CN103114351A - Preparation method and dry-wet spinning method of regenerated protein chitosan blended solution - Google Patents

Preparation method and dry-wet spinning method of regenerated protein chitosan blended solution Download PDF

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Publication number
CN103114351A
CN103114351A CN2013100726945A CN201310072694A CN103114351A CN 103114351 A CN103114351 A CN 103114351A CN 2013100726945 A CN2013100726945 A CN 2013100726945A CN 201310072694 A CN201310072694 A CN 201310072694A CN 103114351 A CN103114351 A CN 103114351A
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solution
regenerated protein
concentration
preparation
dry
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CN2013100726945A
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CN103114351B (en
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赵振强
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Henan Dingda Biological Science & Technology Co Ltd
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Henan Dingda Biological Science & Technology Co Ltd
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Abstract

The invention relates to a preparation method and a dry-wet spinning method of a regenerated protein chitosan blended solution. The preparation method comprises the steps of: carrying out ultrafine grinding on raw materials of leftovers of reeling silks and leftovers of animal coarse hairs such as goat hairs, pig hairs, camel hairs and wools, dissolving the crushed raw materials in an ionic liquid to obtain a regenerated protein solution with high molecular weight, and blending the regenerated protein solution with a chitosan liquid to obtain a spinning solution. The spinning solution is molded by using a dry-wet spinning technology, the structure uniformity and the orientation degree of fibers are enhanced through solidification and drafting, and the elongation and the elasticity of the fibers are improved through oxidation crosslinking. The regenerated protein chitosan blended fiber has high protein content, and has functions of bacteria resistance, moisture prevention and promotion of blood coagulation and wound healing; and all compositions in the fiber are in biomass states, have good biodegradability and biocompatibility and can be applied to textile fibers and biomedical materials.

Description

The preparation of regenerated protein chitosan blend solution and the method for dry-wet spinning
Technical field
The invention belongs to biomass resource regeneration field, relate to a kind of preparation method of the regenerated protein that contains shitosan, be specifically related to a kind of raw egg again that adopts dry-wet spinning technique
The preparation of white chitosan blend solution and the method for dry-wet spinning.
Background technology
Protein fibre has good moisture pick-up properties and antistatic property, with human body skin, good compatibility is arranged, and in recent years, utilizes the marketization of soybean protein, milk protein and pupa albumen fiber of Protein processing, and demonstrates certain premium properties.But, the preparation of these azelons is all as copolymerization or blend such as polyvinyl alcohol, polyacrylonitrile by protein and synthetic high polymer, through wet spinning, obtain, in fiber, the content of albumen is very low, generally be no more than 15%, the main body composition remains synthetic macromolecule, so described azelon is not the azelon on complete meaning, does not also just possess the good characteristic of natural protein fiber.
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Summary of the invention
The objective of the invention is in order to overcome the existing defect of utilizing synthetic high polymer to prepare protein fibre, invent a kind of preparation of the regenerated protein chitosan blend solution that utilizes the chitosan to replace synthetic high polymer and the method for dry-wet spinning.Shitosan claims again chitin, chitin or chitin, at occurring in nature, shitosan extensively is present in the shell of the cell of rudimentary plant mushroom algae and arthropod shrimp crab insect, use the chitosan to replace synthetic high polymer, can make blended fiber possess the good characteristic of natural protein fiber, greatly improve comfortableness, health and the health of fiber.
The objective of the invention is to realize as follows:
Described regenerated protein chitosan blend solution be take silk, animal hair and shitosan and is made as raw material, and its preparation is to realize by following step:
(1) silk is put the Na that concentration is 0.5% under the condition of boiling 2cO 3in solution, come unstuck, the 1%-4% that the weight of silk is solution weight, come unstuck 3 times altogether, and each 10-90 minute comes unstuck rear with hot water injection 3 times, then under 50-90 ℃, dries, shreds;
(2) silk fiber will dry, shredded mixes according to the ratio of quality 1:0.1-20 with animal hair, then by the air-flow micronizer, is ground into the albumen fine powder of diameter 0.01-30 micron;
(3) the albumen fine powder is joined in ionic liquid solution, 60-150 ℃ of lower strong agitation, dissolve 20-240 minute, filter and obtain the regenerated protein solution that concentration is 5-35%;
(4) shitosan is joined in ionic liquid solution, dissolve 30-180 minute under 50-135 ℃ of condition, filter and obtain the chitosan solution that concentration is 1.5-35%;
(5) by regenerated protein solution and chitosan solution blend, the regenerated protein chitosan blend solution that to obtain concentration be 5-35%, wherein the mass ratio of regenerated protein and shitosan is 1-10:1.
The dry-wet spinning method of described regenerated protein chitosan blend solution, its technological process comprises: solidify-preliminary draft-drawing-off-compacting by drying-HEAT SETTING, the process conditions of each step are as follows:
solidify
Coagulation bath composition: the ionic liquid aqueous solution that concentration is 5-70%
Coagulation bath temperature: 10-35 ℃
Air layer height: 1-20 centimetre (being the distance of spinning head surface and coagulating bath liquid level)
Spinning speed: 2-25 m/min
preliminary draft
Preliminary draft is bathed and is formed: the ionic liquid aqueous solution that concentration is 1-50%
Preliminary draft bath temperature: 30-65 ℃
Pre-draft multiple: 1.2-4.5
drawing-off
Drawing-off is bathed and is formed: the aqueous oxidizing agent solution that concentration is 0.5-5.0%
Drawing-off bath temperature: 50-98 ℃
Drafting multiple: 2.5-8 doubly
compacting by drying
Compacting by drying temperature: 100-145 ℃
The compacting by drying time: 5-25 minute
The tension force condition: length is fixed, nervous state (maintenance fiber tension)
hEAT SETTING
HEAT SETTING medium: steam
Steam pressure: 2-10 kg/cm 2
Shaping time: 1-25 minute.
The molecular weight of described shitosan is 10,000-200,000, and deacetylation is more than or equal to 90%.
Described animal hair is pig hair, goats hair, the rabbit hair, camel hair, consumption ox hair, and the sheep's wool of on-woven value.
Described ionic liquid is 1-butyl-3-methylimidazole villaumite, 1-butyl-3-methyl imidazolium tetrafluoroborate or 1-ethyl-3-methylimidazole diethyl phosphate.
Described oxidant is Peracetic acid or hydrogen peroxide.
Good effect of the present invention is as follows: the present invention adopts the dry jet wet spinning technology to realize the fibration of regenerated protein chitosan blend solution, by solidifying and drawing-off, improve the uniformity and the degree of orientation of fibre structure, by oxidation cross-linked, improved elongation and the elasticity of fiber.Regenerated protein chitosan blend fiber of the present invention, there is higher protein content, and there is the function of antibiotic, moisturizing, promotion blood coagulation and wound healing, in fiber, all the components is living beings, there is good biological degradability and biocompatibility, not only can apply to textile fabric, also can be used as bio-medical material.
 
The specific embodiment
case study on implementation 1
The present embodiment be take regenerated protein chitosan blend solution and is produced composite fibre as raw material adopts dry-wet spinning technique;
Regenerated protein chitosan blend solution, take silk, animal hair and shitosan to make as raw material, and its preparation process is as follows:
(1) silk is put the Na that concentration is 0.5% under the condition of boiling 2cO 3in solution, come unstuck, the consumption of silk is solution weight 1.5%, come unstuck altogether 3 times, and each 15 minutes, come unstuck rear with hot water injection 3 times, then under 90 ℃, dry, shred;
(2) silk fiber will dry, shredded and pig hair are ground into the albumen fine powder of 25 microns left and right of diameter by the air-flow micronizer after according to mass ratio 1:0.2 blend.
(3) the albumen fine powder is joined in 1-butyl-3-methylimidazole chloride aqueous solution, dissolve 140 minutes 80 ℃ of lower strong agitation, filter and obtain the regenerated protein solution that concentration is 25%.
(4) by molecular weight be 12,000, deacetylation is more than or equal to 90% shitosan and joins in 1-butyl-3-methylimidazole chloride aqueous solution, under 75 ℃ of conditions, dissolves 150 minutes, filter and obtain the chitosan solution that concentration is 5%.
(5) by regenerated protein solution and chitosan solution blend, the regenerated protein chitosan blend solution that to obtain concentration be 23%, the mass ratio of regenerated protein and shitosan is 9:1.
The technological process that utilizes above-mentioned regenerated protein chitosan blend solution to carry out dry-wet spinning comprises: solidify-preliminary draft-drawing-off-compacting by drying-HEAT SETTING, the process conditions of each step are as follows:
solidify
Coagulation bath composition: the 1-butyl that concentration is 70%-3-methylimidazole chloride aqueous solution
Coagulation bath temperature: 15 ℃
Air layer height: 7 centimetres
Spinning speed: 10 m/mins
preliminary draft
Preliminary draft is bathed and is formed: the 1-butyl that concentration is 30%-3-methylimidazole chloride aqueous solution
Preliminary draft bath temperature: 65 ℃
Pre-draft multiple: 1.5
drawing-off
Drawing-off is bathed and is formed: the aqueous hydrogen peroxide solution that concentration is 5.0%
Drawing-off bath temperature: 98 ℃
Drafting multiple: 8 times
compacting by drying
Compacting by drying temperature: 135 ℃
The compacting by drying time: 5 minutes
The tension force condition: length is fixed, nervous state
hEAT SETTING
HEAT SETTING medium: steam
Steam pressure: 5.0 kg/cm 2
Shaping time: 5.0 minutes.
 
case study on implementation 2
The present embodiment be take regenerated protein chitosan blend solution and is produced composite fibre as raw material adopts dry-wet spinning technique;
Regenerated protein chitosan blend solution, take silk, animal hair and shitosan to make as raw material, and its preparation process is as follows:
(1) silk is put the Na that concentration is 0.5 under the condition of boiling 2cO 3in solution, come unstuck, the consumption of silk is solution weight 2.0%, come unstuck altogether 3 times, and each 50 minutes, come unstuck rear with hot water injection 3 times, then under 60 ℃, dry, shred.
(2) silk fiber will dry, shredded and goats hair are ground into the albumen fine powder of 5.0 microns left and right of diameter by the air-flow micronizer after according to mass ratio 1:5 blend.
(3) the albumen fine powder is joined in 1-butyl-3-methyl imidazolium tetrafluoroborate aqueous solution, dissolve 80 minutes 100 ℃ of lower strong agitation, filter and obtain the regenerated protein solution that concentration expressed in percentage by weight is 20%.
(4) by molecular weight be 15,000, deacetylation is more than or equal to 90% shitosan and joins in 1-butyl-3-methyl imidazolium tetrafluoroborate aqueous solution, under 105 ℃ of conditions, dissolves 30 minutes, filter and obtain the chitosan solution that concentration expressed in percentage by weight is 3.5%.
(5) by regenerated protein solution and chitosan solution blend, the regenerated protein chitosan blend solution that to obtain concentration be 16.7%, the mass ratio of regenerated protein and shitosan is 4:1;
The technological process that utilizes above-mentioned regenerated protein chitosan blend solution to carry out dry-wet spinning comprises: solidify-preliminary draft-drawing-off-compacting by drying-HEAT SETTING, the process conditions of each step are as follows:
solidify
Coagulation bath composition: the 1-butyl that concentration is 40%-3-methyl imidazolium tetrafluoroborate aqueous solution
Coagulation bath temperature: 10 ℃
Air layer height: 3 centimetres
Spinning speed: 3.5 m/mins
preliminary draft
Preliminary draft is bathed and is formed: the 1-butyl that concentration is 10%-3-methyl imidazolium tetrafluoroborate aqueous solution
Preliminary draft bath temperature: 45 ℃
Pre-draft multiple: 2.5
drawing-off
Drawing-off is bathed and is formed: the peroxide acetate aqueous solution that concentration is 0.5%
Drawing-off bath temperature: 88 ℃
Drafting multiple: 6.0 times
compacting by drying
Compacting by drying temperature: 115 ℃
The compacting by drying time: 15 minutes
The tension force condition: length is fixed, nervous state
hEAT SETTING
HEAT SETTING medium: steam
Steam pressure: 8 kg/cm 2
Shaping time: 5.5 minutes.
?
case study on implementation 3
The present embodiment be take regenerated protein chitosan blend solution and is produced composite fibre as raw material adopts dry-wet spinning technique;
Regenerated protein chitosan blend solution, take silk, animal hair and shitosan to make as raw material, and its preparation process is as follows:
(1) silk is put the Na that concentration is 0.5% under the condition of boiling 2cO 3in solution, come unstuck, the consumption of silk is solution weight 3.5%, come unstuck altogether 3 times, and each 40 minutes, come unstuck rear with hot water injection 3 times, then under 70 ℃, dry, shred.
(2) silk fiber will dry, shredded and camel hair are ground into the albumen fine powder of 2.0 microns left and right of diameter by the air-flow micronizer after according to mass ratio 1:10 blend.
(3) the albumen fine powder is joined in 1-ethyl-3-methylimidazole p diethylaminobenzoic acid aqueous solution of ester, dissolve 100 minutes 115 ℃ of lower strong agitation, filter and obtain the regenerated protein solution that concentration is 30%.
(4) by molecular weight be 18,000, deacetylation is more than or equal to 90% shitosan and joins in 1-ethyl-3-methylimidazole p diethylaminobenzoic acid aqueous solution of ester, under 85 ℃ of conditions, dissolves 90 minutes, filter and obtain the chitosan solution that concentration expressed in percentage by weight is 7.5%.
(5) by regenerated protein solution and chitosan solution blend, the regenerated protein chitosan blend solution that to obtain concentration be 24.4%, the mass ratio of regenerated protein and shitosan is 3:1.
The technological process that utilizes above-mentioned regenerated protein chitosan blend solution to carry out dry-wet spinning comprises: solidify-preliminary draft-drawing-off-compacting by drying-HEAT SETTING, the process conditions of each step are as follows:
solidify
Coagulation bath composition: concentration is 55% from 1-ethyl-3-methylimidazole p diethylaminobenzoic acid aqueous solution of ester
Coagulation bath temperature: 25 ℃
Air layer height: 4 centimetres
Spinning speed: 8 m/mins
preliminary draft
Preliminary draft is bathed and is formed: the 1-ethyl-3-methylimidazole p diethylaminobenzoic acid aqueous solution of ester that concentration is 18%
Preliminary draft bath temperature: 55 ℃
Pre-draft multiple: 2.1 times
drawing-off
Drawing-off is bathed and is formed: the aqueous hydrogen peroxide solution that concentration is 1.5%
Drawing-off bath temperature: 90 ℃
Drafting multiple: 6.5 times
compacting by drying:
Compacting by drying temperature: 125 ℃
The compacting by drying time: 12 minutes
The tension force condition: length is fixed, nervous state
hEAT SETTING
HEAT SETTING medium: steam
Steam pressure: 3.0 kg/cm 2
Shaping time: 10 minutes.

Claims (7)

1. the preparation of a regenerated protein chitosan blend solution is characterized in that: this solution be take silk, animal hair and shitosan and is made as raw material, and its preparation is to realize by following step:
(1) silk is put the Na that concentration is 0.5% under the condition of boiling 2cO 3in solution, come unstuck, the 1%-4% that the weight of silk is solution weight, come unstuck 3 times altogether, and each 10-90 minute comes unstuck rear with hot water injection 3 times, then under 50-90 ℃, dries, shreds;
(2) silk fiber will dry, shredded mixes according to the ratio of quality 1:0.1-20 with animal hair, then by the air-flow micronizer, is ground into the albumen fine powder of diameter 0.01-30 micron;
(3) the albumen fine powder is joined in ionic liquid solution, 60-150 ℃ of lower strong agitation, dissolve 20-240 minute, filter and obtain the regenerated protein solution that concentration is 5-35%;
(4) shitosan is joined in ionic liquid solution, dissolve 30-180 minute under 50-135 ℃ of condition, filter and obtain the chitosan solution that concentration is 1.5-35%;
(5) by regenerated protein solution and chitosan solution blend, the regenerated protein chitosan blend solution that to obtain concentration be 5-35%, wherein the mass ratio of regenerated protein and shitosan is 1-10:1.
2. a method of carrying out dry-wet spinning with regenerated protein chitosan blend solution claimed in claim 1 is characterized in that:
The dry-wet spinning method of described regenerated protein chitosan blend solution, its technological process comprises: solidify-preliminary draft-drawing-off-compacting by drying-HEAT SETTING, the process conditions of each step are as follows:
solidify
Coagulation bath composition: the ionic liquid aqueous solution that concentration is 5-70%
Coagulation bath temperature: 10-35 ℃
Air layer height: 1-20 centimetre (being the distance of spinning head surface and coagulating bath liquid level)
Spinning speed: 2-25 m/min
preliminary draft
Preliminary draft is bathed and is formed: the ionic liquid aqueous solution that concentration is 1-50%
Preliminary draft bath temperature: 30-65 ℃
Pre-draft multiple: 1.2-4.5
drawing-off
Drawing-off is bathed and is formed: the aqueous oxidizing agent solution that concentration is 0.5-5.0%
Drawing-off bath temperature: 50-98 ℃
Drafting multiple: 2.5-8 doubly
compacting by drying
Compacting by drying temperature: 100-145 ℃
The compacting by drying time: 5-25 minute
The tension force condition: length is fixed, nervous state
hEAT SETTING
HEAT SETTING medium: steam
Steam pressure: 2-10 kg/cm 2
Shaping time: 1-25 minute.
3. the preparation of regenerated protein chitosan blend solution according to claim 1 is characterized in that: the molecular weight of described shitosan is 10,000-200,000, and deacetylation is more than or equal to 90%.
4. the preparation of regenerated protein chitosan blend solution according to claim 1 is characterized in that: described animal hair is pig hair, goats hair, the rabbit hair, camel hair, consumption ox hair, and the sheep's wool of on-woven value.
5. the preparation of regenerated protein chitosan blend solution according to claim 1 is characterized in that: described ionic liquid is 1-butyl-3-methylimidazole villaumite, 1-butyl-3-methyl imidazolium tetrafluoroborate or 1-ethyl-3-methylimidazole diethyl phosphate.
6. method of carrying out dry-wet spinning with regenerated protein chitosan blend solution according to claim 2, it is characterized in that: described ionic liquid is 1-butyl-3-methylimidazole villaumite, 1-butyl-3-methyl imidazolium tetrafluoroborate or 1-ethyl-3-methylimidazole diethyl phosphate.
7. method of carrying out dry-wet spinning with regenerated protein chitosan blend solution according to claim 2, it is characterized in that: described oxidant is Peracetic acid or hydrogen peroxide.
CN201310072694.5A 2013-03-07 2013-03-07 Preparation method and dry-wet spinning method of regenerated protein chitosan blended solution Expired - Fee Related CN103114351B (en)

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CN107299447A (en) * 2017-07-16 2017-10-27 长沙秋点兵信息科技有限公司 Process for preparing moisture-absorbing stretch-proof fabric by using silk
CN108950721A (en) * 2018-07-10 2018-12-07 安徽省宇鸿纺织工艺制品有限公司 A kind of production technology of fibroin albumen composite fibre
CN110512304A (en) * 2019-08-23 2019-11-29 大连工业大学 A kind of preparation method of chitosan/Antarctic krill protein composite fiber
CN111962174A (en) * 2020-08-30 2020-11-20 上海视物科技有限公司 Goat milk shred and preparation method and application thereof
US10982381B2 (en) 2014-10-06 2021-04-20 Natural Fiber Welding, Inc. Methods, processes, and apparatuses for producing welded substrates
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CN114622304A (en) * 2022-02-07 2022-06-14 江南大学 Preparation method of functional keratin composite fiber based on ionic liquid
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Publication number Priority date Publication date Assignee Title
CN103451770A (en) * 2013-09-04 2013-12-18 东华大学 Preparation method of green low-carbon flame retardant wig fiber
US11555263B2 (en) 2014-10-06 2023-01-17 Natural Fiber Welding, Inc. Methods, processes, and apparatuses for producing dyed and welded substrates
US12091815B2 (en) 2014-10-06 2024-09-17 Natural Fiber Welding, Inc. Methods, processes, and apparatuses for producing welded substrates
US10982381B2 (en) 2014-10-06 2021-04-20 Natural Fiber Welding, Inc. Methods, processes, and apparatuses for producing welded substrates
US11766835B2 (en) 2016-03-25 2023-09-26 Natural Fiber Welding, Inc. Methods, processes, and apparatuses for producing welded substrates
US11920263B2 (en) 2016-05-03 2024-03-05 Natural Fiber Welding, Inc. Methods, processes, and apparatuses for producing dyed and welded substrates
US11085133B2 (en) 2016-05-03 2021-08-10 Natural Fiber Welding, Inc. Methods, processes, and apparatuses for producing dyed and welded substrates
CN107299447A (en) * 2017-07-16 2017-10-27 长沙秋点兵信息科技有限公司 Process for preparing moisture-absorbing stretch-proof fabric by using silk
CN108950721A (en) * 2018-07-10 2018-12-07 安徽省宇鸿纺织工艺制品有限公司 A kind of production technology of fibroin albumen composite fibre
CN110512304A (en) * 2019-08-23 2019-11-29 大连工业大学 A kind of preparation method of chitosan/Antarctic krill protein composite fiber
CN113005532A (en) * 2019-12-19 2021-06-22 武汉大学 Method for continuously preparing silk nanofiber and chitin or chitosan composite fiber
CN111962174A (en) * 2020-08-30 2020-11-20 上海视物科技有限公司 Goat milk shred and preparation method and application thereof
CN114622304A (en) * 2022-02-07 2022-06-14 江南大学 Preparation method of functional keratin composite fiber based on ionic liquid
CN115852506A (en) * 2022-12-01 2023-03-28 温州佳远生物科技有限公司 A kind of drying method for wet spinning of chitosan fiber
CN116716669A (en) * 2023-06-17 2023-09-08 张家港扬子染整有限公司 Regenerated keratin fiber tow and wet spinning method thereof

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