CN106299102A - A kind of thermoelectricity colloidal materials and the preparation method of device and product - Google Patents
A kind of thermoelectricity colloidal materials and the preparation method of device and product Download PDFInfo
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- CN106299102A CN106299102A CN201610735613.9A CN201610735613A CN106299102A CN 106299102 A CN106299102 A CN 106299102A CN 201610735613 A CN201610735613 A CN 201610735613A CN 106299102 A CN106299102 A CN 106299102A
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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
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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
- H10N19/00—Integrated devices, or assemblies of multiple devices, comprising at least one thermoelectric or thermomagnetic element covered by groups H10N10/00 - H10N15/00
- H10N19/101—Multiple thermocouples connected in a cascade arrangement
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Abstract
The invention discloses a kind of thermoelectricity colloidal materials and the preparation method of device and product, after being mixed mutually with redox electrolytes matter by polymer solution, product is prepared thermoelectricity colloid through cured;Thermoelectricity colloid regulates and controls thermoelectrochemistry Seebeck coefficient and thermoelectricity output performance by changing redox electrolytes matter;Owing to this thermoelectricity colloid has the characteristic of flexible extensible, by mould, this thermoelectricity colloid is prepared as required solid shape;It is integrated that the thermoelectricity colloid of solid-state is applicable to large-area encapsulation;Integrated it is prepared as thermo-electric device by thermoelectricity colloid and electrode being packaged;Low yardstick heat energy can be converted into electric energy by this thermo-electric device effectively, has wide application prospect on flexible electronic device and wearable device.
Description
Technical field
The invention belongs to technical field of new energies, more particularly, to a kind of thermoelectricity colloidal materials and the preparation side of device
Method and product.
Background technology
Along with wearable electronic device and the development of electronic skin, their energy resource supply gradually causes the concern of people.
In numerous self-driven energy supplyystems, heat energy be widely present in environment and commercial production, especially human body and environment it
Between heat energy, electric energy can be converted into wearable device energy supply.
The thermoelectrochemistry Seebeck coefficient of traditional quasiconductor and polymer thermoelectric material is the least, and this two classes material
Flex capability poor, cost is higher, preparation process is loaded down with trivial details;These factors seriously limit their extensive application.Prior art
In thermo-electric converting device, utilize thermoelectrochemistry effect (Thermogalvanic Effect), can obtain the biggest
Seebeck coefficient, in this kind of thermoelectrochemistry device, containing redox electrolytes matter, when two electrodes are maintained at different temperatures
Just can produce electric energy output;But the participation due to liquid electrolyte so that this kind of thermoelectrochemistry device is in encapsulation and big face
Productive set is very limited on becoming, it is difficult to be applied to the energy supply of wearable electronic.
Summary of the invention
For disadvantages described above or the Improvement requirement of prior art, the invention provides a kind of thermoelectricity colloidal materials and device
Preparation method and product, its object is to be difficult to by improving thermoelectricity colloidal materials to solve existing thermoelectrochemistry device
Encapsulation and integrated technical problem.
For achieving the above object, according to one aspect of the present invention, it is provided that the preparation method of a kind of thermoelectricity colloidal materials,
Comprise the steps:
(1) at a temperature of 80~90 DEG C, it is equipped with the polymer solution of 0.01~0.1g/mL;
(2) under the mixing speed of 200~500 rpms, the speed with 0.05~0.1mL/s is molten toward above-mentioned polymer
Liquid is slowly added to redox electrolytes matter, and mixes to uniformly, it is thus achieved that middleware;
(3) above-mentioned middleware mould is carried out cured, prepare variously-shaped thermoelectricity colloid.
Preferably, the preparation method of above-mentioned thermoelectricity colloidal materials, polymer uses polyvinyl alcohol (PVA), polymethyl
Acid methyl ester (PMMA) or polyethylene glycol oxide (PEO).
Preferably, the preparation method of above-mentioned thermoelectricity colloidal materials, redox electrolytes matter uses Fe2+/Fe3+、Np3+/Np4+
Or Fe (CN)6 4-/Fe(CN)6 3-。
For realizing the purpose of the present invention, according to another aspect of the present invention, it is provided that the preparation side of a kind of thermo-electric device
Method, comprises the steps:
(1) formation of deposits metal electrode on a flexible substrate;
(2) thermoelectricity colloid is placed between two panels metal electrode, uses polydimethylsiloxane (PDMS) or asphalt mixtures modified by epoxy resin
Fat is packaged around the thermoelectricity colloid between metal electrode, it is thus achieved that thermo-electric device.
Preferably, the preparation method of above-mentioned thermo-electric device, metal electrode uses cr-au electrode;Flexible substrates uses polyamides sub-
Amine (PI) or polyethylene terephthalate (PET).
For realizing the purpose of the present invention, according to another aspect of the present invention, it is provided that a kind of thermoelectricity colloid, it is specially
PVA-FeCl2/FeCl3Colloid, PVA-K4Fe(CN)6/K3Fe(CN)6Colloid or PVA-Np (NO3)3/Np(NO3)4Colloid.
It is another aspect of this invention to provide that provide a kind of thermo-electric device, by the thermoelectricity colloid of opposed polarity is utilized
The series connection of cross over metal electrode is formed;Series connection formed thermo-electric device, its output voltage equal to single thermoelectricity colloid output voltage it
With.
Preferably, above-mentioned thermo-electric device, its thermoelectricity colloid uses PVA-FeCl2/FeCl3Colloid and PVA-K4Fe(CN)6/
K3Fe(CN)6Colloid.
In general, by the contemplated above technical scheme of the present invention compared with prior art, it is possible to show under acquirement
Benefit effect:
(1) preparation method of thermoelectricity colloid that the present invention provides, by composition polymer with have thermoelectrochemistry performance
Redox electrolytes matter prepares the colloid with thermoelectricity capability, owing to have employed polymeric material, and prepared colloid tool
There is certain mechanical performance, the required various form of the application such as column or bulk can be solidified into, and maintain oxidoreduction
The thermoelectrochemistry performance of electrolyte, prepared thermoelectricity colloid has the highest Seebeck coefficient, has under the temperature difference of low yardstick
Bigger thermoelectric voltage is had to export, it is adaptable to prepare thermo-electric device;
The Seebeck coefficient ratio semi-conductor thermoelectric material of thermoelectrochemistry material is much larger, and this is the excellent of thermoelectrochemistry effect
Gesture, but the material (redox electrolytes matter) with focus chemical effect mostly is liquid;Use liquid to prepare device to exist
In encapsulation extremely complex, use solid-state material then can solve encapsulation problem;The preparation method that the present invention provides, utilizes polymerization
Thing reaches the purpose processed by redox electrolytes matter semi-solid preparation, had both been had solid mechanical performance, and had had again pyroelectric effect
Colloid;
(2) according to the thermoelectricity colloid prepared by preparation method provided by the present invention, compared to liquid heat electrochemical material,
It is easier to encapsulation acquisition and determines thermo-electric device;
(3) according to the thermo-electric device prepared by preparation method provided by the present invention, by by the thermoelectricity glue of opposed polarity
Body carries out series connection, and to realize large area integrated, it is thus achieved that possesses the thermo-electric device of flexible wearable characteristic.
Accompanying drawing explanation
Fig. 1 is to utilize the PVA-FeCl prepared by embodiment 12/FeCl3The thermoelectricity capability of the thermo-electric device that colloid is made shows
It is intended to;
Fig. 2 is the PVA-K prepared by embodiment 24Fe(CN)6/K3Fe(CN)6The pyroelectricity of the thermo-electric device that colloid is made
Can schematic diagram;
Fig. 3 is the PVA-FeCl of embodiment 12/FeCl3Thermo-electric device and the PVA-K of embodiment 24Fe(CN)6/K3Fe(CN)6
The thermoelectricity capability schematic diagram of thermo-electric device series connection;
Fig. 4 is the PVA-FeCl of embodiment 32/FeCl3Thermo-electric device and PVA-K4Fe(CN)6/K3Fe(CN)6Thermoelectricity device
The integrated schematic diagram of part;
Fig. 5 is the thermoelectricity capability schematic diagram of the integrated focus device of embodiment 3;
In all of the figs, identical reference is used for representing identical element or structure, wherein:
1-electrode, 2-flexible substrates, 3-PVA-FeCl2/FeCl3Thermoelectricity colloid,
4-PVA-K4Fe(CN)6/K3Fe(CN)6Thermoelectricity colloid.
Detailed description of the invention
In order to make the purpose of the present invention, technical scheme and advantage clearer, below in conjunction with drawings and Examples, right
The present invention is further elaborated.Should be appreciated that specific embodiment described herein only in order to explain the present invention, and
It is not used in the restriction present invention.If additionally, technical characteristic involved in each embodiment of invention described below
The conflict of not constituting each other just can be mutually combined.
Embodiment 1
The thermoelectricity colloid preparation method that embodiment 1 provides, comprises the steps:
(1) 4g polymer powder is dissolved at 80 DEG C 40mL water, it is thus achieved that the polymer solution of clarification;
(2) when above-mentioned polymer solution is clarified, with the speed of 0.1mL/s by the FeCl of 10mL0.1M2/FeCl3(contain
1mL HCl, precaution of hydrolysis) it is slowly added into the polymer solution of above-mentioned clarification, stir under the mixing speed of 200 rpms
Uniformly, it is thus achieved that PVA-FeCl2/FeCl3Colloid;
(3) using mould to be solidified by above-mentioned PVA-FeCl2/FeCl3 colloid, make a diameter of 3mm, thickness is the circle of 1mm
Column colloid.
Thermoelectricity colloid prepared by embodiment 1 utilize polydimethylsiloxane (PDMS) be packaged in two panels cr-au electrode it
Between, it is thus achieved that thermo-electric device;Wherein, cr-au electrode is plated on PI (polyimide, polyimides) film.
Shown in Fig. 1, it is the PVA-FeCl prepared by preparation method utilizing embodiment 12/FeCl3The thermoelectricity device that colloid is made
The thermoelectricity capability schematic diagram of part;Its Seebeck coefficient is 1.02mV K-1, temperature end electrode voltage is just, short under 20 DEG C of temperature difference
Road electric current is 2.96Am-2。
Embodiment 2
The thermoelectricity colloid preparation method that embodiment 2 provides, comprises the steps:
(1) 4g polyvinyl alcohol is dissolved at 85 DEG C 400mL water, it is thus achieved that polymer solution;
(2) when above-mentioned polymer solution is clarified, with the speed of 0.07mL/s by the K of 10mL0.1M4Fe(CN)6/K3Fe
(CN)6Being slowly added into the polymer solution of clarification, under the mixing speed of 300 rpms, stirring is allowed to uniform dissolution, obtains
Obtain PVA-K4Fe(CN)6/K3Fe(CN)6Colloid;
(3) use mould by above-mentioned PVA-K4Fe(CN)6/K3Fe(CN)6Colloid solidifies, and makes a diameter of 3mm, and thickness is
The cylindric colloid of 1mm;
Thermoelectricity colloid prepared by embodiment 2 utilize polydimethylsiloxane (PDMS) be packaged in two panels cr-au electrode it
Between, it is thus achieved that thermo-electric device;Wherein, cr-au electrode is plated on PI film.
Utilize the PVA-K prepared by the preparation method of embodiment 24Fe(CN)6/K3Fe(CN)6The thermo-electric device that colloid is made
Thermoelectricity capability as in figure 2 it is shown, its Seebeck coefficient is-1.21mV K-1, temperature end electrode voltage is negative, under 20 DEG C of temperature difference
Short circuit current is-0.86Am-2。
By the PVA-FeCl prepared by embodiment 12/FeCl3Thermo-electric device and the PVA-K prepared by embodiment 24Fe
(CN)6/K3Fe(CN)6Thermo-electric device is connected;Specifically, by PVA-FeCl2/FeCl3Thermo-electric device and PVA-K4Fe(CN)6/K3Fe
(CN)6Thermo-electric device hot junction connects together, and picks out electrode respectively from the cold end of the two thermo-electric device and tests;This serializer
The thermoelectricity capability curve of part as it is shown on figure 3, under 10 DEG C of temperature difference open-circuit voltage be 23mV, short circuit current is 3.5 μ A;Test result
Show, PVA-FeCl2/FeCl3Thermo-electric device and PVA-K4Fe(CN)6/K3Fe(CN)6Thermo-electric device is effectively cascaded, can
Greatly strengthen the thermoelectricity output performance of thermo-electric device.
Embodiment 3
In order to improve the thermoelectricity output performance of thermo-electric device further, increase output voltage and electric current, by made for embodiment 1
Standby PVA-FeCl2/FeCl3Thermo-electric device and the PVA-K prepared by embodiment 24Fe(CN)6/K3Fe(CN)6Thermo-electric device is carried out
Integrated process as shown in Figure 4, comprises the steps:
(1) deposition intersection cr-au electrode in PI flexible substrates;
(2) on intersection cr-au electrode, it is arranged in order 59 PVA-FeCl2/FeCl3Colloid cylinder and 59 PVA-K4Fe
(CN)6/K3Fe(CN)6Colloid cylinder, it is thus achieved that middleware;
(3) the surrounding employing PDMS of above-mentioned middleware is packaged, it is thus achieved that wearable flexible thermal electrical part;
Human body heat energy directly can be converted into electric energy by this wearable flexible thermal electrical part of embodiment 3 encapsulation preparation,
Its thermoelectricity capability schematic diagram is as shown in Figure 5: in the environment of 5 degrees Celsius, this wearable flexible thermal electrical part is attached to arm
On, output voltage can reach 0.6V, and output electric current reaches 2 μ A;Voltage reaches volts, close to functional need, has played
Effect land productivity Studies of Human Body Heat energy and the effect of low yardstick heat energy.
Embodiment 4
The thermoelectricity colloid preparation method that embodiment 4 provides, comprises the steps:
(1) at 90 DEG C, 4g polyethylene glycol oxide is dissolved in 60mL water, it is thus achieved that polymer solution;
(2) when above-mentioned polymer solution is clarified, with the speed of 0.05mL/s by the FeCl of 20mL 0.1M2/FeCl3(contain
Have 1mL HCl, precaution of hydrolysis) it is slowly added into the polymer solution of clarification, under the mixing speed of 400 rpms, stirring is all
Even, it is thus achieved that PEO-FeCl2/FeCl3Colloid;
(3) use mould by above-mentioned PEO-FeCl2/FeCl3Colloid solidifies, and makes a diameter of 3mm, and thickness is the cylinder of 1mm
Body.
Thermoelectricity colloid embodiment 4 prepared utilizes epoxy encapsulation between cr-au electrode (being plated on PET film), obtains
Obtain thermo-electric device;The Seebeck coefficient of this thermo-electric device is 0.90mV K-1, temperature end electrode voltage is just, under 20 DEG C of temperature difference
Short circuit current is 2.3Am-2。
The thermoelectricity colloid preparation method that embodiment 5 provides, comprises the steps:
(1) 10mL is contained Np and the 1M salpeter solution of 0.05M, under the electric current of 10mA, utilizes gold electrode electrolysis to obtain
Np3+/Np4+Redox electrolytes matter;
(2) 4g polymethyl methacrylate is dissolved at 87 DEG C 100mL water, it is thus achieved that polymer solution;
(3) when above-mentioned polymer solution is clarified, with the speed of 0.08mL/s by 10mLNp3+/Np4+Redox electrolytes
Matter is slowly added into the polymer solution of clarification, stirs, it is thus achieved that PMMA-Np under the mixing speed of 500 rpms
(NO3)3/Np(NO3)4Colloid;
(4) use mould by above-mentioned PMMA-Np (NO3)3/Np(NO3)4Colloid solidifies, and makes a diameter of 3mm, thickness is
The cylinder of 1mm.
Thermoelectricity colloid prepared by embodiment 5 utilize epoxy encapsulation in two panels cr-au electrode (being plated on PET film) it
Between, it is thus achieved that thermo-electric device;The Seebeck coefficient of this thermo-electric device is 1.5mV K-1, temperature end electrode voltage is just, 20 DEG C of temperature
The lower short circuit current of difference is 2.8Am-2。
As it will be easily appreciated by one skilled in the art that and the foregoing is only presently preferred embodiments of the present invention, not in order to
Limit the present invention, all any amendment, equivalent and improvement etc. made within the spirit and principles in the present invention, all should comprise
Within protection scope of the present invention.
Claims (8)
1. the preparation method of a thermoelectricity colloidal materials, it is characterised in that comprise the steps:
(1) at 80~90 DEG C, it is equipped with the polymer solution of 0.01~0.1g/mL;
(2) under the mixing speed of 200~500 rpms, the speed with 0.05~0.1mL/s is toward in described polymer solution
It is slowly added to redox electrolytes matter, and mixes to uniformly, it is thus achieved that middleware;
(3) described middleware is carried out cured to obtain thermoelectricity colloid.
2. preparation method as claimed in claim 1, it is characterised in that described polymer uses polyvinyl alcohol, polymethyl
Acid methyl ester or polyethylene glycol oxide.
3. preparation method as claimed in claim 1 or 2, it is characterised in that described redox electrolytes matter uses Fe2+/Fe3+、
Np3+/Np4+Or Fe (CN)6 4-/Fe(CN)6 3-。
4. a thermoelectricity colloid, it is characterised in that described thermoelectricity colloid is PVA-FeCl2/FeCl3Colloid, PVA-K4Fe(CN)6/
K3Fe(CN)6Colloid or PVA-Np (NO3)3/Np(NO3)4Colloid.
5. the preparation method of a thermo-electric device, it is characterised in that comprise the steps:
(1) formation of deposits metal electrode on a flexible substrate;
(2) thermoelectricity colloid is placed between two panels metal electrode, uses polydimethylsiloxane or epoxy resin, to described thermoelectricity
The periphery of colloid is packaged, it is thus achieved that thermo-electric device.
6. preparation method as claimed in claim 5, it is characterised in that described metal electrode uses cr-au electrode, described flexibility
Substrate uses polyimides or polyethylene terephthalate.
7. a thermo-electric device, it is characterised in that described thermo-electric device by utilizing intersection gold by the thermoelectricity colloid of opposed polarity
Belong to electrode series connection to be formed.
8. thermo-electric device as claimed in claim 7, it is characterised in that described thermoelectricity colloid uses PVA-FeCl2/FeCl3Colloid
And PVA-K4Fe(CN)6/K3Fe(CN)6Colloid.
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CN110364617A (en) * | 2018-04-10 | 2019-10-22 | 深圳光启尖端技术有限责任公司 | A kind of manufacturing method of flexibility thermo-electric device and its flexible thermo-electric device obtained |
KR102123319B1 (en) * | 2019-09-23 | 2020-06-17 | 재단법인대구경북과학기술원 | Flexible thermoelectric module and manufacturing methods thereof |
CN111392690A (en) * | 2020-03-20 | 2020-07-10 | 北京航空航天大学杭州创新研究院 | Pressure sensing system based on thin film thermoelectric device power supply and preparation method thereof |
CN112713233A (en) * | 2019-10-25 | 2021-04-27 | 南方科技大学 | Quasi-solid-state ionic thermoelectric conversion material, thermoelectric conversion device and application thereof |
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CN110364617A (en) * | 2018-04-10 | 2019-10-22 | 深圳光启尖端技术有限责任公司 | A kind of manufacturing method of flexibility thermo-electric device and its flexible thermo-electric device obtained |
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CN112713233B (en) * | 2019-10-25 | 2023-09-26 | 南方科技大学 | Quasi-solid ionic thermoelectric conversion material, thermoelectric conversion device and application thereof |
CN111392690A (en) * | 2020-03-20 | 2020-07-10 | 北京航空航天大学杭州创新研究院 | Pressure sensing system based on thin film thermoelectric device power supply and preparation method thereof |
CN111392690B (en) * | 2020-03-20 | 2023-04-07 | 北京航空航天大学杭州创新研究院 | Pressure sensing system based on thin film thermoelectric device power supply and preparation method thereof |
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