Significant Reduction in Lattice Thermal Conductivity of (PbTe)0.95 - (PbS)0.05 Thermoelectric Materials Through Liquid Silicon Quenching
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Keywords:
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Binary PbTe-PbS System, Lattice Thermal Conductivity, Sustainable Energy, Silicon Quenching, Thermoelectric
Abstract
Thermoelectric materials are game-changers, that have the ability to transform waste heat into electrical energy, making them a potential renewable energy solution to reduce reliance on fossil fuels. The standard metric for evaluating thermoelectric materials is the dimensionless figure of merit, ZT, which is markedly influenced by lattice thermal conductivity (ĸl ). Higher thermal transport through the lattice lowers the ZT value, reducing the material’s efficiency. Therefore, finding ways to decrease ????l is critical for boosting thermoelectric performance. In our research, we explored an innovative approach by applying a quenching technique using liquid silicon to reduce thermal conductivity (ĸT ) due to lattice vibrations. We compared the lattice conductivity (ĸl ) of materials with and without this liquid silicon quenching process. The results were striking: at 300 K, quenching lowers the lattice thermal conductivity by about 40.1 %, and at 800 K, it is still reduced by roughly 24.7%compared with pristine PbTe. Even more impressive, when compared to non-quenched (PbTe)0.95 − (PbS)0.05 alloys, at 300 K, the silicon-quenched sample attains an additional ĸl reduction of roughly 16.1 %, while at 800 K the extra decrease is about 13.0%. These findings highlight that liquid silicon quenching is a highly effective method for lowering ĸl of PbTe thermoelectric materials. This approach paves the way for developing next-generation thermoelectric materials that are more efficient, particularly for eco-friendly waste heat recovery applications. Our work opens new possibilities for sustainable energy innovation.
References
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Tan, G., L. D. Zhao, and M. G. Kanatzidis (2016). Rationally Designing High-Performance Bulk Thermoelectric Materials. Chemical Reviews, 116(19); 12123–12149
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Zebarjadi, M., K. Esfarjani, M. S. Dresselhaus, Z. Ren, and G. Chen (2012). Perspectives on Thermoelectrics: From Fundamentals to Device Applications. Energy & Environmental Science, 5(1); 5147–5162
Zhang, X. and L. D. Zhao (2015). Thermoelectric Materials: Energy Conversion Between Heat and Electricity. Journal of Materiomics, 1(2); 92–105
Zhao, L. D., C. Chang, G. Tan, and M. G. Kanatzidis (2016). SnSe: A Remarkable New Thermoelectric Material. Energy & Environmental Science, 9(10); 3044–3060
Zhao, L. D., V. P. Dravid, and M. G. Kanatzidis (2014a). The Panoscopic Approach to High Performance Thermoelectrics. Energy & Environmental Science, 7(1); 251–268
Zhao, L. D., S.-H. Lo, Y. Zhang, H. Sun, G. Tan, C. Uher, C. Wolverton, V. P. Dravid, and M. G. Kanatzidis (2014b). Ultralow Thermal Conductivity and High Thermoelectric Figure of Merit in SnSe Crystals. Nature, 508(7496); 373–377
Zhao, W., Z. Liu, P. Wei, Q. Zhang, W. Zhu, X. Su, X. Tang, J. Yang, Y. Liu, J. Shi, Y. Chao, S. Lin, and Y. Pei (2021). Flexible, Stretchable, and High-Temperature Thermoelectric Module Based on Solution-Synthesized Tellurium Nanowires. Nature Communications, 12(1); 1–10
Zhu, T., Y. Liu, C. Fu, J. P. Heremans, G. J. Snyder, and X. Zhao (2017). Compromise and Synergy in High-Efficiency Thermoelectric Materials. Advanced Materials, 29(14); 1605884
Biswas, K., J. He, I. D. Blum, C.-I. Wu, T. P. Hogan, D. N. Seidman, V. P. Dravid, and M. G. Kanatzidis (2012). High-Performance Bulk Thermoelectrics with All-Scale Hierarchical Architectures. Nature, 489(7416); 414–418
Chen, Z., X. Zhang, and Y. Pei (2018). Manipulation of Phonon Transport in Thermoelectrics. Advanced Materials, 30(43); 1705617
Delaire, O., J. Ma, K. Marty, A. F. May, M. A. McGuire, M.-H. Du, D. J. Singh, A. Podlesnyak, G. Ehlers, M. D. Lumsden, and B. C. Sales (2011). Giant Anharmonic Phonon Scattering in PbTe. Nature Materials, 10(8); 614–619
Dughaish, Z. H. (2002). Lead Telluride as a Thermoelectric Material for Thermoelectric Power Generation. Physica B: Condensed Matter, 322(1–2); 205–223
Fu, C., H. Wu, Y. Liu, J. He, X. Zhao, and T. Zhu (2021). Enhancing Thermoelectric Properties by Engineering Crystal Defects. Advanced Science, 8(1); 2002328
Gayner, C. and K. K. Kar (2016). Recent Advances in Thermoelectric Materials. Progress in Materials Science, 83; 330–382
Ginting, D., C.-C. Lin, L. Rathnam, B.-K. Yu, S.-J. Kim, R. A. Al Orabi, and J.-S. Rhyee (2016). Enhancement of Thermoelectric Properties by Effective K-Doping and Nano Precipitation in Quaternary Compounds of (Pb1-xKxTe) 0.70(PbSe) 0.25(PbS) 0.05. RSC Advances, 6(67); 62958–62967
Ginting, D., C.-C. Lin, and J.-S. Rhyee (2019). Synergetic Approach for Superior Thermoelectric Performance in PbTe-PbSe-PbS Quaternary Alloys and Composites. Energies, 13(1); 72
Girard, S. N., K. Schmidt-Rohr, T. C. Chasapis, E. Hatzikraniotis, B. Njegic, E. M. Levin, A. Rawal, K. M. Paraskevopoulos, and M. G. Kanatzidis (2021). Analysis of Phase Separation in High-Performance PbTe–PbS Thermoelectric Materials. Advanced Functional Materials, 31(13); 2100258
Han, M.-K., Y. Jin, D.-H. Lee, and S.-J. Kim (2017). Thermoelectric Properties of Bi2Te3: CuI and the Effect of Its Doping with Pb Atoms. Materials, 10(11); 1235
Hanus, R., M. T. Agne, A. J. E. Rettie, and et al. (2019). Lattice Softening Significantly Reduces Thermal Conductivity and Leads to High Thermoelectric Efficiency. Advanced Materials, 31(21); 1900108
He, J. and T. M. Tritt (2017). Advances in Thermoelectric Materials Research: Looking Back and Moving Forward. Science, 357(6358); eaak9997
Heremans, J. P., V. Jovovic, E. S. Toberer, A. Saramat, K. Kurosaki, A. Charoenphakdee, S. Yamanaka, and G. J. Snyder (2008). Enhancement of Thermoelectric Efficiency in PbTe by Distortion of the Electronic Density of States. Science, 321(5888); 554–557
Jahiding, M., M. Mashuni, H. Hamid, W. O. S. Ilmawati, and R. Hamdana (2024). The Production of Renewable Fuels Sago Dregs and Low-Density Polyethylene by Pyrolysis and Its Characterization. Science and Technology Indonesia, 9(3); 565–576
Johnsen, S., J. He, J. Androulakis, V. P. Dravid, I. Todorov, D. Y. Chung, and M. G. Kanatzidis (2011). Nanostructures Boost the Thermoelectric Performance of PbS. Journal of the American Chemical Society, 133(10); 3460–3470
Kim, J. H., M. J. Kim, S. Oh, and J.-S. Rhyee (2014). Thermoelectric Properties of Se-Deficient and Pb-/Sn-Codoped In4Pb0.01Sn0.03Se3-x Polycrystalline Compounds. Journal of Alloys and Compounds, 615; 933–936
Korrapati, V., G. Sumanasekera, and M. K. Sunkara (2022). Recent Advances in Bulk Thermoelectric Materials: Strategies to Enhance Figure of Merit. Dalton Transactions, 51(8); 2845–2869
Lee, M. H., K.-R. Kim, J.-S. Rhyee, S.-D. Park, and G. J. Snyder (2015). High Thermoelectric Figure-of-Merit in Sb2Te3/Ag2Te Bulk Composites as Pb-Free p-Type Thermoelectric Materials. Journal of Materials Chemistry C, 3; 10494–10499
Lee, Y., S.-H. Lo, J. Androulakis, C.-I. Wu, L. Zhao, D. Y. Chung, T. P. Hogan, V. P. Dravid, and M. G. Kanatzidis (2013). High-Performance Tellurium-Free Thermoelectrics: All-Scale Hierarchical Structuring of p-Type PbSe-MSe Systems (M = Ca, Sr, Ba). Journal of the American Chemical Society, 135(13); 5152–5160
Li, J., X. Zhang, S. Lin, Z. Chen, and Y. Pei (2020). Realizing the High Thermoelectric Performance of GeTe by Sb-Doping and Se-Alloying. Chemistry of Materials, 32(11); 4786–4793
Liu, Z., J. Mao, J. Liu, and Z. Ren (2022). Advances in Thermoelectrics: The Roles of Microstructures and Processing Techniques. Materials Today Physics, 23; 100683
Mao, J., G. Chen, and Z. Ren (2020). Thermoelectric Cooling Materials. Nature Materials, 20(4); 454–461
Nielsen, M. D., V. Ozolins, and J. P. Heremans (2013). Lone Pair Electrons Minimize Lattice Thermal Conductivity. Energy & Environmental Science, 6(2); 570–578
Parashchuk, T., B. Wiendlocha, and et al. (2021). High Thermoelectric Performance of p-Type PbTe Enabled by the Synergy of Resonance Scattering and Lattice Softening. ACS Applied Materials & Interfaces, 13(39); 46773–46784
Pei, Y., X. Shi, A. LaLonde, H. Wang, L. Chen, and G. J. Snyder (2011). Convergence of Electronic Bands for High Performance Bulk Thermoelectrics. Nature, 473(7345); 66–69
Pei, Y., H. Wang, and G. J. Snyder (2012). Band Engineering of Thermoelectric Materials. Advanced Materials, 24(46); 6125–6135
Petsagkourakis, I., K. Tybrandt, X. Crispin, I. Ohkubo, N. Satoh, and T. Mori (2018). Thermoelectric Materials and Applications for Energy Harvesting Power Generation. Science and Technology of Advanced Materials, 19(1); 836–862
Rohendi, D., I. Amelia, N. F. Sya’baniah, D. H. Yulianti, N. Syarif, A. Rachmat, Fatmawati, and E. H. Majlan (2024). The Influence of Catalyst Loading on Electrocatalytic Activity and Hydrogen Production in PEM Water Electrolysis. Science and Technology Indonesia, 9(3); 556–564
Romero, A. H., E. K. U. Gross, M. J. Verstraete, and O. Hellman (2015). Thermal Conductivity in PbTe from First Principles. Physical Review B, 91(21); 214310
Samanta, M., K. Biswas, and N. R. Desai (2018). Hole-Doping and Temperature Induced Band Inversion in Topological PbSe: Enhanced Thermoelectric Properties via Convergence of Electronic Bands. Chemistry of Materials, 30(3); 989–998
Sasidharan, N. T., V. Vaiyapuri, K. Elamurugan, N. Mani, and K. Annamalai (2025). Phonon Engineering Enabled Reduction in Thermal Conductivity of SnS/Cu2Se Composites: An Experimental and Numerical Insights. Surfaces and Interfaces, 56; 105488
Snyder, G. J. and E. S. Toberer (2008). Complex Thermoelectric Materials. Nature Materials, 7(2); 105–114
Tan, G., L. D. Zhao, and M. G. Kanatzidis (2016). Rationally Designing High-Performance Bulk Thermoelectric Materials. Chemical Reviews, 116(19); 12123–12149
Telussa, I., E. G. Fransina, E. R. M. A. P. Lilipaly, and A. M. I. Efruan (2022). Effect of Photosynthetic Pigment Composition of Tropical Marine Microalgae from Ambon Bay Navicula sp. Tad on Dye-sensitized Solar Cell Efficiency. Science and Technology Indonesia, 7(4); 486–491
Tian, Z., J. Garg, K. Esfarjani, T. Shiga, J. Shiomi, and G. Chen (2012). Phonon Conduction in PbSe, PbTe, and PbTe1-xSex from First-Principles Calculations. Physical Review B, 85(18); 184303
Wang, H., Z. M. Gibbs, Y. Takagiwa, and G. J. Snyder (2019). Tuning Bands of PbSe for Better Thermoelectric Efficiency. Energy & Environmental Science, 7(2); 804–811
Widianingsih, S., I. Yanti, A. Kamari, and I. Fatimah (2024). Thermal Conversion of Coral Waste and its Utilization as Low-Cost Catalyst for Biodiesel Production. Science and Technology Indonesia, 9(4); 866–875
Wu, H. J., L. D. Zhao, F. S. Zheng, D. Wu, Y. L. Pei, X. Tong, M. G. Kanatzidis, and J. Q. He (2014). Broad Temperature Plateau for Thermoelectric Figure of Merit ZT > 2 in Phase-Separated PbTe0.7S0.3. Nature Communications, 5(1); 5515
Wu, L., J.-C. Zheng, J. Zhou, Q. Li, J. Yang, and Y. Zhu (2015). Nanostructures and Defects in Thermoelectric AgPb18SbTe20 Single Crystal. Journal of Applied Physics, 105(9); 094317
Xiao, Y. and L. D. Zhao (2018). Charge and Phonon Transport in PbTe-Based Thermoelectric Materials. npj Quantum Materials, 3(1); 29
Yamini, S. A., T. Ikeda, A. LaLonde, Y. Pei, S. X. Dou, and G. J. Snyder (2014). Rational Design of p-Type Thermoelectric PbTe: Temperature Dependent Sodium Solubility. Journal of Materials Chemistry A, 1(31); 8725–8730
Yang, L., Z.-G. Chen, G. Han, M. Hong, and J. Zou (2020). Impacts of Cu Deficiency on the Thermoelectric Properties of Cu2-XSe Nanoplates. Nano Energy, 69; 104394
Yang, S., J. Si, Q. Su, and H. Wu (2022). Machine Learning in Thermoelectric Materials: A Perspective. Energy & Environmental Materials, 5(1); 150–171
Zebarjadi, M., K. Esfarjani, M. S. Dresselhaus, Z. Ren, and G. Chen (2012). Perspectives on Thermoelectrics: From Fundamentals to Device Applications. Energy & Environmental Science, 5(1); 5147–5162
Zhang, X. and L. D. Zhao (2015). Thermoelectric Materials: Energy Conversion Between Heat and Electricity. Journal of Materiomics, 1(2); 92–105
Zhao, L. D., C. Chang, G. Tan, and M. G. Kanatzidis (2016). SnSe: A Remarkable New Thermoelectric Material. Energy & Environmental Science, 9(10); 3044–3060
Zhao, L. D., V. P. Dravid, and M. G. Kanatzidis (2014a). The Panoscopic Approach to High Performance Thermoelectrics. Energy & Environmental Science, 7(1); 251–268
Zhao, L. D., S.-H. Lo, Y. Zhang, H. Sun, G. Tan, C. Uher, C. Wolverton, V. P. Dravid, and M. G. Kanatzidis (2014b). Ultralow Thermal Conductivity and High Thermoelectric Figure of Merit in SnSe Crystals. Nature, 508(7496); 373–377
Zhao, W., Z. Liu, P. Wei, Q. Zhang, W. Zhu, X. Su, X. Tang, J. Yang, Y. Liu, J. Shi, Y. Chao, S. Lin, and Y. Pei (2021). Flexible, Stretchable, and High-Temperature Thermoelectric Module Based on Solution-Synthesized Tellurium Nanowires. Nature Communications, 12(1); 1–10
Zhu, T., Y. Liu, C. Fu, J. P. Heremans, G. J. Snyder, and X. Zhao (2017). Compromise and Synergy in High-Efficiency Thermoelectric Materials. Advanced Materials, 29(14); 1605884
Authors
Ginting, D., Nurlela, A., Nanto, D. ., Mashadi, Sudiro, T., Kristiantoro, T. ., & Rhye, J.-S. (2025). Significant Reduction in Lattice Thermal Conductivity of (PbTe)0.95 - (PbS)0.05 Thermoelectric Materials Through Liquid Silicon Quenching. Science and Technology Indonesia, 10(4), 1087–1095. https://doi.org/10.26554/sti.2025.10.4.1087-1095
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