CN106816523A - The composite thermoelectric material being made up of conducting polymer - Google Patents
The composite thermoelectric material being made up of conducting polymer Download PDFInfo
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- CN106816523A CN106816523A CN201710049491.2A CN201710049491A CN106816523A CN 106816523 A CN106816523 A CN 106816523A CN 201710049491 A CN201710049491 A CN 201710049491A CN 106816523 A CN106816523 A CN 106816523A
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- pvdf
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
- H10N10/80—Constructional details
- H10N10/85—Thermoelectric active materials
- H10N10/856—Thermoelectric active materials comprising organic compositions
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
- H10N10/01—Manufacture or treatment
Abstract
A kind of composite thermoelectric material being made up of conventional conductive polymer and pn-junction lamination-type thermoelectric conversion device.Its p type conductive layer is mixed with PVDF by P3HT and constitutes, and n types conductive layer is made up of PANI and PVDF mixing, is isolated by PVDF polymer insulation layers between p types and n type conductive layers.This kind of pn-junction lamination-type thermoelectric conversion device is prepared by spraying process, preparation process is simple, with low cost.
Description
Technical field
The present invention relates to a kind of composite thermoelectric material being made up of conducting polymer, i.e. pn-junction lamination-type heat to electricity conversion dress
Put.Under certain condition, this kind of special thermoelectric material（Device）The electric energy of offer can be applicable to various MEMSs and micro-nano
Device power supply and other micro battery application fields.
Background technology
Thermoelectric material is a kind of functional material that can be realized and mutually be changed between electric energy and heat energy, and it can provide one kind both
The again safe generation mode of cleaning, is with a wide range of applications.The problem that current thermoelectric material is present is its heat to electricity conversion effect
Rate is still relatively low, expensive and TRT manufacturing process is complicated.
The conversion efficiency of thermoelectric of thermoelectric material can be characterized with thermoelectric figure of merit ZT,, here,It is electrical conductivity,It is thermal conductivity factor,It is Seebeck (Seebeck) coefficient, T is absolute temperature.Material to be improved can be seen that by the expression formula of ZT
The conversion efficiency of thermoelectric of material, should select the thermoelectric material with larger electrical conductivity and alap thermal conductivity.But it is true
On, at a certain temperature, 3 factors for determining ZT values are all the functions of carrier concentration, are to be mutually related, it is impossible to while
Optimized them, this is the main cause for hindering pyroelectric material performance further to improve at present.
At present, pyroelectric of the manufacture with ZT values higher is still relatively difficult and expensive.Such as the most frequently used is inorganic
Bi2Te3And Bi2Se3The manufacturing cost of thermoelectric material is time-consuming and expensive, and also has pollution to environment.Further, since manufacture is required
With the requirement of tolerance, also limit some thermoelectric materials and collected and the application in TRT in various heat.
In recent years, with deepening continuously that conducting polymer is studied, countries in the world researcher has carried out a series of using each
Class conducting polymer prepares the research work of new organic composite thermoelectric material and TRT.Because conducting polymer has preferably
Electrical conductivity and mechanical property, relatively low thermal conductivity factor the features such as, by composite optimization, conducting polymer is possible to substitution and passes
The materials such as the semiconductor of system, metal and superconduction, as classic thermoelectric material.Designed by conducting polymer thermoelectric material and opened
The various TRTs of hair, are expected to be applied to MEMS or microelectronic component power supply and other field.
The content of the invention
Further to improve the thermoelectric (al) power factor of existing polymer thermoelectric composite material, its thermoelectric figure of merit ZT is improved,
Higher in order to solve the problems, such as expensive current organic composite thermoelectric material, production, manufacturing cost, the purpose of the present invention is to carry
The conducting polymer composite thermoelectric material that a kind of price is low, be simple to manufacture is supplied, and has been constructed using this special combination
Thermoelectric conversion device that can be practical.
The pn-junction type composite thermoelectric material being made up of conducting polymer of the present invention, including backing material, in substrate
The n-type conductive layer mixed by PANI and PVDF is sprayed in material layer, n-type conductive layer is prepared as follows：By PANI
With PVDF powder mixing after pour into a certain proportion of 1-METHYLPYRROLIDONE solvent, through strength ultrasonic agitation mix, after be put into
Bakeed in 90 DEG C of baking ovens, after after the 1-METHYLPYRROLIDONE solvent evaporation of 60 %, mixed liquor becomes colloidal liquid, using spraying
Technique is sprayed on backing material, and it is the n-type conductive layer of 0.01-0.1mm to constitute thickness；The consumption of PANI accounts for PANI and PVDF
The 75%~90% of quality summation, the consumption of 1-METHYLPYRROLIDONE is identical with the gross mass of PANI and PVDF mixtures；
Then the dielectric isolation layer being made up of PVDF is sprayed again on the n-type conductive layer for preparing, dielectric isolation layer is as follows
Prepare：PVDF polymer powders are dissolved in 1-METHYLPYRROLIDONE solvent, after mixing through strength ultrasonic agitation, in 90 DEG C of baking ovens
Middle baking, after after the 1-METHYLPYRROLIDONE solvent evaporation of 60 %, mixture will become agglutination viscous liquid, using spraying work
Skill is sprayed on n-type conductive layer, prepares dielectric isolation layer, and dielectric isolation layer thickness is 0.01-0.1mm；Preparation is dielectrically separated from
During layer, PVDF polymer powders are 1 ︰ 3 with the mass ratio of 1-METHYLPYRROLIDONE；
Finally, p-type conductive layer is coated with dielectric isolation layer, p-type conductive layer is prepared as follows：Will be a certain proportion of
PVDF powder is mixed into 1-METHYLPYRROLIDONE solvent, strength ultrasonic agitation, after after fully dissolving, pours into P3HT powder, is continued
Strength ultrasonic agitation is uniform, is put into baking in 90 DEG C of baking ovens, and after after 60% 1-METHYLPYRROLIDONE solvent evaporation, mixture will
Become agglutination viscous liquid, sprayed on dielectric isolation layer using spraying coating process, prepare p-type conductive coating, coating layer thickness is
0.01-0.1mm；Described P3HT consumptions account for 75%~90%, the PVDF polymer powders and N- first of P3HT and PVDF mass summations
The mass ratio of base pyrrolidones is 1 ︰ 5；
Adjacent p-type conductive layer and n-type conductive layer are only connected with each other at one end.
Described p-type conductive layer, n-type conductive layer and dielectric isolation layer are sandwich construction.
Described PANI, P3HT, PVDF polymer is technical grade articles for use.
N-type conductive layer, p-type conductive layer and the elementary cell formed positioned at middle dielectric isolation layer overlap and repeat to match somebody with somebody
Put, be external sys-tems by string and/or parallel way.
The composite thermoelectric material being made up of conducting polymer of the invention（Electric heating TRT）It is by different conduction-types
Electroconductive polymer coating stacked combination, in embodiments, electroconductive polymer coating stacked structure at least includes one
The pn knots that individual n-type layer, a p-type layer are constituted, and it is at least partially disposed in being dielectrically separated between p-type layer and n-type layer
Layer is combined.This kind of conducting polymer composite thermoelectric material has the advantages that simple structure, low production cost, easily fabricated,
Pyroelecthc properties are sufficient for being actually subjected to for various MEMSs and micro-nano device power supply and other micro battery application fields
Ask.
N-type conductive layer of the present invention, p-type conductive layer and the elementary cell formed positioned at middle dielectric isolation layer
Can be dissolved in organic solvent of the conducting polymer materials characteristic without other influences, and use after by different mixed with polymers
Spraying process, different conduction-types composition polymer is sprayed in substrates of different and is completed, in addition, manufacturing various thermoelectric device realities
Apply in mode, each is tied by a pn, and be at least partially disposed in the dielectric isolation layer combination between p-type layer and n-type layer
The arrangement of thermoelectricity basic structure stackable configuration, also dependent on needing to constitute any series and parallel structure.
Conducting polymer composite thermoelectric material of the invention specifically has the beneficial effect that：
1. n-type coating material of the invention is meeting conductive wanting directly using PANI the and PVDF polymeric materials of technical grade
Under conditions of asking, manufacturing cost is not only reduced, and after introducing PVDF in conducting polymer PANI, can further drop
The thermal conductivity of low composite, is conducive to the raising of thermoelectric figure of merit.
2. p-type coating material of the invention is directly constituted using technical grade P3HT and PVDF polymer are compound, P3HT tools
There is natural p-type conductive characteristic and environmental stability, by the connection with n-type layer at one end, constitute pn knots, improve electricity
The transference efficiency and conversion efficiency of thermoelectric of son.
3. p-type of the present invention and the overlapping design structure of n-type layer, under extraneous action of thermal difference, can make carrier
Alternately flowed in p-type and n-type layer, can further increase conducting carriers transports densitometer efficiency, improves to phonon
Scattering section, significantly improves the thermoelectric figure of merit of material.
4. pn knots elementary cell of the present invention can be isolated using intermediate insulation thermal insulation layer, be constituted back with connection in series-parallel
Road, can obtain bigger thermoelectromotive force or electric current, be external sys-tems.
5. n-type of the present invention and p-type thermoelectricity coating are sprayable in any organic flexible material and substrate surface,
The foldable bending of material, material proportion is light, price is low, easy preparation, can be widely applied to new micro electronmechanical system, cogeneration and
In the power supply of device.
6. all organic high molecular polymers of material of the present invention, can replace traditional commercialized Bi2Te3
Etc. inorganic thermoelectric material, greatly reduce manufacturing cost, reduce environmental pollution, and aboundresources, be easily-synthesized, easy processing,
Size can be arbitrarily devised, there is broader answering compared with the existing thermoelectric material prepared by expensive other nano materials
Use prospect.
7. experiment shows that size is the thermoelectricity device of one group of pn-junction stromatolithic structure composition of 80 × 20 mm with test result
Part, under high/low temperature heat source temperature gradient is 90 degrees celsius in fig. 1, the open circuit thermoelectrical potential of output is about 1.0 volts.
Brief description of the drawings
Fig. 1 is conducting polymer composite thermoelectric material basic structural unit of the invention and pyroelecthc properties side view.
Specific embodiment
As shown in Figure 1：Wherein（1）It is the n-type conductive layer prepared using spraying coating process after PANI/PVDF mixing；（2）For
The p-type conductive layer prepared using spraying coating process after P3HT/PVDF mixing；（3）For the dielectric isolation layer that PVDF is constituted；（4）It is lining
Bottom material；（5）It is low-temperature heat source；（6）It is high temperature heat source；（7）It is measurement pyroelecthc properties wire；（8）It is voltmeter.
Conducting polymer composite thermoelectric material of the invention includes organic polymer substrate material（4）, in organic polymer
Backing material（4）It is upper to spray the n-type conductive layer mixed by PANI, PVDF（2）；In conductive layer（2）On be coated with by PVDF
The dielectric isolation layer that organic polymer is constituted（3）；In dielectric isolation layer（3）On be coated with the p- mixed by P3HT, PVDF
Type conductive layer（1）；P-type conductive layer（1）, dielectric isolation layer（3）, n-type conductive layer（2）Prepared by solution blended process,
Will its it is well mixed after be dissolved in it is different, in the organic solvent being had no effect to polymer physical chemistry characteristic, to ensure
Dispersed can mix between PANI and PVDF, between P3HT and PVDF；
To form reliable pn-junction, p-type conductive layer（1）With n-type conductive layer（2）Only it is connected with each other at one end.
N-type conductive layer（2）, p-type conductive layer（1）And positioned at middle dielectric isolation layer（3）The elementary cell of formation can
It is overlapping to repeat to configure, and loop is constituted by series-parallel system.
The present invention is further described through below in conjunction with the accompanying drawings, as shown in figure 1, conducting polymer of the invention is compound
P-type and n-type layer that thermoelectric material is linked together by one end respectively, centre plus one layer of polymeric insulating barrier laminate combination structure
Into.Mainly include：The p-type conductive layer that P3HT/PVDF is mixed（1）, n-type conductive layer is mixed by PANI/PVDF
（2）, the dielectric isolation layer being separately formed by PVDF polymer（3）, and other flexible organic polymer backing materials（4）.
P-type conductive layer（1）Prepared using solution blended process.First, the PVDF powder of the ratio is mixed into N- methyl pyrroles
In pyrrolidone solvent, strength ultrasonic agitation, after after fully dissolving, pours into P3HT powder, continues strength ultrasonic agitation, makes its uniform
Mixing.After mixing, put it into 90 DEG C of baking ovens and bakee, after after 60% 1-METHYLPYRROLIDONE solvent evaporation, mixture by
Gradual change agglutination viscous liquid, composition p-type conductive coating is sprayed using spraying coating process on any substrate.Coating layer thickness one
As 0.01-0.1mm；
Prepare n-type conductive layer（2）When, technical grade PANI and the PVDF powder of the ratio is poured into 1-METHYLPYRROLIDONE molten
In agent, after mixing through strength ultrasonic agitation, bakeed in 90 DEG C of baking ovens, after after 60% 1-METHYLPYRROLIDONE solvent evaporation, mixed
Closing liquid will become colloidal liquid, spray composition n-type conductive coating on any substrate using spraying coating process.Coating layer thickness one
As also be 0.01-0.1mm；
Prepare dielectric isolation layer（3）When, the PVDF polymer powders of the ratio are dissolved in 1-METHYLPYRROLIDONE solvent, pass through
Strength ultrasonic agitation mixing after, in 90 DEG C of baking ovens bakee, treat 60% 1-METHYLPYRROLIDONE solvent evaporation, mixture by
After gradual change agglutination viscous liquid, spray composition on any substrate using spraying coating process and be dielectrically separated from coating.Coating layer thickness
General 0.01-0.1mm；
Described flexible organic polymer backing material（4）Can be any other materials such as glass, plastics, polyester piece, specifically
In actual applications as needed depending on；
P-type of the present invention and n-type layer are all made up of technical grade conducting polymer, and preparation method is simple, in composite bed also not
Including any expensive nanoparticle conductive added material, great application and popularization value；
Various coatings in the present invention can also be prepared with methods such as spin coating, spraying or brushings；
Dielectric isolation layer of the invention（3）Can be substituted with any nonconducting polymer foil；
The physical dimension of thermoelectric material of the present invention can be arbitrarily devised.
Foundation needs, and mass percents of the PANI in the present invention in n-type layer can change between 75-90% scopes.
Mass percents of the P3HT in p-type layer can also change between 75-90% scopes.
Conducting polymer composite thermoelectric material of the present invention, by being present in the temperature gradient at thermoelectric material two ends, makes n-type
Thermal diffusion campaign is carried out with the carrier in p-type conductive, differential thermal electromotive force is produced at material two ends, can be applied to each
In the power supply and association area of the micro electronmechanical system of kind and device.
Conducting polymer composite thermoelectric material unit shown in accompanying drawing 1 can be carried out stacked combination configuration by connection in series-parallel,
Under certain temperature gradient conditions, bigger thermoelectromotive force or thermocurrent is obtained.
Claims (5)
1. a kind of composite thermoelectric material being made up of conducting polymer, it is characterised in that：
Including backing material（4）, in substrate material layer（4）The n-type conductive layer that upper spraying is mixed by PANI and PVDF（2）,
N-type conductive layer（2）It is prepared as follows：A certain proportion of N- crassitudes are poured into after PANI and PVDF powder is mixed
In ketone solvent, mix through strength ultrasonic agitation, after be put into 90 DEG C of baking ovens and bakee, treat the 1-METHYLPYRROLIDONE solvent of 60 %
After evaporation, mixed liquor becomes colloidal liquid, using spraying coating process in backing material（4）Upper spraying, composition thickness is 0.01-
The n-type conductive layer of 0.1mm（2）；The consumption of PANI accounts for the 75%~90% of PANI and PVDF mass summations, 1-METHYLPYRROLIDONE
Consumption it is identical with the gross mass of PANI and PVDF mixtures；
Then in the n-type conductive layer for preparing（2）On spray the dielectric isolation layer being made up of PVDF again（3）, dielectric isolation layer（3）
It is prepared as follows：PVDF polymer powders are dissolved in 1-METHYLPYRROLIDONE solvent, after mixing through strength ultrasonic agitation,
Bakeed in 90 DEG C of baking ovens, after after the 1-METHYLPYRROLIDONE solvent evaporation of 60 %, mixture will become agglutination viscous liquid,
Using spraying coating process in n-type conductive layer（2）Upper spraying, prepares dielectric isolation layer（3）, dielectric isolation layer（3）Thickness is
0.01-0.1mm；Prepare dielectric isolation layer（3）When, PVDF polymer powders are 1 ︰ 3 with the mass ratio of 1-METHYLPYRROLIDONE；
Finally, in dielectric isolation layer（3）On be coated with p-type conductive layer（1）, p-type conductive layer（1）It is prepared as follows：Will
A certain proportion of PVDF powder is mixed into 1-METHYLPYRROLIDONE solvent, strength ultrasonic agitation, after after fully dissolving, pours into P3HT
Powder, continues strength ultrasonic agitation uniformly, is put into baking in 90 DEG C of baking ovens, after 60% 1-METHYLPYRROLIDONE solvent evaporates,
Mixture will become agglutination viscous liquid, using spraying coating process in dielectric isolation layer（3）Upper spraying, prepares p-type conductive coating
（1）, coating layer thickness is 0.01-0.1mm；75%~90%, the PVDF that described P3HT consumptions account for P3HT and PVDF mass summations gathers
Compound powder is 1 ︰ 5 with the mass ratio of 1-METHYLPYRROLIDONE.
2. the composite thermoelectric material being made up of conducting polymer according to claim 1, it is characterised in that：Adjacent p-type
Conductive layer（1）With n-type conductive layer（2）Only it is connected with each other at one end.
3. the composite thermoelectric material being made up of conducting polymer according to claim 1, it is characterised in that：Described p-type
Conductive layer（1）, n-type conductive layer（2）And dielectric isolation layer（3）It is sandwich construction.
4. the composite thermoelectric material being made up of conducting polymer according to claim 1, it is characterised in that：Described
PANI, P3HT, PVDF polymer are technical grade articles for use.
5. the composite thermoelectric material being made up of conducting polymer according to claims 1 to 4, it is characterised in that：N-type is led
Electric layer（2）, p-type conductive layer（1）And positioned at middle dielectric isolation layer（3）The elementary cell of formation is overlapping to be repeated to configure, and is passed through
String and/or parallel way are external sys-tems.
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Cited By (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| WO2022171982A1 (en) * | 2021-02-11 | 2022-08-18 | Oxford University Innovation Limited | Thermoelectric generator device |
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| CN105210203A (en) * | 2013-03-14 | 2015-12-30 | 韦克森林大学 | Thermoelectric apparatus and articles and applications thereof |
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2017
- 2017-01-23 CN CN201710049491.2A patent/CN106816523A/en active Pending
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| CN101931043A (en) * | 2009-06-19 | 2010-12-29 | 清华大学 | Thermoelectric conversion material |
| CN103283049A (en) * | 2010-10-18 | 2013-09-04 | 韦克森林大学 | Thermoelectric apparatus and applications thereof |
| CN105210203A (en) * | 2013-03-14 | 2015-12-30 | 韦克森林大学 | Thermoelectric apparatus and articles and applications thereof |
| CN104518078A (en) * | 2014-11-26 | 2015-04-15 | 辽宁师范大学 | Electroconductive polymer composite thermoelectric material |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| WO2022171982A1 (en) * | 2021-02-11 | 2022-08-18 | Oxford University Innovation Limited | Thermoelectric generator device |
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