CN115466491A - High-modulus degradable PBAT/PLA compound and preparation method thereof - Google Patents
High-modulus degradable PBAT/PLA compound and preparation method thereof Download PDFInfo
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Abstract
The invention discloses a high-modulus degradable PBAT/PLA compound, which is mainly prepared by copolymerizing PBAT, PLA and a needle-shaped or sheet-shaped inorganic filler with an epoxy group, wherein the needle-shaped or sheet-shaped inorganic filler with the epoxy group is modified by an epoxy silane coupling agent. The PBAT/PLA compound is reinforced by the in-situ compatibilization of the needle-shaped or flake-shaped inorganic filler with the epoxy functional group. The epoxide group on the surface of the acicular or flaky filler reacts with hydroxyl/carboxyl at the chain end of PBAT and PLA to form a chemical bond, and a block copolymer of PBAT and PLA is generated in situ, so that the molecular weight of the polymer in the system is effectively increased, the compatibility of PBAT/PLA is improved, the interfacial adhesion of PBAT/filler and PLA/filler is enhanced, and the high-modulus degradable PBAT/PLA compound is obtained.
Description
Technical Field
The invention relates to the field of high polymer materials, in particular to a high-modulus degradable PBAT/PLA compound.
Background
There is considerable interest in natural, biological and synthetic polymers that are renewable resources in reducing the prospects of world petroleum resources and limiting the contribution of plastics to waste treatment. Since the policy of global plastic limit and plastic prohibition is continuously released in 2020, the price of PBAT has risen to 2.4-2.6 ten thousand yuan/ton from 2-2.2 ten thousand yuan/ton, and the price of polylactic acid PLA has risen to 3.5 ten thousand yuan/ton.
The polybutylene adipate terephthalate PBAT has the characteristics of both the polybutylene adipate and the polybutylene terephthalate, has better ductility, heat resistance and impact property, and also has excellent biodegradability. Furthermore, PBAT is more affordable than PLA. However, PBAT has a low modulus and is easily deformed when color register printing is performed, and therefore, it is necessary to increase the tensile modulus while reducing the cost. Polylactic acid is a completely biodegradable polymer material, has good thermal stability, can be processed in various ways, such as biaxial stretching and injection blow molding, has high modulus, and is suitable for chromatography printing. The disadvantages are high price and lack of market competitiveness. In consideration of economic benefits, the invention finds a method for blending and compatibilizing high-modulus PLA and PBAT, thereby not only reducing the cost, but also improving the tensile modulus of the compound.
Disclosure of Invention
The invention overcomes the defects of the prior art, fully exerts the function of raw materials, improves the tensile modulus of the compound by using the needle-shaped or sheet-shaped filler with the epoxy functional group, enhances the degradable PBAT/PLA compound by in-situ compatibilization, reduces the cost and improves the economic benefit.
The invention provides a high-modulus degradable PBAT/PLA compound, which is mainly prepared by copolymerizing PBAT, PLA and a needle-shaped or sheet-shaped inorganic filler with epoxy groups according to a certain proportion. The acicular or flaky inorganic filler with epoxy groups is an acicular or flaky inorganic filler modified by a coupling agent, the acicular or flaky inorganic filler comprises but is not limited to at least one of talcum powder (flaky), graphite (flaky), cellulose (acicular), wollastonite (acicular), calcium sulfate whiskers (acicular) and the like, and the inorganic filler is generally ground into powder when in use. The coupling agent is an epoxy silane coupling agent including but not limited to gamma- (2,3-glycidoxy) propyltrimethoxysilane (KH 560). Wherein, the dosage of PBAT is 61-72 wt%, the dosage of PLA is 15-18 wt%, and the dosage of the needle-shaped or flake-shaped inorganic filler with epoxy functional groups is 11-24 wt% based on the total weight of the compound.
The invention also provides a preparation method of the PBAT/PLA compound, which comprises the steps of preparing the needle-shaped or sheet-shaped inorganic filler with the epoxy group and preparing the PBAT/PLA compound by extruding in a double-screw extruder.
In the above preparation method, preferably, the preparation of the needle-like or sheet-like inorganic filler with epoxy groups comprises: preparing coupling agent into hydrolysate, adding needle-shaped or flake-shaped inorganic filler into the hydrolysate, and carrying out surface treatment to obtain the needle-shaped or flake-shaped inorganic filler with 1-3% of epoxy groups, wherein the dosage of the coupling agent is 1-3 parts by weight based on 100 parts by weight of the needle-shaped or flake-shaped inorganic filler.
In the above preparation method, preferably, the step of preparing the coupling agent into a hydrolysate is to mix the coupling agent solution, anhydrous ethanol and water according to a mass ratio of 4:3:1, pouring the mixture into a beaker, pouring the beaker into the beaker, and putting the beaker into a circulating water bath kettle for stirring and hydrolyzing.
In the above preparation method, preferably, the extruding preparation of the PBAT/PLA composite in the twin-screw extruder means that PLA, PBAT, and a needle-shaped and sheet-shaped inorganic filler with epoxy groups are uniformly stirred and put into a co-rotating twin-screw extruder for extrusion, and the length-diameter ratio of the twin-screw extruder is 30-50:1; the temperature of a first zone of the co-rotating double-screw extruder is 156-163 ℃, the temperature of a second zone is 163-166 ℃, the temperature of a third zone is 164-168 ℃, the temperature of a fourth zone is 164-168 ℃, the temperature of a fifth zone is 164-168 ℃, the temperature of a sixth zone is 164-168 ℃, the temperature of a machine head is 164-168 ℃, and the temperature of a melt is 156-163 ℃; the rotating speed of the screw is 300-500r/min. More preferably, the twin-screw extruder has a length to diameter ratio of 40:1; the temperature of a first zone of the co-rotating double-screw extruder is 160 ℃, the temperature of a second zone is 165 ℃, the temperature of a third zone is 165 ℃, the temperature of a fourth zone is 165 ℃, the temperature of a fifth zone is 165 ℃, the temperature of a sixth zone is 165 ℃, the temperature of a machine head is 165 ℃, and the temperature of a melt is 160 ℃; the screw rotation speed is 400r/min.
In the preparation method, preferably, during preparation, the raw materials are respectively weighed according to the specified weight parts and put into an oven, wherein the needle-shaped and sheet-shaped inorganic filler with epoxy groups is dried for 2-4h at 95-105 ℃, PBAT is dried for 2-4h at 95-105 ℃, and PLA is dried for 2-4h at 140-1600 ℃.
In the preparation method, preferably, the melt index of the PLA is 5-8g/10min; the PBAT melt index is 2-5g/10min.
The invention uses the needle-shaped or flake-shaped inorganic filler with the epoxy functional group to improve the tensile modulus of the compound, and the in-situ compatibilization enhances the PBAT/PLA compound. The epoxide group on the surface of the acicular or flaky filler reacts with hydroxyl/carboxyl at the chain ends of PBAT and PLA to form a chemical bond, and a block copolymer of PBAT and PLA is generated in situ, so that the molecular weight of the polymer in the system is effectively increased, the compatibility between PBAT and PLA is improved, and the interfacial adhesion between PBAT/filler and PLA/filler is enhanced. Strengthening by needle-shaped or sheet-shaped filler, in-situ compatibilization of PBAT/PLA, in-situ enhancement of the adhesive force of a polymer/filler interface, and introducing high-modulus PLA to obtain the high-modulus degradable PBAT/PLA compound.
Detailed Description
The following examples are further illustrative of the present invention as to the technical content of the present invention, but the essence of the present invention is not limited to the following examples, and one of ordinary skill in the art can and should understand that any simple changes or substitutions based on the essence of the present invention should fall within the protection scope of the present invention.
In the following examples, PLA: natureWorks7001D, USA, the melt index is 6g/10min; PBAT is THJS-6801 of TUN river in blue mountain of Xinjiang with a melt index of 2-5g/10min; the modified talcum powder contains talcum powder and a modifier, wherein the modifier is an epoxy coupling agent, specifically KH560 containing epoxy functional groups, and the content of the modifier is 1-3 parts by weight based on 100 parts by weight of talcum powder.
Example 1
A high-modulus degradable PBAT/PLA compound is mainly prepared from the following raw materials in parts by weight:
KH560 0.40kg, absolute ethanol 0.30kg, water 0.10kg, talc 40kg, PBAT 0.8kg, PLA 0.2kg.
1 percent of KH560-talcum powder modifier comprises the following steps:
(1) Pouring 0,40kgKH560 solution, 0.30kg absolute ethyl alcohol and 0.10kg water into a beaker, putting the beaker into a circulating water bath, stirring and hydrolyzing for 30 minutes at 30 ℃, thus obtaining KH560 hydrolysate;
(2) Weighing 40kg of talcum powder, pouring the talcum powder into a high-speed stirrer at 100 ℃ and 1000rpm/min, and pouring the KH560 hydrolysate into the high-speed stirrer for three times, wherein the interval between the first time and the second time is 5min, and the interval between the second time and the third time is 15min, so that the KH 560-talcum powder modifier with the content of 1 percent can be prepared.
A preparation method of a high-modulus degradable PBAT/PLA compound comprises the following steps:
s1, weighing 1 percent of KH560-talcum powder 0.12kg, PBAT 0.8kg and PLA 0.2kg;
s2, putting PLA, PBAT,1 percent of KH560-talcum powder modifier into an oven, wherein 1 percent of KH560-talcum powder is dried at 100 ℃ for 3h, PBAT is dried at 100 ℃ for 3h, and PLA is dried at 150 ℃ for 3h.
S3, uniformly stirring the dried PLA, PBAT,1 percent KH560-talcum powder, putting the mixture into a co-rotating double-screw extruder for extrusion, wherein the length-diameter ratio of the double-screw extruder is 40:1; the temperature of a first zone of the co-rotating double-screw extruder is 160 ℃, the temperature of a second zone is 165 ℃, the temperature of a third zone is 165 ℃, the temperature of a fourth zone is 165 ℃, the temperature of a fifth zone is 165 ℃, the temperature of a sixth zone is 165 ℃, the temperature of a machine head is 165 ℃ and the temperature of a melt is 160 ℃; the screw rotation speed is 400r/min. And (4) cooling the extrudate obtained in the step S3, and crushing the extrudate into particles with the diameter of about 20-30mm in a crusher. And pouring the crushed particles into an injection molding machine for injection molding, wherein the processing temperature is set to be 160-170 ℃, and the injection molding pressure is 45Bar.
Comparative example 1
The difference compared to example 1 is that the inorganic filler is selected from irregularly spherical silica.
Example 2
A high-modulus degradable PBAT/PLA compound mainly comprises the following raw materials in parts by weight:
KH560 0.40kg, absolute ethanol 0.30kg, water 0.10kg, talc 40kg, PBAT 0.8kg, PLA 0.2kg.
1 percent of KH560-talcum powder modifier comprises the following steps:
(1) Pouring 0,40kgKH560 solution, 0.30kg absolute ethyl alcohol and 0.10kg water into a beaker, putting the beaker into a circulating water bath, stirring and hydrolyzing for 30 minutes at 30 ℃, thus obtaining KH560 hydrolysate;
(2) Weighing 40kg of talcum powder, pouring the talcum powder into a high-speed stirrer at 100 ℃ and 1000rpm/min, and pouring the KH560 hydrolysate into the high-speed stirrer for three times, wherein the interval between the first time and the second time is 5min, and the interval between the second time and the third time is 15min, so that the KH 560-talcum powder modifier with the content of 1 percent can be prepared.
A preparation method of a high-modulus degradable PBAT/PLA compound comprises the following steps:
s1, weighing 1 percent of KH560-talcum powder 0.18kg, PBAT 0.8kg and PLA 0.2kg;
s2, placing PLA, PBAT,1% KH560-talc modifier in an oven, wherein 1% KH560-talc is dried at 100 ℃ for 3h, PBAT at 100 ℃ for 3h, PLA at 150 ℃ for 3h.
S3, uniformly stirring the dried PLA, PBAT,1 percent KH560-talcum powder, putting the mixture into a co-rotating double-screw extruder for extrusion, wherein the length-diameter ratio of the double-screw extruder is 40:1; the temperature of a first zone of the co-rotating double-screw extruder is 160 ℃, the temperature of a second zone is 165 ℃, the temperature of a third zone is 165 ℃, the temperature of a fourth zone is 165 ℃, the temperature of a fifth zone is 165 ℃, the temperature of a sixth zone is 165 ℃, the temperature of a machine head is 165 ℃ and the temperature of a melt is 160 ℃; the screw rotation speed is 400r/min.
And (3) cooling the extrudate obtained in the step S3, and then putting the extrudate into a crusher to be crushed into particles with the diameter of about 20-30 mm.
Pouring the crushed particles into an injection molding machine for injection molding, wherein the processing temperature is set to be 160-170 ℃, and the injection molding pressure is 45Bar.
Comparative example 2
The difference compared to example 2 is that the inorganic filler is selected from irregularly spherical silica.
Example 3
A high-modulus degradable PBAT/PLA compound mainly comprises the following raw materials in parts by weight:
KH560 0.40kg, absolute ethanol 0.30kg, water 0.10kg, talcum powder 40kg, PBAT 0.8kg, PLA 0.2kg.
1 percent of KH560-talcum powder modifier comprises the following steps:
(1) Pouring 0,40kg of KH560 solution, 0.30kg of absolute ethyl alcohol and 0.10kg of water into a beaker, putting the beaker into a circulating water bath, stirring and hydrolyzing for 30 minutes at 30 ℃, thus obtaining KH560 hydrolysate;
(2) Weighing 40kg of talcum powder, pouring the talcum powder into a high-speed stirrer at 100 ℃ and 1000rpm/min, and pouring the KH560 hydrolysate into the high-speed stirrer for three times, wherein the interval between the first time and the second time is 5min, and the interval between the second time and the third time is 15min, so that the KH 560-talcum powder modifier with the content of 1 percent can be prepared.
A preparation method of a high-modulus degradable PBAT/PLA compound comprises the following steps:
s1, weighing 1 percent of KH560-talcum powder 0.24kg, PBAT 0.8kg and PLA 0.2kg;
s2, putting PLA, PBAT,1 percent of KH560-talcum powder modifier into an oven, wherein 1 percent of KH560-talcum powder is dried at 100 ℃ for 3h, PBAT is dried at 100 ℃ for 3h, and PLA is dried at 150 ℃ for 3h.
S3, uniformly stirring the dried PLA, PBAT,1 percent KH560-talcum powder, putting the mixture into a co-rotating double-screw extruder for extrusion, wherein the length-diameter ratio of the double-screw extruder is 40:1; the temperature of a first zone of the co-rotating double-screw extruder is 160 ℃, the temperature of a second zone is 165 ℃, the temperature of a third zone is 165 ℃, the temperature of a fourth zone is 165 ℃, the temperature of a fifth zone is 165 ℃, the temperature of a sixth zone is 165 ℃, the temperature of a machine head is 165 ℃ and the temperature of a melt is 160 ℃; the screw rotation speed is 400r/min.
And (4) cooling the extrudate obtained in the step S3, and crushing the extrudate into particles with the diameter of about 20-30mm in a crusher.
Pouring the crushed particles into an injection molding machine for injection molding, wherein the processing temperature is set to be 160-170 ℃, and the injection molding pressure is 45Bar.
Comparative example 3
Example 3 is compared with the difference that the inorganic filler is selected from irregularly spherical silica.
Example 4
A high-modulus degradable PBAT/PLA compound mainly comprises the following raw materials in parts by weight:
KH560 0.40kg, absolute ethanol 0.30kg, water 0.10kg, talcum powder 40kg, PBAT 0.8kg, PLA 0.2kg.
1 percent of KH560-talcum powder modifier comprises the following steps:
(1) Pouring 0,40kgKH560 solution, 0.30kg absolute ethyl alcohol and 0.10kg water into a beaker, putting the beaker into a circulating water bath, stirring and hydrolyzing for 30 minutes at 30 ℃, thus obtaining KH560 hydrolysate;
(2) Weighing 40kg of talcum powder, pouring the talcum powder into a high-speed stirrer at 100 ℃ and 1000rpm/min, and pouring the KH560 hydrolysate into the high-speed stirrer for three times, wherein the interval between the first time and the second time is 5min, and the interval between the second time and the third time is 15min, so that the KH 560-talcum powder modifier with the content of 1 percent can be prepared.
A preparation method of a high-modulus degradable PBAT/PLA compound comprises the following steps:
s1, weighing 1 percent of KH560-talcum powder 0.30kg, PBAT 0.8kg and PLA 0.2kg;
s2, putting PLA, PBAT,1 percent of KH560-talcum powder modifier into an oven, wherein 1 percent of KH560-talcum powder is dried at 100 ℃ for 3h, PBAT is dried at 100 ℃ for 3h, and PLA is dried at 150 ℃ for 3h.
S3, uniformly stirring the dried PLA, PBAT,1 percent KH560-talcum powder, putting the mixture into a co-rotating double-screw extruder for extrusion, wherein the length-diameter ratio of the double-screw extruder is 40:1; the temperature of a first zone of the co-rotating double-screw extruder is 160 ℃, the temperature of a second zone is 165 ℃, the temperature of a third zone is 165 ℃, the temperature of a fourth zone is 165 ℃, the temperature of a fifth zone is 165 ℃, the temperature of a sixth zone is 165 ℃, the temperature of a machine head is 165 ℃, and the temperature of a melt is 160 ℃; the screw rotation speed is 400r/min.
And (3) cooling the extrudate obtained in the step S3, and then putting the extrudate into a crusher to be crushed into particles with the diameter of about 20-30 mm.
Pouring the crushed particles into an injection molding machine for injection molding, wherein the processing temperature is set to be 160-170 ℃, and the injection molding pressure is 45Bar.
Comparative example 4
The difference compared to example 4 is that the inorganic filler is selected from irregularly spherical silica.
Comparative example 5
The difference compared with example 4 is that the coupling agent used is KH550 which does not contain epoxy groups.
Comparative example 6
The difference compared to example 4 is that the coupling agent used is KH570 without epoxy groups.
Example 5
Compared with example 4, the difference is that the inorganic filler is selected from wollastonite powder.
Example 6
Compared with the example 4, the difference is that the inorganic filler is calcium sulfate whisker powder.
Example 7
Compared with example 4, the difference is that the inorganic filler is graphite powder.
COMPARATIVE EXAMPLE 7 (preparation of PBAT directly without addition of inorganic Filler)
Putting the PBAT into an oven, drying for 3h at 100 ℃, and then putting the dried PBAT into a co-rotating twin-screw extruder for extrusion, wherein the length-diameter ratio of the twin-screw extruder is 40:1; the temperature of a first zone of the co-rotating double-screw extruder is 160 ℃, the temperature of a second zone is 165 ℃, the temperature of a third zone is 165 ℃, the temperature of a fourth zone is 165 ℃, the temperature of a fifth zone is 165 ℃, the temperature of a sixth zone is 165 ℃, the temperature of a machine head is 165 ℃, and the temperature of a melt is 160 ℃; the screw rotation speed is 400r/min. Cooling the extrudate, and crushing the extrudate into particles with the diameter of about 20-30mm in a crusher. Pouring the crushed particles into an injection molding machine for injection molding, wherein the processing temperature is set to be 160-170 ℃, and the injection molding pressure is 45Bar.
COMPARATIVE EXAMPLE 8 preparation of PBAT/PLA Compound without addition of inorganic Filler
Drying PBAT at 100 ℃ for 3h, drying PLA at 150 ℃ for 3h, and drying PBAT and PLA in the proportion of 80:20, putting the mixture into a co-rotating twin-screw extruder for extrusion, wherein the length-diameter ratio of the twin-screw extruder is 40:1; the temperature of a first zone of the co-rotating double-screw extruder is 160 ℃, the temperature of a second zone is 165 ℃, the temperature of a third zone is 165 ℃, the temperature of a fourth zone is 165 ℃, the temperature of a fifth zone is 165 ℃, the temperature of a sixth zone is 165 ℃, the temperature of a machine head is 165 ℃, and the temperature of a melt is 160 ℃; the screw rotation speed is 400r/min. Cooling the extrudate, and crushing the extrudate into granules with the diameter of about 20-30mm in a crusher. And pouring the crushed particles into an injection molding machine for injection molding, wherein the processing temperature is set to be 160-170 ℃, and the injection molding pressure is 45Bar.
The final products obtained in examples 1 to 7 and comparative examples 1 to 8 were subjected to the performance test, the test results of which are shown in Table 1:
TABLE 1
Item | Example 1 | Example 2 | Example 3 | Example 4 | Example 5 |
Tensile modulus (Mpa) | 110 | 116.4 | 120 | 152 | 141 |
Item | Comparative example 1 | Comparative example 2 | Comparative example 3 | Comparative example 4 | Example 6 |
Tensile modulus (Mpa) | 101.7 | 101.5 | 102.4 | 100.7 | 123 |
Item | Comparative example 5 | Comparative example 6 | Comparative example 7 | Comparative example 8 | Example 7 |
Tensile modulus (Mpa) | 76.7 | 82.4 | 62.4 | 90.1 | 134 |
The above examples and comparative studies show that: the multifunctional epoxy grafted acicular or flaky filler can increase the tensile modulus of the PBAT/PLA compound, thereby increasing the rigidity of the compound and making the compound more suitable for the application of complicated technical scenes such as chromatography printing.
It should be noted that the technical contents described above are only explained and illustrated to enable those skilled in the art to know the technical spirit of the present invention, and therefore, the technical contents are not to limit the scope of the present invention. The scope of the invention is defined by the appended claims. It should be understood by those skilled in the art that any modification, equivalent replacement, and improvement made based on the spirit of the present invention should be considered to be within the spirit and scope of the present invention.
Claims (10)
1. A high-modulus degradable PBAT/PLA compound is mainly prepared by copolymerizing PBAT, PLA and a needle-shaped or sheet-shaped inorganic filler with an epoxy group according to a certain proportion; the needle-shaped or sheet-shaped inorganic filler with the epoxy group is a needle-shaped or sheet-shaped inorganic filler modified by a coupling agent, the needle-shaped or sheet-shaped inorganic filler comprises at least one of talcum powder, graphite, cellulose, wollastonite and calcium sulfate whisker, and the coupling agent is an epoxy silane coupling agent.
2. The PBAT/PLA composite of claim 1, wherein the PBAT is present in an amount of 61-72 wt%, the PLA is present in an amount of 15-18 wt%, and the acicular or platy inorganic filler with epoxy groups is present in an amount of 11-24 wt%, based on the total weight of the composite.
3. A method of preparing the PBAT/PLA composite of claim 1 or 2, comprising the preparation of a needle-like or plate-like inorganic filler with epoxy groups, extrusion in a twin screw extruder to prepare the PBAT/PLA composite.
4. The method according to claim 3, wherein the preparation of the acicular or tabular inorganic filler having an epoxy group comprises: preparing coupling agent into hydrolysate, adding needle-shaped or sheet-shaped inorganic filler, and performing surface treatment.
5. The method of claim 4, wherein the coupling agent is used in an amount of 1 to 3 parts by weight, based on 100 parts by weight of the acicular or platy inorganic filler.
6. The method according to claim 4, wherein the coupling agent is prepared as a hydrolysate by mixing the coupling agent, absolute ethanol and water in a weight ratio of 4:3:1, pouring the mixture into a beaker, pouring the beaker into the beaker, and putting the beaker into a circulating water bath kettle for stirring and hydrolyzing.
7. The preparation method of claim 3, wherein the extruding preparation of PBAT/PLA composite in the twin-screw extruder is that PLA, PBAT, needle-shaped or flake-shaped inorganic filler with epoxy groups are stirred uniformly and put into a co-rotating twin-screw extruder for extruding, and the length-diameter ratio of the twin-screw extruder is 30-50:1; the temperature of a first zone of the co-rotating double-screw extruder is 156-163 ℃, the temperature of a second zone is 163-166 ℃, the temperature of a third zone is 164-168 ℃, the temperature of a fourth zone is 164-168 ℃, the temperature of a fifth zone is 164-168 ℃, the temperature of a sixth zone is 164-168 ℃, the temperature of a machine head is 164-168 ℃, and the temperature of a melt is 156-163 ℃; the rotating speed of the screw is 300-500r/min.
8. The method of claim 7, wherein the twin screw extruder has a length to diameter ratio of 40:1; the temperature of a first zone of the co-rotating double-screw extruder is 160 ℃, the temperature of a second zone is 165 ℃, the temperature of a third zone is 165 ℃, the temperature of a fourth zone is 165 ℃, the temperature of a fifth zone is 165 ℃, the temperature of a sixth zone is 165 ℃, the temperature of a machine head is 165 ℃, and the temperature of a melt is 160 ℃; the screw rotation speed is 400r/min.
9. The preparation method of claim 3, wherein the preparation method comprises the steps of weighing the raw materials according to the specified parts by weight, and placing the raw materials into an oven, wherein the needle-shaped or sheet-shaped inorganic filler with epoxy groups is dried at 95-105 ℃ for 2-4h, the PBAT is dried at 95-105 ℃ for 2-4h, and the PLA is dried at 140-160 ℃ for 2-4h.
10. The method of claim 3, wherein the PLA melt index is 5 to 8g/10min; the PBAT melt index is 2-5g/10min.
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