Nano Structured Composite Materials for Thermoelectric Applications. Ewha Womans University. April 5, 2010
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1 Nano Structured Composite Materials for Thermoelectric Applications Sung-Jin Kim Ewha Womans University Department of Chemistry and Nano Science April 5, 2010
2 Thermoelectricity 연구분야 온도차에의해기전력이발생하는현상 (Seebeck 효과 ) 또는전류에의해열이흡수, 발생이생기는현상 (Peltier 효과 ) 응용분야 열전냉각 (Thermoelectric cooling) 열전발전 (Power generation) NAS A 2
3 Configuration of Thermoelectric Module HEAT IN thermoelement electrical conductor electrical insulator p n p n p n p n + HEAT OUT Laser Cooling Modules
4 Thermoelectric Figure of Merit Z=α 2 σ/κ Seebeck coeff. (α) : morphology, doping state Electrical l conductivity(σ) it : carrier concentration ti Thermal conductivity (κ) : phonon scattering
5 Optimum Transport Coefficients Figure of Merit : ZT S κ tot ZT = 2 S σt k κ = κ + κ κ el k κ = κe + κph el κ latt K L - High Seebeck coefficient - High electrical l conductivity it - Low thermal conductivity ZT Insul ators 5 Met tals Semiconductor Carrier Concentration Difficulties in increasing ZT in bulk materials : S σ σ S and k
6 Selection Criteria for Candidate Materials Z max T γ τ mm m 3/2 x y k latt z e ( r+ 1/2) m = effective mass τ = scattering time r = scattering parameter k latt = lattice thermal conductivity T = temperature γ = band degeneracy Guiding Principles: Narrow band-gap semiconductors : Single carrier systems Heavy elements : High μ, low κ Large unit cell, complex structure : low κ Highly anisotropic or highly symmetric Complex compositions : low κ, complex electronic structure Mass Fluctuation : low κ High density of states t near the Fermi level l : high h Seebeck coefficient Science, 303, 818
7 New direction : Nano-based Thermoelectrics Minimizing the thermal conductivity : Thermal conductivity can be significantly reduced by the scattering of unwanted heat flow at the interfaces Phonons Electrons Mean Free Path Λ = nm Λ = 1-10 nm Wavelength λ = nm λ = 1 nm Interfaces that Scatter Phonons but not Electrons Maximizing Seebeck coefficient: Electronic properties may be dramatically modified due to the electron confinement in nanostructures which exhibit low- dimensional behaviors.
8 New Classes of Promising Thermoelectric Materials Nature 413, 597 (2001) Science 297, 2229 (2002) Science 303, 818 (2004) Ag-Sb rich Majumdar, Science 303, 777 (2004) PbSeTe/PbTe QD Super-lattices AgPb18SbTe20 ZT = 800K Science 321, 554 (2008) 0K (ZT) Nature 451, 168 (2008) Nano materials Bulk materials 0.5 Tl0.02Pb0.98Te ZT = 773K Year Nature 459 (2009) Science 320, 634 (2008) Sb rich In 4 Se 3 ZT = 700K Bi x Sb 2-x Te 3 Nanocomposite
9 Theoretical studies Nanodot Nanocomposites Nanograined Nanocomposites 2.5 Λ = nm < L Electron mean free path Woochul Kim, Yunsei Univ.
10 New Approach Nanoparticles Embedded in Bulk Thermoelectric Materials Electron Phonon + nanorod nanoparticles Coherent interface (Matrix/nanoparticl es) Matrix Matrix + nanorod, nanoparticles Type of Bull Matrixes Nanoparticles Nanorods PbTe Bi 2 Te 3 In 2 Te 3 Bi 2 Te 3 Bi 2 Se 3 Sb 2 Te 3 Bi x Sb 2 x Te 3 Bi 2 3 x 2-x 3 Bi 2 Te 3 CdSe Te
11 Synthesis of Various Nanoparticles Bi(C 2 H 3 O 2 ) 3 (or Sb(C 2 H 3 O 2 ) 3 ) + Te-TOP (or Se-TOP) 1-Dodecanthiol Oleylamine, 1-Octadecene Various reaction temperature Size Control 75 o C 80 o C Various Source 85 o C 90 o C Morphology Control 140 o C Composition Control Bi 2 Se o C Bi Bi Bi 09(3) 09(2) Te 15(3) 05(1) 19(3) 01(1) 2 Te 3 0.9(3)Sb 0.9(2) 3 Bi 1.5(3) Sb 0.5(1) Te 3 Bi 1.9(3) Sb 0.1(1) Te 3 11
12 Sample preparation and measurements Sample Preparation Rocking furnace Nanocomposite ingot sawing Polishing ( micro) Data Analysis 900 Measurements Temperature(K) Seebeck Coefficient & Electrical conductivity measurement Nanocomposite sample Temperature(K) Thermal conductivity measurement
13 Nano-structured Bulk Thermoelectirc Material PbTe ingot with Bi 2 Te 3 nanoparticle + PbTe Bi 2 Te 3 nanoparticles(~150nm) incoherent interface Materials Lattice parameter Structure Lattice mismatch PbTe A Rock salt Bi 2 Te 3 a=4.385a, c=30.48a Rhomboh edral 30% (a/a) PbTe with Bi 2Te 3 ingot
14 Nano-Bulk Composite Thermoelectric Material PbTe ingot with Bi 2 Se 3 nanoparticle PbTe + Bi2Se3 + PbTe Bi 2 Se 3 nanoparticles(~80nm) Coherent(stress) incoherent interface
15 Nano-Bulk Composite Thermoelectric Material In2Te3 ingot with Bi2Te3 nanoparticle coherent interface (Particle size < 20nm) + Bi2Te3 nanoparticles (~150nm) In2Te3 Matrix In2Te3 ingot with Bi2Se3 nanoparticle + coherent interface In2Te3 Matrix 15 Bi2Se3 nanoparticles (~80nm)
16 Nano-Bulk Composite Thermoelectric Material Composition dependent of electrical properties PbTe + 2.7% Bi 2 Te 3 PbTe + 10% Bi 2 Te 3 PbTe + 20% Bi Te 2 3 PbTe + 2.7% bulk Bi 2 Te 3 Elect trical Condu uctivity (S/cm m) Electrical Conductivity (S/cm) Temperature (K) See ebeck Coef fficient (μv/k K) Seebeck Coefficient (μv/k) Power Factor (μw/cmk 2 ) Temperature (K) 2 ) Power Facto or (μw/cmk Temperature (K) The values : Negative value The values : ~1000 S/cm at R.T. Majority of charge carriers : 1.5 ~9 W/cmK 2 Electrons The values : ~ -60~-220μV/K Power Factor increase with decreasing nanoparticle content
17 Nano-Bulk Composite Thermoelectric Material Rela ative int tensity Bulk Bi 2 Te 3 * Bi 2 Te 3 * *** * θ Relativ ve intens sity Nanoparticle Bi 2 Te θ
18 1. Remove 2. Electrochemically deposition barrier oxide layer Bi nanowire material 3. Electrochemically deposition Te nanowire material 4. Remove AAO template
19 1. Remove 2. Electrochemically deposition barrier oxide layer nanowire material 1. Remove 2. Remove Ag film AAO template Scheme 1. Schamatic of the process employed to produce (a) superlattice structure (b) one element or binary nanowire arrays by pulsed-potential potential deposition into porous anodic alumina template
20 SEM image Bi and Te NWs
21 Summary 열전재료용나노입자, 나노선제조 Bulk 에나노입자, 나노선삽입 Hydrothermal 법을이용한 Bi 2 Te 3 의 morphologies PbTe ingot with Bi 2 Te 3 Colloidal 법을이용한 Bi 2 Te 3 나노입자 Bi 2 Se 3 나노입자 PbTe ingot with Bi 2 Se 3 Sb 2 Te 3 나노입자 Bi x Sb 2-x Te 3 나노입자 InTe ingot with Bi 2 Se 3 Bi 나노입자 CdSe 나노선 전기화학법을이용한 Bi, Te 나노선 InTe ingot with Bi 2 Te 3
22 Conclusions Nanostructured bulk CompositeTE materials - New approaches are promising in raising ZT - Strong thermal conductivity reduction can be achieved through nanostructuring - Doping studies and processing conditions are important in ZT optimization Nanoparticles - Nano particles of various TE materials are obtained Nanocomposites - New approaches was provide to control the size and concentration of the nanocomponent in bulk TE materials 22
23 Ha Yeong Kim Jieun Park, Hee Jin Kim Dr. Mi-Kyung Han Prof. WooChul Kim Yonsei University Prof. Wooyoung Lee Yonsei University Acknowledgment Grant: 21st Century Frontier R&D Programs NRF, 23
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