Skip to main content
Log in

Solution-processed n-type Bi2Te3−xSex nanocomposites with enhanced thermoelectric performance via liquid-phase sintering

液相烧结增强溶液法制备的n型碲化铋基纳米复合材料的热电性能

  • Articles
  • Published:
Science China Materials Aims and scope Submit manuscript

Abstract

The much slower progress in enhancing the thermoelectric performance of n-type Bi2Te3 than that of p-type Bi2Te3 based materials in the past decade hinders the widespread use in power generation and refrigeration. Here, a facile bottom-up solution-synthesis with spark plasma sintering (SPS) process has been developed to build n-type Bi2Te3−xSex bulk nanocomposites, which substantially improves the power factor and decreases the lattice thermal conductivity by tuning the interface scattering of phonons and electrons. The stoichiometric composition in ternary Bi2Te3−xSex nanocomposites is also tuned to optimize the carrier concentration and lattice thermal conductivity. The optimized bulk nanocomposite Bi2Te2.7Se0.3 exhibits a ZT of 1.1 at ~371 K, which is comparable to the corresponding commercially available ingots. Our results demonstrate the great potential of the solution-processed n-type Bi2Te3−xSex nanocomposites for cost-effective thermoelectric applications.

摘要

近十多年来Bi2Te3基材料热电性能研究中, n型材料的热电性能提升要比p型慢很多, 这极大限制了Bi2Te3基材料在发电和制冷应用 领域中的广泛推广. 本文介绍了一种简单的“自下而上”的溶液合成方法, 并结合放电等离子体烧结工艺来构建n型Bi2Te3−xSex纳米复合块 体材料. 在化学溶液合成过程中引入过量的碲源, 实现在烧结制备样品的过程中引入液相烧结过程. 这一过程优化了声子和电子在界面的 散射行为, 从而增强了材料的功率因子并降低了晶格热导率. 通过调整Bi2Te3−xSex 纳米复合材料中的化学成分进一步实现了载流子浓度和 晶格热导率的优化. 优化的Bi2Te2.7Se0.3材料在~371K下的ZT值达到了1.1, 与商业化碲化铋材料的ZT值相当. 本研究表明溶液法制备的n型 碲化铋基纳米复合材料在大规模低成本的热电应用领域具有重要前景.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Similar content being viewed by others

References

  1. Bell LE. Cooling, heating, generating power, and recovering waste heat with thermoelectric systems. Science, 2008, 321: 1457–1461

    Article  Google Scholar 

  2. Snyder GJ, Toberer ES. Complex thermoelectric materials. Nat Mater, 2008, 7: 105–114

    Article  Google Scholar 

  3. Ortega S, Ibáñez M, Liu Y, et al. Bottom-up engineering of thermoelectric nanomaterials and devices from solution-processed nanoparticle building blocks. Chem Soc Rev, 2017, 46: 3510–3528

    Article  Google Scholar 

  4. Farooq MU, Butt S, Gao K, et al. Pronounced effect of ZnTe nanoinclusions on thermoelectric properties of Cu2-xSe chalcogenides. Sci China Mater, 2016, 59: 135–143

    Article  Google Scholar 

  5. Zhu T, Liu Y, Fu C, et al. Compromise and synergy in highefficiency thermoelectric materials. Adv Mater, 2017, 29: 1605884

    Article  Google Scholar 

  6. Yang G, Yao Y, Ma D. Structural, electronic, and thermoelectric properties of La2CuBiS5. Sci China Mater, 2017, 60: 151–158

    Article  Google Scholar 

  7. Pei Y, Wang H, Snyder GJ. Band engineering of thermoelectric materials. Adv Mater, 2012, 24: 6125–6135

    Article  Google Scholar 

  8. Ding D, Lu C, Tang Z. Bottom up chalcogenide thermoelectric materials from solution-processed nanostructures. Adv Mater Interfaces, 2017, 4: 1700517

    Article  Google Scholar 

  9. Poudel B, Hao Q, Ma Y, et al. High-thermoelectric performance of nanostructured bismuth antimony telluride bulk alloys. Science, 2008, 320: 634–638

    Article  Google Scholar 

  10. Xie W, He J, Kang HJ, et al. Identifying the specific nanostructures responsible for the high thermoelectric performance of (Bi,Sb)2Te3 nanocomposites. Nano Lett, 2010, 10: 3283–3289

    Article  Google Scholar 

  11. Xu Z, Wu H, Zhu T, et al. Attaining high mid-temperature performance in (Bi,Sb)2Te3 thermoelectric materials via synergistic optimization. NPG Asia Mater, 2016, 8: e302

    Article  Google Scholar 

  12. Kim SI, Lee KH, Mun HA, et al. Dense dislocation arrays embedded in grain boundaries for high-performance bulk thermoelectrics. Science, 2015, 348: 109–114

    Article  Google Scholar 

  13. Liu WS, Zhang Q, Lan Y, et al. Thermoelectric property studies on Cu-doped n-type CuxBi2Te2.7Se0.3 nanocomposites. Adv Energy Mater, 2011, 1: 577–587

    Article  Google Scholar 

  14. Yan X, Poudel B, Ma Y, et al. Experimental studies on anisotropic thermoelectric properties and structures of n-type Bi2Te2.7Se0.3. Nano Lett, 2010, 10: 3373–3378

    Article  Google Scholar 

  15. Hu L, Zhu T, Liu X, et al. Point defect engineering of high-performance bismuth-telluride-based thermoelectric materials. Adv Funct Mater, 2014, 24: 5211–5218

    Article  Google Scholar 

  16. Hu L, Wu H, Zhu T, et al. Tuning multiscale microstructures to enhance thermoelectric performance of n-type bismuth-telluridebased solid solutions. Adv Energy Mater, 2015, 5: 1500411

    Article  Google Scholar 

  17. Tang Z, Hu L, Zhu T, et al. High performance n-type bismuth telluride based alloys for mid-temperature power generation. J Mater Chem C, 2015, 3: 10597–10603

    Article  Google Scholar 

  18. Ao WQ, Sun WA, Li JQ, et al. Hydrothermal synthesis of nanosized AgPb18SbTe20 thermoelectric powders. J Alloys Compd, 2009, 475: L22–L24

    Article  Google Scholar 

  19. Mehta RJ, Zhang Y, Karthik C, et al. A new class of doped nanobulk high-figure-of-merit thermoelectrics by scalable bottom-up assembly. Nat Mater, 2012, 11: 233–240

    Article  Google Scholar 

  20. Son JS, Choi MK, Han MK, et al. n-Type nanostructured thermoelectric materials prepared from chemically synthesized ultrathin Bi2Te3 nanoplates. Nano Lett, 2012, 12: 640–647

    Article  Google Scholar 

  21. Zhang Y, Day T, Snedaker ML, et al. A mesoporous anisotropic ntype Bi2Te3 monolith with low thermal conductivity as an efficient thermoelectric material. Adv Mater, 2012, 24: 5065–5070

    Article  Google Scholar 

  22. Min Y, Roh JW, Yang H, et al. Surfactant-free scalable synthesis of Bi2Te3 and Bi2Se3 nanoflakes and enhanced thermoelectric properties of their nanocomposites. Adv Mater, 2013, 25: 1425–1429

    Article  Google Scholar 

  23. Hong M, Chasapis TC, Chen ZG, et al. n-Type Bi2Te3–xSex nanoplates with enhanced thermoelectric efficiency driven by widefrequency phonon scatterings and synergistic carrier scatterings. ACS Nano, 2016, 10: 4719–4727

    Article  Google Scholar 

  24. Li S, Xin C, Liu X, et al. 2D hetero-nanosheets to enable ultralow thermal conductivity by all scale phonon scattering for highly thermoelectric performance. Nano Energy, 2016, 30: 780–789

    Article  Google Scholar 

  25. Li S, Fan T, Liu X, et al. Graphene quantum dots embedded in Bi2Te3 nanosheets to enhance thermoelectric performance. ACS Appl Mater Interfaces, 2017, 9: 3677–3685

    Article  Google Scholar 

  26. Min Y, Park G, Kim B, et al. Synthesis of multishell nanoplates by consecutive epitaxial growth of Bi2Se3 and Bi2Te3 nanoplates and enhanced thermoelectric properties. ACS Nano, 2015, 9: 6843–6853

    Article  Google Scholar 

  27. Zhao XB, Ji XH, Zhang YH, et al. Bismuth telluride nanotubes and the effects on the thermoelectric properties of nanotube-containing nanocomposites. Appl Phys Lett, 2005, 86: 062111

    Article  Google Scholar 

  28. Dirmyer MR, Martin J, Nolas GS, et al. Thermal and electrical conductivity of size-tuned bismuth telluride nanoparticles. Small, 2009, 5: 933–937

    Article  Google Scholar 

  29. Fang H, Bahk JH, Feng T, et al. Thermoelectric properties of solution-synthesized n-type Bi2Te3 nanocomposites modulated by Se: An experimental and theoretical study. Nano Res, 2015, 9: 117–127

    Article  Google Scholar 

  30. Scheele M, Oeschler N, Meier K, et al. Synthesis and thermoelectric characterization of Bi2Te3 nanoparticles. Adv Funct Mater, 2009, 19: 3476–3483

    Article  Google Scholar 

  31. German RM, Suri P, Park SJ. Review: liquid phase sintering. J Mater Sci, 2008, 44: 1–39

    Article  Google Scholar 

  32. Zhang C, Ng H, Li Z, et al. Minority carrier blocking to enhance the thermoelectric performance of solution-processed BixSb2–xTe3 nanocomposites via a liquid-phase sintering process. ACS Appl Mater Interfaces, 2017, 9: 12501–12510

    Article  Google Scholar 

  33. Zhang C, de la Mata M, Li Z, et al. Enhanced thermoelectric performance of solution-derived bismuth telluride based nanocomposites via liquid-phase sintering. Nano Energy, 2016, 30: 630–638

    Article  Google Scholar 

  34. Li JQ, Li LF, Song SH, et al. High thermoelectric performance of GeTe–Ag8GeTe6 eutectic composites. J Alloys Compd, 2013, 565: 144–147

    Article  Google Scholar 

  35. Zhang C, Peng Z, Li Z, et al. Controlled growth of bismuth antimony telluride BixSb2-xTe3 nanoplatelets and their bulk thermoelectric nanocomposites. Nano Energy, 2015, 15: 688–696

    Article  Google Scholar 

  36. Soni A, Yanyuan Z, Ligen Y, et al. Enhanced thermoelectric properties of solution grown Bi2Te3–xSex nanoplatelet composites. Nano Lett, 2012, 12: 1203–1209

    Article  Google Scholar 

  37. Lu Z, Tan LP, Zhao X, et al. Aqueous solution synthesis of (Sb, Bi)2 (Te, Se)3 nanocrystals with controllable composition and morphology. J Mater Chem C, 2013, 1: 6271

    Article  Google Scholar 

  38. Fu J, Song S, Zhang X, et al. Bi2Te3 nanoplates and nanoflowers: Synthesized by hydrothermal process and their enhanced ther-moelectric properties. CrystEngComm, 2012, 14: 2159

    Article  Google Scholar 

  39. Kim HS, Gibbs ZM, Tang Y, et al. Characterization of Lorenz number with Seebeck coefficient measurement. APL Mater, 2015, 3: 041506

    Article  Google Scholar 

  40. Puneet P, Podila R, Karakaya M, et al. Preferential scattering by interfacial charged defects for enhanced thermoelectric performance in few-layered n-type Bi2Te3. Sci Rep, 2013, 3: 3212

    Article  Google Scholar 

  41. Pan Y, Li JF. Thermoelectric performance enhancement in n-type Bi2(TeSe)3 alloys owing to nanoscale inhomogeneity combined with a spark plasma-textured microstructure. NPG Asia Mater, 2016, 8: e275

    Article  Google Scholar 

  42. Borup KA, de Boor J, Wang H, et al. Measuring thermoelectric transport properties of materials. Energy Environ Sci, 2015, 8: 423–435

    Article  Google Scholar 

Download references

Acknowledgements

This work was supported by the Natural Science Foundation of SZU (2017003), Shenzhen Science and Technology Research Grant (JCYJ20150324141711684), Singapore National Research Foundation (NRF-RF2009-06) and an Investigator-ship Award (NRFNRFI2015- 03), Ministry of Education (Singapore) via an AcRF Tier2 Grant (MOE2012-T2-2-086). We also thank Dr. Zhong Li and Prof. Khiam Aik Khor for the support on the spark-plasma-sintering experiments.

Author information

Authors and Affiliations

Authors

Corresponding authors

Correspondence to Chaohua Zhang  (张朝华) or Qihua Xiong  (熊启华).

Additional information

Author contributions Zhang C and Xiong Q designed the experiments. Zhang C conducted the material synthesis and characterization. Ng H performed part of the solution-synthesis of the samples. Zhang CX contributed to the SEM characterization. Zhang C wrote the paper with support from Xiong Q. All authors contributed to the general discussion.

Conflict of interest The authors declare no conflicts of interest.

Supplementary information Experimental results including the image of expelled items, EDX, comparison of the thermoelectric properties and the anisotropy of the thermal conductivity test are available in the online version of the paper.

Chaohua Zhang received his BSc degree in physics from Lanzhou University in 2008, and received his PhD degree in physical chemistry under the supervision of Prof. Zhongfan Liu from Peking University in 2013. After three years postdoctoral experience in Prof. Qihua Xiong’s group at Nanyang Technological University, he joined Shenzhen University as an associate professor in 2017. His current research is focused on the controllable growth of 2D materials, synthesis and characterization of thermoelectric materials.

Qihua Xiong received his BSc degree in physics from Wuhan University in 1997, and then finished three years graduate studies at Shanghai Institute of Applied Physics, Chinese Academy of Sciences. He received a PhD degree under the supervision of Prof. Peter C. Eklund from Pennsylvania State University in 2006. After three years postdoctoral experience in Prof. Charles M. Lieber’s group at Harvard University, he joined Nanyang Technological University as an assistant professor in 2009 and was promoted to Professor in 2016. His research focuses on light-matter interactions of emergent quantum matter by optical spectroscopy approaches. He recently ventured into the field of 2D layered materials and laser cooling of solids.

Electronic supplementary material

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Zhang, C., Zhang, C., Ng, H. et al. Solution-processed n-type Bi2Te3−xSex nanocomposites with enhanced thermoelectric performance via liquid-phase sintering. Sci. China Mater. 62, 389–398 (2019). https://doi.org/10.1007/s40843-018-9312-5

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s40843-018-9312-5

Keywords

Navigation