CN106637489A - Polymer sheath-core composite fiber with thermoelectric effect as well as preparation method and application thereof - Google Patents
Polymer sheath-core composite fiber with thermoelectric effect as well as preparation method and application thereof Download PDFInfo
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- CN106637489A CN106637489A CN201611250721.3A CN201611250721A CN106637489A CN 106637489 A CN106637489 A CN 106637489A CN 201611250721 A CN201611250721 A CN 201611250721A CN 106637489 A CN106637489 A CN 106637489A
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- D—TEXTILES; PAPER
- D01—NATURAL OR MAN-MADE THREADS OR FIBRES; SPINNING
- D01F—CHEMICAL FEATURES IN THE MANUFACTURE OF ARTIFICIAL FILAMENTS, THREADS, FIBRES, BRISTLES OR RIBBONS; APPARATUS SPECIALLY ADAPTED FOR THE MANUFACTURE OF CARBON FILAMENTS
- D01F8/00—Conjugated, i.e. bi- or multicomponent, artificial filaments or the like; Manufacture thereof
- D01F8/04—Conjugated, i.e. bi- or multicomponent, artificial filaments or the like; Manufacture thereof from synthetic polymers
- D01F8/06—Conjugated, i.e. bi- or multicomponent, artificial filaments or the like; Manufacture thereof from synthetic polymers with at least one polyolefin as constituent
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- D—TEXTILES; PAPER
- D01—NATURAL OR MAN-MADE THREADS OR FIBRES; SPINNING
- D01D—MECHANICAL METHODS OR APPARATUS IN THE MANUFACTURE OF ARTIFICIAL FILAMENTS, THREADS, FIBRES, BRISTLES OR RIBBONS
- D01D5/00—Formation of filaments, threads, or the like
- D01D5/28—Formation of filaments, threads, or the like while mixing different spinning solutions or melts during the spinning operation; Spinnerette packs therefor
- D01D5/30—Conjugate filaments; Spinnerette packs therefor
- D01D5/34—Core-skin structure; Spinnerette packs therefor
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- D—TEXTILES; PAPER
- D01—NATURAL OR MAN-MADE THREADS OR FIBRES; SPINNING
- D01F—CHEMICAL FEATURES IN THE MANUFACTURE OF ARTIFICIAL FILAMENTS, THREADS, FIBRES, BRISTLES OR RIBBONS; APPARATUS SPECIALLY ADAPTED FOR THE MANUFACTURE OF CARBON FILAMENTS
- D01F1/00—General methods for the manufacture of artificial filaments or the like
- D01F1/02—Addition of substances to the spinning solution or to the melt
- D01F1/10—Other agents for modifying properties
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- D—TEXTILES; PAPER
- D01—NATURAL OR MAN-MADE THREADS OR FIBRES; SPINNING
- D01F—CHEMICAL FEATURES IN THE MANUFACTURE OF ARTIFICIAL FILAMENTS, THREADS, FIBRES, BRISTLES OR RIBBONS; APPARATUS SPECIALLY ADAPTED FOR THE MANUFACTURE OF CARBON FILAMENTS
- D01F8/00—Conjugated, i.e. bi- or multicomponent, artificial filaments or the like; Manufacture thereof
- D01F8/04—Conjugated, i.e. bi- or multicomponent, artificial filaments or the like; Manufacture thereof from synthetic polymers
- D01F8/12—Conjugated, i.e. bi- or multicomponent, artificial filaments or the like; Manufacture thereof from synthetic polymers with at least one polyamide as constituent
-
- D—TEXTILES; PAPER
- D01—NATURAL OR MAN-MADE THREADS OR FIBRES; SPINNING
- D01F—CHEMICAL FEATURES IN THE MANUFACTURE OF ARTIFICIAL FILAMENTS, THREADS, FIBRES, BRISTLES OR RIBBONS; APPARATUS SPECIALLY ADAPTED FOR THE MANUFACTURE OF CARBON FILAMENTS
- D01F8/00—Conjugated, i.e. bi- or multicomponent, artificial filaments or the like; Manufacture thereof
- D01F8/04—Conjugated, i.e. bi- or multicomponent, artificial filaments or the like; Manufacture thereof from synthetic polymers
- D01F8/14—Conjugated, i.e. bi- or multicomponent, artificial filaments or the like; Manufacture thereof from synthetic polymers with at least one polyester as constituent
Abstract
The invention discloses a polymer sheath-core composite fiber with a thermoelectric effect as well as a preparation method and application thereof. The polymer sheath-core composite fiber is composed of a polymer sheath layer and a thermoelectric master batch material core layer, wherein the mass ratio of the sheath layer to the core layer ranges from (2 to 1) to (1 to 2); the polymer sheath layer is prepared from one of polypropylene, polyamide 6, polyamide 66 and polyethylene terephthalate resin; the thermoelectric master batch material core layer is composed of ternary components including carbon nanotubes/graphene, bismuth telluride and resin. According to the polymer sheath-core composite fiber disclosed by the invention, the graphene, the bismuth telluride and the macromolecule resin are used as raw materials, and are subjected to methods including melting and commixing, solid-phase force shearing and the like, so that uniform dispersion of a graphene and bismuth telluride compound phase is realized in one step. After thermoelectric master batches are prepared, a melting compounded spinning technology is adopted to prepare a sheath-core composite thermoelectric fiber material. The fiber material has an important application prospect in the field of thermoelectric conversion. The polymer sheath-core composite fiber can be made into a thermoelectric refrigerating device which is arranged in a fabric and clothes; the temperature can be adjusted and the temperature is comfortable and adjustable.
Description
Technical field
The invention belongs to thermoelectric material and device preparation field, are related to the fiber with thermoelectric property and by this fiber system
Into device.Specially a kind of polymer core-skin composite fiber with pyroelectric effect and preparation method and application.
Background technology
A global difficult problem.Therefore, develop and become very urgent using new green power.And in commercial production
And have many that it cannot be avoided to generate but the heat energy that go out of use in life, for example：Underground heat, frictional heat, vehicle exhaust, pot
Vapourss, steel plant's waste heat that fire grate is put etc., if can carry out effectively recycling by these used heat that alleviation will be become not
A kind of effective means of regenerative resource crisis.And thermoelectric material exactly one kind can realize that heat energy and electric energy are directly mutually changed
Functional material.
Thermoelectric material refers to by material internal carrier moving realize the green that heat energy and electric energy are directly mutually changed
Environment protection type functional material, it is mainly characterized by environmentally safe and utilization of energy multiformity, is expected to alleviate what the mankind were faced
Two hang-ups -- energy crisis and environmental pollution.Thermoelectric generation technology is imitated using the Sai Beike (Seebeck) of semi-conducting material
The technology that energy is directly changed should be carried out with Peltier (Peltier) effect, conversion efficiency depends primarily on the dimensionless of material
Performance index, i.e. ZT values (Z=α2σ/k, wherein α are Seebeck coefficients；σ is electrical conductivity；K is thermal conductivity).As all solid state
Electricity and refrigerator, thermo-electric device has the advantages that other materials is incomparable, for example movement-less part, noiseless, easily miniature
The features such as change, high easily controllable, reliability, life-span length.Inorganic thermoelectric material because its ZT value is up to 1.0 or so, always
Receive significant attention, but it there is also high cost, the shortcoming of machinability difference simultaneously.And Organic thermoelectric material has raw material
Abundant, low cost, light weight, it is readily synthesized and the significant advantage such as machinability height.In addition, Organic thermoelectric material has thermal conductivity
The low advantage of rate, generally its numerical value only has 1/10th of inorganic thermoelectric material.However, Organic thermoelectric material electrical conductivity and Sai Bei
Gram coefficient is low so that its thermoelectric (al) power factor is low, is only equivalent to the thousand of current comparatively ideal inorganic thermoelectric material power factor
/ mono-.
In conventional semiconductor material, improve while carrier mobility can bring electrical conductivity and Seebeck coefficient and carry
It is high.In Organic thermoelectric material, the transmission of carrier mainly by polaron in strand and interchain transition realizing, therefore
The doping of polymer molecule chain configuration, arrangement mode and conductive nano has a significant impact to carrier mobility.In organic thermoelectricity
In material, carrier is mainly transmitted in polymer molecular chain by polaron with the transition of interchain, therefore polymer point
Subchain configuration and strand arrangement mode have a significant impact to carrier mobility.Strengthen the ductility of strand, improve molecule
The order of chain arrangement is to realize the important channel of the raising of thermoelectricity capability in Organic thermoelectric material.
Graphene as a kind of new material, with other materials it is incomparable the characteristics of and advantage, so by Graphene with
The materials such as polymer combine improvement, strengthen the electric conductivity of composite.In the polymer/graphene with electric conductivity
In, micron order Tellurobismuthite. is introduced, can make organic polymer that there is thermoelectricity effect, meanwhile, can be processed using conventional polymer
Technique is processed.
The content of the invention
The present invention proposes a kind of using Graphene, Tellurobismuthite., macromolecule resin（Polypropylene, polyamide 6, polyamide 66,
Pet resin）For raw material, method is sheared etc. by melt blending, solid phase power, a step realize Graphene,
Tellurobismuthite. compound phase it is dispersed.After preparing thermoelectricity master batch, using melt composite spinning technology, core-sheath thermoelectricity is prepared
Fibrous material.
It is an object of the invention to provide a kind of polymer core-skin composite fiber with pyroelectric effect and preparation method thereof
And application.The fiber has important application prospect in thermo-electric conversion field.Can be fabricated to thermoelectric cooling device be placed in fabric and
In clothes, temperature is adjustable to realize that temperature pleasant is adjustable.Preparation process is simple, can be prepared using conventional spinning processes, be prepared
Efficiency high, technological parameter is easily controlled.
For achieving the above object, the invention discloses following technology contents：
A kind of polymer core-skin composite fiber with pyroelectric effect, it is characterised in that it is by polymeric skin and thermoelectricity master batch
Material sandwich layer is constituted；Cortex is 1 with the mass ratio of sandwich layer:2 to 2:1；
The polymeric skin be polypropylene, polyamide 6, polyamide 66, one kind of pet resin；
The thermoelectricity agglomerate material sandwich layer is made up of CNT or Graphene, Tellurobismuthite., resin ternary component, wherein：
The content of CNT or graphite olefinic constituents is 5wt%-30wt%；
The content of Tellurobismuthite. component is 20wt%-50wt%；
The content of resin components is 20wt%-75wt%；
The resin components be polypropylene, polyamide 6, polyamide 66, the one kind in pet resin.
The properties of product of the polymer core-skin composite fiber with pyroelectric effect prepared by the present invention are as follows：
（1）Composite fibre sandwich layer electrical conductivity is 10-5To 10-1In the range of S/cm；
（2）Composite fibre Seebeck coefficient can realize 10-4To 10-2It is adjustable in the range of V/k；
（3）Composite fibre can realize energization cooling-down effect and thermo-electric generation function.
The present invention further discloses the preparation method of the polymer core-skin composite fiber with pyroelectric effect, its feature exists
Carry out in as follows：
（1）After weighing CNT or Graphene, Tellurobismuthite. mixing, carry out after electromagnetism crushing under inert gas shielding, then enter
Row secondary ball milling, is fully disperseed the two, and at 30-50 μm, graphene layer numerical control is made as 1-2 to the Tellurobismuthite. powder prepared
Layer；
（2）After weighing resin and mixing ball milling gained powder body, under inert gas shielding, using the melting of twin screw blender altogether
Mixed, thermoelectricity agglomerate material is prepared in pelletize；
（3）Melt composite spinning technique prepares core-skin composite fiber：By polymeric skin, thermoelectricity agglomerate material sandwich layer, mixing, skin
Layer be polypropylene, polyamide 6, polyamide 66, one kind of pet resin, sandwich layer be thermoelectricity master batch material
Material, the different shoe designings of control, prepares the core-skin composite fiber for possessing thermoelectricity function.
The step（1）、（2）In noble gases be A r.The technological parameter of ball milling is in step (1)：Ratio of grinding media to material
For 13:1, rotating speed is 350 revs/min, and Ball-milling Time is 9-20 hours.Step（3）Middle melt composite spinning technological parameter is：
Spinning temperature：130-270℃；Screw speed：13r/min;Cortex screw metering pump pump for amount be set to for：20 g/min；Core
Layer screw metering pump arranges speed：20 g/min；Winding speed is 100-1000m/min-1。
The present invention further discloses the polymer core-skin composite fiber with pyroelectric effect in thermo-electric conversion field side
The application in face.Particularly thermoelectric cooling device is placed in fabric and clothes, reaches the adjustable purpose of temperature（See Fig. 3）.Experiment knot
Fruit shows：Polymer core-skin composite fiber with pyroelectric effect is fabricated to into thermoelectric cooling device to be placed in fabric and clothes,
Temperature is adjustable to realize that temperature pleasant is adjustable（For example, fiber prepared by this patent is fixed on into summer special work post as liner
In protective garment, it is possible to achieve under 38 DEG C of ambient temperature, can lower the temperature after energization 4 DEG C, make body-sensing comfortable）.
Polymer core-skin composite fiber with pyroelectric effect disclosed by the invention and its preparation method and application is had
Good effect be：
（1）The present invention is combined using electromagnetism disintegrating process and ball-milling method, dispersing Nano carbon tubes, Graphene, Tellurobismuthite., the time
It is short, energy- and time-economizing.
（2）Material prepared by the present invention has excellent thermoelectricity capability.
（3）Preparation process is simple of the present invention, preparation time is short, technological parameter is easily controlled, it is reproducible, with low cost,
Industrialization prospect is good.
（4）Thermoelectric fiber prepared by this method can change doping type and prepare with P, N structure thermoelectric fiber.It is made
Standby polymer core-skin composite fiber has important application prospect in thermo-electric conversion field.
Description of the drawings
Fig. 1 is the SEM figures of thermoelectricity composite fibre prepared in embodiment 1；
Fig. 2 is field emission scanning electron microscope (FESEM) picture of thermoelectricity composite fibre cross section in embodiment 2；
Fig. 3 is the schematic diagram that thermoelectric cooling device is placed in fabric.
Specific embodiment
With reference to specific embodiment, the present invention is expanded on further.It should be understood that these embodiments are merely to illustrate the present invention
Rather than restriction the scope of the present invention.In addition, it is to be understood that after the content for having read instruction of the present invention, people in the art
Member can make various changes or modifications to the present invention, and these equivalent form of values equally fall within the application appended claims and limited
Scope.Wherein Tellurobismuthite., Graphene, polypropylene（PP）, polyamide 6（PA6）, polyamide 66（PA66）And poly- terephthaldehyde
Sour glycol ester resin (PET) is by commercially available.
Embodiment 1
With high-purity Tellurobismuthite., Graphene（3-6 layers）Powder is raw material, according to the g of Tellurobismuthite. 50, the g stoichiometric proportions of Graphene 30
Example dispensing, weighs the powder that total amount is 80 g, loads ball grinder, carries out ball milling, and ratio of grinding media to material is 13:1, rotating speed is 350 r/
Min, Ball-milling Time is 12 hours, obtains micron powder.By resulting micron powder and PP（20g）After mixing, input
In twin screw blender, extruder temperature is set as 180 DEG C, extruded velocity is 5 kg/h, subsequently, in extruded stock immersion water bath
Cooling, pelletizing, drying is obtained thermoelectricity master batch.
Double-component Compound spinning screw extruderIn, thermoelectricity master batch input core hopper, cortex input is pure
PP, cortex is 1 with the mass ratio of sandwich layer:2；Set spinning technology parameter as：Spinning temperature：130-250 degree；Screw speed：
13r/min;Cortex screw metering pump pump for amount be set to for：10 g/min；Sandwich layer screw metering pump arranges speed：20 g/
min；Winding speed is 100-1000m/min-1.Obtained thermoelectric fiber Seebeck coefficient is 0.62 μ V/K.
Embodiment 2
With high-purity Tellurobismuthite., Graphene（3-6 layers）Powder is raw material, according to the g of Tellurobismuthite. 20, the g stoichiometric ratios of Graphene 5
Dispensing, weighs the powder that total amount is 25 g, loads ball grinder, carries out ball milling, and ratio of grinding media to material is 13:1, rotating speed is 350 r/min,
Ball-milling Time is 12 hours, obtains micron powder.By resulting micron powder and PA6（75 g）After mixing, input is double
In screw rod blender, extruder temperature is set as 270 DEG C, extruded velocity is 5 kg/h, subsequently, drop in extruded stock immersion water bath
Temperature, pelletizing, drying is obtained thermoelectricity master batch.
Double-component Compound spinning screw extruderIn, thermoelectricity master batch input core hopper, cortex input is pure
PA6, cortex is 1 with the mass ratio of sandwich layer：1；Set spinning technology parameter as：Spinning temperature：220-270 degree；Screw speed：
13r/min;Cortex screw metering pump pump for amount be set to for：20 g/min；Sandwich layer screw metering pump arranges speed：20 g/
min；Winding speed is 100-1000m/min-1.Thermoelectric fiber Seebeck coefficient is 0.35 μ V/K.
Embodiment 3
With high-purity Tellurobismuthite., Graphene（3-6 layers）Powder is raw material, according to the g of Tellurobismuthite. 40, the g stoichiometric proportions of Graphene 20
Example dispensing, weighs the powder that total amount is 60 g, loads ball grinder, carries out ball milling, and ratio of grinding media to material is 13:1, rotating speed is 350 r/
Min, Ball-milling Time is 12 hours, obtains micron powder.By resulting micron powder and PET（40 g）After mixing, throw
In entering twin screw blender, extruder temperature is set as 220 DEG C, extruded velocity is 5 kg/h, subsequently, extruded stock immersion water bath
Middle cooling, pelletizing, drying is obtained thermoelectricity master batch.
Double-component Compound spinning screw extruderIn, thermoelectricity master batch input core hopper, cortex input is pure
PET, cortex is 2 with the mass ratio of sandwich layer：1；Set spinning technology parameter as：Spinning temperature：240℃；Screw speed：13r/
min;Cortex screw metering pump pump is set to for amount：20 g/min；Sandwich layer screw metering pump arranges speed：10 g/min；Volume
It is 100-1000m/min around speed-1.Thermoelectric fiber Seebeck coefficient is 0.58 μ V/K.
Embodiment 4
With high-purity Tellurobismuthite., Graphene（3-6 layers）Powder is raw material, according to the g of Tellurobismuthite. 40, the g stoichiometries of CNT 10
Ratio dispensing, weighs the powder that total amount is 50 g, loads ball grinder, carries out ball milling, and ratio of grinding media to material is 13:1, rotating speed is 350 r/
Min, Ball-milling Time is 12 hours, obtains micron powder.
By resulting micron powder and PA6（50 g）After mixing, in input twin screw blender, extruder temperature is set
For 260 DEG C, extruded velocity is 5 kg/h, subsequently, is lowered the temperature in extruded stock immersion water bath, and pelletizing, drying is obtained thermoelectricity female
Grain.
Double-component Compound spinning screw extruderIn, thermoelectricity master batch input core hopper, cortex input is pure
PA6, cortex is 1 with the mass ratio of sandwich layer：1；Set spinning technology parameter as：Spinning temperature：220-270 degree；Screw speed：
13r/min;Cortex screw metering pump pump is set to for amount：20 g/min；Sandwich layer screw metering pump arranges speed：20 g/
min；Winding speed is 100-1000 m/min-1.Thermoelectric fiber Seebeck coefficient is 0.55 μ V/K.
Embodiment 5
By the fiber in embodiment 1, suitable length is intercepted（50 cm）, fiber cold end is placed in fabric and fixed；Hot junction winding is solid
Be set to it is discoid concentrate on the fabric lower left corner, and configure radiator fan, concentrate radiating.Power from commercially available normal charge is precious（2A；
5V）, from commercially available silver wire as wire, connection fiber two ends, thermoelectric fiber heat is concentrated to hot junction after power supply, cold junction temperature drop
Low, fabric temperature is lowered the temperature 4 DEG C, and fabric schematic diagram is as shown in Figure 3.
Claims (6)
1. a kind of polymer core-skin composite fiber with pyroelectric effect, it is characterised in that it is female by polymeric skin and thermoelectricity
Grain material sandwich layer composition；Cortex is 2 with the mass ratio of sandwich layer:1 to 1:2；
The polymeric skin be polypropylene, polyamide 6, polyamide 66, one kind of pet resin；
The thermoelectricity agglomerate material sandwich layer is made up of CNT or Graphene, Tellurobismuthite., resin ternary component, wherein：
The content of CNT or graphite olefinic constituents is 5wt%-30wt%；
The content of Tellurobismuthite. component is 20wt%-50wt%；
The content of resin components is 20wt%-75wt%；
The resin components be polypropylene, polyamide 6, polyamide 66, the one kind in pet resin.
2. there is the preparation method of the polymer core-skin composite fiber of pyroelectric effect, it is characterised in that by such as described in claim 1
Lower step is carried out：
（1）After weighing CNT or Graphene, Tellurobismuthite. mixing, carry out after electromagnetism crushing under inert gas shielding, then enter
Row secondary ball milling, is fully disperseed the two, prepares 30-50 μm of Tellurobismuthite. powder, and graphene layer numerical control is made as 1-2 layers；
（2）After weighing resin and mixing ball milling gained powder body, under inert gas shielding, using the melting of twin screw blender altogether
Mixed, thermoelectricity agglomerate material is prepared in pelletize；
（3）Melt composite spinning technique prepares core-skin composite fiber：By polymeric skin, thermoelectricity agglomerate material sandwich layer, mixing, control
The different shoe designings of system, prepare the core-skin composite fiber for possessing thermoelectricity function；Wherein melt composite spinning technological parameter is：Spinning
Temperature：130-270 ℃；Screw speed：13r/min;Cortex screw metering pump pump is set to for amount：20 g/min；Sandwich layer screw rod
Dosing pump arranges speed：20 g/min；Winding speed is 100-1000m/min-1。
3. the preparation method described in claim 2, wherein the noble gases in the step (1), (2) are A r.
4. the preparation method described in claim 2, wherein the technological parameter of ball milling is in the step (1)：Ratio of grinding media to material is 13:
1, rotating speed is 350 revs/min, and Ball-milling Time is 9-20 hours.
5. application of the polymer core-skin composite fiber with pyroelectric effect in terms of thermo-electric conversion field described in claim 1.
6. the application in terms of the application described in claim 5, wherein thermo-electric conversion field is referred to：Thermoelectric cooling device is placed in be knitted
In thing, knapsack and clothes, adjustable supply voltage is adjusting temperature.
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| CN108385204A (en) * | 2018-01-30 | 2018-08-10 | 宁波三邦超细纤维有限公司 | Graphene terylene antistatic composite fiber and preparation method thereof |
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