by Iris Ohyama Co., Ltd.) to obtain press-cut chips of about 4 mm ⁇ 13 mm.
  • a molded body containing pulp fibers was obtained in the same manner as in Example 1.
  • the density of the pulp fiber-containing compact was 1.02 g/cm 3 .
  • the screw used for kneading was divided into 7 parts, and only the 5th part counted from the raw material inlet side used a kneading part consisting of 6 parts, and the other parts were all composed of feed screws. It was a kneaded configuration. As for the kneading parts, the one closest to the discharge port was L type, and the others were all R type.
  • a molding composition (resin composition) obtained by melt-kneading was extruded into a strand shape and then cut into pellets.
  • a type A1 multipurpose test piece specified in JIS K 7139:2009 was injection molded under the conditions of a molding temperature of 165 ° C., a mold temperature of 40 ° C., and an injection speed of 100 mm / sec to obtain a pulp fiber-containing molded product. rice field.
  • the density of the pulp fiber-containing compact was 0.95 g/cm 3 .
  • the average fiber length and average fiber diameter of the pulp fibers were measured using a fiber image analyzer (Valmet FS5, manufactured by Valmet Co., Ltd.). Also, the ratio of fine fibers of 0.1 mm or less in the measured length-weighted average fiber length distribution was defined as the fine fiber ratio.
  • Method for measuring melting point of polyolefin fiber 5 mg of polyolefin fiber is cut out, and the melting point of the polyolefin fiber is measured with a differential scanning calorimeter (DSC). The melting point is measured by increasing the temperature from 30° C. to 280° C. at a rate of 20° C./min under a nitrogen atmosphere using a Diamond DSC manufactured by Perkin-Elmer. If there are catalog values for polyolefin fibers, etc., the catalog values may be adopted.
  • DSC differential scanning calorimeter
  • the bulk specific gravity of the bulky fiber assembly sheet and the dense fiber assembly sheet was calculated by measuring the thickness and weight of the sheet after conditioning the humidity of the 50 mm square sheet under conditions of 23° C. and 50% RH for 24 hours.
  • the thickness of the sheet was measured with a digital thickness gauge (DG-127, manufactured by Ozaki Seisakusho Co., Ltd.).
  • the flow direction (running direction of the conveyor 10) in the manufacturing process of the obtained fiber assembly is the first direction, the direction orthogonal to the first direction is the second direction, and the tensile strength is measured according to JIS P 8113:2006.
  • the thickness (unit is N/m) was measured.
  • the tensile strength in each direction was calculated by dividing this tensile strength by the thickness of the test piece (unit: MPa).
  • a strip of 15 mm ⁇ 180 mm was measured at a speed of 20 mm/min using Tensilon manufactured by A&D Co., Ltd. as a tensile tester.
  • the obtained molded article (molded body) was cut into a strip-shaped test piece having a length of 80 mm and a width of 10 mm.
  • the thickness of the strip-shaped test piece was measured with a constant pressure thickness measuring device (manufactured by Teclock Co., Ltd., model number PG-02J), and the volume of the strip-shaped test piece was calculated. Furthermore, the density was calculated by measuring the mass of the strip-shaped test piece.
  • the molded articles produced using the pulp fiber-containing pellets of the present invention are excellent in flexural modulus and flexural strength, and excellent in rigidity and strength against bending. It was excellent in impact resistance.
  • Comparative Example 1 when ethylene-vinyl alcohol copolymer (EVOH) fibers were used in place of polyolefin fibers and a slurry containing pulp and EVOH was made into paper to obtain a fiber aggregate. was inferior in rigidity and strength against bending and in impact resistance as compared with the examples. Further, in Comparative Example 2, in which the fiber assembly was not formed into a fiber aggregate but was melt-kneaded and then injection-molded, the strength against bending was improved, but the rigidity against bending and the impact resistance were inferior.
  • EVOH ethylene-vinyl alcohol copolymer

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