JP5214695B2 - 熱電材料とそれを原料とした複合材料及びその製造方法 - Google Patents
熱電材料とそれを原料とした複合材料及びその製造方法 Download PDFInfo
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- 238000004519 manufacturing process Methods 0.000 title claims description 121
- 239000000463 material Substances 0.000 title claims description 114
- 239000002131 composite material Substances 0.000 title claims description 63
- 239000000243 solution Substances 0.000 claims description 72
- 239000011812 mixed powder Substances 0.000 claims description 70
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 69
- 239000002041 carbon nanotube Substances 0.000 claims description 67
- 229910021393 carbon nanotube Inorganic materials 0.000 claims description 67
- 238000000034 method Methods 0.000 claims description 50
- 239000011259 mixed solution Substances 0.000 claims description 30
- 229910052751 metal Inorganic materials 0.000 claims description 27
- 239000002184 metal Substances 0.000 claims description 27
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 claims description 21
- 238000002156 mixing Methods 0.000 claims description 18
- 239000000843 powder Substances 0.000 claims description 16
- 150000003839 salts Chemical class 0.000 claims description 16
- 239000002994 raw material Substances 0.000 claims description 15
- 238000006243 chemical reaction Methods 0.000 claims description 11
- 229910052714 tellurium Inorganic materials 0.000 claims description 10
- PORWMNRCUJJQNO-UHFFFAOYSA-N tellurium atom Chemical compound [Te] PORWMNRCUJJQNO-UHFFFAOYSA-N 0.000 claims description 10
- 239000006185 dispersion Substances 0.000 claims description 9
- USIUVYZYUHIAEV-UHFFFAOYSA-N diphenyl ether Chemical compound C=1C=CC=CC=1OC1=CC=CC=C1 USIUVYZYUHIAEV-UHFFFAOYSA-N 0.000 claims description 8
- 238000005245 sintering Methods 0.000 claims description 8
- 239000004094 surface-active agent Substances 0.000 claims description 8
- QYIGOGBGVKONDY-UHFFFAOYSA-N 1-(2-bromo-5-chlorophenyl)-3-methylpyrazole Chemical compound N1=C(C)C=CN1C1=CC(Cl)=CC=C1Br QYIGOGBGVKONDY-UHFFFAOYSA-N 0.000 claims description 7
- 150000001462 antimony Chemical class 0.000 claims description 7
- JHXKRIRFYBPWGE-UHFFFAOYSA-K bismuth chloride Chemical compound Cl[Bi](Cl)Cl JHXKRIRFYBPWGE-UHFFFAOYSA-K 0.000 claims description 7
- RXPAJWPEYBDXOG-UHFFFAOYSA-N hydron;methyl 4-methoxypyridine-2-carboxylate;chloride Chemical compound Cl.COC(=O)C1=CC(OC)=CC=N1 RXPAJWPEYBDXOG-UHFFFAOYSA-N 0.000 claims description 7
- 238000010298 pulverizing process Methods 0.000 claims description 7
- 238000000746 purification Methods 0.000 claims description 7
- 238000002490 spark plasma sintering Methods 0.000 claims description 7
- QGLWBTPVKHMVHM-KTKRTIGZSA-N (z)-octadec-9-en-1-amine Chemical compound CCCCCCCC\C=C/CCCCCCCCN QGLWBTPVKHMVHM-KTKRTIGZSA-N 0.000 claims description 6
- NKJOXAZJBOMXID-UHFFFAOYSA-N 1,1'-Oxybisoctane Chemical compound CCCCCCCCOCCCCCCCC NKJOXAZJBOMXID-UHFFFAOYSA-N 0.000 claims description 6
- QAOWNCQODCNURD-UHFFFAOYSA-N Sulfuric acid Chemical compound OS(O)(=O)=O QAOWNCQODCNURD-UHFFFAOYSA-N 0.000 claims description 6
- 239000003638 chemical reducing agent Substances 0.000 claims description 6
- 238000000227 grinding Methods 0.000 claims description 6
- RMZAYIKUYWXQPB-UHFFFAOYSA-N trioctylphosphane Chemical compound CCCCCCCCP(CCCCCCCC)CCCCCCCC RMZAYIKUYWXQPB-UHFFFAOYSA-N 0.000 claims description 6
- 238000001035 drying Methods 0.000 claims description 5
- 238000000605 extraction Methods 0.000 claims description 5
- 238000007306 functionalization reaction Methods 0.000 claims description 5
- 239000012298 atmosphere Substances 0.000 claims description 4
- 125000000524 functional group Chemical group 0.000 claims description 4
- 238000010438 heat treatment Methods 0.000 claims description 4
- 239000002798 polar solvent Substances 0.000 claims description 4
- 238000000926 separation method Methods 0.000 claims description 4
- QTBSBXVTEAMEQO-UHFFFAOYSA-M Acetate Chemical compound CC([O-])=O QTBSBXVTEAMEQO-UHFFFAOYSA-M 0.000 claims description 3
- GRYLNZFGIOXLOG-UHFFFAOYSA-N Nitric acid Chemical compound O[N+]([O-])=O GRYLNZFGIOXLOG-UHFFFAOYSA-N 0.000 claims description 3
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 3
- 229910017604 nitric acid Inorganic materials 0.000 claims description 3
- 229910052760 oxygen Inorganic materials 0.000 claims description 3
- 239000001301 oxygen Substances 0.000 claims description 3
- 239000000126 substance Substances 0.000 claims description 3
- 238000007254 oxidation reaction Methods 0.000 claims description 2
- 238000003825 pressing Methods 0.000 claims description 2
- 125000003748 selenium group Chemical class *[Se]* 0.000 claims 3
- 230000000052 comparative effect Effects 0.000 description 12
- 230000000694 effects Effects 0.000 description 8
- 229910052797 bismuth Inorganic materials 0.000 description 5
- JCXGWMGPZLAOME-UHFFFAOYSA-N bismuth atom Chemical compound [Bi] JCXGWMGPZLAOME-UHFFFAOYSA-N 0.000 description 5
- 239000013078 crystal Substances 0.000 description 5
- 239000000758 substrate Substances 0.000 description 5
- 239000002159 nanocrystal Substances 0.000 description 4
- 150000003342 selenium Chemical class 0.000 description 4
- 238000010299 mechanically pulverizing process Methods 0.000 description 3
- 229910044991 metal oxide Inorganic materials 0.000 description 3
- 150000004706 metal oxides Chemical class 0.000 description 3
- 230000002776 aggregation Effects 0.000 description 2
- 239000000919 ceramic Substances 0.000 description 2
- 238000010586 diagram Methods 0.000 description 2
- 150000002500 ions Chemical class 0.000 description 2
- 238000003701 mechanical milling Methods 0.000 description 2
- 239000011858 nanopowder Substances 0.000 description 2
- 239000002245 particle Substances 0.000 description 2
- 239000011669 selenium Substances 0.000 description 2
- 239000004065 semiconductor Substances 0.000 description 2
- 239000002904 solvent Substances 0.000 description 2
- XSOKHXFFCGXDJZ-UHFFFAOYSA-N telluride(2-) Chemical compound [Te-2] XSOKHXFFCGXDJZ-UHFFFAOYSA-N 0.000 description 2
- GMAVRNRAOGOYIT-UHFFFAOYSA-N C(CCCCCCCCCCCCCCC)(O)O.C(CCCCCCCCCCCCCCC)(O)O Chemical compound C(CCCCCCCCCCCCCCC)(O)O.C(CCCCCCCCCCCCCCC)(O)O GMAVRNRAOGOYIT-UHFFFAOYSA-N 0.000 description 1
- VEXZGXHMUGYJMC-UHFFFAOYSA-N Hydrochloric acid Chemical compound Cl VEXZGXHMUGYJMC-UHFFFAOYSA-N 0.000 description 1
- 230000005679 Peltier effect Effects 0.000 description 1
- 230000005678 Seebeck effect Effects 0.000 description 1
- BUGBHKTXTAQXES-UHFFFAOYSA-N Selenium Chemical compound [Se] BUGBHKTXTAQXES-UHFFFAOYSA-N 0.000 description 1
- 230000005680 Thomson effect Effects 0.000 description 1
- 238000005054 agglomeration Methods 0.000 description 1
- 238000004220 aggregation Methods 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 229910052787 antimony Inorganic materials 0.000 description 1
- WATWJIUSRGPENY-UHFFFAOYSA-N antimony atom Chemical compound [Sb] WATWJIUSRGPENY-UHFFFAOYSA-N 0.000 description 1
- 229910052799 carbon Inorganic materials 0.000 description 1
- 125000003178 carboxy group Chemical group [H]OC(*)=O 0.000 description 1
- 238000005119 centrifugation Methods 0.000 description 1
- 238000004891 communication Methods 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 238000001816 cooling Methods 0.000 description 1
- 238000001914 filtration Methods 0.000 description 1
- 239000002048 multi walled nanotube Substances 0.000 description 1
- 239000002105 nanoparticle Substances 0.000 description 1
- 239000002071 nanotube Substances 0.000 description 1
- 230000003287 optical effect Effects 0.000 description 1
- 238000010248 power generation Methods 0.000 description 1
- 230000000630 rising effect Effects 0.000 description 1
- 229910052711 selenium Inorganic materials 0.000 description 1
- 230000002195 synergetic effect Effects 0.000 description 1
- 238000009210 therapy by ultrasound Methods 0.000 description 1
Classifications
-
- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
- H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
- H01B1/14—Conductive material dispersed in non-conductive inorganic material
- H01B1/18—Conductive material dispersed in non-conductive inorganic material the conductive material comprising carbon-silicon compounds, carbon or silicon
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F9/00—Making metallic powder or suspensions thereof
- B22F9/02—Making metallic powder or suspensions thereof using physical processes
- B22F9/04—Making metallic powder or suspensions thereof using physical processes starting from solid material, e.g. by crushing, grinding or milling
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F9/00—Making metallic powder or suspensions thereof
- B22F9/16—Making metallic powder or suspensions thereof using chemical processes
- B22F9/18—Making metallic powder or suspensions thereof using chemical processes with reduction of metal compounds
- B22F9/24—Making metallic powder or suspensions thereof using chemical processes with reduction of metal compounds starting from liquid metal compounds, e.g. solutions
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C12/00—Alloys based on antimony or bismuth
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C26/00—Alloys containing diamond or cubic or wurtzitic boron nitride, fullerenes or carbon nanotubes
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C47/00—Making alloys containing metallic or non-metallic fibres or filaments
- C22C47/14—Making alloys containing metallic or non-metallic fibres or filaments by powder metallurgy, i.e. by processing mixtures of metal powder and fibres or filaments
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C49/00—Alloys containing metallic or non-metallic fibres or filaments
- C22C49/02—Alloys containing metallic or non-metallic fibres or filaments characterised by the matrix material
- C22C49/12—Intermetallic matrix material
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C49/00—Alloys containing metallic or non-metallic fibres or filaments
- C22C49/14—Alloys containing metallic or non-metallic fibres or filaments characterised by the fibres or filaments
-
- 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
-
- 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
- H10N10/855—Thermoelectric active materials comprising inorganic compositions comprising compounds containing boron, carbon, oxygen or nitrogen
-
- 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
- H10N10/857—Thermoelectric active materials comprising compositions changing continuously or discontinuously inside the material
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F2998/00—Supplementary information concerning processes or compositions relating to powder metallurgy
- B22F2998/10—Processes characterised by the sequence of their steps
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Mechanical Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Inorganic Chemistry (AREA)
- Dispersion Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Manufacturing & Machinery (AREA)
- Powder Metallurgy (AREA)
- Carbon And Carbon Compounds (AREA)
- Manufacture Of Alloys Or Alloy Compounds (AREA)
- Manufacture Of Metal Powder And Suspensions Thereof (AREA)
Description
また、本発明による熱電材料は、上記の熱電材料の製造方法で製造されたことを特徴とする。
また、本発明による複合材料は、上記の複合材料の製造方法で製造されたことを特徴とする。
S120:精製過程
S140:官能化過程
S160:抽出過程
S180:分散過程
S200:混合溶液製造ステップ
S300:混合粉末製造ステップ
S320:化学反応過程
S340:混合粉末製造過程
S360:粉末分離過程
S380:粉末乾燥過程
S400:混合粉末粉砕ステップ
S500:熱電材料製造ステップ
S600:複合材料製造ステップ
Claims (15)
- カーボンナノチューブが分散した第1溶液と金属塩が混合した第2溶液を製造する第1溶液及び第2溶液製造ステップと、
前記第1溶液と第2溶液を混合して混合溶液を製造する混合溶液製造ステップと、
前記混合溶液を化学反応させてカーボンナノチューブと金属が混合した混合粉末を生成及び成長させる混合粉末製造ステップと、
前記混合粉末を機械的に粉砕及び混合する混合粉末粉砕ステップと、
前記粉砕及び混合した混合粉末を熱処理して熱電材料を製造する熱電材料製造ステップとからなることを特徴とする熱電材料の製造方法。 - 前記金属塩は、ビスマスアセテート(Bi acetate)、ビスマスクロライド(Bi chloride)、ビスマス硝酸塩(BiNO3)の少なくとも1つとテルルクロライド(Te chloride)とを必ず含み、アンチモン塩とセレン塩の少なくとも1つを含むことを特徴とする請求項1に記載の熱電材料の製造方法。
- 前記第1溶液には、ジオクチルエーテル(Dioctylether)、ジフェニルエーテル(Diphenylether)の少なくとも1つを含む極性溶媒が含まれることを特徴とする請求項1に記載の熱電材料の製造方法。
- 前記混合粉末製造ステップは、
前記混合溶液を10℃/分で250〜280℃まで昇温して2時間保持して熱電材料を生成する化学反応過程と、
生成された熱電材料の周囲にカーボンナノチューブが位置する混合粉末を製造する混合粉末製造過程とからなることを特徴とする請求項1に記載の熱電材料の製造方法。 - 前記第2溶液には、オレイルアミン(Oleylamine)とトリオクチルホスフィン(Trioctylphosphine)の少なくとも1つが適用されることを特徴とする請求項1に記載の熱電材料の製造方法。
- 前記混合粉末粉砕ステップは、
フレーク(flake)形状の混合粉末を円形にし、前記金属と分離していたカーボンナノチューブの一部が金属内部に挿入されるようにする過程であることを特徴とする請求項1に記載の熱電材料の製造方法。 - 前記第1溶液及び第2溶液製造ステップは、
前記カーボンナノチューブを精製する精製過程と、
前記カーボンナノチューブに官能基を形成する官能化過程と、
前記カーボンナノチューブを抽出する抽出過程と、
抽出されたカーボンナノチューブを極性溶媒に界面活性剤と共に分散する分散過程とを順次行って第1溶液を製造すると共に、
ビスマスアセテート(Bi acetate)、ビスマスクロライド(Bi chloride)、ビスマス硝酸塩(BiNO3)の少なくとも1つ、テルルクロライド(Te chloride)、還元剤、及び界面活性剤を必ず含み、セレン塩とアンチモン塩の少なくとも1つを選択的に含むように混合して第2溶液を製造する過程であることを特徴とする請求項1に記載の熱電材料の製造方法。 - 前記熱電材料製造ステップは、
還元雰囲気で熱処理して前記混合粉末に含まれる酸素、酸化物及び有機物を除去する過程であることを特徴とする請求項1に記載の熱電材料の製造方法。 - 前記精製過程は、
硫酸と硝酸が3:1の体積比で混合した溶液で行われることを特徴とする請求項7に記載の熱電材料の製造方法。 - 前記混合粉末製造ステップの後には、
前記混合粉末を分離する粉末分離過程と、
分離した混合粉末を80〜100℃の真空雰囲気で加熱して酸化反応を中断する粉末乾燥過程とが行われることを特徴とする請求項1に記載の熱電材料の製造方法。 - カーボンナノチューブが分散した第1溶液と金属塩が混合した第2溶液を製造する第1溶液及び第2溶液製造ステップと、
前記第1溶液と第2溶液を混合して混合溶液を製造する混合溶液製造ステップと、
前記混合溶液を化学反応させてカーボンナノチューブと金属が混合した混合粉末を生成及び成長させる混合粉末製造ステップと、
前記混合粉末を機械的に粉砕及び混合する混合粉末粉砕ステップと、
前記粉砕及び混合した混合粉末を熱処理して熱電材料を製造する熱電材料製造ステップと、
前記熱電材料にスパークプラズマ焼結工程を行ってバルク化した複合材料を製造する複合材料製造ステップとからなることを特徴とする熱電材料を原料とした複合材料の製造方法。 - 前記金属塩は、ビスマスアセテート(Bi acetate)、ビスマスクロライド(Bi chloride)、ビスマス硝酸塩(BiNO3)の少なくとも1つとテルルクロライド(Te chloride)とを必ず含み、アンチモン塩とセレン塩の少なくとも1つを含むことを特徴とする請求項11に記載の熱電材料を原料とした複合材料の製造方法。
- 前記複合材料製造ステップは、300〜350℃の温度、30〜70MPaの圧力で加圧して焼結する過程であることを特徴とする請求項12に記載の熱電材料を原料とした複合材料の製造方法。
- 請求項1に記載の熱電材料の製造方法で製造されたことを特徴とする熱電材料。
- 請求項11に記載の複合材料の製造方法で製造されたことを特徴とする複合材料。
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KR1020100047880A KR101180263B1 (ko) | 2010-05-24 | 2010-05-24 | 열전분말과 이를 원료로 한 복합재료 및 이들의 제조방법 |
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JP5214695B2 true JP5214695B2 (ja) | 2013-06-19 |
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Cited By (1)
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US10460850B2 (en) | 2014-11-12 | 2019-10-29 | Korea Institute Of Machinery & Materials | Thermoelectric composite material and method for preparing thermoelectric composite material |
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TWI472069B (zh) * | 2011-12-19 | 2015-02-01 | Ind Tech Res Inst | 熱電複合材料 |
JP2013219116A (ja) * | 2012-04-05 | 2013-10-24 | Toyota Motor Corp | ナノコンポジット熱電変換材料 |
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