CN101894905B - Flexible thermoelectric semiconductor power generator and preparation method thereof - Google Patents
Flexible thermoelectric semiconductor power generator and preparation method thereof Download PDFInfo
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Abstract
The invention relates to a flexible thermoelectric semiconductor power generator and a preparation method thereof. In the method, a cold end ceramic plate is cut along the gaps between the p/n elements of each pair of thermocouples connected along hot end electrodes on the basis of obtaining mutually independent p-n thermocouple pairs by spraying high temperature end electrodes; the hot ends of each pair of p-n thermocouple pairs are mutually independent, and each pair of p/n elements forming the thermocouple pair is mutually independent at the cold end along the directions of heat expansion and cold contraction of hot end flow guide bars; and certain spaces for the cold surface and the hot surface of each pair of thermocouples are reserved under thermal shock so as to release the stress of the thermal shock, so that flexible connection is realized and the non-rigid connection thermoelectric power generator, namely the flexible-connection thermoelectric power generator, which can completely release the thermal shock stress is obtained. The flexible thermoelectric semiconductor power generator has the characteristics of simple process, low cost, high conversion efficiency, suitability for recycling of waste heat with different low grades, high thermal shock resistance, high performance stability after long-term use and long service life and the like, and is suitable for industrialized mass preparation of the flexible thermoelectric semiconductor power generator.
Description
Technical field
The present invention relates to a kind of flexible thermoelectric semiconductor power generator and preparation method thereof, belong to thermoelectric power generation device technical field.
Background technology
The thermoelectric semiconductor thermo-electric generation utilizes semi-conductive Seebeck effect that heat energy directly is converted to electric energy, possess movement-less part, noiselessness, free of contamination advantage, low-grade heat energy (＜350 ℃) is difficult to reclaim one of difficult point that becomes the raising energy utilization rate simultaneously.Therefore, thermoelectric power generation becomes in the world competitively one of focus of research as a kind of new and high technology of energy field, and will produce great influence to mankind's 21 century economic life and social development.
Though thermoelectric power generation device movement-less part, on it is applied to low-grade exhaust heat generating, as: vehicle exhaust, engine, incineration firing, factory's used heat, family expenses charcoal burner etc., the variations in temperature of used heat is big and fast.Electrothermal module must through heating end from room temperature-40 ℃～100 ℃ to serviceability temperature-40 ℃～400 ℃, cold junction is-40 ℃～200 ℃ thermal shock.Since thermocouple between for being rigidly connected, the thermal stress that the thermal shock of thermoelectric power generation device causes down is difficult to discharge, and causes solder joint loosening until coming off, and constantly increases with prolongation interchange (AC) resistance of service time, finally causes component failure.How discharging the thermal stress of thermoelectric power generation device thermal shock in low-grade heat source reclaims, is the unique channel that guarantees that its stable performance life-span is long.Be in technical know-how and experimental results show that it all is the use field of expansion thermoelectric power generation and the effective ways that improve energy utilization rate.
With the thermocouple in the thermoelectric power generation device between connection become and flexibly connect, be to solve the effective way that the thermoelectric device thermal stress is difficult to discharge.At present, flexibly connecting the method for preparing electrothermal module has: the thermoelectric cooling module cold junction adopts printing screen plate formula soldering layer to connect soldering layer and flow deflector, flexibly connects the cold junction potsherd and flow guide bar discharges thermal stress with the heat-conducting glue conduct; Electrothermal module rubber-like fine metal mesh is installed between first electrode and the thermoelectric element as conducting element, can be released in the thermal stress of short transverse.Yet the flexibly connecting of thermoelectric cooling has only huyashi-chuuka (cold chinese-style noodles) to exist, and this method can only be used for serviceability temperature below 100 ℃, simultaneously the every pair of thermocouple to hot side still be rigidly connected, thermal stress can't discharge fully.The interpolation wire can only solve thermal stress release longitudinally in the electrothermal module, laterally is still to be rigidly connected, and can't discharge the thermoelectric device thermal stress that thermal shock produces in Waste Heat Recovery fully.
Summary of the invention
The objective of the invention is to, provide that a kind of technology is simple, rate of finished products is high, cost is low, conversion efficiency of thermoelectric is high, high temperature resistant, thermal shock resistance strong, long-term serviceability good stability, reliability height, is applicable to that industrial mass prepares the product and the technology of preparing of flexible thermoelectric semiconductor power generator.
Technical scheme of the present invention is, the thermoelectric device of the present invention's preparation is to adopt spraying to obtain on the right basis of p-n thermocouple independent of each other at existing (seeing application number 201010148997.7 for details) temperature end electrode, the cold junction ceramic wafer is cut open width of slit 0.2 ± 0.1mm along the right interelement slit of p/n of every pair of thermocouple that the hot junction electrode connects.Connect hot-end coating electrode and blank pottery with heat-conducting cream.So the right hot junction of the every pair of p-n thermocouple is independently of one another, it is also independently of one another along the hot junction flow guide bar direction of expanding with heat and contract with cold at cold junction to constitute every pair of right p/n element of this thermocouple simultaneously.Under thermal shock every pair independently the cold thermocouple hot side all have certain space to discharge the stress that thermal shock produces, realization flexibly connects, and obtains the thermoelectric generator that a kind of thermoelectric generator that can discharge the non-rigid connection of thermal shock stress fully promptly flexibly connects.
Flexible thermoelectric semiconductor power generator of the present invention is " sandwich " version, and described thermoelectric power generation device possesses:
Light face ceramic insulating substrate as the high temperature hot junction;
The ceramic insulating substrate of the band metallic pattern that separates as low temperature cold junction polylith;
Bismuth telluride-base p/n type element between cold and hot end ceramic insulating substrate;
As the water conservancy diversion copper sheet of low-temperature end electrode and the coating electrode of temperature end.
The preparation method of flexible thermoelectric semiconductor power generator of the present invention is:
(1) is raw material with the thermoelectric crystal bar of the p/n type for preparing, cuts into thickness, will cut into bottom surface 0.6 * 0.6mm～6.0 * 6.0mm, tall and big behind the large stretch of surface metalation of the p/n that cut in the p/n of 0.6mm type element greater than the thick p/n sheet of 0.6mm.
(2) will hang up the flow deflector of burn-oning behind the lead-free solder of Sn95Sb5 of 227 ℃ Sn93Cu7 or 240 ℃ with the huyashi-chuuka (cold chinese-style noodles) ceramic wafer surface of metallic pattern (as shown in Figure 2); Porous mold is placed on the ceramic substrate that is covered with the low-temperature end electrode, p/n type element is put into the vestibule of porous mold, cross continuous tunnel furnace and add thermal weld, welded and taken off porous mold; After the device interelement that welds on the huyashi-chuuka (cold chinese-style noodles) ceramic wafer is filled a kind of technology filler, be cured, after the curing oxide layer of p/n type element hot end surface removed.
(3) on p/n type element hot end surface, cover the grid barrier layer, make the element surface metallization by figure spray nickel dam shown in Figure 1 and allumen layer, as the temperature end electrode, p/n type element hot junction is together in series, spraying finishes the grid barrier layer is taken off; After the hot junction electrode is ground to required thickness, cleans up interelement curing process filler and dry the lead-in wire of burn-oning; Charges are optional can select white cement or talcum powder for use with the technology filler.
(4) figure of cold and hot surface ceramic wafer and cutting route determines;
According to cutting, spraying coating process is the easiest, can satisfy every pair of hot junction requirement independent of each other that the p-n thermocouple is right, determines cutting route (1) cutting route as shown in Figure 3.
(5) select for use the high equipment of production efficiency (as laser cutting machine) that the cold junction ceramic wafer is cut along (1) cutting route among Fig. 3, be divided into several, width of slit is 0.2 ± 0.1mm, cut back huyashi-chuuka (cold chinese-style noodles) porcelain plate and do not have picture surface as shown in Figure 4, the device side figure as shown in Figure 5, (2) are the huyashi-chuuka (cold chinese-style noodles) ceramic wafer among Fig. 5, (3) are flow deflector, (4) be P/N type element, (5) are nickel dam and allumen layer;
Select high power for use, as the CO of 200W
2Laser cutter cuts along (1) cutting route shown in Figure 3.
(6) heat-conducting cream that is provided with between the faying face of hot junction electrode and hot junction white pottery porcelain plate reaches seamless link, and the thickness of heat-conducting cream is 0.1～0.15mm, the heat-conducting cream that heat-conducting cream selects for use the high temperature of heat conduction non-conducting not solidify;
With the hot junction white pottery porcelain plate that scribbles conductive paste topped with the hot junction electrode of huyashi-chuuka (cold chinese-style noodles) porcelain plate on, alignment is ceramic wafer up and down, uses resistant to elevated temperatures heat-conducting glue edge sealing all around, dries.
It is independently of one another to obtain the right hot junction of the every pair of p-n thermocouple, and it is also independently of one another at cold junction to constitute every pair of right p/n element of this thermocouple simultaneously.Can discharge the hot junction from room temperature-40 ℃～100 ℃ to 50 ℃～400 ℃ of serviceability temperatures, the thermal stress of cold junction under-40 ℃～200 ℃ Rapid Thermal is impacted, long-term serviceability is stable, the thermoelectric power generation device of long service life.
The present invention's beneficial effect compared with the prior art is, the present invention is independently of one another in the right hot junction of the every pair of p-n thermocouple, it is also independently of one another along the hot junction flow guide bar direction of expanding with heat and contract with cold at cold junction to constitute every pair of right p/n element of this thermocouple simultaneously, under thermal shock every pair independently the cold thermocouple hot side all have certain space to discharge the stress that thermal shock produces, be a kind of thermoelectric generator that flexibly connects that can discharge thermal shock stress fully.
Technology of the present invention is simple, rate of finished products is high, cost is low, conversion efficiency of thermoelectric is high, high temperature resistant, thermal shock resistance strong, long-term serviceability good stability, reliability height, is applicable to that industrial mass prepares the product and the technology of preparing of flexible thermoelectric semiconductor power generator.The right cold and hot surface of every pair of thermocouple independent of each other of the thermoelectric semiconductor generator that is obtained all flexibly connects, can discharge the hot junction from room temperature-40 ℃～100 ℃ to 50 ℃～400 ℃ of serviceability temperatures, the thermal stress of cold junction under-40 ℃～200 ℃ Rapid Thermal is impacted, guarantee that the use job stability is stable under the long-term thermal shock of device in different low-grade exhaust heat reclaims, reliability is high, the life-span is long, having lowered the use cost of thermoelectric device, is the use field of expansion thermoelectric power generation and the effective ways that improve energy utilization rate.
The present invention is applicable to the batch preparation of industrialization of stable performance, highly reliable type, long service life thermoelectric semiconductor power generator.
Description of drawings
Fig. 1 thermoelectric generator hot side electrode pattern;
Fig. 2 thermoelectric generator huyashi-chuuka (cold chinese-style noodles) electrode pattern;
Fig. 3 huyashi-chuuka (cold chinese-style noodles) ceramic wafer cutting route figure;
Fig. 4 cuts back huyashi-chuuka (cold chinese-style noodles) ceramic wafer and is not with the picture surface figure;
Fig. 5 cuts the side view of back device.
Picture in picture number expression: (1) cutting route: (2) huyashi-chuuka (cold chinese-style noodles) ceramic wafer; (3) flow deflector; (4) P/N type element; (5) nickel dam and allumen layer.
Embodiment
Embodiment 1:
Below for preparing the embodiment of the flexible thermoelectric power generating device of TEP1-12635-3.4:
The thermoelectric crystal bar of the p/n type that the raw material that the embodiment of the invention adopts is, ceramic wafer, heat-conducting cream etc.
(1) is raw material with the thermoelectric crystal bar of the p/n type for preparing, cuts into thickly, cut into bottom surface 1.31 * 1.31 behind the large stretch of surface metalation of the p/n that will cut greater than the thick p/n sheet of 2.0mm
± 0.02Mm, high by 2.0
± 0.01The p/n type element of mm.
(2) will hang up the flow deflector of burn-oning behind 240 ℃ the lead-free solder of Sn95Sb5 with the huyashi-chuuka (cold chinese-style noodles) ceramic wafer surface of metallic pattern; Porous mold is placed on the ceramic substrate that is covered with the low-temperature end electrode, p/n type element is put into the hole of porous die cavity, cross continuous tunnel furnace and carry out thermal weld, welded and taken off porous mold; Behind the mixture of device interelement filling concrete that welds on the huyashi-chuuka (cold chinese-style noodles) ceramic wafer and glue, be cured, after the curing oxide layer of p/n type element hot end surface removed.
(3) on p/n type element hot end surface, cover the grid barrier layer, spray nickel dam and allumen layer make the element surface metallization, as the temperature end electrode, p/n type element hot junction are together in series, and spraying finishes the grid barrier layer is taken off; The hot junction electrode is ground to 0.3
± 0.02Mm thickness is removed interelement curing process filler and is dried the lead-in wire of burn-oning.
(4) determining of the figure of cold and hot surface ceramic wafer and cutting route:
According to cutting, spraying coating process is the easiest, can satisfy every pair of hot junction requirement independent of each other that the p-n thermocouple is right, determines that hot side spraying figure is shown in Figure 1, huyashi-chuuka (cold chinese-style noodles) ceramic wafer figure is shown in Figure 2, cutting route is shown in (1) among Fig. 3.
(5) select the CO of power 250W for use
2Laser cutter cuts along (1) cutting route shown in Figure 3, cuts back width of slit 0.22mm; Cutting back huyashi-chuuka (cold chinese-style noodles) porcelain plate does not have picture surface as shown in Figure 4, device side figure as shown in Figure 5, (2) are the huyashi-chuuka (cold chinese-style noodles) ceramic wafer among Fig. 5, (3) are flow deflector, (4) are P/N type element, (5) are nickel dam and allumen layer.
(6) on the blank ceramic wafer of hot junction, evenly smear the thick heat-conducting cream of a bed thickness 0.12mm, make between the faying face of hot junction ceramics and coating electrode together by the heat-conducting cream seamless link.Alignment is ceramic wafer up and down, uses resistant to elevated temperatures heat-conducting glue edge sealing all around, dries.It is independently of one another to obtain the right hot junction of the every pair of p-n thermocouple, and it is also independently of one another along the hot junction flow guide bar direction of expanding with heat and contract with cold at cold junction to constitute every pair of right p/n element of this thermocouple simultaneously.Can discharge the hot junction from room temperature-40 ℃～100 ℃ to 50 ℃～400 ℃ of serviceability temperatures, the thermal stress of cold junction under-40 ℃～200 ℃ Rapid Thermal is impacted, long-term serviceability is stable, the flexible thermoelectric power generating device of long service life.
Embodiment 2:
Below for preparing the embodiment of the flexible thermoelectric power generating device of TEP1-12656-0.6.
The thermoelectric crystal bar of the p/n type that the raw material that present embodiment adopts is, ceramic wafer, heat-conducting cream etc.
(1) is raw material with the thermoelectric crystal bar of the p/n type for preparing, cuts into thickly, cut into bottom surface 2.5 * 2.5 behind the large stretch of surface metalation of the p/n that will cut greater than the thick p/n sheet of 1.5mm
± 0.02Mm, high by 1.5
± 0.01The p/n type element of mm.
(2) will hang up the flow deflector of burn-oning behind 240 ℃ the lead-free solder of Sn95Sb5 with the huyashi-chuuka (cold chinese-style noodles) ceramic wafer surface of metallic pattern; Porous mold is placed on the ceramic substrate that is covered with the low-temperature end electrode, p/n type element is put into the hole of porous die cavity, cross continuous tunnel furnace and carry out thermal weld, welded and taken off porous mold; Behind the mixture of device interelement filling concrete that welds on the huyashi-chuuka (cold chinese-style noodles) ceramic wafer and glue, be cured, throw the oxide layer of p/n type element hot end surface bright after the curing.
(3) on p/n type element hot end surface, cover the barrier layer, spray nickel dam and allumen layer make the element surface metallization, as the temperature end electrode, p/n type element hot junction are together in series, and spraying finishes the grid barrier layer is taken off; The hot junction electrode is ground to 0.4
± 0.02Mm thickness is removed interelement curing process filler and is dried the lead-in wire of burn-oning.
(4) figure of cold and hot surface ceramic wafer and cutting route determines;
According to cutting, spraying coating process is the easiest, can satisfy every pair of hot junction requirement independent of each other that the p-n thermocouple is right, determines that hot side spraying figure is shown in Figure 1, huyashi-chuuka (cold chinese-style noodles) ceramic wafer figure is shown in Figure 2, cutting route is shown in (1) among Fig. 3.
(5) select the CO of power 250W for use
2Laser cutter, cut, cut back width of slit 0.27mm along (1) cutting route shown in Figure 3; Cutting back huyashi-chuuka (cold chinese-style noodles) porcelain plate does not have picture surface as shown in Figure 4, device side figure as shown in Figure 5, (2) are the huyashi-chuuka (cold chinese-style noodles) ceramic wafer among Fig. 5, (3) are flow deflector, (4) are P/N type element, (5) are nickel dam and allumen layer.
(6) on the blank ceramic wafer of hot junction, evenly smear the thick heat-conducting cream of a bed thickness 0.15mm, make between the faying face of hot junction ceramics and coating electrode together by the heat-conducting cream seamless link.Alignment is ceramic wafer up and down, uses resistant to elevated temperatures heat-conducting glue edge sealing all around, dries.It is independently of one another to obtain the right hot junction of the every pair of p-n thermocouple, and it is also independently of one another along the hot junction flow guide bar direction of expanding with heat and contract with cold at cold junction to constitute every pair of right p/n element of this thermocouple simultaneously.Can discharge the hot junction from room temperature-40 ℃～100 ℃ to 50 ℃～400 ℃ of serviceability temperatures, the thermal stress of cold junction under-40 ℃～200 ℃ Rapid Thermal is impacted, long-term serviceability is stable, the flexible thermoelectric power generating device of long service life, has lowered the use cost of thermoelectric power generation device and the use field of expansion thermoelectric power generation greatly.
Claims (5)
1. the preparation method of a flexible thermoelectric semiconductor power generator, be included in welding p/n type thermoelectric element on the cold junction ceramic wafer, it is characterized in that, described method is to adopt spraying to obtain on the right basis of p-n thermocouple independent of each other at the temperature end electrode, along the right interelement slit of p/n of every pair of thermocouple that the hot junction electrode connects the cold junction ceramic wafer is cut open; The right hot junction of the every pair of p-n thermocouple is independently of one another, and it is also independently of one another along the hot junction flow guide bar direction of expanding with heat and contract with cold at cold junction to constitute every pair of right p/n element of this thermocouple simultaneously; The cold and hot surface of every pair of thermocouple all has certain space to discharge the stress of thermal shock under thermal shock, realizes flexibly connecting, and obtains the thermoelectric power generation device that a kind of thermoelectric generator that can discharge the non-rigid connection of thermal shock stress fully promptly flexibly connects.
2. the preparation method of a kind of flexible thermoelectric semiconductor power generator according to claim 1 is characterized in that, the width of slit of described cutting cold junction ceramic wafer is 0.2 ± 0.1mm.
3. the preparation method of a kind of flexible thermoelectric semiconductor power generator according to claim 1 is characterized in that, the mode of described cutting cold junction ceramic wafer adopts CO
2Laser cutter cuts.
4. the preparation method of a kind of flexible thermoelectric semiconductor power generator according to claim 1, it is characterized in that, the heat-conducting cream that is provided with between the faying face of hot junction electrode and hot junction ceramic wafer in the described method reaches seamless link, and the thickness of heat-conducting cream is 0.1～0.15mm.
5. the preparation method of a kind of flexible thermoelectric semiconductor power generator according to claim 5 is characterized in that, the heat-conducting cream that the heat-conducting cream that described hot junction electrode is connected with the hot junction ceramic wafer selects for use the high temperature of heat conduction non-conducting not solidify.
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| DE102015224020A1 (en) | 2015-12-02 | 2017-06-08 | Deutsches Zentrum für Luft- und Raumfahrt e.V. | Thermoelectric module |
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| CN102506515A (en) * | 2011-09-21 | 2012-06-20 | 中国电子科技集团公司第十八研究所 | Small-sized high-reliability thermoelectric refrigerator |
| CN102425879B (en) * | 2011-09-21 | 2015-03-11 | 中国电子科技集团公司第十八研究所 | Preparation method of thermoelectric refrigerator for high orbit space |
| US9859486B2 (en) | 2012-07-19 | 2018-01-02 | Nec Corporation | Thermoelectric conversion element and manufacturing method for same |
| CN103325935B (en) * | 2013-05-24 | 2015-10-28 | 深圳大学 | A kind of flexible thin film thermobattery and preparation method thereof |
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| CN110069084A (en) * | 2018-01-24 | 2019-07-30 | 思纳福(北京)医疗科技有限公司 | Temperature control device |
| CN108305935A (en) * | 2018-02-08 | 2018-07-20 | 南方科技大学 | Flexible thermo-electric device and preparation method |
| CN110265538A (en) * | 2019-05-30 | 2019-09-20 | 清华大学 | Flexible thermoelectric generator and its preparation method and application system |
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| US20040114665A1 (en) * | 2002-12-12 | 2004-06-17 | Sun Park | Cantilevered thermocouple rake |
| JP5212762B2 (en) * | 2005-05-17 | 2013-06-19 | 日産自動車株式会社 | Temperature control method for fuel cell stack structure and fuel cell stack structure |
| CN101717848A (en) * | 2009-12-17 | 2010-06-02 | 哈尔滨电机厂有限责任公司 | Stability heat processing process of elastic key bar of 200MW turbonator |
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