CN106898690A - A kind of rear-earth-doped SnTe base thermoelectricity materials - Google Patents
A kind of rear-earth-doped SnTe base thermoelectricity materials Download PDFInfo
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- CN106898690A CN106898690A CN201710112857.6A CN201710112857A CN106898690A CN 106898690 A CN106898690 A CN 106898690A CN 201710112857 A CN201710112857 A CN 201710112857A CN 106898690 A CN106898690 A CN 106898690A
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- 239000000463 material Substances 0.000 title claims abstract description 90
- 230000005619 thermoelectricity Effects 0.000 title claims abstract description 68
- 229910005642 SnTe Inorganic materials 0.000 title claims abstract description 64
- 229910052761 rare earth metal Inorganic materials 0.000 claims abstract description 42
- 150000002910 rare earth metals Chemical class 0.000 claims abstract description 10
- 238000005266 casting Methods 0.000 claims description 6
- 238000007731 hot pressing Methods 0.000 claims description 5
- 238000002844 melting Methods 0.000 claims description 4
- 230000008018 melting Effects 0.000 claims description 4
- 229910052684 Cerium Inorganic materials 0.000 claims description 3
- 229910052691 Erbium Inorganic materials 0.000 claims description 3
- 229910052688 Gadolinium Inorganic materials 0.000 claims description 3
- 229910052779 Neodymium Inorganic materials 0.000 claims description 3
- 229910052777 Praseodymium Inorganic materials 0.000 claims description 3
- 229910052772 Samarium Inorganic materials 0.000 claims description 3
- 229910052769 Ytterbium Inorganic materials 0.000 claims description 3
- 239000003708 ampul Substances 0.000 claims description 3
- 238000003801 milling Methods 0.000 claims description 3
- 239000010453 quartz Substances 0.000 claims description 3
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N silicon dioxide Inorganic materials O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims description 3
- 229910052714 tellurium Inorganic materials 0.000 claims description 3
- 229910052718 tin Inorganic materials 0.000 claims description 3
- 229910052727 yttrium Inorganic materials 0.000 claims description 3
- 239000002994 raw material Substances 0.000 claims description 2
- 238000003746 solid phase reaction Methods 0.000 claims description 2
- 238000010348 incorporation Methods 0.000 claims 2
- 238000000498 ball milling Methods 0.000 claims 1
- 238000006467 substitution reaction Methods 0.000 abstract description 3
- 239000000203 mixture Substances 0.000 description 14
- 238000002360 preparation method Methods 0.000 description 13
- 230000006872 improvement Effects 0.000 description 6
- 238000000034 method Methods 0.000 description 6
- 238000001816 cooling Methods 0.000 description 5
- 238000010248 power generation Methods 0.000 description 4
- 230000008901 benefit Effects 0.000 description 3
- 238000005516 engineering process Methods 0.000 description 3
- 238000011160 research Methods 0.000 description 3
- 229910052692 Dysprosium Inorganic materials 0.000 description 2
- 230000009286 beneficial effect Effects 0.000 description 2
- 238000003912 environmental pollution Methods 0.000 description 2
- 229910052746 lanthanum Inorganic materials 0.000 description 2
- 238000005457 optimization Methods 0.000 description 2
- 239000000843 powder Substances 0.000 description 2
- 230000009467 reduction Effects 0.000 description 2
- 238000005057 refrigeration Methods 0.000 description 2
- 238000012360 testing method Methods 0.000 description 2
- 239000011800 void material Substances 0.000 description 2
- 239000002918 waste heat Substances 0.000 description 2
- 230000003796 beauty Effects 0.000 description 1
- 150000004770 chalcogenides Chemical class 0.000 description 1
- 230000008859 change Effects 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 238000004891 communication Methods 0.000 description 1
- 230000006835 compression Effects 0.000 description 1
- 238000007906 compression Methods 0.000 description 1
- 238000009792 diffusion process Methods 0.000 description 1
- 239000002019 doping agent Substances 0.000 description 1
- 235000013399 edible fruits Nutrition 0.000 description 1
- 230000005611 electricity Effects 0.000 description 1
- 230000021824 exploration behavior Effects 0.000 description 1
- 239000002440 industrial waste Substances 0.000 description 1
- 239000003350 kerosene Substances 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 230000004044 response Effects 0.000 description 1
- 239000000523 sample Substances 0.000 description 1
- 238000010583 slow cooling Methods 0.000 description 1
- 238000002791 soaking Methods 0.000 description 1
- 239000002887 superconductor Substances 0.000 description 1
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
- H10N10/80—Constructional details
- H10N10/85—Thermoelectric active materials
- H10N10/851—Thermoelectric active materials comprising inorganic compositions
- H10N10/852—Thermoelectric active materials comprising inorganic compositions comprising tellurium, selenium or sulfur
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- H—ELECTRICITY
- H10—SEMICONDUCTOR DEVICES; ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N—ELECTRIC SOLID-STATE DEVICES NOT OTHERWISE PROVIDED FOR
- H10N10/00—Thermoelectric devices comprising a junction of dissimilar materials, i.e. devices exhibiting Seebeck or Peltier effects
- H10N10/01—Manufacture or treatment
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Abstract
The invention discloses a kind of rear-earth-doped SnTe base thermoelectricity materials, rare earth element is mixed in the SnTe base thermoelectricity materials, the rare earth doped atomic percentage conc is 0.1 ~ 2%.Existing SnTe base thermoelectricity materials are better than using the thermoelectricity capability of the rear-earth-doped SnTe base thermoelectricity materials of technical scheme, its electrical conductivity is suitable, and thermoelectricity capability is high；After rare earth element is added, easily substitution Sn reduces intrinsic Sn hole concentrations as alms giver, optimizes carrier concentration, so as to improve the thermoelectricity capability of material.
Description
Technical field
The invention belongs to field of thermoelectric material technique, more particularly to a kind of rear-earth-doped SnTe base thermoelectricity materials.
Background technology
The material of thermoelectric generator or thermoelectric cooling module is referred to as thermoelectric material, be one kind can realize electric energy interacted with heat energy turn
The material of change.The thermo-electric generation and refrigeration device made by thermoelectric material have pollution-free, noiseless, easy to maintain, safety can
By the advantages of.The earliest Soviet Union is that household radio electricity receiver is powered in outlying district by the use of kerosene lamp or timber as thermal source.With
Space exploration interest increase and in the increasingly increased resource survey of the earth and Exploratory behavior, it is necessary to develop a class can
Itself energy supply and the power-supply system that need not be looked after, thermoelectric power generation are particularly suitable to these applications.For remote space probe
For, the thermoelectric generator of radio isotope heat supply is unique electric power system.It is successfully applied to NASA
On more than 20 spacecrafts such as the Apollo of NASA transmittings, Pioneer, Voyager and Ulysses.In Russia, there are more than 1000
The ocean lighthouse that similar radiosotope thermoelectric generator device is used near the Arctic Circle, sets with non-maintaining 20 years of operation
The meter life-span.Nearly more than ten years, China has been also carried out substantial amounts of research on using the nature temperature difference and industrial waste heat thermoelectric power generation, and
Larger progress is achieved, with good comprehensive social benefit.There is thermoelectric cooler mechanical compression refrigeration machine to be difficult to match in excellence or beauty
Advantage：Size is small, light weight, without any mechanical rotation part, work noiseless, without liquid or gaseous medium, therefore does not deposit
In the problem of pollution environment, accurate temperature controlling, fast response time, device long service life are capable of achieving.It can also be making for superconductor
With offer low temperature environment.The micro element prepared furthermore with thermoelectric material is used to prepare micro power, microcell cooling, optic communication
Swash the thermoregulating system of laser diode and infrared ray sensor, the application field of thermoelectric material has been expanded significantly.In electronic product
Radiating, biomedicine operation in temperature control aspect be respectively provided with good application prospect.Should say, thermoelectric material is a kind of
The material of extensive application prospect, in environmental pollution and energy crisis increasingly serious today, carries out new thermoelectric materials
Research has very strong realistic meaning.
Thermoelectric generation technology can realize that heat energy and electric energy are directly mutually changed, and be the emphasis problem of current new energy research
One of.Greatly develop application of the thermoelectric power generation technology in solar thermal energy generating (increasing income) and waste heat waste-heat power generation (throttling) etc. field
The current energy scarcity of China and problem of environmental pollution can effectively be alleviated, with important strategic importance.The performance of thermoelectric material
By dimensionless figure of merit ZT=[S2σ/(κe+κL)] T signs, conductivityσ and Seebeck coefficient S are improved, while reducing thermal conductivity κ (κ
It is carrier thermal conductivity κeWith phonon thermal conductivity κLSum) be optimization of material key, but three physical quantitys are interrelated, make
The optimization for obtaining performance is limited by reality.In recent years, by not turning off using energy band engineering, nanometer engineering and new material
Hair, achieves a large amount of progress in terms of peak value thermoelectric figure of merit is improved.
Unleaded SnTe has with the same face-centred cubic structure of chalcogenide lead, because SnTe has intrinsic Sn higher empty
Position, causes intrinsic carrier concentration higher so that the thermal conductivity of the material is higher, and Seeebeck coefficients and ZT values are relatively low,
Therefore do not paid attention to for a long time.If the performance of unleaded group IV-VI thermoelectric material SnTe can be improved further,
There is the group IV-VI thermoelectric material of other commonly used lead bases to be replaced.And undoped p SnTe sills have it is higher intrinsic
Sn rooms, cause intrinsic carrier concentration higher so that the thermal conductivity of the material is higher, and Seeebeck coefficients and Z values compared with
It is low.Although can improve the Seebeck coefficients of material by introducing resonance level using In doping, the method is to dopant
It is required that higher, performance increase rate is limited, and the introducing of resonance level can reduce carrier mobility.
The content of the invention
For above technical problem, the invention discloses a kind of rear-earth-doped SnTe base thermoelectricity materials, current-carrying is directly adjusted
Sub- concentration reduction void content, improves the Seebeck coefficients of material, and method is simple, and Modulatory character is strong.
In this regard, the technical solution adopted by the present invention is：
A kind of rear-earth-doped SnTe base thermoelectricity materials, mix rare earth element, the rare earth in the SnTe base thermoelectricity materials
The atomic percentage conc of element doping is 0.1~2%.This technical scheme is mixed SnTe base thermoelectricity materials using rare earth element
It is miscellaneous, carrier concentration reduction void content can be directly adjusted, the Seebeck coefficients of material are improved, method is simple, Modulatory character
By force, rare earth element earth rich reserves, are proved to that Beneficial Effect can be produced to the regulation and control of SnTe sills carrier.When rare earth unit
After element is mixed, easily substitution Sn reduces intrinsic Sn hole concentrations as alms giver, optimizes carrier concentration, so as to improve material
The thermoelectricity capability of material.
As a further improvement on the present invention, rare earth element, the rare earth element are mixed in the SnTe base thermoelectricity materials
The atomic percentage conc of doping is 0.5~1.5%.Wherein, the atomic percentage conc is atom number percentage composition.
As a further improvement on the present invention, rare earth element, the rare earth element are mixed in the SnTe base thermoelectricity materials
The atomic percentage conc of doping is 0.5%.
Preferably, the rare earth element is LREE or heavy rare earth element.
As a further improvement on the present invention, the rare earth element is at least one in La, Ce, Pr, Nd, Sm or Gd.
Described La, Ce, Pr, Nd, Sm, Gd are LREE.
As a further improvement on the present invention, the rare earth element is at least one in Dy, Er, Yb or Y.It is described to be
Dy, Er, Yb, Y are heavy rare earth element.
As a further improvement on the present invention, the rear-earth-doped SnTe base thermoelectricity materials can use melting, hot pressing, ball
Various methods such as mill, solid phase reaction are obtained.Rear-earth-doped SnTe base thermoelectricity materials, method letter are prepared using traditional preparation methods
It is single.
As a further improvement on the present invention, it uses following steps to prepare：Weigh Sn, Te, rare earth metal conduct
Raw material；Material vacuum is enclosed in quartz ampoule carries out intensification melting, and cooling obtains ingot casting after the completion of reaction, and the ingot casting that will be obtained exists
Milling is cleaned in glove box, then by powder hot pressing under 550~650 DEG C of direct current hot press, 70~90MPa.Wherein, reacted
Ingot casting is obtained into rear Slow cooling.
Compared with prior art, beneficial effects of the present invention are：
It is better than using the thermoelectricity capability of the rear-earth-doped SnTe base thermoelectricity materials of technical scheme existing
SnTe base thermoelectricity materials, its electrical conductivity is suitable, and thermoelectricity capability is high；After rare earth element is added, easily substitution Sn, as alms giver
Intrinsic Sn hole concentrations are reduced, optimizes carrier concentration, so as to improve the thermoelectricity capability of material.
Specific embodiment
Preferably embodiment of the invention is described in further detail below.It should be appreciated that tool discussed below
Body embodiment is only used to explain the present invention, is not intended to limit the present invention.
The thermal conductivity κ of the thermoelectric material of following examples is according to using Netzsch LFA-457 type laser pulse heat analysis
The densitometer of the thermal diffusion coefficient of instrument measurement, the specific heat measured using Netzsch DSC-404 type difference specific heats instrument and material
Obtain.The conductivityσ and Seebeck coefficient S of material are obtained using ZEM-3 electrical conductivity with the test of Seebeck coefficient tester.Material
The thermoelectric figure of merit Z of material is calculated according to above-mentioned measured value.
Embodiment 1
A kind of rear-earth-doped SnTe base thermoelectricity materials, mix rare-earth elements La, the La in the SnTe base thermoelectricity materials
The atomic percentage conc of doping is 0.2%.
The rare-earth elements La doping SnTe base thermoelectricity materials are prepared using following steps：
Step S1：By La, Sn, Te according to vacuum seal is matched in quartz ampoule, it is warmed up to the programming rate of 200 DEG C/h
1000 DEG C, soaking time is 6h.
Step S2：Then 600 DEG C are dropped to the cooling rate of 200 DEG C/h, anneal 50h at such a temperature, finally with 200
DEG C/cooling rate of h drops to room temperature.
Step S3：The ingot casting that will be obtained cleans milling in glove box, by powder with direct current hot press in 600 DEG C, 80MPa
Lower hot pressing 2 minutes.
Embodiment 2
A kind of rear-earth-doped SnTe base thermoelectricity materials, rare-earth elements La is mixed with the SnTe base thermoelectricity materials, described
The atomic percentage conc of La doping is 0.5%.Preparation method is with embodiment 1.
Embodiment 3
A kind of rear-earth-doped SnTe base thermoelectricity materials, mix rare-earth elements La, the La in the SnTe base thermoelectricity materials
The atomic percentage conc of doping is 1%.Preparation method is with embodiment 1.
Embodiment 4
A kind of rear-earth-doped SnTe base thermoelectricity materials, mix rare-earth elements La, the La in the SnTe base thermoelectricity materials
The atomic percentage conc of doping is 2%.Preparation method is with embodiment 1.
Embodiment 5
A kind of rear-earth-doped SnTe base thermoelectricity materials, mix rare earth element ce, the Ce in the SnTe base thermoelectricity materials
The atomic percentage conc of doping is 0.5%.Preparation method is with embodiment 1.
Embodiment 6
A kind of rear-earth-doped SnTe base thermoelectricity materials, mix rare earth element Pr, the Pr in the SnTe base thermoelectricity materials
The atomic percentage conc of doping is 0.5%.Preparation method is with embodiment 1.
Embodiment 7
A kind of rear-earth-doped SnTe base thermoelectricity materials, mix rare earth element nd, the Nd in the SnTe base thermoelectricity materials
The atomic percentage conc of doping is 0.5%.Preparation method is with embodiment 1.
Embodiment 8
A kind of rear-earth-doped SnTe base thermoelectricity materials, mix rare earth element Sm, the Sm in the SnTe base thermoelectricity materials
The atomic percentage conc of doping is 0.5%.Preparation method is with embodiment 1.
Embodiment 9
A kind of rear-earth-doped SnTe base thermoelectricity materials, mix rare earth Gd, the Gd in the SnTe base thermoelectricity materials
The atomic percentage conc of doping is 0.5%.Preparation method is with embodiment 1.
Embodiment 10
A kind of rear-earth-doped SnTe base thermoelectricity materials, mix rare earth element Dy, the Dy in the SnTe base thermoelectricity materials
The atomic percentage conc of doping is 0.5%.Preparation method is with embodiment 1.
Embodiment 11
A kind of rear-earth-doped SnTe base thermoelectricity materials, mix rare earth element er, the Er in the SnTe base thermoelectricity materials
The atomic percentage conc of doping is 0.5%.Preparation method is with embodiment 1.
Embodiment 12
A kind of rear-earth-doped SnTe base thermoelectricity materials, mix rare earth element y b, the Yb in the SnTe base thermoelectricity materials
The atomic percentage conc of doping is 0.5%.Preparation method is with embodiment 1.
Embodiment 13
A kind of rear-earth-doped SnTe base thermoelectricity materials, mix rare earth element y in the SnTe base thermoelectricity materials, the Y mixes
Miscellaneous atomic percentage conc is 0.5%.Preparation method is with embodiment 1.
The rear-earth-doped SnTe base thermoelectricity materials that 1~embodiment of embodiment 13 is obtained are carried out into thermoelectricity capability test, and with
The SnTe base thermoelectricity materials not being doped embodiment, the data knot of conductivityσ and thermoelectric figure of merit Z at 600 DEG C as a comparison
Fruit is as shown in table 1.
Table 1
From above-mentioned table 1, using the thermoelectricity capability of the rear-earth-doped SnTe base thermoelectricity materials of technical solution of the present invention
Than undoped p SnTe base thermoelectricity materials it is higher.
Above content is to combine specific preferred embodiment further description made for the present invention, it is impossible to assert
Specific implementation of the invention is confined to these explanations.For general technical staff of the technical field of the invention,
On the premise of not departing from present inventive concept, some simple deduction or replace can also be made, should be all considered as belonging to of the invention
Protection domain.
Claims (7)
1. a kind of rear-earth-doped SnTe base thermoelectricity materials, it is characterised in that：Rare earth element is mixed in the SnTe base thermoelectricity materials,
The rare earth doped atomic percentage conc is 0.1 ~ 2%.
2. rear-earth-doped SnTe base thermoelectricity materials according to claim 1, it is characterised in that：The SnTe base thermoelectricity materials
Middle incorporation rare earth element, the rare earth doped atomic percentage conc is 0.5 ~ 1.5%.
3. rear-earth-doped SnTe base thermoelectricity materials according to claim 2, it is characterised in that：The SnTe base thermoelectricity materials
Middle incorporation rare earth element, the rare earth doped atomic percentage conc is 0.5%.
4. rear-earth-doped SnTe base thermoelectricity materials according to claim 1, it is characterised in that：The rare earth element be La,
At least one in Ce, Pr, Nd, Sm or Gd.
5. rear-earth-doped SnTe base thermoelectricity materials according to claim 1, it is characterised in that：The rare earth element be Dy,
At least one in Er, Yb or Y.
6. rear-earth-doped SnTe base thermoelectricity materials according to claim 1 ~ 5 any one, it is characterised in that：The rare earth
Doping SnTe base thermoelectricity materials are obtained using melting, hot pressing, ball milling, solid phase reaction.
7. rear-earth-doped SnTe base thermoelectricity materials according to claim 6, it is characterised in that：It uses following steps system
It is standby to obtain：Sn, Te, rare earth metal are weighed as raw material；Material vacuum is enclosed in quartz ampoule carries out intensification melting, has reacted
Cool down the ingot casting that obtains into rear, the ingot casting that will be obtained cleans milling in glove box, then 550 ~ 650 DEG C of direct current hot press,
Hot pressing under 70 ~ 90 MPa.
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Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107768512A (en) * | 2017-10-16 | 2018-03-06 | 四川大学 | The method for improving SnTe thermoelectricity capabilities is adulterated by Zn |
| CN109273583A (en) * | 2018-08-29 | 2019-01-25 | 宁波革鑫新能源科技有限公司 | One kind mixing gadolinium SnTe base thermoelectricity material and preparation method thereof |
| CN111081857A (en) * | 2019-12-25 | 2020-04-28 | 哈尔滨工业大学（深圳） | Zintl phase thermoelectric material with hexagonal ZrBeSi structure and preparation method thereof |
| CN111517292A (en) * | 2020-04-30 | 2020-08-11 | 西华大学 | Tin telluride-based thermoelectric material and preparation method thereof |
| CN112670394A (en) * | 2020-12-24 | 2021-04-16 | 合肥工业大学 | Method for improving thermoelectric performance of p-type SnTe base material by introducing stable nano heterojunction |
| CN116903370A (en) * | 2023-06-02 | 2023-10-20 | 江苏万新光学有限公司 | SnTe-based thermoelectric material with multi-scale nano composite structure and preparation method thereof |
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| CN101965312A (en) * | 2008-01-14 | 2011-02-02 | 俄亥俄州立大学研究基金会 | Improve by the thermoelectric figure of merit that improves density of electronic states |
| CN105304808A (en) * | 2015-09-29 | 2016-02-03 | 涂艳丽 | SnTe-In2Te3 series thermoelectric material and preparation method thereof |
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2017
- 2017-02-28 CN CN201710112857.6A patent/CN106898690A/en active Pending
Patent Citations (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN101965312A (en) * | 2008-01-14 | 2011-02-02 | 俄亥俄州立大学研究基金会 | Improve by the thermoelectric figure of merit that improves density of electronic states |
| CN105304808A (en) * | 2015-09-29 | 2016-02-03 | 涂艳丽 | SnTe-In2Te3 series thermoelectric material and preparation method thereof |
Cited By (7)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN107768512A (en) * | 2017-10-16 | 2018-03-06 | 四川大学 | The method for improving SnTe thermoelectricity capabilities is adulterated by Zn |
| CN107768512B (en) * | 2017-10-16 | 2019-09-13 | 四川大学 | The method for improving SnTe thermoelectricity capability is adulterated by Zn |
| CN109273583A (en) * | 2018-08-29 | 2019-01-25 | 宁波革鑫新能源科技有限公司 | One kind mixing gadolinium SnTe base thermoelectricity material and preparation method thereof |
| CN111081857A (en) * | 2019-12-25 | 2020-04-28 | 哈尔滨工业大学（深圳） | Zintl phase thermoelectric material with hexagonal ZrBeSi structure and preparation method thereof |
| CN111517292A (en) * | 2020-04-30 | 2020-08-11 | 西华大学 | Tin telluride-based thermoelectric material and preparation method thereof |
| CN112670394A (en) * | 2020-12-24 | 2021-04-16 | 合肥工业大学 | Method for improving thermoelectric performance of p-type SnTe base material by introducing stable nano heterojunction |
| CN116903370A (en) * | 2023-06-02 | 2023-10-20 | 江苏万新光学有限公司 | SnTe-based thermoelectric material with multi-scale nano composite structure and preparation method thereof |
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Application publication date: 20170627 |