Degradable polyester composite material with controllable interface network as well as preparation method and application of degradable polyester composite material

Abstract

The invention belongs to the technical field of polymer blends, and particularly relates to a degradable polyester composite material with a controllable interface network as well as a preparation method and application of the degradable polyester composite material. The length-diameter ratio of carbon nanotubes (CNTs) is controlled within the range of 50-800, a Pickering emulsion is adopted to prepare CNT-poly (butylene succinate) (PBS) composite master batch, the CNT-poly (butylene succinate) (PBS) composite master batch and polylactic acid matrix resin are subjected to melt blending, and the composite material which is stable in interface structure and uniform in dispersion is obtained. The material forms a continuous conductive and polarized network at an interface, so that the charge capture and storage capability is effectively improved. Compared with a traditional direct melt blending system, the triboelectricity output performance is remarkably enhanced, the open-circuit voltage can reach 1129.5 V, the short-circuit current reaches up to 57.8 microamperes, the transfer charge reaches up to 471.7 nC, excellent charge generation and accumulation characteristics are shown, and the material is suitable for high-output degradable triboelectricity energy collection devices.

Description

Technical Field

[0001] This application belongs to the field of polymer blend technology, specifically relating to a composite material with polylactic acid matrix as the continuous phase and polybutylene succinate coated with carbon nanotubes as the dispersed phase. Background Technology

[0002] With the rapid development of flexible electronics, wearable devices, and the Internet of Things, the demand for green, functional, and sustainable energy materials in the field of materials science is constantly increasing. How to achieve efficient energy conversion and signal response while maintaining biodegradability has become an important direction in current polymer composite material research. Polylactic acid (PLA) and polybutylene succinate (PBS) are representative biodegradable polyesters derived from renewable resources, possessing both good biocompatibility and processing properties. However, due to their thermodynamic incompatibility, direct blending easily forms coarse phase regions and weak interfaces, making it difficult to establish stable energy transfer and charge storage channels, thus limiting their performance in structure-function integrated composite materials.

[0003] In PLA / PBS blends, the construction of the interfacial network is crucial for multi-scale performance. Introducing nanofillers at the phase interface can form nanoscale bridging and polarization networks, achieving synergistic coupling of mechanical reinforcement and charge transport. Carbon nanotubes (CNTs), due to their excellent conductivity, high specific surface area, and anisotropic structure, are widely used to improve interfacial adhesion and regulate phase morphology. Existing technologies (such as patent application number 202411806158.8) disclose a PLA / PBS composite material using CNTs as a solid emulsifier. CNT-coated PBS particles are prepared via an emulsion method and then melt-blended with PLA, positioning the CNTs at the phase interface. This significantly improves compatibility and charge transport pathways, thereby enhancing triboelectric output performance. When this material is used as a material for a contact-separated triboelectric nanogenerator, its triboelectric output performance is improved by approximately three times compared to PLA / PBS blends without CNTs. Performance test results show that the open-circuit voltage of this material reaches 184.94V, and the short-circuit current density is 21.14mA / m². 2 The surface charge density reaches 496.14 μC / m². 2 All three core indicators performed excellently.

[0004] However, this technology only involves CNTs with a single aspect ratio, and its mechanism of action is mainly limited to the dispersion of fillers at the interfacial reinforcement level. In fact, CNTs with different aspect ratios exhibit significantly different interfacial localization behaviors, network building capabilities, and charge migration characteristics in polymer blends, which directly affect phase structure evolution and interfacial polarization. Existing technologies have not systematically studied the intrinsic relationship between CNT aspect ratio and interfacial network formation, charge trapping efficiency, and macroscopic output performance, nor have they provided operable parameter control strategies. Therefore, how to achieve precise interfacial structure construction and charge dynamics optimization through differentiated aspect ratio control remains a key scientific and technological problem that urgently needs to be solved in this field. Summary of the Invention

[0005] The purpose of this invention is to provide a biodegradable polyester composite material with controllable interface network and strong charge storage capacity, as well as its preparation method and application, to solve the problems of significant phase separation, weak interfacial bonding, and low charge capture and storage efficiency in polylactic acid (PLA) and polybutylene succinate (PBS) blend systems. To achieve the above objective, this invention adopts the following technical solution:

[0006] A biodegradable polyester composite material, characterized in that:

[0007] The composite material uses polylactic acid (PLA) as the continuous phase and polybutylene succinate (PBS) coated with carbon nanotubes (CNTs) as the dispersed phase; the mass ratio of PLA, PBS and CNTs is (90-50):(10-50):1; the aspect ratio of the carbon nanotubes is 50-800.

[0008] Preferably, the mass ratio of PLA, PBS, and CNT is 70:30:1.

[0009] Preferably, the aspect ratio of the CNT is 50, 157, 300 or 800, more preferably 300.

[0010] A method for preparing the composite material includes the following steps:

[0011] (1) Dissolve PBS in dichloromethane to prepare an oil phase; disperse CNT in an aqueous phase at a volume ratio of oil phase to aqueous phase of 1:(2.5-3.5), preferably 1:3, and homogenize using a homogenizer at a speed of 10000-12000 rpm for 2-3 min to obtain Pickering emulsion;

[0012] (2) The emulsion was stirred under ventilation conditions to volatilize dichloromethane. The stirring speed was 300-350 rpm and the time was 20-24 h. After that, it was filtered, washed with deionized water and dried at 50-60℃ for 20-24 h to obtain CNT@PBS composite masterbatch.

[0013] (3) The composite masterbatch and polylactic acid are melt-blended at 160-180°C and 40-60 r / min for 6-8 min to obtain the composite material.

[0014] As a preferred option, the aspect ratio of carbon nanotubes can be adjusted during the preparation process to control their distribution behavior and network structure in the polymer interface region, thereby achieving synergistic optimization of the phase structure and charge storage capacity of the composite system.

[0015] The present invention also provides the application of the above-mentioned composite material in charge trapping and storage functional materials, preferably as a triboelectric layer for triboelectric nanogenerators.

[0016] By adopting the above technical solution, the present invention has the following beneficial effects:

[0017] (1) By adjusting the aspect ratio of CNTs to within the range of 50 to 800, their selective distribution at the interface of PLA / PBS blend system can be achieved, a stable interfacial polarization network can be constructed, phase separation can be suppressed, and the interfacial bonding strength can be improved, thereby enhancing the charge capture and storage capacity of the system.

[0018] (2) By preparing CNT@PBS composite masterbatch by Pickering emulsion method and melt blending it with PLA, a composite material with uniform dispersion and stable interfacial network can be obtained with regular microstructure and good processing adaptability.

[0019] (3) Under the same ratio conditions, the composite material exhibits higher charge storage and output performance. Test results show that the charge storage potential of the material can reach 486 mV, and when used as a friction layer, the open circuit voltage is 1129.5 V, the short circuit current is 57.8 μA, and the transferred charge is 471.7 nC, which is significantly improved compared with the system without CNTs or without optimized aspect ratio;

[0020] (4) Compared with the cited patent in the background art (application number 202411806158.8), the present invention does not require changing the matrix composition or introducing new components. It can significantly improve the interface structure and electrical properties by simply adjusting the aspect ratio of carbon nanotubes, thereby achieving predictable adjustment of material properties. The process is simple, highly controllable, and has good degradability and large-scale preparation potential. Attached Figure Description

[0021] The attached diagram will be briefly described below:

[0022] Figure 1 Scanning electron microscope (SEM) images of the phase structure morphology of the composite materials obtained in Examples 1-4 and Comparative Example 1.

[0023] Figure 2Surface potential diagrams of the composite materials prepared in Examples 1-4 and Comparative Example 1;

[0024] Figure 3 For the open-circuit voltage diagram, short-circuit current diagram, and charge transfer diagram in performance test 1;

[0025] Figure 4 The graph shows the charge accumulation and accumulation rate in performance test 1;

[0026] Figure 5 The open-circuit voltage diagram, current density diagram, and charge density diagram are shown in Performance Test 2. Detailed Implementation

[0027] The present application will now be further described by way of specific embodiments. Those skilled in the art will be able to implement the present application based on these descriptions. Furthermore, the embodiments of the present application described below are generally only a part of the embodiments of the present application, and not all of the embodiments. Therefore, all other embodiments obtained by those skilled in the art based on the embodiments of the present application without inventive effort should fall within the scope of protection of the present application.

[0028] Example 1

[0029] Pretreatment stage: Polybutylene succinate granules (Xinjiang Lanshan Tunhe Polyester Co., Ltd., brand name TH801, density 1.25 g / cm³) were processed. 3 The following materials were used: melting point 113℃, melt index 10-20 g / 10min; carbon nanotube powder (Jiangsu Xianfeng Nanomaterials Technology Co., Ltd., grade XFM22, aspect ratio L / D=50); and polylactic acid (NatureWorks, USA, grade 4032D, melt index 6.17 g / 10min, density 1.24 g / cm³). 3 Its melting point is 148–160℃, and its weight-average molecular weight and number-average molecular weight are 1.85 × 10⁻⁶. 5 g / mol, 1.22×10 5 (g / mol) was dried in a forced-air oven at 60℃ for 12 hours.

[0030] Step 1: Weigh 1 part by mass of carbon nanotube (CNT) powder with an aspect ratio (L / D) of 50 and disperse it uniformly in deionized water to prepare an aqueous phase. Separately, dissolve 30 parts by mass of PBS in dichloromethane to form an oil phase. Mix the oil phase and aqueous phase at an oil-to-water ratio of 1:3 and homogenize using a homogenizer at 12,000 rpm for 3 minutes to form a PBS@CNT emulsion. Stir the emulsion at 350 rpm for 24 hours in a fume hood to fully volatilize the dichloromethane, then filter and dry in a 60°C forced-air oven for 24 hours to obtain PBS@CNT composite masterbatch.

[0031] Step 2: 70 parts by mass of PLA and dried PBS@CNT composite masterbatch were melt-blended at 180℃ and 60 r / min for 8 min to obtain a PLA / PBS@CNT composite material with carbon nanotube L / D=50. The obtained PLA / PBS@CNT composite material has PLA matrix as the continuous phase and 1 part by mass of CNT with L / D=50 as the filler coated on the PBS surface as the dispersed phase. Scanning electron microscopy images of the sample phase structure morphology are shown below. Figure 1 As shown.

[0032] Example 2

[0033] The only difference between Example 2 and Example 1 is that the carbon nanotube powder (Belgian Nanocyl, grade NC7000) has an aspect ratio (L / D) of 157. All other parameters, including oil-to-water ratio, homogenization speed, evaporation time, and melt blending conditions, are the same. Specific preparation methods are detailed below.

[0034] Pretreatment stage: Polybutylene succinate granules (Xinjiang Lanshan Tunhe Polyester Co., Ltd., brand name TH801, density 1.25 g / cm³) were processed. 3 The following materials were used: melting point 113℃, melt index 10-20 g / 10min; carbon nanotube powder (Jiangsu Xianfeng Nanomaterials Technology Co., Ltd., grade XFM22, aspect ratio L / D=157); and polylactic acid (NatureWorks, USA, grade 4032D, melt index 6.17 g / 10min, density 1.24 g / cm³). 3 Its melting point is 148–160℃, and its weight-average molecular weight and number-average molecular weight are 1.85 × 10⁻⁶. 5 g / mol, 1.22×10 5 (g / mol) was dried in a forced-air oven at 60℃ for 12 hours.

[0035] Step 1: Weigh 1 part by mass of carbon nanotube (CNT) powder with an aspect ratio (L / D) of 157 and disperse it uniformly in deionized water to prepare an aqueous phase. Separately, dissolve 30 parts by mass of PBS in dichloromethane to form an oil phase. Mix the oil phase and aqueous phase at an oil-to-water ratio of 1:3 and homogenize using a homogenizer at 12,000 rpm for 3 minutes to form a PBS@CNT emulsion. Stir the emulsion at 350 rpm for 24 hours in a fume hood to fully volatilize the dichloromethane, then filter and dry in a 60°C forced-air oven for 24 hours to obtain PBS@CNT composite masterbatch.

[0036] Step 2: 70 parts by mass of PLA and dried PBS@CNT composite masterbatch were melt-blended at 180℃ and 60 r / min for 8 min to obtain a PLA / PBS@CNT composite material with carbon nanotube L / D=157. The obtained PLA / polyPBS@CNT composite material has PLA matrix as the continuous phase and 1 part by mass of CNT with L / D=157 as the filler coated on the PBS surface as the dispersed phase. Scanning electron microscopy images of the sample phase structure morphology are shown below. Figure 1 As shown.

[0037] Example 3

[0038] The steps of Example 1 were repeated in Example 3. The only difference was that the carbon nanotube powder (Jiangsu Xianfeng Nanomaterials Technology Co., Ltd., grade XFM2) had an aspect ratio L / D of 300; all other conditions were the same. Please refer to the following text for specific preparation methods.

[0039] Pretreatment stage: Polybutylene succinate granules (Xinjiang Lanshan Tunhe Polyester Co., Ltd., brand name TH801, density 1.25 g / cm³) were processed. 3 The following materials were used: melting point 113℃, melt index 10-20 g / 10min; carbon nanotube powder (Jiangsu Xianfeng Nanomaterials Technology Co., Ltd., grade XFM22, aspect ratio L / D=300); and polylactic acid (NatureWorks, USA, grade 4032D, melt index 6.17 g / 10min, density 1.24 g / cm³). 3 Its melting point is 148–160℃, and its weight-average molecular weight and number-average molecular weight are 1.85 × 10⁻⁶. 5 g / mol, 1.22×10 5 (g / mol) was dried in a forced-air oven at 60℃ for 12 hours.

[0040] Step 1: Weigh 1 part by mass of carbon nanotube (CNT) powder with an aspect ratio (L / D) of 300 and disperse it uniformly in deionized water to prepare an aqueous phase. Separately, dissolve 30 parts by mass of PBS in dichloromethane to form an oil phase. Mix the oil phase and aqueous phase at an oil-to-water ratio of 1:3 and homogenize using a homogenizer at 12,000 rpm for 3 minutes to form a PBS@CNT emulsion. Stir the emulsion at 350 rpm for 24 hours in a fume hood to fully volatilize the dichloromethane, then filter and dry in a 60°C forced-air oven for 24 hours to obtain PBS@CNT composite masterbatch.

[0041] Step 2: 70 parts by mass of PLA and dried PBS@CNT composite masterbatch were melt-blended at 180℃ and 60 r / min for 8 min to obtain a PLA / PBS@CNT composite material with carbon nanotube L / D=300. The obtained PLA / PBS@CNT composite material has a polylactic acid matrix as the continuous phase and 1 part by mass of CNT with L / D=300 as the filler coated on the PBS surface as the dispersed phase. Scanning electron microscopy images of the sample phase structure morphology are shown below. Figure 1 As shown.

[0042] Example 4

[0043] Repeat the steps of Example 1, using carbon nanotube powder with an L / D ratio of 800 (Jiangsu Xianfeng Nanomaterials Technology Co., Ltd., grade XFM16), and keep all other conditions the same. See below for specific preparation methods.

[0044] Pretreatment stage: Polybutylene succinate granules (Xinjiang Lanshan Tunhe Polyester Co., Ltd., brand name TH801, density 1.25 g / cm³) were processed. 3 The following materials were used: melting point 113℃, melt index 10~20 g / 10min; carbon nanotube powder (Jiangsu Xianfeng Nanomaterials Technology Co., Ltd., grade XFM22, aspect ratio L / D=800); and polylactic acid (NatureWorks, USA, grade 4032D, melt index 6.17 g / 10min, density 1.24 g / cm³). 3 Its melting point is 148–160℃, and its weight-average molecular weight and number-average molecular weight are 1.85 × 10⁻⁶. 5 g / mol, 1.22×10 5 (g / mol) was dried in a forced-air oven at 60℃ for 12 hours.

[0045] Step 1: Weigh 1 part by mass of carbon nanotube (CNT) powder with an aspect ratio (L / D) of 800 and disperse it uniformly in deionized water to prepare an aqueous phase. Separately, dissolve 30 parts by mass of PBS in dichloromethane to form an oil phase. Mix the oil phase and aqueous phase at an oil-to-water ratio of 1:3 and homogenize using a homogenizer at 12,000 rpm for 3 minutes to form a PBS@CNT emulsion. Stir the emulsion at 350 rpm for 24 hours in a fume hood to fully volatilize the dichloromethane, then filter and dry in a 60°C forced-air oven for 24 hours to obtain PBS@CNT composite masterbatch.

[0046] Step 2: 70 parts by mass of PLA and dried PBS@CNT composite masterbatch were melt-blended at 180℃ and 60 r / min for 8 min to obtain a PLA / PBS@CNT composite material with carbon nanotube L / D=800. The obtained PLA / PBS@CNT composite material has PLA matrix as the continuous phase and 1 part by mass of CNT with L / D=800 as the filler coated on the PBS surface as the dispersed phase. Scanning electron microscopy images of the sample phase structure morphology are shown below. Figure 1 As shown.

[0047] Comparative Example 1

[0048] Compared with Examples 1, 2, 3, and 4, Comparative Example 1 differs in that no carbon nanotube filler was added during the preparation process; PLA and PBS were directly melt-blended to obtain a PLA / PBS binary blend. The specific preparation method is as follows:

[0049] Pretreatment stage: Polylactic acid (PLA, grade 4032D, NatureWorks LLC, USA, melt index 6.2 g / 10 min, density 1.24 g / cm³) was added. 3 Melting point 148–160℃, weight-average molecular weight 1.85 × 10⁻⁶ 5 g / mol, number-average molecular weight 1.22 × 10 5 (g / mol) and polybutylene succinate (PBS, brand name TH801, Xinjiang Lanshan Tunhe Polyester Co., Ltd., melt index 10-20 g / 10 min, density 1.25 g / cm³) 3 The raw materials (with a melting point of 113℃) were placed in a 60℃ forced-air drying oven and dried for 12 hours to remove any moisture and volatile impurities that may be present in the raw materials.

[0050] Step 1: Thoroughly dried polylactic acid (PLA) and polybutylene succinate (PBS) were melt-blended using a torque rheometer. The blending conditions were: temperature 180℃, rotation speed 60 r / min, and blending time 8 min, to obtain the PLA / PBS blend. Scanning electron microscopy (SEM) images of the sample phase structure morphology are shown below. Figure 1 As shown.

[0051] Performance Test 1

[0052] The composite materials prepared in Examples 1-4 and Comparative Example 1 were used to prepare thin films of the same size for testing their surface potential. The testing methods and conditions are as follows: Kelvin probe microscopy (KPFM) was used for the test, with a test area of ​​4 cm². 2 The test results are as follows Figure 2 As shown. From Figure 2It can be seen that the surface potential of the composite material after CNT introduction changes from negative to positive. Among them, the PLA / PBS@CNT composite material with L / D=300 (Example 3) exhibits the largest surface potential, which fully demonstrates the excellent charge storage capacity of this interfacial charge network.

[0053] Performance Test 2

[0054] The composite materials prepared in Examples 1-4 and Comparative Example 1 were used as the friction layer of a rotary triboelectric nanogenerator, and their open-circuit voltage (V) was tested under the same rotational speed conditions. oc The test method and test settings are as follows: A rotary TENG device is used for the test, with the rotor and stator kept in contact. The rotational speed is set to 60 rpm, and the test area is 113.04 cm². 2 The test results are as follows Figure 3 As shown. From Figure 3 It can be seen that the open-circuit voltage of the composite material after introducing carbon nanotubes is better than that of the PLA / PBS blend provided in Comparative Example 1. Among them, the PLA / PBS@CNT composite material with L / D=300 (Example 3) exhibits the highest open-circuit voltage. Compared with Examples 1, 2, and 4 and Comparative Example 1, the composite material prepared in Example 3 has an open-circuit voltage as high as 1129.5V, which is nearly 3.1 times that of Comparative Example 1.

[0055] The PLA / PBS@CNT composite materials prepared in Examples 1-4 and Comparative Example 1 were used as the friction layer of a rotary triboelectric nanogenerator. Their short-circuit current (I0.05) was tested under the same rotational speed conditions. sc The test method and test settings are as follows: A rotary TENG device is used for the test, with the rotor and stator kept in contact. The rotational speed is set to 60 rpm, and the test area is 113.04 cm². 2 The test results are as follows Figure 3 As shown. From Figure 3 It can be seen that the PLA / PBS@CNT composite material with L / D=300 carbon nanotubes (Example 3) exhibits the highest short-circuit current. Compared with Examples 1, 2, and 4 and Comparative Example 1, the composite material prepared in Example 3 has a short-circuit current as high as 57.8 μA, which is nearly 2.8 times that of Comparative Example 1.

[0056] The PLA / PBS@CNT composite materials prepared in Examples 1-4 and Comparative Example 1 were used as the friction layer of a rotary triboelectric nanogenerator. Their transferred charge (Q) was tested under the same rotational speed conditions. scd The test method and test settings are as follows: A rotary TENG device is used for the test, with the rotor and stator kept in contact. The rotational speed is set to 60 rpm, and the test area is 113.04 cm². 2 The test results are as follows Figure 3As shown. From Figure 3 It can be seen that the PLA / PBS@CNT composite material with L / D=300 carbon nanotubes (Example 3) exhibits the highest transfer charge. Compared with Examples 1, 2, and 4 and Comparative Example 1, the composite material prepared in Example 3 has a transfer charge as high as 471.7 nC, which is nearly 2.8 times that of Comparative Example 1.

[0057] The PLA / PBS@CNT composite materials prepared in Examples 1-4 and Comparative Example 1 were used as the friction layer of a rotary triboelectric nanogenerator. The charge accumulation and accumulation rate were tested under the same rotational speed conditions. The test methods and settings are as follows: a rotary TENG device was used, with the rotor and stator kept in contact; the rotational speed was set to 60 rpm; and the test area was 113.04 cm². 2 The test results are as follows Figure 4 As shown. From Figure 4 As can be seen, the PLA / PBS@CNT composite material with L / D=300 carbon nanotubes (Example 3) achieved a charge accumulation of 4.9 μC within 248 s. Compared with Examples 1, 2, and 4 and Comparative Example 1, the composite material prepared in Example 3 exhibited the largest charge accumulation and the fastest charge accumulation rate, demonstrating an unexpected technical effect.

[0058] Performance Test 3

[0059] The difference between this performance test and Performance Test 1 is that the composite materials prepared in Examples 1-4 and Comparative Example 1 are used as materials for contact-separated triboelectric nanogenerators, and their open-circuit voltage, current density, and charge density are tested (the test methods are the same as in Performance Test 1, and the test area is 1×1cm). 2 The test results are attached. Figure 5 ).

[0060] From the appendix Figure 5 The open-circuit voltage test results show that the open-circuit voltage of the PLA / PBS@CNT composite material with carbon nanotubes is significantly better than that of the PLA / PBS blend in Comparative Example 1. Among them, the PLA / PBS@CNT composite material with L / D=300 (Example 3) exhibits the highest open-circuit voltage, which is significantly higher than that of Comparative Example 1, demonstrating the positive role of carbon nanotubes in enhancing the voltage output of contact-separated TENGs.

[0061] The current density test results showed that the composite material prepared in Example 3 exhibited the best current density performance. Compared with Comparative Example 1, its current density was significantly improved, further demonstrating the synergistic optimization effect of carbon nanotubes with L / D=300 on the interface network and triboelectric properties of the composite material, thus greatly enhancing the current output capability of the contact-separated TENG.

[0062] The charge density test results show that the composite material of Example 3 has the highest charge density. Compared with Examples 1, 2, and 4 and Comparative Example 1, Example 3 has a significant advantage in charge density performance, indicating that the charge transfer efficiency of this material is significantly improved during the contact separation friction process.

[0063] In summary, through observation of the appendix Figure 5 It can be seen that the composite material prepared in this application can be applied not only to rotary triboelectric nanogenerators, but also to contact-separated triboelectric nanogenerators. It exhibits excellent triboelectric properties in both working modes. In particular, the PLA / PBS@CNT composite material with L / D=300 (Example 3) has significantly surpassed the traditional blend (Comparative Example 1) in terms of open-circuit voltage, short-circuit current and transferred charge, demonstrating its wide applicability and excellent performance stability in the field of triboelectric nanogenerators.

Claims

1. A biodegradable polyester composite material with controllable interface network, characterized in that, The composite material uses polylactic acid matrix as the continuous phase and polybutylene succinate coated with carbon nanotubes as the dispersed phase; the mass ratio of polylactic acid, polybutylene succinate and carbon nanotubes is (50-90):(10-50):1; and the aspect ratio of the carbon nanotubes is 50-800.

2. The composite material according to claim 1, characterized in that, The mass ratio of polylactic acid, polybutylene succinate, and carbon nanotubes is 70:30:

1.

3. The composite material according to claim 1, characterized in that, The aspect ratio of the carbon nanotubes is 50, 157, 300 or 800.

4. A method for preparing the composite material according to any one of claims 1 to 3, characterized in that, Includes the following steps: A composite masterbatch was prepared by mixing polybutylene succinate with carbon nanotubes using the Pickering emulsion template method; the prepared composite masterbatch was then melt-blended with polylactic acid to obtain a composite material.

5. The method for preparing a composite material according to claim 4, characterized in that, Includes the following steps: Polybutylene succinate was dissolved in dichloromethane as the oil phase, and carbon nanotubes were dispersed in an aqueous solution as the aqueous phase. The oil phase and the aqueous phase were then subjected to Pickering emulsion blending, and the blend was post-treated to obtain a composite masterbatch.

6. The method for preparing a composite material according to claim 5, characterized in that, The post-processing includes: stirring the blend to volatilize dichloromethane, then filtering, washing with deionized water, and drying to obtain the composite masterbatch.

7. The method for preparing a composite material according to claim 4, characterized in that, The conditions for melt blending are: temperature 160–180°C, rotation speed 40–60 r / min, and time 6–8 min.

8. The application of the composite material according to any one of claims 1 to 3 in charge capture and storage functional materials.

9. The application according to claim 8, characterized in that, The applications include using composite materials as the friction layer of a rotary triboelectric nanogenerator or a contact-separated triboelectric nanogenerator.

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