CN208111483U - A kind of thermo-electric device with adaptive connection layer - Google Patents
A kind of thermo-electric device with adaptive connection layer Download PDFInfo
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- CN208111483U CN208111483U CN201820784196.1U CN201820784196U CN208111483U CN 208111483 U CN208111483 U CN 208111483U CN 201820784196 U CN201820784196 U CN 201820784196U CN 208111483 U CN208111483 U CN 208111483U
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Abstract
The utility model relates to a kind of thermo-electric devices with adaptive connection layer, it is characterized in that, the thermo-electric device includes substrate, and the thermoelectricity pair that at least one of connection on the substrate is made of N-shaped thermoelectric element, p-type thermoelectric element and flow deflector for connecting N-shaped thermoelectric element and p-type thermoelectric element；The temperature end of the N-shaped thermoelectric element and/or p-type thermoelectric element is connect with flow deflector by the first adaptive connection layer and/or the low-temperature end of the N-shaped thermoelectric element and/or p-type thermoelectric element is connect with substrate by the second adaptive connection layer.In the thermo-electric device of the utility model, articulamentum（First adaptive connection layer or/and the second adaptive connection layer）Be with excellent ductility, and can occur under smaller stress larger plastic deformation material its with good electric heating property, to ensure lower interface additional thermal resistance and resistance.
Description
Technical field
The utility model relates to a kind of thermo-electric devices with adaptive connection layer, belong to thermoelectric material and device technology neck
Domain.
Background technique
The thermoelectric material hot and cold side temperature difference can be directly changed into electric energy using the Seebeck effect of thermoelectric material.Based on the original
The thermoelectric heat generation system structure of reason is simple, compact layout, no rotation/transmission parts and work liquid, can long-term static work,
Deep space exploration, special power supply and remaining waste-heat power generation field have broad application prospects.
The thermoelectricity capability of material indicates that high ZT peak value is the primary mesh of thermoelectric material research with dimensionless thermoelectric figure of merit ZT
Mark.ZT value usually varies with temperature, and is based on the corresponding temperature of ZT peak value, at present can the thermoelectric material system of practical application mainly have
CoSb suitable for the Bi-Te (20~300 DEG C) of low-temperature space, suitable for middle warm area3Base filled skutterudite (SKD, 400~700
DEG C), Pb-Te (400~800 DEG C), Half-Heusler (400~800 DEG C) and suitable for high-temperature region Si-Ge (600~
1000 DEG C) and oxide (600~1000 DEG C) etc..
The basic function component thermoelectric element of thermoelectric generator (TEG), by the metalization layer structure of thermoelectric material and both ends of the surface
At.By a N-shaped thermoelectric element and a p-type thermoelectric element, arranged in parallel and hot end is rigidly connected by flow deflector, that is, is constituted
One π type thermoelectricity pair.It integrates multiple thermoelectricity and further integrates TEG system to thermo-electric device, multiple devices are obtained.π type heat
The structure of electricity pair designs so that when integrated thermal electric device and TEG system no longer needs to handle element hot end, all subsequent behaviour
Make more easily to complete in cold end.Specifically, can be by the cold end of multiple π type thermoelectricity pair and metallization by low-temperature welding
Ceramic substrate rigid connection, so that N-shaped and the cold end of p-type element be made alternately to be connected in series, obtains corresponding thermo-electric device.Device
When the work of part/system, π type thermoelectricity to be rigidly fixed in high temperature heat source and low temperature it is heat sink between, and make in enough compression
Under, to ensure good thermo-contact.
In the longitudinal direction for being parallel to element arm, N-shaped and p-type element by rigid constraint heat source and it is heat sink between.In general, N-shaped
It is had a certain difference with the thermal expansion coefficient of p-type thermoelectric material, element arm longitudinal extension amount when leading to temperature end temperature change
Difference, so that compression or tensile stress can be generated inside N-shaped or p-type element.Tensile stress therein easily causes thermoelectricity first
The cracking of electrode and thermoelectric material interface, seriously affects interface contact performance and mechanical strength in part, leads to device performance substantially
Deteriorate, or even failure.By taking filled skutterudite thermo-electric device as an example, the thermal expansion coefficient of p-type is higher than n-type material by 20% or so,
It during temperature end heats up and cools down, will appear very big tensile stress respectively inside N-shaped element and p-type element, be easy
Interface micro-crack is caused, even results in and falls off；On the other hand, in the transverse direction perpendicular to element arm, N-shaped and p-type element are by height
The rigid constraint of warm end rigidity flow deflector and low-temperature end metallized ceramic substrate.When device works, temperature end usually has hundreds of degree
Temperature rise, flow deflector generates apparent lateral expansion, and low-temperature end metallized ceramic substrate temperature change is small, and swell increment is negligible,
To thermoelectric element, at high/low temperature end, the shearing force by flow deflector and ceramic substrate acting in opposition, respective interface easily go out respectively
Existing mechanical damage, to cause hidden trouble to device/system performance.
In the interfacial stress for alleviating thermoelectric element, has numerous studies report at present in terms of improving interface cohesion.This respect
Most common Research Thinking is optimization electrode/flow deflector thermal expansion coefficient.Such as Zhao Degang is mixed with Mo-Cu (CN100524867C)
Object is closed as electrode material, electrode thermal expansion coefficient is adjusted by optimization element ratio, electrode and thermoelectric material has been effectively relieved
Interfacial stress.Li Fei etc. then by design Mo/Cu/Mo/Cu ... sandwich, has equally reached adjusting electrode thermal expansion system
Number reduces the effect (CN104347788A) of thermoelectric element interfacial stress.Bai Sheng is equal between Bi-Te thermoelectric material and Al electrode by force
Introduce Cu buffer layer (CN10343889B), Yan Yong is high introduced in Mg-Si-Sn base thermoelectric element by the first Ni-Al layers,
The 2nd Ni-Al layers of layered electrode (CN104362249B) formed with Ag layers, Cui Jiaolin etc. pass through in thermoelectric element and Cu water conservancy diversion
Three transition zones (Ni layers of spray, plating Ni layers and Sn95Ag5 solder layer) (CN103698035B) is introduced between piece, the studies above is equal
The interfacial stress of thermoelectric element has been effectively relieved.Furthermore also there is the trial for improving interface portion geometric configuration, as rattan original stretches one
Notch features are introduced Deng in thermoelectric element high temperature termination electrode and flow deflector joint portion, by adjusting kerf and optimization high/low temperature
The relative area of termination electrode and flow deflector joint portion can also mitigate the interfacial stress of engaging portion to a certain extent
(CN105765749A).Obviously, current research work, which is concentrated mainly on, reduces thermoelectric material and high temperature in single thermoelectric element
Between termination electrode, and the interfacial stress between single thermoelectric element and temperature end flow deflector, but in thermoelectricity pair and thermo-electric device
In level, the studies above is helpless to alleviate between N-shaped and p-type element and temperature end flow deflector and low-temperature end metallized ceramic
Interfacial stress caused by thermal expansion coefficient difference between substrate.
Utility model content
In view of the above-mentioned problems, the research work for alleviating interfacial stress has been extended to thermoelectricity pair and heat for the first time by the utility model
This level of electrical part, and then a kind of thermo-electric device with adaptive connection layer is provided, the thermo-electric device includes substrate,
With at least one of connection on the substrate by N-shaped thermoelectric element, p-type thermoelectric element and for connecting N-shaped thermoelectric element
The thermoelectricity pair formed with the flow deflector of p-type thermoelectric element；The temperature end of the N-shaped thermoelectric element and/or p-type thermoelectric element with lead
Flow is connected by the first adaptive connection layer and/or the low-temperature end and base of the N-shaped thermoelectric element and/or p-type thermoelectric element
Plate is connected by the second adaptive connection layer.
In the thermo-electric device of the utility model, articulamentum (the first adaptive connection layer or/and the second adaptive connection
Layer) it is that and the material of larger plastic deformation can occur under smaller stress with excellent ductility, such as composition can be
The alloy that simple substance or any at least two in In, Ga, Cu, Al, Ag, Au, Li, Na, K, Ge, Te etc. are formed, has good
Electric heating property, to ensure lower interface additional thermal resistance and resistance.Secondly, selected adaptive connection layer material also have it is excellent
Ductility, thus articulamentum itself can under smaller stress by tangentially or the deformation of normal direction discharges stress in time,
To avoid internal stress excessive buildup, the protection to device is realized.
Preferably, the composition of the first adaptive connection layer and/or the second adaptive connection layer be selected from In, Ga, Cu,
The alloy that simple substance or any at least two in Al, Ag, Au, Li, Na, K, Ge, Te are formed.Preferably, described first is adaptive
The group of articulamentum or the second adaptive connection layer becomes In, Ga, Cu, Al, Ag, Au, Li, Na, K, Ge、Te、In-Ga、Gu-In、Al-
In、Cu- Ga, Al-Ga, Cu-In-Ga, Al-In-Ga, Al-Cu-Ga or Al-Cu-In.
Preferably, the first adaptive connection layer or the second adaptive connection layer with a thickness of 5nm~500 μm, preferably
It is 1~500 μm.Thickness is too thin, and extension amplitude of deformation is limited, cannot be fully absorbed interfacial stress, while being unfavorable for ensuring good
Heat, electrical contact.Thickness is too thick, and deformation is excessive, then will affect the structural rigidity of device and system, and may cause articulamentum material
Material is excessive to be squeezed out, and the performance of thermo-electric device is influenced.
Preferably, the thermoelectricity pair is configured as π type structure or ring structure.Specifically, when with adaptive connection layer
Thermo-electric device at work, the temperature end temperature of thermoelectricity pair is significantly raised, and N-shaped thermoelectric element and p-type thermoelectric element are along longitudinal direction
Obvious expansion occurs, high/low temperature end interface pressure increases, and adaptive connection layer can be by extending outward or inwardly receiving at this time
Contracting, suitably adjusting thickness, the difference of compensated n-type thermoelectric element and p-type thermoelectric element longitudinal dilatation amount.Temperature end is led simultaneously
Flow transversely occurs obviously to expand, and pushes the temperature end of N-shaped thermoelectric element and p-type thermoelectric element away from each other, and low-temperature end
Substrate temperature varies less, and swell increment can be ignored relatively.The adaptive connection layer of respective interface is in lesser shearing force at this time
The lower sliding that certain amplitude can transversely occur of effect, compensates the lateral expansion of temperature end flow deflector, so that height be effectively relieved
The transverse shear stresses at low-temperature end interface；When temperature end temperature, which has, to be declined by a relatively large margin, N-shaped thermoelectric element and p-type thermoelectricity member
Part occurs obviously to shrink along longitudinal direction, and in the process, the biggish element of thermal expansion coefficient, longitudinal shrinkage is bigger, corresponding material
Material is internal and tensile stress will occur in interface, and the adaptive connection layer of respective interface can increase thickness by longitudinal stretching at this time,
The difference of compensated n-type thermoelectric element and p-type thermoelectric element longitudinal shrinkage, so that the drawing being subject to inside respective element be effectively reduced
Stretch stress.Temperature end flow deflector transversely occurs obviously to shrink simultaneously, pulls the high temperature of N-shaped thermoelectric element and p-type thermoelectric element
End is mutually drawn close, and the temperature change of low-temperature end substrate can be ignored relatively, the low temperature of N-shaped thermoelectric element and p-type thermoelectric element
End relative position is tended to remain unchanged, and the adaptive connection layer of respective interface is under the effect of lesser interfacial shear force at this time
The cross-direction shrinkage of temperature end flow deflector can be compensated, so that high/low temperature end circle be effectively relieved along the horizontal sliding that certain amplitude occurs
The transverse shear stresses in face.
Preferably, only adaptive there are first between the N-shaped thermoelectric element or the temperature end and flow deflector of p-type thermoelectric element
Answer articulamentum.
Preferably, only adaptive there are second between the N-shaped thermoelectric element or the low-temperature end and substrate of p-type thermoelectric element
Articulamentum.
Preferably, the N-shaped thermoelectric element and p-type thermoelectric element can be single segment structure or multi-segment structure.
Preferably, further including high temperature termination electrode, institute between the N-shaped thermoelectric element and/or p-type thermoelectric element and flow deflector
State high temperature termination electrode with a thickness of 50~500 μm.
Also, preferably, the high temperature termination electrode is located at N-shaped thermoelectric element and/or p-type thermoelectric element adaptively connects with first
It connects between layer.If the first adaptive connection layer is not present in thermo-electric device, high temperature termination electrode is located at N-shaped thermoelectric element and/or p-type
Between thermoelectric element and flow deflector；If high temperature termination electrode is located at N-shaped thermoelectricity member there are the first adaptive connection layer in thermo-electric device
Between part and/or p-type thermoelectric element and the first adaptive connection layer.
Preferably, further include low temperature termination electrode between the N-shaped thermoelectric element and/or p-type thermoelectric element substrate, it is described low
Warm termination electrode with a thickness of 50~500 μm.It is preferred that the low temperature termination electrode be located at N-shaped thermoelectric element and/or p-type thermoelectric element with
Between second adaptive connection layer.
Also, preferably, the low temperature termination electrode is located at N-shaped thermoelectric element and/or p-type thermoelectric element adaptively connects with second
It connects between layer.If the second adaptive connection layer is not present in thermo-electric device, high temperature termination electrode is located at N-shaped thermoelectric element and/or p-type
Between thermoelectric element and substrate；If there are the second adaptive connection layer in thermo-electric device, high temperature termination electrode is located at N-shaped thermoelectric element
And/or between p-type thermoelectric element and the second adaptive connection layer.
Also, preferably, between the high temperature termination electrode or low temperature termination electrode and N-shaped thermoelectric element and/or p-type thermoelectric element
Further include barrier layer, the barrier layer with a thickness of 1~200 μm.In addition, having both the material of excellent ductility and electrical and thermal conductivity performance
Material is usually relatively more active, therefore also reply linkage interface optimizes (such as setting diffusion barrier layer) if necessary, avoids
Because interface is spread, excessive (or even complete) consumes selected adaptive connection layer during the work time, influences its adaptive ability.
Preferably, the substrate be metallized ceramic substrate, the metallized ceramic substrate include cold end ceramic substrate and
Be distributed in the metalization layer of cold end ceramic base plate surface, the metalization layer with a thickness of 10~300 μm.
In the present invention, to alleviate, thermoelectricity draws the longitudinal direction that certain positions occur inside thermo-electric device in the course of work
Stress and transverse shear stresses are stretched, in thermoelectricity pair in the connection procedure of N-shaped thermoelectric element and p-type thermoelectric element and flow deflector,
Or in thermoelectricity pair in the cold end of thermoelectric element and the welding process of metallized ceramic substrate, the utility model is in N-shaped thermoelectricity member
The cold end of part and p-type thermoelectric element or/and hot end addition suitable thickness, with excellent ductility and good conductive heating conduction
Connect layer material, while ensuring that interface has low additional resistance and thermal resistance, make interface for internal stress have it is certain from
Adaptability.Since other positions of device are rigid connection, from mechanical angle, above-mentioned adaptive connection layer
Mechanical strength is minimum.When thermo-electric device internal stress is accumulated to a certain extent, stress will pass through the shape of adaptive connection layer first
Change is released, to achieve the purpose that protect other rigid interfaces of thermo-electric device.
Detailed description of the invention
Fig. 1 is the thermo-electric device schematic diagram in the utility model with adaptive connection layer；
Fig. 2 is thermo-electric device Thermal Cycling high temperature end flow deflector temperature and time relation curve；
Appended drawing reference：
1 N-shaped thermoelectric material；
6 p-type thermoelectric materials
2, the high temperature termination electrode of 8 thermoelectricity pair；
3, the low temperature termination electrode of 7 thermoelectricity pair；
5 temperature end flow deflectors；
4, the first adaptive connection layer of 9 high temperature termination electrodes and flow deflector；
10 cold end ceramic substrates；
The metalization layer of 11 cold end ceramic base plate surfaces；
12, the second adaptive connection layer between 13 low temperature termination electrodes and metalization layer.
Specific embodiment
The utility model is further illustrated below by way of following embodiments, it should be appreciated that following embodiments are only used for
Bright the utility model, rather than limit the utility model.
In the present invention, the adaptive connection layer of the thermo-electric device with adaptive connection layer is located at thermoelectric element (P
Type thermoelectric element or/and N-type thermoelectric element) and substrate (such as metallized ceramic substrate) between, or/and be located at thermoelectricity centering n
Between type thermoelectric element and/or the temperature end and flow deflector of p-type thermoelectric element.The thermoelectricity is to by N-shaped thermoelectric element, p-type heat
Electric device and for connecting N-shaped thermoelectric element and p-type thermoelectric element flow deflector composition.Specifically, thermo-electric device includes
Flow deflector (high temperature flow deflector) positioned at temperature end, is distributed between the flow deflector and substrate the substrate positioned at low-temperature end
One N-shaped thermoelectric element and a p-type thermoelectric element and for connecting thermoelectric element (N-shaped thermoelectric element and/or p-type thermoelectricity
Element) and flow deflector the first adaptive connection layer or/and for connecting thermoelectric element (N-shaped thermoelectric element and/or p-type thermoelectricity
Element) and substrate the second adaptive connection layer.Substrate can be metallized ceramic substrate.The metallized ceramic substrate includes cold
End ceramic substrate and be distributed in the metalization layer of cold end ceramic base plate surface, the metalization layer with a thickness of 10~300 μm.
In the present invention, adaptive connection layer (the first adaptive connection layer and the second adaptive connection layer) is that have
Larger plastic deformation, and the material with high conductance and thermal conductivity can occur under smaller stress for excellent ductility
Material, the including but not limited to simple substance such as In, Ga, Cu, Al, Ag, Au, Li, Na, K, Ge, Te and their alloy.It is alloy type adaptive
The ingredient for answering articulamentum includes but is not limited to In-Ga, Gu-In, Al-In, Cu-Ga, Al-Ga, Cu-In-Ga, Al-Cu-In etc..
The thickness of first adaptive connection layer or the second adaptive connection layer can be 5nm~500 μm, preferably 1~500 μm.Optional
Embodiment in, the material of high temperature flow deflector can be one of Ni, Fe, Co, Cu, Mo-Cu, W-Cu and Al.
In alternative embodiments, the thermoelectricity of thermo-electric device is constituted to comprising a N-shaped thermoelectric element and a p-type heat
Electric device and flow deflector for connecting N-shaped thermoelectric element and p-type thermoelectric element.Wherein, the configuration of thermoelectricity pair can be biography
The π type structure of system, it is abnormally-structured to be also possible to annular etc..Constitute the N-shaped thermoelectric element of thermoelectricity pair and the thermoelectricity of p-type thermoelectric element
Material includes but is not limited to Bi-Te base thermoelectricity material, SKD base thermoelectricity material, Si-Ge base thermoelectricity material, Half-Heusler base
Thermoelectric material, Pb-Te base thermoelectricity material, Cu base fast-ionic conductor, liquid-like phase material, diamond-like materials, oxide-base thermoelectricity
The thermoelectric material systems such as material.In addition, constituting the N-shaped thermoelectric element of thermoelectricity pair and p-type thermoelectric element can be from same material
The single segment structure of Material system is also possible to can also be multi-segment structure respectively from the single segment structure of different materials system.This reality
With novel ingredient, structure and thickness by designing suitable adaptive connection layer, ensuring that interface is low electric, thermal losses same
When, it has been effectively relieved by the deformation absorption interface stress of its own because of n using the excellent ductility of adaptive connection layer
The tensile stress that type thermoelectric element is different with p-type thermoelectric element longitudinal extension amount and generates at related interfaces, and because of thermoelectricity
To the shear stress that temperature end flow deflector is different with low-temperature end ceramic substrate transversal stretching amount and generates at related interfaces, thus
Significantly improve the military service stability of thermo-electric device.
In alternative embodiments, when the thermoelectric element temperature end of each thermoelectricity pair of composition thermo-electric device passes through just
Property articulamentum connect with high temperature flow deflector, the low-temperature end and metallization of the N-shaped thermoelectric element of thermoelectricity centering and p-type thermoelectric element are made pottery
Pass through an adaptive connection layer and a rigid connection layer connection between porcelain substrate respectively, that is to say, that only in N-shaped thermoelectricity member
There are the second adaptive connection layers between part or the low-temperature end and metallized ceramic substrate of p-type thermoelectric element.Alternatively, when composition heat
The thermoelectric element low-temperature end of each thermoelectricity pair of electrical part passes through rigid connection layer and connect with metallized ceramic substrate, thermoelectricity pair
In N-shaped thermoelectric element and p-type thermoelectric element temperature end and high temperature flow deflector between respectively pass through an adaptive connection layer
It is connected with a rigid connection layer, that is to say, that only make pottery in the temperature end of N-shaped thermoelectric element or p-type thermoelectric element and metallization
There are the first adaptive connection layers between porcelain substrate.As an example, the N-shaped thermoelectric element of each thermoelectricity pair and p-type heat
Rigid connection can be used in the temperature end and high temperature flow deflector of electric device, meanwhile, in the welding of cold end and metallized ceramic substrate
Cheng Zhong can add adaptive connection layer in a kind of cold end of wherein thermoelectric element, realize adaptive with metallized ceramic substrate
Connection, and adaptive connection layer is not added in the cold end of another thermoelectric element, it realizes and connects with the rigidity of metallized ceramic substrate
It connects.That is, the inside of each thermoelectricity pair and its in all multiple joining interfaces of low-temperature end ceramic substrate, an only thermoelectric element
Cold end and ceramic substrate interface there are adaptive connection layer, remaining interface be rigid connection.The advantages of above structure, exists
In：Single adaptive connection layer influences less the structural strength of thermo-electric device, and by adaptive connection layer material, structure
The corresponding thermoelectricity pair in thermo-electric device can be equally effectively relieved in reasonable screening and design, single adaptive connection layer with thickness
The stretching of each interface internal and shear stress when temperature change at high/low temperature end, realize protection thermoelectricity to and device purpose.
It in alternative embodiments, further include high temperature between N-shaped thermoelectric element and/or p-type thermoelectric element and flow deflector
Termination electrode, the preferably described high temperature termination electrode be located at N-shaped thermoelectric element and/or p-type thermoelectric element and the first adaptive connection layer it
Between, the high temperature termination electrode with a thickness of 50~500 μm.Wherein, the group of high temperature termination electrode become Ni, Fe, Co, Cu, Mo-Cu,
At least one of W-Cu and Al.In alternative embodiments, between N-shaped thermoelectric element and/or p-type thermoelectric element substrate also
Including low temperature termination electrode, the preferably described low temperature termination electrode is located at N-shaped thermoelectric element and/or p-type thermoelectric element and second adaptively
Between articulamentum, the low temperature termination electrode with a thickness of 50~500 μm.Wherein, the group of low temperature termination electrode become Ni, Fe, Co,
At least one of Cu, Mo-Cu, W-Cu and Al.In alternative embodiments, high temperature termination electrode or low temperature termination electrode and N-shaped
It further include barrier layer between thermoelectric element and/or p-type thermoelectric element, the thickness on the barrier layer can be 1~200 μm.Wherein, it hinders
The composition of barrier can be at least one of Ti, Mo, Cr, Nb, Ta, Ti-Al alloy, Ti-Mo alloy.In optional embodiment
In, metallized ceramic substrate includes cold end ceramic substrate and the metalization layer for being distributed in cold end ceramic base plate surface, the metal
Change layer with a thickness of 10~300 μm.
Below using tradition π type filled skutterudite thermoelectricity to deposited copper aluminum oxide ceramic substrate as description object, but
Those skilled in the art should understand that other configurations, the thermoelectricity pair of other materials system cooperate the rigid insulation of other materials
Each corresponding component in the alternative following embodiments of heat-conducting substrate and realize the utility model.Therefore, the utility model and unlimited
Documented any certain material and structure in following embodiments.N-shaped thermoelectricity member is prepared by sintering and cutting technique first
Part 1 and p-type thermoelectric element 6.As shown in Figure 1, N-shaped thermoelectric material 1 and p-type thermoelectric material 6 are respectively included, 2 He of high temperature termination electrode
8 and low temperature termination electrode 3 and 7.Then by the first adaptive connection layer 4 and 9 by N-shaped thermoelectric element and p-type thermoelectric element
Temperature end is connected with high temperature flow deflector 5, obtains π type thermoelectricity pair.Certain circuit design is pressed later, selects suitable metallization pottery
Porcelain substrate, by the second adaptive connection layer 12 and 13 by the cold end (low-temperature end) of N-shaped thermoelectric element and p-type thermoelectric element and cold
It holds the metalization layer 11 on 10 surface of ceramic substrate to be connected, obtains by several pairs of thermoelectricity to the thermo-electric device being connected in series.It measures and remembers
Record device internal resistance.Then device is placed in thermal cycle test platform.Low-temperature end ceramic substrate is close to test platform low-temperature end electricity
Pole, temperature end flow deflector surface carry out insulating heat-conductive processing, are then close to test platform temperature end and heat electrode.Test platform is set
Under vacuum state.Platform low-temperature end keeps certain temperature, and temperature end is followed through multiple thermal cycle epiphysiometer part internal resistance with heat
Data before ring are compared, to judge influence of the different articulamentums for thermo-electric device thermal cycling stability.
In Thermal Cycling, when temperature end temperature change, N-shaped thermoelectric element and p-type thermoelectric element occur along longitudinal direction
Apparent contraction or expansion, but the difference of thermal expansion coefficient causes the longitudinal shrinkage of the two or swell increment different, when device is each
When interface is rigid connection, inside the element that longitudinal dilatation amount is small or shrinkage is big and related interfaces are stretched stress, when
To when being more than material or interface tensile strength, mechanical damage will occur in material internal or interface, cause to connect for tensile stress accumulation
Performance decline is touched, resistance increases.And in a thermoelectricity pair, when N-shaped thermoelectric element and p-type thermoelectric element and temperature end flow deflector
Between low-temperature end metallized ceramic substrate 4 at when thering are in interface one or more interfaces to connect by adaptive connection layer,
Adaptive connection layer can suitably adjust thickness, compensated n-type under lower stress by extending outward or to contract
With the difference of p-type element longitudinal shrinkage or swell increment, it even is eliminated the stretching that related interfaces are subject to so as to significantly reduce and answers
Power makes material and interface from damage.At the same time, when temperature end temperature change, temperature end flow deflector transversely occurs bright
Aobvious expansion or shrinkage pushes the temperature end of N-shaped thermoelectric element and p-type thermoelectric element away from each other or draws close, and low-temperature end metal
Change ceramic substrate temperature change very little, expansion or shrinkage amount can be ignored relatively, therefore N-shaped thermoelectric element and p-type thermoelectric element
With there are transverse shear stresses on the inside and linkage interface of high temperature flow deflector and metallized ceramic substrate.When shear stress is accumulated
To when being more than the shear strength of material or interface, mechanical damage will occur in material internal or interface, and contact performance is caused to decline,
Resistance increases.And in a thermoelectricity pair, when N-shaped thermoelectric element and p-type thermoelectric element and temperature end flow deflector and low-temperature end gold
Between categoryization ceramic substrate 4 at when thering are in interface one or more interfaces to connect by adaptive connection layer, adaptive connection
The horizontal sliding of certain amplitude can occur under lower shear stress for layer, compensate temperature end flow deflector cross-direction shrinkage or
Expansion, is effectively relieved inside element and the transverse shear stresses at high/low temperature end interface, reduction material and interface are mechanically damaged,
To avoid device internal resistance excessively rapid growth, improve the stability of device performance.
Enumerate embodiment further below the utility model is described in detail.It will similarly be understood that following embodiment is served only for
The utility model is further described, should not be understood as the limitation to scope of protection of the utility model, the technology of this field
Some nonessential modifications and adaptations that personnel's above content according to the present utility model is made belong to the guarantor of the utility model
Protect range.Following specific technological parameters of example etc. are also only an examples in OK range, i.e. those skilled in the art can
It is done in suitable range and is selected with the explanation by this paper, and do not really want to be defined in hereafter exemplary specific value.
Embodiment 1
Being sintered diameter respectively by one-step method sintering process is 50mm, with a thickness of the N-shaped with barrier layer and electrode of 8mm
With P-type skutterudite sample, structure is respectively Ni/Ti-Al/Yb0.3Co4Sb12/ Ti-Al/Ni and Ni/Ti-Al/CeFe4Sb12/
Ti-Al/Ni, wherein Ni is electrode, and about 120 μm of thickness, Ti-Al is barrier layer, about 100 μm of thickness.Wire cutting obtains corresponding heat
Electric device, having a size of 4*4*8mm3.Then by soldering processes, by Cu-Ag solder, by the high temperature of above-mentioned N-shaped and p-type element
End is by having a size of 5*12*2mm3Mo-Cu flow deflector rigid connection, obtain corresponding thermoelectricity pair；
Circuit design is carried out to thermo-electric device cold end, accordingly the suitably deposited copper ceramic substrate of selection, will pass through connection heat
Electric device cold end and copper-clad (300 μm of thickness) are obtained by 8 pairs of thermoelectricity to the thermo-electric device being connected in series.From above-mentioned sample with
Machine takes out 8 thermoelectricity pair, and the cold end of above-mentioned deposited copper ceramic substrate and thermoelectricity pair is cleaned by ultrasonic and is dried.
Deposited copper ceramic base plate surface is placed on heating platform, applies copper face upward.Correspond to N-shaped on substrate copper-clad surface
It places having a size of 4*4*0.2mm the position of the cold end of thermoelectric element and p-type thermoelectric element3Sn foil (with a thickness of 300 μm), will be hot
The cold end (low-temperature end) of electricity pair is placed on corresponding Sn foil, is applied 0.01~0.5MPa pressure to the cold end of thermoelectricity pair and is kept.
Heating platform is opened, it is made to be to slowly warm up to 260 DEG C, keeps the temperature 5min.It is then shut off heating platform, heating platform surface temperature drop
Cold end pressure is removed when to 50 DEG C or less, the cold end for obtaining N-shaped thermoelectric element and p-type thermoelectric element passes through soldering-tin layer and rigidly connects
The filled skutterudite thermo-electric device connect, is indicated with device A.
As a comparison, then at random 8 thermoelectricity pair are taken out, the cold end of above-mentioned deposited copper ceramic substrate and thermoelectricity pair is cleaned by ultrasonic
And it dries.Deposited copper ceramic base plate surface is placed on heating platform, applies copper face upward.Correspond to N-shaped on substrate copper-clad surface
It places with the position of p-type element cold end having a size of 4*4*0.02mm3In foil (with a thickness of 300 μm), thermoelectricity is placed in cold end
On corresponding In foil, 0.01~0.5MPa pressure is applied to cold end to thermoelectricity and is kept.Heating platform is opened, it is made slowly to heat up
To 145 DEG C, 5min is kept the temperature.It is then shut off heating platform, cold end pressure is removed when heating platform surface temperature is down to 50 DEG C or less
Power obtains N-shaped with p-type thermoelectric element cold end and passes through the filled skutterudite thermo-electric device that adaptive connection layer In is connected, with device
Part B is indicated.
The room temperature internal resistance of above-mentioned device is tested first, it is found that the room temperature internal resistance of device A and device B is essentially identical, respectively
It is 39.4m Ω and 38.8m Ω.
Then device A and device B are placed in thermal cycle test platform respectively.Low-temperature end ceramic substrate is close to test platform
Low-temperature end Cu electrode, temperature end flow deflector are close to test platform temperature end Ni and heat electrode.Above-mentioned thermo-electric device in test process
The pressure that low-temperature end ceramic substrate is born is 3MPa.In single Thermal Cycling, temperature end Ni heats electrode temperature 550
DEG C and 200 DEG C between change, low-temperature end temperature is maintained at 35 DEG C or so, and test platform is placed under low vacuum state, air pressure <
20Pa.Through 500 thermal cycle epiphysiometer part internal resistances, find device A and device B room temperature internal resistance be respectively 52.2m Ω and
39.1mΩ。
Since the influence of related interfaces diffusion couple interface contact performance can be ignored in device under 500 DEG C and lower temperature,
Therefore device A is the main reason for internal resistance steeply rises after thermal cycling：Thermoelectricity centering N-shaped thermoelectric element and p-type thermoelectric element
Between and temperature end flow deflector and low-temperature end ceramic substrate between thermal expansion coefficient mismatch cause respective interface to stretch
And shear stress.Since each interface device A is rigid connection at 35 DEG C, above-mentioned stress lacks in Thermal Cycling to be had
The release approach of effect, is easy to accumulate, to make to the interface of certain weaknesses such as the interface of skutterudite material and the barrier layer Ti-Al
At mechanical damage, contact resistance is caused to increase, so that the internal resistance for causing device A total dramatically increases.The result of device B is formed therewith
Stark contrast：Since there are In adaptive connection layers between the cold end and deposited copper ceramic substrate of thermoelectricity pair.In works warm in cold end
Degree is lower to have excellent ductility, can produce obvious deformation under the stress of very little.Higher device temperature end Thermal Cycling
In, In articulamentum passes through the longitudinally extending or timely compensated n-type thermoelectric element of contraction and p-type under the interfacial stress effect of very little
The difference (micron order) of longitudinal dilatation amount between thermoelectric element, while by lateral extension or shrinking compensation temperature end water conservancy diversion in time
The difference (micron order) of lateral expansion amount effectively avoids to discharge interfacial stress in time between piece and low-temperature end ceramic substrate
Interface damage, it is ensured that the contact performance at each interface, and then device internal resistance raising is substantially eliminated, it significantly improves thermo-electric device and exists
Stability under thermal cycle conditions.
Embodiment 2
Referring to the step of embodiment 1 be prepared each interface it is rigidly connected by 8 thermoelectricity to the thermoelectricity being composed in series
Device C.As a comparison, then at random 8 thermoelectricity pair are taken out, simultaneously by the ultrasonic cleaning of the cold end of above-mentioned deposited copper ceramic substrate and thermoelectricity pair
Drying.Deposited copper ceramic base plate surface is placed on heating platform, applies copper face upward.Correspond to N-shaped and p on substrate copper-clad surface
It is placed respectively having a size of 4*4*0.02mm the position of type element cold end3In foil (with a thickness of 300 μm) and Sn foil (with a thickness of 300 μ
M), cold end of the thermoelectricity to N-shaped thermoelectric element and p-type thermoelectric element is respectively placed on In foil and Sn foil, to thermoelectricity to cold end
Apply 0.01~0.5MPa pressure and keeps.Heating platform is opened, it is made to be to slowly warm up to 250 DEG C, keeps the temperature 5min.It is then shut off
Heating platform, heating platform surface temperature are down to 50 DEG C or less and remove cold end pressure, obtain p-type element cold end by scolding tin with
The rigid connection of copper ceramic substrate is applied, and N-shaped element cold end passes through the filling that In adaptive connection layer is connect with deposited copper ceramic substrate
Skutterudite thermoelectric device is indicated with device D.
The room temperature internal resistance of above-mentioned device is tested first, it is found that the room temperature internal resistance of device C and device D is essentially identical, respectively
It is 38.6m Ω and 39.1m Ω.
Thermal cycle processing is carried out respectively to device C and device D referring to the method and parameter of embodiment 1, after 500 thermal cycles
The room temperature internal resistance of measurement device internal resistance, discovery device C and device D is respectively 50.3m Ω and 40.7m Ω.With the situation class of device A
Seemingly, the internal resistance of device C significantly rises after thermal cycle, embodies good repeatability, while also illustrating that rigid connection interface exists
Fragility under thermal cycle conditions.In contrast, the internal resistance of device D is only than increasing 4% before thermal cycle.It can be seen that one
A thermoelectricity centering only introduces an adaptive connection layer, it is same it is possible to prevente effectively from device internal stress accumulation and interface damage,
Significantly improve the stability of device under thermal cycle conditions.Two low-temperature ends of each thermoelectricity pair, which pass through, in device B adaptively connects
Layer is connect to be connected with ceramic substrate, such design increases the deformation freedom degree of device low-temperature end, but compared with full rigidity connection,
The structural strength of device is decreased obviously, and each thermoelectricity centering of device D has an element cold end rigidly to connect with ceramic substrate
It connects, such structure design significantly enhances the overall structural strength of device, thus to the structural strength of corresponding heat and power system
To have and be obviously improved.
Claims (12)
1. a kind of thermo-electric device with adaptive connection layer, which is characterized in that the thermo-electric device includes substrate, and is connected to
At least one on the substrate is by N-shaped thermoelectric element, p-type thermoelectric element and for connecting N-shaped thermoelectric element and p-type heat
The thermoelectricity pair of the flow deflector composition of electric device；The temperature end of the N-shaped thermoelectric element and/or p-type thermoelectric element and flow deflector are logical
The low-temperature end for crossing the connection of the first adaptive connection layer and/or the N-shaped thermoelectric element and/or p-type thermoelectric element passes through with substrate
The connection of second adaptive connection layer.
2. thermo-electric device according to claim 1, which is characterized in that the first adaptive connection layer and/or second is certainly
Simple substance or any at least two of the composition of articulamentum in In, Ga, Cu, Al, Ag, Au, Li, Na, K, Ge, Te is adapted to be formed
Alloy.
3. thermo-electric device according to claim 1, which is characterized in that the first adaptive connection layer and/or second is certainly
Adapt to articulamentum with a thickness of 5nm~500 μm.
4. thermo-electric device according to claim 1, which is characterized in that the thermoelectricity pair is configured as π type structure or annular
Structure.
5. thermo-electric device according to claim 1, which is characterized in that only the N-shaped thermoelectric element or p-type thermoelectric element
There are the first adaptive connection layers between temperature end and flow deflector.
6. thermo-electric device according to claim 1, which is characterized in that only the N-shaped thermoelectric element or p-type thermoelectric element
There are the second adaptive connection layers between low-temperature end and substrate.
7. thermo-electric device according to claim 1, which is characterized in that the N-shaped thermoelectric element and/or p-type thermoelectric element
Further include high temperature termination electrode between flow deflector, the high temperature termination electrode with a thickness of 50~500 μm.
8. thermo-electric device according to claim 7, which is characterized in that the high temperature termination electrode be located at N-shaped thermoelectric element and/
Or between p-type thermoelectric element and the first adaptive connection layer.
9. thermo-electric device according to claim 1, which is characterized in that the N-shaped thermoelectric element and/or p-type thermoelectric element
Further include low temperature termination electrode between substrate, the low temperature termination electrode with a thickness of 50~500 μm.
10. thermo-electric device according to claim 9, which is characterized in that the low temperature termination electrode is located at N-shaped thermoelectric element
And/or between p-type thermoelectric element and the second adaptive connection layer.
11. the thermo-electric device according to claim 7 or 9, which is characterized in that the high temperature termination electrode or low temperature termination electrode with
Further include barrier layer between N-shaped thermoelectric element and/or p-type thermoelectric element, the barrier layer with a thickness of 1~200 μm.
12. thermo-electric device according to claim 1, which is characterized in that the substrate is metallized ceramic substrate, the gold
Categoryization ceramic substrate includes cold end ceramic substrate and the metalization layer for being distributed in cold end ceramic base plate surface, the metalization layer
With a thickness of 10~300 μm.
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
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| CN108550688A (en) * | 2018-05-24 | 2018-09-18 | 中国科学院上海硅酸盐研究所 | A kind of thermo-electric device with adaptive connection layer |
| CN114551707A (en) * | 2021-03-10 | 2022-05-27 | 中国科学院理化技术研究所 | Low-temperature thermoelectric device and preparation method thereof |
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2018
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Cited By (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108550688A (en) * | 2018-05-24 | 2018-09-18 | 中国科学院上海硅酸盐研究所 | A kind of thermo-electric device with adaptive connection layer |
| CN114551707A (en) * | 2021-03-10 | 2022-05-27 | 中国科学院理化技术研究所 | Low-temperature thermoelectric device and preparation method thereof |
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