CN109627702A - A kind of Degradable environment protection polymer composite - Google Patents
A kind of Degradable environment protection polymer composite Download PDFInfo
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- CN109627702A CN109627702A CN201811260923.5A CN201811260923A CN109627702A CN 109627702 A CN109627702 A CN 109627702A CN 201811260923 A CN201811260923 A CN 201811260923A CN 109627702 A CN109627702 A CN 109627702A
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L67/00—Compositions of polyesters obtained by reactions forming a carboxylic ester link in the main chain; Compositions of derivatives of such polymers
- C08L67/02—Polyesters derived from dicarboxylic acids and dihydroxy compounds
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- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07D—HETEROCYCLIC COMPOUNDS
- C07D209/00—Heterocyclic compounds containing five-membered rings, condensed with other rings, with one nitrogen atom as the only ring hetero atom
- C07D209/02—Heterocyclic compounds containing five-membered rings, condensed with other rings, with one nitrogen atom as the only ring hetero atom condensed with one carbocyclic ring
- C07D209/44—Iso-indoles; Hydrogenated iso-indoles
- C07D209/48—Iso-indoles; Hydrogenated iso-indoles with oxygen atoms in positions 1 and 3, e.g. phthalimide
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- C—CHEMISTRY; METALLURGY
- C07—ORGANIC CHEMISTRY
- C07D—HETEROCYCLIC COMPOUNDS
- C07D405/00—Heterocyclic compounds containing both one or more hetero rings having oxygen atoms as the only ring hetero atoms, and one or more rings having nitrogen as the only ring hetero atom
- C07D405/02—Heterocyclic compounds containing both one or more hetero rings having oxygen atoms as the only ring hetero atoms, and one or more rings having nitrogen as the only ring hetero atom containing two hetero rings
- C07D405/04—Heterocyclic compounds containing both one or more hetero rings having oxygen atoms as the only ring hetero atoms, and one or more rings having nitrogen as the only ring hetero atom containing two hetero rings directly linked by a ring-member-to-ring-member bond
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2201/00—Properties
- C08L2201/06—Biodegradable
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2201/00—Properties
- C08L2201/08—Stabilised against heat, light or radiation or oxydation
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L2205/00—Polymer mixtures characterised by other features
- C08L2205/03—Polymer mixtures characterised by other features containing three or more polymers in a blend
- C08L2205/035—Polymer mixtures characterised by other features containing three or more polymers in a blend containing four or more polymers in a blend
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Abstract
The present invention relates to technical field of polymer materials, and in particular to a kind of Degradable environment protection polymer composite.The material is made of the raw material comprising following parts by weight: 50~80 parts of poly butylene succinate;40~60 parts of polylactic acid;20~30 parts of starch;10~20 parts of carragheen;1~5 part of toughener;0.5~2 part of coupling agent;0.5~2 part of antiager.Since material of the present invention is made of the degradable raw material such as poly butylene succinate, polylactic acid, starch, composite material of the present invention has good degradation;In addition, again since the composite material joined toughener and antiager, which also has good intensity, toughness and anti-aging effect.
Description
Technical field
The present invention relates to technical field of polymer materials, and in particular to a kind of Degradable environment protection polymer composite.
Background technique
3D printing is one kind based on digital model file, with adhesive materials such as powdery metal or plastics, is led to
The technology of object is constructed after the mode successively printed.With the development of 3D printing technique, industrial design, engineering, automobile,
The fields such as aerospace, dentistry and medical treatment have been more and more widely used.
As society is to the attention degree of environmental protection, Degradable environment protection polymer composite has widely in 3D printing
Demand;In the prior art, the raw materials such as poly butylene succinate (PBS), polylactic acid (PLA) and starch have drop well
Solve performance;Therefore, usually by the raw material as degradable environment-friendly material;But the anti-aging property of existing degradable environment-friendly material
It is further improved.
Summary of the invention
The technical problem to be solved by the invention is to provide a kind of Degradable environment protection polymer composite, described can
Degradation environment protection polymer composite has good anti-aging effect.
Above-mentioned technical problem to be solved by this invention, is achieved by the following technical programs:
A kind of Degradable environment protection polymer composite, is made of the raw material comprising following parts by weight:
50~80 parts of poly butylene succinate;40~60 parts of polylactic acid;20~30 parts of starch;Carragheen 10~20
Part;1~5 part of toughener;0.5~2 part of coupling agent;0.5~2 part of antiager.
Preferably, the Degradable environment protection polymer composite, is made of the raw material comprising following parts by weight:
70~80 parts of poly butylene succinate;50~60 parts of polylactic acid;25~30 parts of starch;Carragheen 15~20
Part;1~3 part of toughener;0.5~1 part of coupling agent;0.5~1 part of antiager.
It is further preferred that the Degradable environment protection polymer composite, by the raw material comprising following parts by weight
It is made:
80 parts of poly butylene succinate;50 parts of polylactic acid;25 parts of starch;15 parts of carragheen;3 parts of toughener;It is even
1 part of agent of connection;1 part of antiager.
Preferably, the toughener is selected from MBS toughener.
Preferably, the coupling agent is selected from silane coupling agent KH-540.
Preferably, the antiager is prepared via a method which to obtain:
2,3,3', 4'- bibenzene tetracarboxylic dianhydride is dissolved in organic solvent, 3- amino normal heptane and 4- diformazan is then added
Aminopyridine carries out 1~3h of heating reflux reaction, must precipitate after cooling is static, i.e. the antiager.
It is further preferred that the organic solvent is toluene.
It is further preferred that 2,3,3', 4'- bibenzene tetracarboxylic dianhydride and 3- amino normal heptane and 4-dimethylaminopyridine
Mass ratio is 2.5~3.0:2.0~4.0:0.2~0.3.
It is further preferred that 2,3,3', 4'- bibenzene tetracarboxylic dianhydride and 3- amino normal heptane and 4-dimethylaminopyridine
Mass ratio be 2.9~3.0:2.5~3.0:0.20~0.25.
Most preferably, the quality of 2,3,3', 4'- bibenzene tetracarboxylic dianhydride and 3- amino normal heptane and 4-dimethylaminopyridine
Than for 2.95:2.5:0.25.
Preferably, the amount ratio of 2,3,3', 4'- bibenzene tetracarboxylic dianhydride and organic solvent is 1g:8~15mL.
The preparation method of above-mentioned Degradable environment protection polymer composite, it includes following steps:
Poly butylene succinate, polylactic acid, starch, carragheen, toughener, coupling agent and antiager are first put into height
It is uniformly mixed in fast mixing machine, is then placed in melt blending in double screw extruder and extruding pelletization is up to the degradable ring
Protect polymer composite.
The utility model has the advantages that the present invention provides the Degradable environment protection polymer composites that one kind completely newly forms;The material
Material by poly butylene succinate, polylactic acid, starch etc. there is degradable material to be made, therefore, what the present invention was prepared
Composite material has good degradation;Again due to the Degradable environment protection polymer composite joined toughener and
Antiager, so that the intensity, toughness and anti-aging property of the Degradable environment protection polymer composite are enhanced;More into
One step, present invention employs the antiager that completely new approach is prepared, used the antiager make it is of the present invention can
The anti-aging property of degradation environment protection polymer composite further enhances;The antiager that the completely new approach is prepared is applied to
In Degradable environment protection polymer composite, antiageing effect is better than existing age resister.
Specific embodiment
The present invention is explained further below in conjunction with specific embodiment, but embodiment does not do any type of limit to the present invention
It is fixed.
The preparation of 1 Degradable environment protection polymer composite of embodiment
Parts by weight of raw materials composition: 80 parts of poly butylene succinate;50 parts of polylactic acid;25 parts of starch;Carragheen 15
Part;3 parts of toughener;1 part of coupling agent;1 part of antiager.
The poly butylene succinate selects the poly butylene succinate that the trade mark of German BASF is H1805;
The polylactic acid selects the polylactic acid that the trade mark of U.S. NatureWorks is 3052d;The starch selects cornstarch;
The MBS toughener that the toughener is EM500 with the trade mark of South Korea LG;The coupling agent is selected from silane coupling agent KH-
540;
The antiager is prepared via a method which to obtain: by 2,3,3', 4'- bibenzene tetracarboxylic dianhydride is dissolved in toluene
In, 3- amino normal heptane is then added and 4-dimethylaminopyridine carries out heating reflux reaction 2h, must be precipitated after cooling is static, i.e.,
The antiager;In above-mentioned reaction, 2,3,3', 4'- bibenzene tetracarboxylic dianhydride and 3- amino normal heptane and 4- dimethylamino pyrrole
The mass ratio of pyridine is 2.95:2.5:0.25;The amount ratio of 2,3,3', 4'- bibenzene tetracarboxylic dianhydride and organic solvent is 1g:
10mL。
Preparation method: first by poly butylene succinate, polylactic acid, starch, carragheen, toughener, coupling agent and anti-
Old agent is put into high-speed mixer and is uniformly mixed, and is then placed in melt blending in double screw extruder and extruding pelletization is up to described
Degradable environment protection polymer composite.
The preparation of 2 Degradable environment protection polymer composite of embodiment
Parts by weight of raw materials composition: 50 parts of poly butylene succinate;40 parts of polylactic acid;30 parts of starch;Carragheen 10
Part;3 parts of toughener;1 part of coupling agent;1 part of antiager.
The poly butylene succinate selects the poly butylene succinate that the trade mark of German BASF is H1805;
The polylactic acid selects the polylactic acid that the trade mark of U.S. NatureWorks is 3052d;The starch selects cornstarch;
The MBS toughener that the toughener is EM500 with the trade mark of South Korea LG;The coupling agent is selected from silane coupling agent KH-
540;
The antiager is prepared via a method which to obtain: by 2,3,3', 4'- bibenzene tetracarboxylic dianhydride is dissolved in toluene
In, 3- amino normal heptane is then added and 4-dimethylaminopyridine carries out heating reflux reaction 2h, must be precipitated after cooling is static, i.e.,
The antiager;In above-mentioned reaction, 2,3,3', 4'- bibenzene tetracarboxylic dianhydride and 3- amino normal heptane and 4- dimethylamino pyrrole
The mass ratio of pyridine is 2.5:3.0:0.2;The amount ratio of 2,3,3', 4'- bibenzene tetracarboxylic dianhydride and organic solvent is 1g:8mL.
Preparation method: first by poly butylene succinate, polylactic acid, starch, carragheen, toughener, coupling agent and anti-
Old agent is put into high-speed mixer and is uniformly mixed, and is then placed in melt blending in double screw extruder and extruding pelletization is up to described
Degradable environment protection polymer composite.
The preparation of 3 Degradable environment protection polymer composite of embodiment
Parts by weight of raw materials composition: 80 parts of poly butylene succinate;60 parts of polylactic acid;20 parts of starch;Carragheen 20
Part;5 parts of toughener;2 parts of coupling agent;2 parts of antiager.
The poly butylene succinate selects the poly butylene succinate that the trade mark of German BASF is H1805;
The polylactic acid selects the polylactic acid that the trade mark of U.S. NatureWorks is 3052d;The starch selects cornstarch;
The MBS toughener that the toughener is EM500 with the trade mark of South Korea LG;The coupling agent is selected from silane coupling agent KH-
540;
The antiager is prepared via a method which to obtain: by 2,3,3', 4'- bibenzene tetracarboxylic dianhydride is dissolved in toluene
In, 3- amino normal heptane is then added and 4-dimethylaminopyridine carries out heating reflux reaction 2h, must be precipitated after cooling is static, i.e.,
The antiager;In above-mentioned reaction, 2,3,3', 4'- bibenzene tetracarboxylic dianhydride and 3- amino normal heptane and 4- dimethylamino pyrrole
The mass ratio of pyridine is 3.0:4.0:0.3;The amount ratio of 2,3,3', 4'- bibenzene tetracarboxylic dianhydride and organic solvent is 1g:15mL.
Preparation method: first by poly butylene succinate, polylactic acid, starch, carragheen, toughener, coupling agent and anti-
Old agent is put into high-speed mixer and is uniformly mixed, and is then placed in melt blending in double screw extruder and extruding pelletization is up to described
Degradable environment protection polymer composite.
The preparation of 1 Degradable environment protection polymer composite of comparative example
Parts by weight of raw materials composition: 80 parts of poly butylene succinate;50 parts of polylactic acid;25 parts of starch;Carragheen 15
Part;3 parts of toughener;1 part of coupling agent.
The poly butylene succinate selects the poly butylene succinate that the trade mark of German BASF is H1805;
The polylactic acid selects the polylactic acid that the trade mark of U.S. NatureWorks is 3052d;The starch selects cornstarch;
The MBS toughener that the toughener is EM500 with the trade mark of South Korea LG;The coupling agent is selected from silane coupling agent KH-
540;
Preparation method: first poly butylene succinate, polylactic acid, starch, carragheen, toughener and coupling agent are put into
It is uniformly mixed in high-speed mixer, is then placed in melt blending in double screw extruder and extruding pelletization up to described degradable
Environmental protection macromolecule composite material.
Comparative example 1 the difference from embodiment 1 is that, be added without antiager in comparative example 1.
The preparation of 2 Degradable environment protection polymer composite of comparative example
Parts by weight of raw materials composition: 80 parts of poly butylene succinate;50 parts of polylactic acid;25 parts of starch;Carragheen 15
Part;3 parts of toughener;1 part of coupling agent;1 part of antiager.
The poly butylene succinate selects the poly butylene succinate that the trade mark of German BASF is H1805;
The polylactic acid selects the polylactic acid that the trade mark of U.S. NatureWorks is 3052d;The starch selects cornstarch;
The MBS toughener that the toughener is EM500 with the trade mark of South Korea LG;The coupling agent is selected from silane coupling agent KH-
540;The antiager is selected from conventional antioxidant 300, chemical name are as follows: 4,4'- thiobis (6- tert-butyl -3- methylbenzene
Phenol);
Preparation method: first by poly butylene succinate, polylactic acid, starch, carragheen, toughener, coupling agent and anti-
Old agent is put into high-speed mixer and is uniformly mixed, and is then placed in melt blending in double screw extruder and extruding pelletization is up to described
Degradable environment protection polymer composite.
Comparative example 2 difference from example 1 is that, antiager in comparative example 2 using conventional antioxidant 300,
And embodiment 1 is using the antiager being prepared by the method for the invention.
The preparation of 3 Degradable environment protection polymer composite of comparative example
Parts by weight of raw materials composition: 80 parts of poly butylene succinate;50 parts of polylactic acid;25 parts of starch;Carragheen 15
Part;3 parts of toughener;1 part of coupling agent;1 part of antiager.
The poly butylene succinate selects the poly butylene succinate that the trade mark of German BASF is H1805;
The polylactic acid selects the polylactic acid that the trade mark of U.S. NatureWorks is 3052d;The starch selects cornstarch;
The MBS toughener that the toughener is EM500 with the trade mark of South Korea LG;The coupling agent is selected from silane coupling agent KH-
540;The antiager is selected from conventional irgasfos 168, chemical name are as follows: three [2.4- di-tert-butyl-phenyl] phosphite esters;
Preparation method: first by poly butylene succinate, polylactic acid, starch, carragheen, toughener, coupling agent and anti-
Old agent is put into high-speed mixer and is uniformly mixed, and is then placed in melt blending in double screw extruder and extruding pelletization is up to described
Degradable environment protection polymer composite.
Comparative example 3 difference from example 1 is that, antiager in comparative example 3 using conventional irgasfos 168,
And embodiment 1 is using the antiager being prepared by the method for the invention.
Experimental example
The Degradable environment protection polymer composite that Examples 1 to 3 and comparative example 1~3 are prepared is made a length of
10cm, width 5cm, with a thickness of the thin sample of 2.0mm, thin sample is put into gravity pair by reference standard GB/T7141-200
In streaming heat aging test chamber, artificial addition aging 1000h is carried out at 100 DEG C;Test Degradable environment protection macromolecule composite wood
Expect tensile strength (tensile strength referring to ASTM D638 standard method test) before and after artificial accelerated aging, cantilever beam notch
Impact strength (Izod notched impact strength is tested referring to ASTM D256 standard method).And tensile strength calculated conservation rate and
Impact strength conservation rate;
The tensile strength before tensile strength/artificial accelerated aging after stretching strength retentivity=artificial accelerated aging ×
100%;
It is outstanding before Izod notched impact strength/artificial accelerated aging after impact strength conservation rate=artificial accelerated aging
Arm beam notch impact strength × 100%;
Before and after artificially roughening, if stretching strength retentivity and impact strength conservation rate closer to 100%,
Then illustrate that Degradable environment protection polymer composite is got over through the change rate of artificial accelerated aging post-tensioning intensity and impact strength
It is small, influenced by thermo-oxidative ageing smaller, the ageing resistance of material is stronger, and test result is shown in Table 1.
The thermal ageing test result of 1. Degradable environment protection polymer composite of table
Experimental material | Stretching strength retentivity (%) | Impact strength conservation rate (%) |
1 composite material of embodiment | 96.2 | 104.4 |
2 composite material of embodiment | 97.1 | 108.2 |
3 composite material of embodiment | 95.5 | 103.2 |
1 composite material of comparative example | 28.7 | 266.9 |
2 composite material of comparative example | 65.3 | 159.8 |
3 composite material of comparative example | 61.2 | 168.1 |
The Degradable environment protection polymer composite that Examples 1 to 3 is prepared it can be seen from 1 experimental data of table its
Stretching strength retentivity is between 90%~100%, and impact strength conservation rate is between 100~110%;It is through artificial acceleration
The change rate of tensile strength and impact strength after senile experiment controls within 10%;This explanation joined system of the present invention
The Degradable environment protection polymer composite being prepared after standby obtained antiager has excellent thermo oxidative aging effect, material
The mechanical property of material is influenced very little by thermal oxide, and performance is stablized.
It can be seen that after artificially roughening from 1 experimental data of comparative example, stretching strength retentivity is
28.7%, impact strength conservation rate is 266.9%, and the change rate of tensile strength and impact strength is big, this illustrates comparative example 1 not
It is poor that its thermo oxidative aging of Degradable environment protection polymer composite effect that antioxidant is prepared is added, by thermal oxide
Afterwards, very greatly, performance is unstable for the mechanical property variation of material.
It can be seen that after artificially roughening from the experimental data of comparative example 2 and 3, stretching strength retentivity point
Not Wei 65.3% and 61.2%, impact strength conservation rate is respectively 159.8% and 168.1%;This says the conventional antiager system of addition
The change rate ratio of standby obtained Degradable environment protection polymer composite, tensile strength and impact strength is added without antioxidant
The Degradable environment protection polymer composite being prepared further decreases, but the degradable ring being prepared with Examples 1 to 3
It protects polymer composite to compare, change rate is still higher.This illustrates conventional antiager, although can improve degradable
The thermo oxidative aging of environmental protection macromolecule composite material acts on, but compared with the antiager that the method for the present invention is prepared, right
The raising degree of the thermo oxidative aging effect of Degradable environment protection polymer composite is much prepared not as good as the method for the present invention
Antiager.
Claims (10)
1. a kind of Degradable environment protection polymer composite, which is characterized in that be made of the raw material comprising following parts by weight:
50~80 parts of poly butylene succinate;40~60 parts of polylactic acid;20~30 parts of starch;10~20 parts of carragheen;Toughening
1~5 part of agent;0.5~2 part of coupling agent;0.5~2 part of antiager.
2. Degradable environment protection polymer composite according to claim 1, which is characterized in that by including following parts by weight
Raw material be made:
70~80 parts of poly butylene succinate;50~60 parts of polylactic acid;25~30 parts of starch;15~20 parts of carragheen;Toughening
1~3 part of agent;0.5~1 part of coupling agent;0.5~1 part of antiager.
3. Degradable environment protection polymer composite according to claim 1, which is characterized in that by including following parts by weight
Raw material be made:
80 parts of poly butylene succinate;50 parts of polylactic acid;25 parts of starch;15 parts of carragheen;3 parts of toughener;1 part of coupling agent;
1 part of antiager.
4. Degradable environment protection polymer composite according to claim 1, which is characterized in that the toughener is selected from
MBS toughener.
5. Degradable environment protection polymer composite according to claim 1, which is characterized in that the coupling agent is selected from
Silane coupling agent KH-540.
6. Degradable environment protection polymer composite according to claim 1, which is characterized in that the antiager passes through
Following method is prepared:
2,3,3', 4'- bibenzene tetracarboxylic dianhydride is dissolved in organic solvent, 3- amino normal heptane and 4- dimethylamino is then added
Pyridine carries out 1~3h of heating reflux reaction, must precipitate after cooling is static, i.e. the antiager.
7. Degradable environment protection polymer composite according to claim 6, which is characterized in that the organic solvent is
Toluene.
8. Degradable environment protection polymer composite according to claim 6, which is characterized in that 2,3,3', 4'- biphenyl four
Formic acid dianhydride and 3- amino normal heptane and the mass ratio of 4-dimethylaminopyridine are 2.5~3.0:2.0~4.0:0.2~0.3;It is excellent
The mass ratio of selection of land, 2,3,3', 4'- bibenzene tetracarboxylic dianhydride and 3- amino normal heptane and 4-dimethylaminopyridine is 2.9~
3.0:2.5~3.0:0.20~0.25;Most preferably, 2,3,3', 4'- bibenzene tetracarboxylic dianhydride and 3- amino normal heptane and 4- bis-
The mass ratio of methylamino pyridine is 2.95:2.5:0.25.
9. Degradable environment protection polymer composite according to claim 6, which is characterized in that 2,3,3', 4'- biphenyl four
The amount ratio of formic acid dianhydride and organic solvent is 1g:8~15mL.
10. the preparation method of Degradable environment protection polymer composite according to any one of claims 1 to 9, which is characterized in that
It comprises the following steps:
It is mixed that poly butylene succinate, polylactic acid, starch, carragheen, toughener, coupling agent and antiager are first put into high speed
It is uniformly mixed in conjunction machine, is then placed in melt blending in double screw extruder and extruding pelletization is high up to the Degradable environment protection
Molecular composite material.
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CN112029245A (en) * | 2020-09-18 | 2020-12-04 | 广州市芮奇塑胶有限公司 | Degradable plastic fastener and preparation method thereof |
CN112662153A (en) * | 2020-12-23 | 2021-04-16 | 广州赢盛塑料制品有限公司 | Environment-friendly degradable packaging bottle and preparation method thereof |
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CN105670248A (en) * | 2014-12-04 | 2016-06-15 | 河南青源天仁生物技术有限公司 | Full-degradable seedling breeding plate with PLA/PBS as base material and preparation method thereof |
KR20170080998A (en) * | 2015-12-31 | 2017-07-11 | 주식회사 휴비스 | Masterbatch composition, and preparation method of polyester resin foam using the same |
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CN105017731A (en) * | 2014-11-26 | 2015-11-04 | 江苏天仁生物材料有限公司 | Fully biodegradable material taking polylactic acid/polybuthylenesuccinate as basic material and preparation method of fully biodegradable material |
CN105670248A (en) * | 2014-12-04 | 2016-06-15 | 河南青源天仁生物技术有限公司 | Full-degradable seedling breeding plate with PLA/PBS as base material and preparation method thereof |
KR20170080998A (en) * | 2015-12-31 | 2017-07-11 | 주식회사 휴비스 | Masterbatch composition, and preparation method of polyester resin foam using the same |
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Publication number | Priority date | Publication date | Assignee | Title |
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CN112029245A (en) * | 2020-09-18 | 2020-12-04 | 广州市芮奇塑胶有限公司 | Degradable plastic fastener and preparation method thereof |
CN112662153A (en) * | 2020-12-23 | 2021-04-16 | 广州赢盛塑料制品有限公司 | Environment-friendly degradable packaging bottle and preparation method thereof |
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