CN113977943A - 4D printing method for controlling deformation of liquid crystal elastomer material - Google Patents
4D printing method for controlling deformation of liquid crystal elastomer material Download PDFInfo
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- 239000000463 material Substances 0.000 title claims abstract description 95
- 239000004997 Liquid crystal elastomers (LCEs) Substances 0.000 title claims abstract description 44
- 238000007639 printing Methods 0.000 title claims abstract description 39
- 238000000034 method Methods 0.000 title claims abstract description 30
- 238000004132 cross linking Methods 0.000 claims abstract description 29
- 239000000758 substrate Substances 0.000 claims abstract description 11
- 239000002243 precursor Substances 0.000 claims abstract description 8
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- 230000002441 reversible effect Effects 0.000 abstract description 5
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- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C64/00—Additive manufacturing, i.e. manufacturing of three-dimensional [3D] objects by additive deposition, additive agglomeration or additive layering, e.g. by 3D printing, stereolithography or selective laser sintering
- B29C64/20—Apparatus for additive manufacturing; Details thereof or accessories therefor
- B29C64/264—Arrangements for irradiation
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B29—WORKING OF PLASTICS; WORKING OF SUBSTANCES IN A PLASTIC STATE IN GENERAL
- B29C—SHAPING OR JOINING OF PLASTICS; SHAPING OF MATERIAL IN A PLASTIC STATE, NOT OTHERWISE PROVIDED FOR; AFTER-TREATMENT OF THE SHAPED PRODUCTS, e.g. REPAIRING
- B29C64/00—Additive manufacturing, i.e. manufacturing of three-dimensional [3D] objects by additive deposition, additive agglomeration or additive layering, e.g. by 3D printing, stereolithography or selective laser sintering
- B29C64/30—Auxiliary operations or equipment
- B29C64/386—Data acquisition or data processing for additive manufacturing
- B29C64/393—Data acquisition or data processing for additive manufacturing for controlling or regulating additive manufacturing processes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B33—ADDITIVE MANUFACTURING TECHNOLOGY
- B33Y—ADDITIVE MANUFACTURING, i.e. MANUFACTURING OF THREE-DIMENSIONAL [3-D] OBJECTS BY ADDITIVE DEPOSITION, ADDITIVE AGGLOMERATION OR ADDITIVE LAYERING, e.g. BY 3-D PRINTING, STEREOLITHOGRAPHY OR SELECTIVE LASER SINTERING
- B33Y30/00—Apparatus for additive manufacturing; Details thereof or accessories therefor
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B33—ADDITIVE MANUFACTURING TECHNOLOGY
- B33Y—ADDITIVE MANUFACTURING, i.e. MANUFACTURING OF THREE-DIMENSIONAL [3-D] OBJECTS BY ADDITIVE DEPOSITION, ADDITIVE AGGLOMERATION OR ADDITIVE LAYERING, e.g. BY 3-D PRINTING, STEREOLITHOGRAPHY OR SELECTIVE LASER SINTERING
- B33Y50/00—Data acquisition or data processing for additive manufacturing
- B33Y50/02—Data acquisition or data processing for additive manufacturing for controlling or regulating additive manufacturing processes
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Physics & Mathematics (AREA)
- Mechanical Engineering (AREA)
- Optics & Photonics (AREA)
- Health & Medical Sciences (AREA)
- Toxicology (AREA)
- Liquid Crystal (AREA)
Abstract
The invention discloses a 4D printing method for controlling deformation of a liquid crystal elastomer material, wherein after the material is extruded and deposited on a substrate, a forming material is selectively cured in an ultraviolet light sweeping mode, and total ultraviolet light irradiation dosage in different areas is controlled by adjusting ultraviolet light irradiation energy intensity emitted by an ultraviolet light controller, or adjusting relative movement speed between the ultraviolet light controller and the forming material, or adjusting and controlling distance between the ultraviolet light controller and the forming material, so that the crosslinking density of the material in different areas is controlled. The invention irradiates different areas of the liquid crystal elastomer precursor sample piece printed by direct writing with ultraviolet light with different doses, so that different parts of the sample piece generate different crosslinking densities, and the temperatures of different parts for generating the directional-non-directional conversion are different. The invention can realize multi-stage reversible shape change of the liquid crystal elastomer sample by utilizing the differential design of the printing structure and the cross-linking density in space.
Description
Technical Field
The invention relates to the technical field of additive manufacturing and intelligent high polymer materials, in particular to a 4D printing method for controlling deformation of a liquid crystal elastomer material.
Background
The liquid crystal elastomer is an intelligent material and has the characteristics of both liquid crystal and polymer. The mesomorphism transformation device can complete the transformation from a nematic phase state to an isotropic state under the stimulation of an external field, such as heat, light, a magnetic field and the like, the mesomorphism in the mesomorphism transformation device is changed from ordered arrangement to disordered, and the shape change and the color change are represented in a macroscopic view, and the transformation is reversible. Due to the excellent excitation-response characteristic and the good cycle characteristic, the material can be used for manufacturing drivers and sensors.
3D printing is a rapid prototyping additive manufacturing technology, which can rapidly manufacture a pre-designed personalized shape, and the use of smart materials as 3D materials enables the printed object to complete the pre-designed shape, color and physical and chemical property changes under the condition of external stimulation, which is called 4D printing. The liquid crystal elastomer can be used as an intelligent material for 4D printing, the type of the liquid crystal elastomer polymerization spacer and the difference of the doped response particles in the precursor material are different, and the prepared driver has different stimulus response behaviors.
At present, the liquid crystal elastomer is mostly homogeneous for 4D printing, which greatly limits the deformation flexibility of the liquid crystal elastomer as an intelligent driver, and the material properties of the 3D printing piece are endowed in the printing process, namely the deformation behavior of the material can be programmed by utilizing the process parameter change in the printing process.
Disclosure of Invention
The invention provides a 4D printing method for controlling deformation of a liquid crystal elastomer material, aiming at the technical problems.
In order to achieve the above purpose, the invention provides the following technical scheme:
A4D printing method for controlling deformation of a liquid crystal elastomer material is characterized in that after the material is extruded and deposited on a substrate, a forming material is selectively cured in an ultraviolet light sweeping mode, and total ultraviolet light irradiation dose in different areas is controlled by adjusting ultraviolet light irradiation energy intensity emitted by an ultraviolet light controller, or adjusting relative movement speed between the ultraviolet light controller and the forming material, or adjusting and controlling distance between the ultraviolet light controller and the forming material, so that cross-linking density in different areas of the material is controlled.
Further, when the same UV light controller scanning speed was used, 50mw/cm, respectively, was used2And 200mw/cm2The ultraviolet head irradiation power is used for carrying out photo-crosslinking on different areas of the liquid crystal elastomer material.
Further, when 100mw/cm is used2The UV irradiation power of (1) is respectively 2mm/s and 4mm/s sweep speed to carry out photocrosslinking on different areas of the liquid crystal elastomer material.
Further, the ultraviolet light controller adopts an ultraviolet light curing head or an ultraviolet light projector.
Furthermore, when the material after extrusion deposition is subjected to digital light projection curing by adopting an ultraviolet projector, the light transmittance of different parts of the projection sheet is controlled, and the dose of the material receiving ultraviolet radiation is controlled, so that different parts generate different crosslinking degrees.
Further, material extrusion uses a direct write extrusion head printer for material build-up.
Further, the head printer is extruded to direct-write includes that the head is extruded to direct-write, ultraviolet curing head and material shaping base plate, and the material shaping base plate can drive through the slip table of below and do the motion along the XYZ axle, and the material is placed and is extruded the deposit by the atmospheric pressure in extruding the head and print on the material shaping base plate, forms liquid crystal elastomer precursor material, and the ultraviolet ray that the ultraviolet curing head sent solidifies the sample spare after printing.
Furthermore, the ultraviolet curing head selects a super-condensing lens as a lens, and the diameter of a condensing light spot of the ultraviolet curing head is phi 2 mm.
Further, the uv curing head may be replaced with a uv projector.
Further, the response stimulus temperature of different areas is in the interval of 95-155 ℃.
Compared with the prior art, the invention has the beneficial effects that:
according to the 4D printing method for controlling the deformation of the liquid crystal elastomer material, the total irradiation dose of ultraviolet light received by different areas is controlled by adjusting the ultraviolet light energy intensity emitted by an ultraviolet light controller, or adjusting the relative movement speed between the ultraviolet light controller and a forming material, or adjusting and controlling the distance between the ultraviolet light controller and the forming material, so that the cross-linking density of different areas of the material is controlled, different cross-linking densities are generated at different parts of the material, and the temperatures for generating the directional-non-directional conversion at different parts are different. The invention can realize multi-stage reversible shape change of the liquid crystal elastomer sample by utilizing the differential design of the printing structure and the cross-linking density in space.
Drawings
In order to more clearly illustrate the embodiments of the present application or technical solutions in the prior art, the drawings needed to be used in the embodiments will be briefly described below, and it is obvious that the drawings in the following description are only some embodiments described in the present invention, and other drawings can be obtained by those skilled in the art according to the drawings.
Fig. 1 is a schematic structural diagram of a direct-write extrusion head printer according to embodiment 2 of the present invention.
Fig. 2 is a schematic flow chart of a deformation process of a curing and heating sample according to embodiment 3 of the present invention.
Fig. 3 is a schematic flow chart of the deformation process of the curing and heating sample provided in embodiment 4 of the present invention.
FIG. 4 is a DSC curve of a sample before curing provided in example 4 of the present invention
Fig. 5 is a DSC curve of a sample after curing provided in example 4 of the present invention.
Detailed Description
The liquid crystal single domain in the liquid crystal elastomer material can be aligned under the action of external force. When the temperature of the oriented liquid crystal elastomer material is increased, the liquid crystal single domain is converted from the oriented state to the non-oriented state, and the property is reversible, namely, when the temperature is reduced, the conversion from the non-oriented state to the oriented state is generated. The liquid crystal elastomer material undergoes shape changes of overall elongation and contraction accompanying the oriented-non-oriented transition of the liquid crystal single domain.
The invention provides a 4D printing method for controlling deformation of a liquid crystal elastomer material, wherein after the material is extruded and deposited on a substrate, different ultraviolet doses are applied to different positions for irradiation crosslinking. The temperature at which deformation occurs at a portion where the irradiation dose is high, and the temperature at which deformation occurs at a portion where the irradiation dose is low.
And selectively curing the molding material by adopting an ultraviolet light sweeping mode, and controlling the total ultraviolet light irradiation dose in different areas by adjusting the ultraviolet light irradiation energy intensity emitted by an ultraviolet light controller, or adjusting the relative movement speed between the ultraviolet light controller and the molding material, or regulating and controlling the distance between the ultraviolet light controller and the molding material, thereby controlling the crosslinking density of the different areas of the material.
Material extrusion was extruded as lines using a direct write extrusion head printer onto a forming substrate to form the original shape of the actuator.
Different heating temperatures are set according to the level of difference in the degree of crosslinking that the printed liquid crystal elastomer material has. For example, the degree of crosslinking 1 corresponds to a temperature 1, the degree of crosslinking 2 corresponds to a temperature 2, and the degree of crosslinking N corresponds to a temperature N.
Based on the difference of the spatial crosslinking degree of the liquid crystal elastomer material, the liquid crystal elastomer material can realize the transformation from one two-dimensional form 1 to another two-dimensional form 2, and can realize the transformation from the two-dimensional form 2 to the two-dimensional form 3 along with the increase of the temperature, and the deformation of the forms can be reversible along with the decrease of the temperature.
In order to make the technical solutions of the present invention better understood by those skilled in the art, the present invention will be further described in detail with reference to the accompanying drawings and examples.
Example 1
The experimental material was prepared using an additive method, mixing liquid crystal monomer C6m (RM82), n-butylamine and photoinitiator in a mass ratio of 1:1: 0.01. The reaction flask was sealed with a stopper having a stirring hole, and the flask was put in an oil bath at 100 ℃ and the mixture was stirred at 80/min for 18 hours with a stirrer. After the reaction is finished, the liquid crystal ink is placed in a refrigerator at the temperature of-5 ℃ for ice-bath quenching for 2h, and then the material is placed in an extrusion printing syringe for direct-writing photocuring printing.
Example 2
The material build-up printing was performed using a custom made direct write extrusion head printer, the printing apparatus being shown in fig. 1, where 1 is a direct write extrusion head, the material being placed in the extrusion head and being extruded by air pressure. 2 is material shaping base plate, can be driven by the slip table of below, does the motion along XYZ axle. And 3, a liquid crystal elastomer precursor material extruded on the molding substrate. And 4, an ultraviolet curing head which can emit an ultraviolet head of 365nm to cure the printed sample piece, wherein the photoinitiator IRGACURE 369 is added in the precursor material, so that the liquid crystal elastomer material can be further polymerized under the irradiation of ultraviolet light, and the orientation direction of the liquid crystal is fixed.
The distance between the ultraviolet illumination curing head and the direct-writing printing extrusion head is 50mm, a super-condensing lens is selected as a lens of the ultraviolet illumination head, the diameter of a condensing light spot of the illumination head is phi 2mm, and an area of about 2mm multiplied by 2mm can be used as a minimum curing unit of ultraviolet light curing to perform selective area curing on a printed sample piece.
The material forming process is that firstly the direct-writing printing head 1 is used for extruding and forming the material, a certain pressure is applied to enable the material to be extruded at a certain speed, and meanwhile the forming platform 2 moves relatively, so that the material is deposited on the substrate in a certain path to form a fixed shape. And then the forming platform moves leftwards, and the ultraviolet curing head 4 is started to perform scanning illumination curing on the formed material at a certain ultraviolet illumination intensity.
In the printing process, the total irradiation measurement can be changed by adjusting the intensity of the illumination energy emitted by the ultraviolet light controller and changing the speed and the times of scanning the sample by the optical head, so that the crosslinking density of different areas is controlled.
When the same print head scanning speed was used, the ultraviolet head irradiation power was changed to 50mw/cm, respectively2And 200mw/cm2. 100mw/cm may also be used2And carrying out photocrosslinking on different areas by using sweep speeds of 2mm/s and 4mm/s respectively.
The photocuring of the printed material can also be carried out using digital light technology, i.e. irradiation of the material using an ultraviolet projector. And 5, an ultraviolet projector is arranged above the forming platform, and after the material is extruded and printed, ultraviolet light emitted by the projector is used for carrying out ultraviolet light irradiation on the material. The intensity of ultraviolet light irradiated on the material is different by utilizing different gray scales (or different colors) of the projection film, so that the crosslinking degree of different parts of the material is different.
In the printing process, the stimulation response shrinkage direction of the printing sample piece can be changed by adjusting the printing path direction of the extrusion head in the direct-writing extrusion process, the cross-linking density is influenced by ultraviolet light measurement so as to control the phase change temperature of the printing sample piece, and therefore a driver with spatial anisotropy is printed, and controllable deformation can be generated along with the temperature change.
Example 3
As shown in FIG. 2, a difference in crosslink density was introduced on both sides of the rectangular bar, with the left side being a high crosslink density region fully cured using high UV light metrology with a total radiation metrology of 200mw/cm2On the right are lightly crosslinked areas cured using a low UV light dose of 50mw/cm total radiation dose2. At a low stimulus temperature of 120 ℃, the low crosslink density region first undergoes phase change shrinkage, causing a difference in length along the long side, and the member is deformed from a rectangular shape to a semicircular shape by in-plane bending in the direction of the low crosslink density region. When the temperature is continuously raised to the high stimulation temperature of 155 ℃, the fully solidified high crosslinking density area also generates phase change shrinkage, and the semicircular sample piece is followedAnd further, when the temperature is continuously reduced, the high crosslinking density area of the rectangular sample strip is firstly lower than the phase transition temperature of the rectangular sample strip to complete the shape recovery, the liquid crystal elastomer sample strip is deformed into a semicircle, and when the temperature is further reduced, the semicircle is restored into the original strip shape.
The maximum bending curvature generated by the deformation with temperature can be controlled by controlling the difference of the crosslinking degree of the lightly crosslinked area and the fully crosslinked area or the size ratio of the lightly crosslinked area and the fully crosslinked area.
The degree of flexure of the liquid crystal elastomer stopper can also be controlled using varying stimulus temperatures.
Example 4
The out-of-plane bending deformation of the two-dimensional member to the three-dimensional shape can be realized by adjusting the ultraviolet irradiation dose to generate the spatial difference of the crosslinking density. And printing a circular structure by using a path planning mode of concentric circles, and performing scanning curing in the circular path planning mode by using an ultraviolet irradiation curing head.
As shown in fig. 3, the sample irradiated on the single surface is heated, when the temperature reaches 120 ℃, the outer layer area with low cross-linking density reaches the phase transition temperature first, the sample is deformed into a trapezoidal cylinder from the original plane-shaped disc, when the temperature is further heated to 155 ℃, the inner area also reaches the phase transition temperature to complete the shape deformation, and the sample is continuously deformed into a pyramid cone from the trapezoidal cylinder.
Placing a precursor liquid crystal sample printed on a substrate under an ultraviolet lamp for curing, setting the vertical irradiation distance of the sample from the ultraviolet lamp to be about 5cm, and measuring the curing intensity of the ultraviolet lamp by using an ultraviolet spectrophotometer with the model UIT-101 of USHIO company to be about 20mw/cm2Setting the ultraviolet curing time to be 2-60 s. The phase transition temperature was measured by DSC, and the DSC curves of the samples before and after curing are shown in FIG. 4 and FIG. 5, respectively.
In FIG. 4, the curve shows an endothermic peak at a position of 90 ℃ indicating that the phase transition temperature of the liquid crystal ink not subjected to the photo-curing reaction is about 90 ℃, whereas in FIG. 5, the test curve shows an endothermic peak at a position of about 155 ℃ in the test curveShowing the phase transition temperature T of the fully cured liquid crystalline elastomeric materialNIAbout 155 deg.c. This shows that the phase transition temperature of the liquid crystal elastomer material from nematic state to isotropic state is changed in the ultraviolet light curing crosslinking process, and the phase transition temperature of the completely polymerized liquid crystal elastomer is about 65 ℃ higher than that of the liquid crystal precursor without photopolymerization. Adjusting the uv dose during printing does affect its uv crosslinking and regulates its phase transition temperature.
The above examples are only intended to illustrate the technical solution of the present invention, but not to limit it; although the present invention has been described in detail with reference to the foregoing embodiments, it will be understood by those of ordinary skill in the art that: it is to be understood that modifications may be made to the technical solutions described in the foregoing embodiments, or equivalents may be substituted for some of the technical features thereof, but such modifications or substitutions do not depart from the spirit and scope of the technical solutions of the embodiments of the present invention.
Claims (10)
1. A4D printing method for controlling deformation of a liquid crystal elastomer material is characterized in that after the material is extruded and deposited on a substrate, a forming material is selectively cured in an ultraviolet light sweeping mode, and total ultraviolet light irradiation dosage in different areas is controlled by adjusting ultraviolet light irradiation energy intensity emitted by an ultraviolet light controller, or adjusting relative movement speed between the ultraviolet light controller and the forming material, or adjusting and controlling distance between the ultraviolet light controller and the forming material, so that cross-linking density of the material in different areas is controlled.
2. The 4D printing method for controlling deformation of liquid crystal elastomer material according to claim 1, wherein 50mw/cm is used when the same UV light controller scanning speed is used2And 200mw/cm2The ultraviolet head irradiation power is used for carrying out photo-crosslinking on different areas of the liquid crystal elastomer material.
3. 4D printing method for controlling deformation of liquid crystal elastomer material according to claim 1The method is characterized in that when 100mw/cm is used2The UV irradiation power of (1) is respectively 2mm/s and 4mm/s sweep speed to carry out photocrosslinking on different areas of the liquid crystal elastomer material.
4. The 4D printing method for controlling the deformation of the liquid crystal elastomer material according to claim 1, wherein the ultraviolet light controller adopts an ultraviolet light curing head or an ultraviolet light projector.
5. The 4D printing method for controlling the deformation of the liquid crystal elastomer material according to claim 4, wherein when the material after extrusion deposition is subjected to digital light projection curing by adopting an ultraviolet projector, the light transmittance of different parts of a projection sheet is controlled, and the dose of ultraviolet radiation received by the material is controlled, so that different parts generate different crosslinking degrees.
6. The 4D printing method for controlling deformation of liquid crystal elastomer material as claimed in claim 1, wherein the material extrusion uses a direct write extrusion head printer for material stacking.
7. The 4D printing method for controlling the deformation of the liquid crystal elastomer material according to claim 5, wherein the direct-writing type extrusion head printer comprises a direct-writing extrusion head (1), an ultraviolet curing head (4) and a material forming substrate (2), the material forming substrate (2) can be driven by a lower sliding table to move along XYZ axes, the material is placed in the extrusion head and is extruded and deposited by air pressure to be printed on the material forming substrate (2) to form the liquid crystal elastomer precursor material (3), and the ultraviolet light emitted by the ultraviolet curing head (4) is used for curing the printed sample.
8. The 4D printing method for controlling the deformation of the liquid crystal elastomer material as claimed in claim 7, wherein the ultraviolet curing head (4) adopts a super-condenser lens as a lens, and the diameter of a light condensing spot of the ultraviolet curing head (4) is phi 2 mm.
9. The 4D printing method for controlling deformation of liquid crystal elastomer material according to claim 7, wherein the uv curing head (4) can be replaced by a uv projector (5).
10. The 4D printing method of controlling the deformation of liquid crystal elastomer material according to claim 1, wherein the response stimulus temperature of different areas is in the interval 95-155 ℃.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN114932690A (en) * | 2022-05-06 | 2022-08-23 | 哈尔滨工业大学 | Preparation method of cross-medium soft robot based on liquid crystal elastomer |
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| CN108481734A (en) * | 2018-02-14 | 2018-09-04 | 北京大学 | 4D micro-nano Method of printings based on three-dimensional laser direct write |
| CN110172116A (en) * | 2019-04-26 | 2019-08-27 | 华中科技大学 | A kind of preparation method and product based on liquid crystal elastic body and 4D printing |
| CN110509546A (en) * | 2019-09-05 | 2019-11-29 | 西安工业大学 | A kind of programmable 4D Method of printing using multi-wavelength UV projection |
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- 2021-11-19 CN CN202111374054.0A patent/CN113977943A/en active Pending
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| CN108481734A (en) * | 2018-02-14 | 2018-09-04 | 北京大学 | 4D micro-nano Method of printings based on three-dimensional laser direct write |
| CN110172116A (en) * | 2019-04-26 | 2019-08-27 | 华中科技大学 | A kind of preparation method and product based on liquid crystal elastic body and 4D printing |
| CN110509546A (en) * | 2019-09-05 | 2019-11-29 | 西安工业大学 | A kind of programmable 4D Method of printing using multi-wavelength UV projection |
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| Title |
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| 汤桂平等: "4D打印液晶弹性体工艺及其性能研究", 机械工程学报, vol. 57, no. 7, 30 April 2021 (2021-04-30), pages 234 - 243 * |
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| CN114932690A (en) * | 2022-05-06 | 2022-08-23 | 哈尔滨工业大学 | Preparation method of cross-medium soft robot based on liquid crystal elastomer |
| CN114932690B (en) * | 2022-05-06 | 2022-11-01 | 哈尔滨工业大学 | Preparation method of cross-medium soft robot based on liquid crystal elastomer |
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