CN112652698B - Thermoelectric conversion material and thermoelectric conversion device - Google Patents
Thermoelectric conversion material and thermoelectric conversion device Download PDFInfo
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- CN112652698B CN112652698B CN202011544475.9A CN202011544475A CN112652698B CN 112652698 B CN112652698 B CN 112652698B CN 202011544475 A CN202011544475 A CN 202011544475A CN 112652698 B CN112652698 B CN 112652698B
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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
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- H10N10/85—Thermoelectric active materials
- H10N10/856—Thermoelectric active materials comprising organic compositions
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- H—ELECTRICITY
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- H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
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Abstract
The invention discloses a thermoelectric conversion material and a thermoelectric conversion device. This thermoelectric conversion material includes a matrix containing hydrogen ions; wherein the matrix comprises a hydrogel. The invention also provides a thermoelectric conversion device based on the thermoelectric conversion material. The thermoelectric conversion material provided by the invention has excellent thermoelectric conversion performance, and a thermoelectric conversion device prepared based on the thermoelectric conversion material has the capabilities of high open-circuit voltage, high output power and continuous output of electric power, and has wide application prospect.
Description
Technical Field
The present invention relates to the field of thermoelectric conversion technology, and in particular, to a thermoelectric conversion material and a thermoelectric conversion device.
Background
Compared with the transition of electrons in a semiconductor material, ions as charge carriers can directionally migrate under the action of a certain external field, and have more excellent characteristics. Through the reasonable material structure, ions realize the selective migration of anions and cations (similar to electrons-holes) in a high molecular aqueous solution system, and the ionic conductor thermoelectric material with the thermoelectric conversion function can be obtained. More importantly, the ions as carriers have the advantages of adjustable carrier concentration, charge number, ion size and species, and the ion migration can improve the open-circuit voltage performance of the thermoelectric conversion device by coupling redox reaction; meanwhile, the polymer aqueous solution system used as the medium has more material and structure controllability. In addition, the thermoelectric material based on the high polymer and the ionic system also has good flexibility, is easy to generate closer interface contact with a heat source, further reduces heat transfer loss and obviously improves thermoelectric conversion efficiency.
However, the ionic type thermoelectric conversion material also has some disadvantages. For example, the migration rate of ions is relatively slow, which causes the problems of low conductivity, low open-circuit voltage and low output power of the material, and most of them cannot form continuous external output electric work. Therefore, the current ionic thermoelectric conversion materials still need to be improved.
Disclosure of Invention
The invention aims to solve the problem of slow ion migration rate of the hydrogel-based thermoelectric material and improve the thermoelectric conversion efficiency of the hydrogel-based thermoelectric material. Accordingly, an object of the present invention is to provide a thermoelectric conversion material having excellent thermoelectric conversion performance, a second object of the present invention is to provide a method for producing the thermoelectric conversion material, and a third object of the present invention is to provide an application of the thermoelectric conversion material.
In order to achieve the purpose, the technical scheme adopted by the invention is as follows:
a first aspect of the invention provides a thermoelectric conversion material including a matrix containing hydrogen ions; the matrix comprises a hydrogel.
The matrix of the thermoelectric conversion material provided by the invention is ion conductor hydrogel which can effectively form a hydrogen bond system and has the advantage of high mobility of hydrogen ions.
Preferably, in the thermoelectric conversion material, the hydrogel includes at least one of a polyacrylamide hydrogel, a polyacrylic acid hydrogel, and a polyvinyl alcohol hydrogel.
Preferably, in the thermoelectric conversion material, the concentration of the hydrogen ions in the matrix is 0.01 to 4 mol/L; more preferably, the concentration of the hydrogen ions in the matrix is 0.1 to 2 mol/L; still more preferably, the concentration of the hydrogen ions in the matrix is 0.5mol/L to 1.5 mol/L.
Preferably, in the thermoelectric conversion material, the matrix further contains an acid ion.
Preferably, in the thermoelectric conversion material, the matrix contains a strong acid having a pKa (acidity coefficient) value of less than 1.
Preferably, the strong acid is at least one selected from the group consisting of sulfuric acid, hydrochloric acid, phosphoric acid, trichloroacetic acid, trinitrobenzenesulfonic acid. In some embodiments of the invention, a strong non-oxidizing inorganic acid is selected, such as sulfuric acid, hydrochloric acid, or phosphoric acid.
A second aspect of the invention provides a method for producing a thermoelectric conversion material according to the first aspect of the invention, comprising the steps of:
and carrying out polymerization reaction on hydrogel monomers in a solvent, and then dialyzing in acid liquor to obtain the thermoelectric conversion material.
Preferably, in the method for producing a thermoelectric conversion material, the hydrogel monomer includes at least one of an acrylamide monomer, an acrylic monomer, and polyvinyl alcohol; further preferably, the hydrogel monomer comprises at least one of acrylamide, methacrylamide, ethylacrylamide, sodium acrylate, potassium acrylate, methyl acrylate, ethyl acrylate, butyl acrylate, cyclohexyl acrylate, lauryl acrylate, isooctyl acrylate, methacrylic acid, methyl methacrylate, ethyl methacrylate, n-butyl methacrylate, isooctyl methacrylate, isobornyl methacrylate, lauryl methacrylate, 2-hydroxyethyl acrylate, 2-hydroxypropyl acrylate, 2-hydroxyethyl methacrylate, 2-hydroxypropyl methacrylate, polyvinyl alcohol; still further preferably, the hydrogel monomer includes at least one of acrylamide, sodium acrylate, potassium acrylate, and polyvinyl alcohol.
Preferably, in the method for producing a thermoelectric conversion material, the solvent is at least one selected from the group consisting of water, an alcohol solvent, an ether solvent, a ketone solvent, and an ester solvent; more preferably, the solvent is at least one selected from the group consisting of water, ethanol, isopropanol, glycerol, ethylene glycol, diethyl ether, acetone, and ethyl acetate. In some embodiments of the invention, the solvent is water.
Preferably, the method for producing a thermoelectric conversion material further includes adding an initiator to participate in a polymerization reaction.
Preferably, the initiator is selected from at least one of persulfate, azo initiators, acyl peroxides and dialkyl peroxides; further preferably, the initiator is at least one selected from the group consisting of potassium persulfate, sodium persulfate, and ammonium persulfate.
Preferably, the mass of the initiator is 0.02-0.1% of the mass of the hydrogel monomer; more preferably, the mass of the initiator is 0.03 to 0.06 percent of the mass of the hydrogel monomer.
Preferably, the method for producing a thermoelectric conversion material further includes adding a crosslinking agent to participate in a polymerization reaction.
Preferably, the crosslinking agent is selected from at least one of acrylamide crosslinking agent and acrylate crosslinking agent; further preferably, the crosslinking agent is at least one selected from the group consisting of methylenebisacrylamide and ethylene glycol dimethacrylate.
Preferably, in the method for producing a thermoelectric conversion material, the mass of the crosslinking agent is 0.08% to 0.15% of the mass of the hydrogel monomer; more preferably, the mass of the crosslinking agent is 0.09% to 0.12% of the mass of the hydrogel monomer.
Preferably, the method for producing a thermoelectric conversion material further comprises adding an accelerator to participate in the polymerization reaction.
Preferably, the accelerator is an amine; further preferably, the accelerator is a diamine and/or a polyamine. In some embodiments of the invention, the accelerator is tetramethylethylenediamine. The dosage of the accelerator can be adjusted according to actual needs, and belongs to the conventional technical means in the field.
Preferably, in the method for producing the thermoelectric conversion material, the temperature of the polymerization reaction is 20 ℃ to 80 ℃; further preferably, the temperature of the polymerization reaction is 20 ℃ to 60 ℃; still more preferably, the temperature of the polymerization reaction is 20 ℃ to 40 ℃. In some embodiments of the invention, the polymerization is carried out at room temperature (25 ℃).
Preferably, in the method for producing a thermoelectric conversion material, the acid solution is at least one selected from sulfuric acid, hydrochloric acid, phosphoric acid, trichloroacetic acid, and trinitrobenzenesulfonic acid; more preferably, the acid solution is at least one selected from sulfuric acid, hydrochloric acid, and phosphoric acid.
Preferably, in the preparation method of the thermoelectric conversion material, the concentration of the acid solution is 0.1mol/L to 2 mol/L; further preferably, the concentration of the acid solution is 0.3-1 mol/L; still more preferably, the concentration of the acid solution is 0.5mol/L to 0.75 mol/L.
A third aspect of the invention provides a thermoelectric conversion device comprising the thermoelectric conversion material according to the first aspect of the invention and an electrode; the electrode is connected to the thermoelectric conversion material.
Preferably, in the thermoelectric conversion device, the electrodes include two inert electrodes provided on both surfaces of the thermoelectric conversion material, respectively.
Preferably, in the thermoelectric conversion device, the thickness of the thermoelectric conversion material is 0.5mm to 15 mm.
Preferably, in the thermoelectric conversion device, the first inert electrode and the second inert electrode are each selected from a platinum electrode, a gold electrode, a carbon electrode, a platinum-plated electrode, or a gold-plated electrode. The carbon electrode is a composite electrode consisting of one or more of a graphite electrode, a carbon nanotube electrode and a carbon fiber material electrode.
Preferably, the thermoelectric conversion device continues to work on the external circuit under the temperature difference. Specifically, when a temperature difference is applied to the thermoelectric conversion device, an open-circuit voltage can be generated, and work can be continuously applied to an external circuit when a loop is formed.
Preferably, the working temperature range of the thermoelectric conversion device is-10 ℃ to 80 ℃. When the working temperature range is-10 ℃ to 80 ℃, the temperature gradient difference is preferably 0.1 ℃ to 79.9 ℃. Wherein, the temperature gradient difference is the difference between the high temperature end and the low temperature end.
More preferably, the operating temperature range of the thermoelectric conversion device is 0 to 40 ℃. When the working temperature range is 0-40 ℃, the temperature gradient difference is preferably 0.1-39.9 ℃.
Preferably, the load of each thermoelectric conversion device in operation is 400 Ω to 10000 Ω; further preferably, the load at the time of operation of each thermoelectric conversion device is 500 Ω to 9000 Ω.
Preferably, the output power of each of the thermoelectric conversion devices is 20 μ W to 60 μ W; further preferably, the output power of each thermoelectric conversion device is 20 μ W to 52 μ W.
A fourth aspect of the present invention provides a use of the thermoelectric conversion material according to the first aspect of the present invention in the field of internet of things, the field of sensing, or the field of wearable.
The invention has the beneficial effects that:
the thermoelectric conversion material provided by the invention has excellent thermoelectric conversion performance, and a thermoelectric conversion device prepared based on the thermoelectric conversion material has the capabilities of high open-circuit voltage, high output power and continuous electric power output.
The thermoelectric conversion material and the thermoelectric conversion device provided by the invention have the advantages of simple and easy preparation method, mild conditions, easily available raw materials and good repeatability, and have good application prospects in the fields of Internet of things, sensor functions, wearable electronics and the like.
Different from a common hydrogel-based thermoelectric conversion device, the device designed by the invention can continuously and stably output electric work to the outside under the condition of stable temperature difference.
Drawings
Fig. 1 is a schematic view of the structure of a thermoelectric conversion device of the present invention;
FIG. 2 is a graph of current versus time for the device of example 1 at a temperature differential of 0-40 ℃ and a 700 Ω load;
FIG. 3 is a graph of open-circuit voltage versus time for the device of example 1 at a temperature differential of 0-40 ℃;
FIG. 4 is a graph of power versus resistance for different loading conditions for the device of example 1 at a temperature differential of 0-40 deg.C.
Detailed Description
The present invention will be described in further detail with reference to specific examples. The starting materials, reagents or equipment used in the examples are, unless otherwise specified, either conventionally commercially available or may be obtained by methods known in the art. Unless otherwise indicated, the testing or testing methods are conventional in the art.
The open circuit voltage of the following examples was tested using the two electrode method.
Example 1
The method for producing the thermoelectric conversion material of this example was as follows:
taking 3.75g of acrylamide, 1.25g of sodium acrylate, 5.0mg of methylene bisacrylamide and an aqueous solution containing 2.0mg of potassium persulfate, adding 18.0mL of deionized water, uniformly mixing, adding 0.05mL of tetramethylethylenediamine serving as an accelerator, carrying out dialysis in 0.5mol/L sulfuric acid after the polymerization reaction at room temperature is finished, and preparing the hydrogel with the sulfuric acid concentration (by hydrogen ion concentration) of 0.5 mol/L.
Fig. 1 is a schematic view of the structure of a thermoelectric conversion device of the present invention. In fig. 1, 1 is an inert electrode plate, 2 is a thermoelectric conversion material, and 3 is an inert electrode plate. Referring to the schematic view of fig. 1, the thermoelectric conversion material having a thickness of 15mm prepared in this example was assembled by connecting platinum sheet electrode plates to the upper and lower surfaces thereof, respectively.
The temperature difference of 0-40 ℃ is loaded on the two polar plates of the thermoelectric conversion device, the output open-circuit voltage of the thermoelectric conversion device is more than 600mV, and the thermoelectric conversion device can continuously and stably output electric work under a certain load. FIG. 2 is a graph of current versus time (i-t plot) for the device of example 1 at 0-40 deg.C differential and 700 Ω load. FIG. 3 is a graph of open-circuit voltage versus time (V-t plot) for the device of example 1 at a temperature differential of 0-40 deg.C. As can be seen from fig. 3, the thermoelectric conversion device of example 1 outputted an open-circuit voltage of more than 600mV at a temperature difference of 0 to 40 ℃. FIG. 4 is a graph of the power versus resistance (P-R plot) of the device of example 1 at different loading conditions at a temperature differential of 0-40 deg.C. As can be seen from fig. 4, the thermoelectric conversion device of example 1 has an output power of 20 μ W to 52 μ W under a load of 500 Ω to 9000 Ω.
Example 2
The method for producing the thermoelectric conversion material of this example was as follows:
taking 3.33g of acrylamide, 1.67g of potassium acrylate, 6.0mg of ethylene glycol dimethacrylate and an aqueous solution containing 3.0mg of potassium persulfate, adding 15.0mL of deionized water, uniformly mixing, adding 0.05mL of tetramethylethylenediamine serving as an accelerator, carrying out dialysis in 0.75mol/L sulfuric acid after the polymerization reaction at room temperature is finished, and preparing the hydrogel with the sulfuric acid concentration (calculated by hydrogen ion concentration) of 0.75 mol/L.
Referring to fig. 1, the thermoelectric conversion material having a thickness of 15mm prepared in this example was assembled by connecting platinum sheet electrode plates to the upper and lower surfaces thereof, respectively. The temperature difference of 0-40 ℃ is loaded on the two polar plates of the thermoelectric conversion device, the output open-circuit voltage is more than 600mV, and the thermoelectric conversion device can continuously and stably output electric work under a certain load.
Example 3
The method for producing the thermoelectric conversion material of this example was as follows:
taking 3.75g of acrylamide, 1.25g of sodium acrylate, 5.0mg of methylene bisacrylamide, 0.3g of polyvinyl alcohol and an aqueous solution containing 2.0mg of potassium persulfate, adding 15.0mL of deionized water, uniformly mixing, adding 0.05mL of tetramethylethylenediamine serving as an accelerator, carrying out dialysis in 0.5mol/L sulfuric acid after the polymerization reaction at room temperature is finished, and preparing the hydrogel with the sulfuric acid concentration (calculated by hydrogen ion concentration) of 0.5 mol/L.
Referring to fig. 1, the thermoelectric conversion material having a thickness of 15mm prepared in this example was assembled by connecting platinum sheet electrode plates to the upper and lower surfaces thereof, respectively. The temperature difference of 0-40 ℃ is loaded on the two polar plates of the thermoelectric conversion device, the output open-circuit voltage is more than 700mV, and the thermoelectric conversion device can continuously and stably output electric work under a certain load.
Through tests, the Seebeck coefficient of the thermoelectric conversion device provided by the embodiment of the invention can reach 25mV/K in the range of 0-40 ℃, and the Seebeck coefficient of the thermoelectric conversion device reported at present is about 10mV/K at most.
Experiments prove that the thermoelectric conversion device which has high open-circuit voltage and output power and can continuously output electric power is obtained by combining the hydrogel and the high mobility of hydrogen ions in the hydrogel. When a temperature difference is given, the device can continuously and stably output electric power to a load.
The invention provides a hydrogel material with low-quality heat energy (the temperature is lower than 100 ℃), and the thermoelectric conversion material and the thermoelectric conversion device can realize the conversion between the heat energy and the electric energy at the temperature lower than 100 ℃, improve the utilization efficiency of the heat energy and have good application value.
The above embodiments are preferred embodiments of the present invention, but the present invention is not limited to the above embodiments, and any other changes, modifications, substitutions, combinations, and simplifications which do not depart from the spirit and principle of the present invention should be construed as equivalents thereof, and all such changes, modifications, substitutions, combinations, and simplifications are intended to be included in the scope of the present invention.
Claims (8)
1. A thermoelectric conversion material characterized in that: comprises a substrate containing hydrogen ions; the matrix comprises a hydrogel;
the hydrogel comprises at least one of polyacrylamide hydrogel, polyacrylic acid hydrogel and polyvinyl alcohol hydrogel;
the concentration of the hydrogen ions in the matrix is 0.01-4 mol/L;
the method for producing the thermoelectric conversion material includes the steps of:
and carrying out polymerization reaction on hydrogel monomers in a solvent, and then dialyzing in acid liquor to obtain the thermoelectric conversion material.
2. A thermoelectric conversion material according to claim 1, characterized in that: the matrix contains a strong acid having a pKa value of less than 1.
3. A method for producing a thermoelectric conversion material according to any one of claims 1 to 2, characterized in that: the method comprises the following steps:
and carrying out polymerization reaction on hydrogel monomers in a solvent, and then dialyzing in acid liquor to obtain the thermoelectric conversion material.
4. A thermoelectric conversion device, characterized in that: comprising the thermoelectric conversion material according to any one of claims 1 to 2 and an electrode; the electrode is connected to the thermoelectric conversion material.
5. The thermoelectric conversion device according to claim 4, wherein: the electrodes include two inert electrodes respectively provided on both surfaces of the thermoelectric conversion material.
6. The thermoelectric conversion device according to claim 5, wherein: the thermoelectric conversion device continuously applies work to the external circuit under the temperature difference.
7. The thermoelectric conversion device according to claim 6, wherein: the working temperature range of the thermoelectric conversion device is-10 ℃ to 80 ℃.
8. Use of the thermoelectric conversion material according to any one of claims 1 to 2 in the field of internet of things, sensing, or wearable.
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| CN113644785B (en) * | 2021-10-14 | 2022-02-22 | 启东市飞宏自动化设备有限公司 | Heat dissipation protection device for motor |
| CN114350094B (en) * | 2021-12-08 | 2022-11-08 | 广东省科学院化工研究所 | Temperature-sensitive thermoelectric hydrogel and preparation method and application thereof |
| CN114479332B (en) * | 2021-12-29 | 2023-12-05 | 广东省科学院化工研究所 | Ion conductor thermoelectric material and preparation method and application thereof |
| CN114497258B (en) * | 2021-12-30 | 2023-04-07 | 广东省科学院化工研究所 | Photoelectric and thermoelectric combined device |
| CN115172579B (en) * | 2022-09-05 | 2023-02-07 | 广东省科学院化工研究所 | Thermoelectric conversion device and preparation method thereof |
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| CN1528029A (en) * | 2001-05-10 | 2004-09-08 | �����֯��ʽ���� | Polymer gel electrlyte-use composition and method of pouring non-aqueous electrolyte solution |
| JP2016018809A (en) * | 2014-07-04 | 2016-02-01 | 国立大学法人広島大学 | Thermoelectric conversion material and method of manufacturing the same |
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| KR102324383B1 (en) * | 2018-12-10 | 2021-11-11 | 연세대학교 산학협력단 | Ionic thermoelectric materials and ionic thermoelectric devices comprising the same |
| US20200299466A1 (en) * | 2019-03-03 | 2020-09-24 | Massachusetts Institute Of Technology | Pure conducting polymer hydrogel and hydrogel precursor materials having extraordinary electrical, mechanical and swelling properties and methods of making |
| CN110808329B (en) * | 2019-11-13 | 2021-03-23 | 四川大学 | Phthalocyanine copper sulfonic acid doped polymer-based thermoelectric material and preparation method and application thereof |
| CN111333868A (en) * | 2020-03-26 | 2020-06-26 | 武汉大学 | Composite hydrogel with synchronous evaporation heat dissipation and waste heat recovery capabilities, preparation method and thermal management method |
| CN111564316B (en) * | 2020-04-13 | 2022-03-04 | 东华大学 | Gel electrode, full-gel-state ion thermoelectric supercapacitor and preparation thereof |
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| CN1528029A (en) * | 2001-05-10 | 2004-09-08 | �����֯��ʽ���� | Polymer gel electrlyte-use composition and method of pouring non-aqueous electrolyte solution |
| JP2016018809A (en) * | 2014-07-04 | 2016-02-01 | 国立大学法人広島大学 | Thermoelectric conversion material and method of manufacturing the same |
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