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Staggered-layer-boosted flexible Bi2Te3 films with high thermoelectric performance

Nature Nanotechnology volume 18, pages 1281–1288 (2023)Cite this article

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Abstract

Room-temperature bismuth telluride (Bi2Te3) thermoelectrics are promising candidates for low-grade heat harvesting. However, the brittleness and inflexibility of Bi2Te3 are far reaching and bring about lifelong drawbacks. Here we demonstrate good pliability over 1,000 bending cycles and high power factors of 4.2 (p type) and 4.6 (n type) mW m−1 K−2 in Bi2Te3-based films that were exfoliated from corresponding single crystals. This unprecedented bendability was ascribed to the in situ observed staggered-layer structure that was spontaneously formed during the fabrication to promote stress propagation whilst maintaining good electrical conductivity. Unexpectedly, the donor-like staggered layer rarely affected the carrier transport of the films, thus maintaining its superior thermoelectric performance. Our flexible generator showed a high normalized power density of 321 W m−2 with a temperature difference of 60 K. These high performances in supple thermoelectric films not only offer useful paradigms for wearable electronics, but also provide key insights into structure–property manipulation in inorganic semiconductors.

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Fig. 1: Exceptional flexibility and high TE performance of Bi2Te3-based films.
Fig. 2: Macroscopic, microscopic and atomic-scale in situ observations of staggered-layer-boosted flexibility for p-type BST films.
Fig. 3: DFT calculations showing the staggered-layer structure transformation in Bi2Te3 thin film.
Fig. 4: Temperature-dependent TE properties and DFT electronic band structures of the p- and n-type SCs and films.
Fig. 5: Electrical output performance of Bi2Te3-based f-TEGs.

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Acknowledgements

J.H. acknowledges support from the National Natural Science Foundation of China (grant 11934007), the Science and Technology Innovation Committee Foundation of Shenzhen (grant JCYJ20200109141205978) and the Outstanding Talents Training Fund in Shenzhen (202108). L.X. acknowledges support from the Science and Technology Innovation Committee Foundation of Shenzhen (grant JCYJ20190809145205497). We thank K. Cai at Tongji University for fruitful discussion, and M. Han at Shenzhen Institute of Advanced Technology, Chinese Academy of Sciences, for support on the thermal diffusion coefficient testing. We acknowledge the assistance of SUSTech Core Research Facilities. We also thank F. Shen and S. Liu from Thermo Fisher Scientific and Z. Li from BestronST for help and discussion on the mechanical in situ TEM testing at Shanghai NanoPort.

Author information

Author notes

  1. These authors contributed equally: Yao Lu, Yi Zhou, Wu Wang, Mingyuan Hu.

Authors and Affiliations

  1. Shenzhen Key Laboratory of Thermoelectric Materials, Department of Physics, Southern University of Science and Technology, Shenzhen, China

    Yao Lu, Yi Zhou, Wu Wang, Mingyuan Hu, Dasha Mao, Shan Huang, Lin Xie, Peijian Lin, Binbin Jiang, Bin Zhu, Jianghe Feng, Jianxu Shi, Qing Lou, Yi Huang, Jianmin Yang, Jinhong Li & Jiaqing He

  2. International School of Microelectronics, Dongguan University of Technology, Dongguan, China

    Yao Lu

  3. Department of Electrical and Computer Engineering, National University of Singapore, Singapore, Singapore

    Yi Zhou

  4. Hubei Key Laboratory of Theory and Application of Advanced Materials Mechanics, Wuhan University of Technology, Wuhan, China

    Xiege Huang & Guodong Li

  5. Guangdong–Hong Kong–Macao Joint Laboratory for Photonic–Thermal–Electrical Energy Materials and Devices, Southern University of Science and Technology, Shenzhen, China

    Jiaqing He

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Contributions

Y.L., Y.Z., W.W., M.H. and J.H. conceived the general idea. J.H. supervised the project. Y.L. prepared the samples and devices, carried out the measurements and characterizations and interpreted the results. Y.Z. constructed the device testing equipment, performed the finite-element simulations and analysed the data. W.W. contributed to the TEM observations, simulations and analysis. M.H. contributed to the growth and optimization of SCs. X.H., S.H. and G.L. conducted the DFT calculations. D.M., L.X., P.L., B.J., B.Z., J.F., J.S. and J.L. contributed to the TE characterizations. Q.L., Y.H. and J.Y. helped to prepare the sample for electron microscopy observations. Y.L., Y.Z., W.W., M.H. and J.H. wrote the paper. All authors discussed and commented on the results.

Corresponding author

Correspondence to Jiaqing He.

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Extended data

Extended Data Fig. 1 STEM-EDS spectrum image and analysis of the staggered layers for p-type BST films.

a, HAADF-STEM image, overall corresponding EDS spectrum image and individual elemental Bi, Sb, Te maps of the p-type Bi0.5Sb1.5Te3 thin film. b, Intensity profiles of the staggered layers (marked in HAADF image of a) from the HAADF and elemental maps.

Source data

Extended Data Fig. 2 In situ TEM investigation of p-type BST films.

a, The protocol of FIB sample preparation for in situ mechanical TEM testing. b, The SEM image of resultant FIB sample. c, Intensity profiles of atomic columns in Te (upper) and BiSb layer (lower) in staggered layers in the marked region tracked from image i to vi in Fig. 2g. d, Strain maps for the nanostructure evolution during in situ deformation tracked from image i to vi in Fig. 2g.

Source data

Extended Data Fig. 3 Cyclic temperature dependent thermoelectric properties.

Temperature dependent thermoelectric properties of p-type samples (a, b, c) and n-type samples under three test cycles (d, e, f).

Source data

Extended Data Fig. 4 The design and performance of the Bi2Te3-based 5-pair p–n f-TEG.

a, The temperature profile of the proposed 5-pair p–n f-TEG with an optimized dimension. b, Digital photo of our f-TEG. Comparison of maximum power density (PDmax) as a function of temperature difference (c) and normalized maximum power density (PDmax×L/ΔT2) (d) among the flexible TE modules.

Source data

Supplementary information

Supplementary Information

Supplementary Notes 1–5, Figs. 1–27 and Tables 1–5.

Supplementary Video 1

In situ SEM observation of p-type Bi2Te3 film under bending.

Supplementary Video 2

In situ SEM observation of n-type Bi2Te3 film under bending.

Supplementary Video 3

Overviewing TEM observation of p-type Bi2Te3 film during in situ mechanical TEM testing.

Supplementary Video 4

HRTEM observation and the corresponding strain map during in situ deformation.

Source data

Source Data Fig. 1

Exceptional flexibility and TE performance of Bi2Te3-based films.

Source Data Fig. 2

Macroscopic, microscopic and atomic-scale in situ observations of staggered-layer-boosted flexibility for p-type BST films.

Source Data Fig. 3

DFT calculations showing the staggered-layer structure transformation in Bi2Te3 thin film.

Source Data Fig. 4

Temperature-dependent TE properties and DFT electronic band structures of the p- and n-type SCs and films.

Source Data Fig. 5

Electrical output performance of Bi2Te3-based f-TEGs.

Source Data Extended Data Fig. 1

STEM–energy-dispersive spectroscopy image and analysis of the staggered layers for p-type BST films.

Source Data Extended Data Fig. 2

In situ TEM investigation of p-type BST films.

Source Data Extended Data Fig. 3

Cyclic temperature-dependent TE properties.

Source Data Extended Data Fig. 4

The design and performance of the Bi2Te3-based five-pair p–n f-TEG.

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Lu, Y., Zhou, Y., Wang, W. et al. Staggered-layer-boosted flexible Bi2Te3 films with high thermoelectric performance. Nat. Nanotechnol. 18, 1281–1288 (2023). https://doi.org/10.1038/s41565-023-01457-5

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