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Title Page

Contents

Abbreviation 14

Abstract 18

Chapter 1. A general introduction to the thermoelectricity 22

1.1. Thermoelectric effect 23

1.2. Challenging to enhance the power factor 26

1.3. Reducing the thermal conductivity (K) 31

1.4. Phonon scattering 33

Chapter 2. Enhancement of thermoelectric performance in coated grain nanocomposite 35

2.1. High thermoelectric performance with coated grain embedded nanocomposites. 36

2.2. High thermoelectric performance in nanocomposite with coated grain boundary 39

2.2.1. Theoretical calculation of the Seebeck coefficient of the coated grain boundary 39

2.2.2. Theoretical calculation of phonon scattering 40

2.3. Synthesis of coated grain boundary contained composite 44

2.3.1. Solubility product (Kₛₚ) 45

2.3.2. Pearson's hard and soft acids and bases (HSAB) theory 46

2.3.3. Crystal structure similarity 49

Chapter 3. Eco-friendly thermoelectric materials: coated grain contained nanocomposite of SnTe / CuInTe₂ 51

3.1. Abstract 52

3.2. Introduction 53

3.3. Experimental Section 54

3.3.1. Chemicals and materials 54

3.3.2. Synthesis of Ag and In co-doped SnTe 54

3.3.3. Cation exchange reaction 55

3.3.4. Characterization of phase 55

3.3.5. Hot press and sintering 56

3.3.6. Characterizations of thermoelectric properties 56

3.4. Results and discussion 58

3.5. Conclusion 61

Chapter 4. Coated grain nanocomposite based on PbSe 67

4.1. Abstract 68

4.2. Introduction 69

4.3. Experimental Section 70

4.3.1. Synthesis 70

4.3.2. Cation exchange reaction 70

4.3.3. Spark plasma sintering (SPS) 71

4.3.4. Characterization of physical properties 72

4.4. Result and discussion 74

4.5. Conclusion 79

Reference 89

국문 초록 94

Table 2-1. Solubility product (Kₛₚ) of metal chalcogenides. 45

Table 2-2. Periodic table classifying elements forming hard and soft acids/bases. 46

Table 3-1. Results of the Hall effect measurement. CG indicates coated grain and the meanings of 1:1,3:3,5 :5 and 7:7 are the molar percentages of Cu and In precursors relative... 64

Table 4-1. Lattice parameter of the PbSe powder samples, (a) Lattice parameter of the 1% Cr doped PbSe. (b) Lattice parameter of the powder samples after cation exchange reaction... 83

Table 4-2. Comparison of the acoustic impedances. Acoustic impedances of between CuInTe₂ and SnTe, and between CdSe and PbSe. 87

Chapter 1. A general introduction to the thermoelectricity 9

Figure 1-1. Schematic of (a) Seebeck effect for the electric energy generator, (b) Peltier effect for refrigerator. 23

Figure 1-2. Relationship between the Seebeck coefficient (S), the electrical conductivity (σ), and the thermoelectric power factor (S²σ). 30

Figure 1-3. Graph of the thermal conductivity (K) as a function of carrier concentration. 31

Figure 1-4. (a) Spring-mass system representing solid phase material, (b) Phonon gas model. 33

Figure 1-5. Different types of scattering processes in crystalline solid. 34

Chapter 2. Enhancement of thermoelectric performance in coated grain nanocomposite 10

Figure 2-1. Schematic of energy filtering effect. Electrons of high energy and low energy are represented as red and blue circles, respectively. 37

Figure 2-2. Schematics of the phonon scattering effect by the embedded materials, (a) scattered phonons by the nanoparticles (b) scattered phonons by the coated grain boundaries. 38

Figure 2-3. Schematic of scattering cross section. The light is represented as arrows. 40

Figure 2-4. Schematic of modeled coated particle for van-de Hulst approximation. 42

Figure 2-5. Schematic of the synthesized coated grain boundary by cation exchange reaction. 44

Figure 2-6. Schematic of cation exchange mechanism on the surface of SnTe. 47

Figure 2-7. Mechanism of the nucleophilic acyl substitution. 48

Figure 2-8. The powder X-ray diffraction (PXRD) pattern of SnTe based composite. ZnO as by-product formed by the nucleophilic acyl substitution was observed. 48

Figure 2-9. Crystal structure similarity of CuInTe₂ and SnTe. 49

Chapter 3. Eco-friendly thermoelectric materials: coated grain contained nanocomposite of SnTe / CuInTe₂ 11

Figure 3-1. PXRD data for coated grain boundary system of SnTe / CuInTe₂. CG means coated grain and the meanings of 1, 3, 5 and 7 are the molar percentages of Cu and In ion... 62

Figure 3-2. Transmission electron microscope (TEM) analysis of the CuInTe₂/ SnTe coated grain nanostructures, (a), (b), (c) and (d) are the BF-STEM images of SnTe coated with 5... 63

Figure 3-3. The results of the STEM- EDS (Scanning TEM-Electron Dispersive Spectroscopy) analysis for SnTe / CuInTe₂ coated grain boundary structure. 64

Figure 3-4. Temperature dependent electrical transport properties of SnTe composite containing coated layer of CuInTe₂ by cation exchange (a) Resistivity, (b) Seebeck... 65

Figure 3-5. Temperature dependent thermal conductivity of the CuInTe₂/ SnTe depending on the mole fraction of the Cu and In precursors for cation exchange reaction. 66

Figure 3-6. Temperature dependent thermoelectric figure of merits (zT) of coated grain CuInTe₂/ SnTe nanocomposites depending on the mole fraction of the Cu and In precursors. 66

Chapter 4. Coated grain nanocomposite based on PbSe 12

Figure 4-1. Schematic of SPS furnace. 71

Figure 4-2. PXRD data for coated grain boundary system of PbSe / Cu₂Se synthesized by cation exchange reaction with 3 molar percent of the Cu(Ace)₂ with respect to the matrix... 80

Figure 4-3. Temperature dependent thermal conductivity of PbSe and surface coated PbSe by cation exchange reaction with 3 molar percent of the Cu(Ace)₂ 81

Figure 4-4. Temperature dependent electrical transport properties of PbSe fabricated by cation exchange reaction with 3 molar percent of the Cu(Ace)₂ with respect to the matrix... 82

Figure 4-5. Schematic of the diffusing Cu ions from Cu₂Se in the PbSe matrix as temperature increases. 83

Figure 4-6. PXRD patterns of the PbSe / Cu₂Se nanocomposite powder samples after annealing process at 460℃ for 40 minutes. 84

Figure 4-7. Temperature dependent electrical transport properties of PbSe composite prepared by cation exchange reaction with 3 molar percent of the Cd(Ace)₂ as a Cd... 85

Figure 4-8. Temperature dependent properties of the PbSe / CdSe nanocomposite, (a) Thermal conductivity, (b) zT. 86

Figure 4-9. Schematic of the phonon scattering depend on the difference of the acoustic impedance. 87

Figure 4-10. Temperature dependence of the thermal conductivity of 1% Cr-doped PbSe. 88

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