Orchestrating phase transition in GeTe thermoelectrics: An investigation into the role of electronegativity

Article

Zhou, Yuwei, Cheng, Jiahui, Hong, Min, Lyu, Tu, Wang, Moran, Luo, Xiaohuan, Zhang, Chaohua, Liu, Fusheng and Hu, Lipeng. 2024. "Orchestrating phase transition in GeTe thermoelectrics: An investigation into the role of electronegativity." Nano Energy. 127. https://doi.org/10.1016/j.nanoen.2024.109723
Article Title

Orchestrating phase transition in GeTe thermoelectrics: An investigation into the role of electronegativity

ERA Journal ID201288
Article CategoryArticle
AuthorsZhou, Yuwei, Cheng, Jiahui, Hong, Min, Lyu, Tu, Wang, Moran, Luo, Xiaohuan, Zhang, Chaohua, Liu, Fusheng and Hu, Lipeng
Journal TitleNano Energy
Journal Citation127
Article Number109723
Number of Pages12
Year2024
PublisherElsevier
Place of PublicationNetherlands
ISSN2211-2855
2211-3282
Digital Object Identifier (DOI)https://doi.org/10.1016/j.nanoen.2024.109723
Web Address (URL)https://www.sciencedirect.com/science/article/abs/pii/S2211285524004713
AbstractIn thermoelectrics, mastering solid-state phase transition is paramount for enhancing the figure of merit and potentially designing novel thermoelectric materials. Focusing on GeTe, its reversible rhombohedral-to-cubic phase transition poses challenge for practical application. The determinant governing this phase transition remains obscure. Here, we introduce a simple, intuitive, and broadly applicable strategy to facilitate this phase transition by exploiting the large electronegativity disparity between cations and anions. Leveraging this concept, we adeptly identify AgInTe2 as a potent alloying agent and incorporate Sb to enhance the dissolution of AgInTe2 within the matrix, hastening the formation of cubic GeTe thanks to the increased electron transfer. These leads to the enhanced band degeneracy, formed multiscale microstructures, enhanced lattice anharmonicity, and reduced sound velocity, substantially increasing the density-of-states effective mass and decreasing the lattice thermal conductivity. Notably, AgInTe2 alloying engenders impurity bands, significantly narrowing the bandgap and rendering it ideal for low-temperature power generation. Consequently, the cubic (Ge0.94Sb0.06Te)0.9(AgInTe2)0.1 achieves a peak zT ∼ 1.01 at 473 K, resulting in a maximum energy-conversion efficiency ∼ 5.3% (9.2%) in a single-leg device under a 300 K (500 K) temperature differential. These results underscore the critical role of electronegativity difference in managing the rhombohedral-cubic phase transition in chalcogenides.
KeywordsChalcogenides; Thermoelectric; GeTe; Electronegativity; Phase transition
Contains Sensitive ContentDoes not contain sensitive content
ANZSRC Field of Research 2020401807. Nanomaterials
Public Notes

The accessible file is the accepted version of the paper. Please refer to the URL for the published version.

Byline AffiliationsShenzhen University, China
School of Engineering
Centre for Future Materials
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Crystal symmetry induced structure and bonding manipulation boosting thermoelectric performance of GeTe
Li, Meng, Hong, Min, Tang, Xiao, Sun, Qiang, Lyu, Wan-Yu, Xu, Sheng-Duo, Kou, Liang-Zhi, Dargusch, Matthew, Zou, Jin and Chen, Zhi-Gang. 2020. "Crystal symmetry induced structure and bonding manipulation boosting thermoelectric performance of GeTe." Nano Energy. 73, pp. 1-10. https://doi.org/10.1016/j.nanoen.2020.104740
Rashba effect maximizes thermoelectric performance of GeTe derivatives
Hong, Min, Lyv, Wanyu, Li, Meng, Xu, Shengduo, Sun, Qiang, Zou, Jin and Chen, Zhi-Gang. 2020. "Rashba effect maximizes thermoelectric performance of GeTe derivatives." Joule. 4 (9), pp. 2030-2043. https://doi.org/10.1016/j.joule.2020.07.021
Computation-guided design of high-performance flexible thermoelectric modules for sunlight-to-electricity conversion
Xu, Shengduo, Hong, Min, Shi, Xiaolei, Li, Meng, Sun, Qiang, Chen, Qixiang, Dargusch, Matthew, Zou, Jin and Chen, Zhigang. 2020. "Computation-guided design of high-performance flexible thermoelectric modules for sunlight-to-electricity conversion." Energy and Environmental Science. 13 (10), pp. 3480-3488. https://doi.org/10.1039/D0EE01895C
Bi0.5Sb1.5Te3/PEDOT:PSS-based flexible thermoelectric film and device
Wang, Yuan, Hong, Min, Liu, Wei-Di, Shi, Xiao-Lei, Xu, Sheng-Duo, Sun, Qiang, Gao, Han, Lu, Siyu, Zou, Jin and Chen, Zhi-Gang. 2020. "Bi0.5Sb1.5Te3/PEDOT:PSS-based flexible thermoelectric film and device." Chemical Engineering Journal. 397, pp. 1-9. https://doi.org/10.1016/j.cej.2020.125360
Enhanced thermoelectric properties of nanostructured n-type Bi2Te3 by suppressing Te vacancy through non-equilibrium fast reaction
Wang, Yuan, Liu, Wei-Di, Shi, XIao-Lei, Hong, Min, Wang, Li-Jun, Li, Meng, Wang, Hao, Zou, Jin and Chen, Zhi-Gang. 2020. "Enhanced thermoelectric properties of nanostructured n-type Bi2Te3 by suppressing Te vacancy through non-equilibrium fast reaction." Chemical Engineering Journal. 391. https://doi.org/10.1016/j.cej.2019.123513
High-Performance PEDOT: PSS Flexible Thermoelectric Materials and Their Devices by Triple Post-Treatments
Xu, Shengduo, Hong, Min, Shi, Xiao-Lei, Wang, Yuan, Ge, Lei, Bai, Yang, Wang, Lianzhou, Dargusch, Matthew, Zou, Jin and Chen, Zhi-Gang. 2019. "High-Performance PEDOT: PSS Flexible Thermoelectric Materials and Their Devices by Triple Post-Treatments." Chemisty of Materials. 31 (14), pp. 5238-5244. https://doi.org/10.1021/acs.chemmater.9b01500
Exploring the underlying mechanisms behind the increased far infrared radiation properties of perovskite-type Ce/Mn co-doped ceramics
Deng, Yi, Zhang, Kewei, Shi, Xiuyuan, Dong, Taosheng, Yang, Lei, Yang, Weizhong, Hong, Min, Wang, Yuan, Dargusch, Matthew and Chen, Zhi-Gang. 2019. "Exploring the underlying mechanisms behind the increased far infrared radiation properties of perovskite-type Ce/Mn co-doped ceramics." Materials Research Bulletin. 109, pp. 233-239. https://doi.org/10.1016/j.materresbull.2018.09.042
Strong phonon–phonon interactions securing extraordinary thermoelectric Ge1–xSbxTe with Zn-alloying-induced band alignment
Hong, Min, Wang, Yuan, Feng, Tianli, Sun, Qiang, Xu, Shengduo, Matsumura, Syo, Pantelides, Sokrates T., Zou, Jin and Chen, Zhi-Gang. 2019. "Strong phonon–phonon interactions securing extraordinary thermoelectric Ge1–xSbxTe with Zn-alloying-induced band alignment." Journal of the American Chemical Society. 141 (4), pp. 1742-1748. https://doi.org/10.1021/jacs.8b12624
High Thermoelectric Performance in p-type Polycrystalline Cd-doped SnSe Achieved by a Combination of Cation Vacancies and Localized Lattice Engineering
Shi, Xiaolei, Wu, Angyin, Feng, Tianli, Zheng, Kun, Liu, Weidi, Sun, Qiang, Hong, Min, Pantelides, Sokrates T., Chen, Zhi-Gang and Zou, Jin. 2019. "High Thermoelectric Performance in p-type Polycrystalline Cd-doped SnSe Achieved by a Combination of Cation Vacancies and Localized Lattice Engineering." Advanced Energy Materials. 9 (11), pp. 1-15. https://doi.org/10.1002/aenm.201803242
High Porosity in Nanostructured n-Type Bi2Te3 Obtaining Ultralow Lattice Thermal Conductivity
Wang, Yuan, Liu, Wei-Di, Gao, Han, Wang, Li-Jun, Li, Meng, Shi, Xiao-Lei, Hong, Min, Wang, Hao, Zou, Jin and Chen, Zhi-Gang. 2019. "High Porosity in Nanostructured n-Type Bi2Te3 Obtaining Ultralow Lattice Thermal Conductivity ." ACS Applied Materials and Interfaces. 11 (34), pp. 31237-31244. https://doi.org/10.1021/acsami.9b12079
Real-time observation of the thermally-induced phase transformation in GeTe and its thermal expansion properties
Tran, Xuan Quy, Hong, Min, Maeno, Hiroshi, Kawami, Youichirou, Toriyama, Takaaki, Jack, Kevin, Chen, Zhi-Gang, Zou, Jin, Matsumura, Syo and Dargusch, Matthew S.. 2019. "Real-time observation of the thermally-induced phase transformation in GeTe and its thermal expansion properties." Acta Materialia. 165, pp. 327-335. https://doi.org/10.1016/j.actamat.2018.11.059
Thermoelectric GeTe with Diverse Degrees of Freedom Having Secured Superhigh Performance
Hong, Min, Zou, Jin and Chen, Zhi-Gang. 2019. "Thermoelectric GeTe with Diverse Degrees of Freedom Having Secured Superhigh Performance." Advanced Materials. 31 (14), pp. 1-23. https://doi.org/10.1002/adma.201807071
High thermoelectric performance in sintered octahedron-shaped Sn(CdIn)xTe1+2x microcrystals
Moshwan, Raza, Shi, Xiao-Lei, Liu, Wei-Di, Yang, Lei, Wang, Yuan, Hong, Min, Auchterlonie, Graeme, Zou, Jin and Chen, Zhi-Gang. 2018. "High thermoelectric performance in sintered octahedron-shaped Sn(CdIn)xTe1+2x microcrystals." ACS Applied Materials and Interfaces. 10 (45), pp. 38944-38952. https://doi.org/10.1021/acsami.8b14233
Dual Ag/ZnO-decorated micro-/nanoporous sulfonated polyetheretherketone with superior antibacterial capability and biocompatibility via layer-by-layer self-assembly strategy
Deng, Yi, Yang, Lei, Huang, Xiaobing, Chen, Junhong, Shi, Xiuyuan, Yang, Weizhong, Hong, Min, Wang, Yuan, Dargusch, Matthew and Chen, Zhi-Gang. 2018. "Dual Ag/ZnO-decorated micro-/nanoporous sulfonated polyetheretherketone with superior antibacterial capability and biocompatibility via layer-by-layer self-assembly strategy." Macromolecular Bioscience. 18 (7), pp. 1-12. https://doi.org/10.1002/mabi.201800028
Achieving high thermoelectric performance of Ni/Cu modified Bi0.5Sb1.5Te3 composites by a facile electroless plating
Huang, Zhong-Yue, Zhang, He, Yang, Lei, Zhu, Bin, Zheng, Kun, Hong, Min, Yu, Yuan, Zu, Fang-Qiu, Zou, Jin and Chen, Zhi-Gang. 2018. "Achieving high thermoelectric performance of Ni/Cu modified Bi0.5Sb1.5Te3 composites by a facile electroless plating." Materials Today Energy. 9, pp. 383-390. https://doi.org/10.1016/j.mtener.2018.06.011
Ag doping induced abnormal lattice thermal conductivity in Cu2Se
Liu, Weidi, Shi, Xiaolei, Hong, Min, Yang, Lei, Moshwan, Raza, Chen, Zhi-Gang and Zou, Jin. 2018. "Ag doping induced abnormal lattice thermal conductivity in Cu2Se." Journal of Materials Chemistry C. 6 (48), pp. 13225-13231. https://doi.org/10.1039/c8tc04129f
Enhancing thermoelectric performance of (Cu1-xAgx)2Se via CuAgSe secondary phase and porous design
Liu, Weidi, Shi, Xiaolei, Moshwan, Raza, Hong, Min, Yang, Lei, Chen, Zhi-Gang and Zou, Jin. 2018. "Enhancing thermoelectric performance of (Cu1-xAgx)2Se via CuAgSe secondary phase and porous design." Sustainable Materials and Technologies. 17, pp. 1-8. https://doi.org/10.1016/j.susmat.2018.e00076
Atomic Insights into Phase Evolution in Ternary Transition-Metal Dichalcogenides Nanostructures
Zou, Yi-Chao, Chen, Zhi-Gang, Aso, Kohei, Zhang, Chenxi, Kong, Fantai, Hong, Min, Matsumura, Syo, Cho, Kyeongjae and Zou, Jin. 2018. "Atomic Insights into Phase Evolution in Ternary Transition-Metal Dichalcogenides Nanostructures." Small. 14 (22), pp. 1-6. https://doi.org/10.1002/smll.201800780
Boosting the thermoelectric performance of p-type heavily Cu-doped polycrystalline SnSe via inducing intensive crystal imperfections and defect phonon scattering
Shi, Xiaolei, Zheng, Kun, Hong, Min, Liu, Weidi, Moshwan, Raza, Wang, Yuan, Qu, Xianlin, Chen, Zhi-Gang and Zou, Jin. 2018. "Boosting the thermoelectric performance of p-type heavily Cu-doped polycrystalline SnSe via inducing intensive crystal imperfections and defect phonon scattering." Chemical Science. 9 (37), pp. 7376-7389. https://doi.org/10.1039/C8SC02397b
Sustainable utilization of municipal solid waste i incineration fly ash for ceramic bricks with eco-friendly biosafety
Deng, Yi, Gong, B., Chao, Y., Dong, T., Yang, W., Hong, Min, Shi, X., Wang, G., Jin, Y. and Chen, Z.-G.. 2018. "Sustainable utilization of municipal solid waste i incineration fly ash for ceramic bricks with eco-friendly biosafety." Materials Today Sustainability. 1-2, pp. 32-38. https://doi.org/10.1016/j.mtsust.2018.11.002
Self-assembled 3D flower-like hierarchical Ti-doped Cu3SbSe4 microspheres with ultralow thermal conductivity and high zT
Zhou, Tian, Wang, Lijun, Zheng, Shuqi, Hong, Min, Fang, Teng, Bai, Peng-Peng, Chang, Siyi, Cui, Wenlin, Shi, Xiaolei, Zhao, Huaizhou and Chen, Zhi-Gang. 2018. "Self-assembled 3D flower-like hierarchical Ti-doped Cu3SbSe4 microspheres with ultralow thermal conductivity and high zT." Nano Energy. 49, pp. 221-229. https://doi.org/10.1016/j.nanoen.2018.04.035
Nano-scale dislocations induced by self-vacancy engineering yielding extraordinary n-type thermoelectric Pb0.96-yInySe
Hong, Min, Chen, Zhi-Gang, Matsumura, Syo and Zou, Jin. 2018. "Nano-scale dislocations induced by self-vacancy engineering yielding extraordinary n-type thermoelectric Pb0.96-yInySe." Nano Energy. 50, pp. 785-793. https://doi.org/10.1016/j.nanoen.2018.06.030
Arrays of planar vacancies in superior thermoelectric Ge1−x−yCdxBiyTe with band convergence
Hong, Min, Wang, Yuan, Liu, Weidi, Matsumura, Syo, Wang, Hao, Zou, Jin and Chen, Zhi-Gang. 2018. "Arrays of planar vacancies in superior thermoelectric Ge1−x−yCdxBiyTe with band convergence." Advanced Energy Materials. 8 (30), pp. 1-10. https://doi.org/10.1002/aenm.201801837
Realizing zT of 2.3 in Ge1−x−ySbxInyTe via Reducing the Phase-Transition Temperature and Introducing Resonant Energy Doping
Hong, Min, Chen, Zhi-Gang, Yang, Lei, Zou, Yi-Chao, Dargusch, Matthew, Wang, Hao and Zou, Jin. 2018. "Realizing zT of 2.3 in Ge1−x−ySbxInyTe via Reducing the Phase-Transition Temperature and Introducing Resonant Energy Doping." Advanced Materials. 30 (11), pp. 1-8. https://doi.org/10.1002/adma.201705942
Achieving zT > 2 in p-Type AgSbTe2−xSex alloys via exploring the extra light valence band and introducing dense stacking faults
Hong, Min, Chen, Zhi-Gang, Yang, Lei, Liao, Zhi-Ming, Zou, Yi-Chao, Chen, Yan-Hui, Matsumura, Syo and Zou, Jin. 2018. "Achieving zT > 2 in p-Type AgSbTe2−xSex alloys via exploring the extra light valence band and introducing dense stacking faults." Advanced Energy Materials. 8 (9), pp. 1-7. https://doi.org/10.1002/aenm.201702333
BixSb2_xTe3 nanoplates with enhanced thermoelectric performance due to sufficiently decoupled electronic transport properties and strong wide-frequency phonon scatterings
Hong, Min, Chen, Zhi G., Yang, Lei and Zou, Jin. 2016. "BixSb2_xTe3 nanoplates with enhanced thermoelectric performance due to sufficiently decoupled electronic transport properties and strong wide-frequency phonon scatterings." Nano Energy. 20, pp. 144-155. https://doi.org/10.1016/j.nanoen.2015.12.009
Enhancing the thermoelectric performance of SnSe1-xTex nanoplates through band engineering
Hong, Min, Chen, Zhi-Gang, Yang, Lei, Chasapis, Thomas C., Kang, Stephen Dongmin, Zou, Yichao, Auchterlonie, Graeme John, Kanatzidis, Mercouri G., Snyder, G. Jeffrey and Zou, Jin. 2017. "Enhancing the thermoelectric performance of SnSe1-xTex nanoplates through band engineering." Journal of Materials Chemistry A. 5 (21), pp. 10713-10721. https://doi.org/10.1039/c7ta02677c
Fundamental and progress of Bi2Te3-based thermoelectric materials
Hong, Min, Chen, Zhigang and Zou, Jin. 2018. "Fundamental and progress of Bi2Te3-based thermoelectric materials." Chinese Physics B. 27 (4), pp. 1-25. https://doi.org/10.1088/1674-1056/27/4/048403
Achieving high Figure of Merit in p-type polycrystalline Sn0.98Se via self-doping and anisotropy-strengthening
Shi, Xiaolei, Chen, Zhi-Gang, Liu, Weidi, Yang, Lei, Hong, Min, Moshwan, Raza, Huang, Liqing and Zou, Jin. 2018. "Achieving high Figure of Merit in p-type polycrystalline Sn0.98Se via self-doping and anisotropy-strengthening." Energy Storage Materials. 10, pp. 130-138. https://doi.org/10.1016/j.ensm.2017.08.014
Scalable growth of high mobility dirac semimetal Cd3As2 microbelts
Chen, Zhi Gang, Zhang, Cheng, Zou, Yichao, Zhang, Enze, Yang, Lei, Hong, Min, Xiu, Faxian and Zou, Jin. 2015. "Scalable growth of high mobility dirac semimetal Cd3As2 microbelts." Nano Letters: a journal dedicated to nanoscience and nanotechnology. 15 (9), pp. 5830-5834. https://doi.org/10.1021/acs.nanolett.5b01885
Limit of zT enhancement in rocksalt structured chalcogenides by band convergence
Hong, Min, Chen, Zhi-Gang, Pei, Yanzhong, Yang, Lei and Zou, Jin. 2016. "Limit of zT enhancement in rocksalt structured chalcogenides by band convergence." Physical Review B: Covering condensed matter and materials physics. 94 (16). https://doi.org/10.1103/PhysRevB.94.161201
Enhancing thermoelectric performance of Bi2Te3-based nanostructures through rational structure design
Hong, Min, Chen, Zhi-Gang, Yang, Lei and Zou, Jin. 2016. "Enhancing thermoelectric performance of Bi2Te3-based nanostructures through rational structure design." Nanoscale. 8 (16), pp. 8681-8686. https://doi.org/10.1039/c6nr00719h
Co-doped Sb2Te3 paramagnetic nanoplates
Yang, Lei, Chen, Zhi-Gang, Nie, Tianxiao, Han, Guang, Zhang, Zhi, Hong, Min, Wang, Kang L. and Zou, Jin. 2016. "Co-doped Sb2Te3 paramagnetic nanoplates." Journal of Materials Chemistry C. 4 (3), pp. 521-525. https://doi.org/10.1039/c5tc03767k
Te-Doped Cu2Se nanoplates with a high average thermoelectric figure of merit
Yang, Lei, Chen, Zhi-Gang, Han, Guang, Hong, Min, Huang, Liqing and Zou, Jin. 2016. "Te-Doped Cu2Se nanoplates with a high average thermoelectric figure of merit." Journal of Materials Chemistry A. 4 (23), pp. 9213-9219. https://doi.org/10.1039/c6ta02998a
Rational design of Bi2Te3 polycrystalline whiskers for thermoelectric applications
Han, Guang, Chen, Zhi Gang, Yang, Lei, Hong, Min, Drennan, John and Zou, Jin. 2015. "Rational design of Bi2Te3 polycrystalline whiskers for thermoelectric applications." ACS Applied Materials and Interfaces. 7 (1), pp. 989-995. https://doi.org/10.1021/am5078528
Enhanced Thermoelectric Performance of Nanostructured Bi2Te3 through Significant Phonon Scattering
Yang, Lei, Chen, Zhi Gang, Hong, Min, Han, Guang and Zou, Jin. 2015. "Enhanced Thermoelectric Performance of Nanostructured Bi2Te3 through Significant Phonon Scattering." ACS Applied Materials and Interfaces. 7 (42), pp. 23694-23699. https://doi.org/10.1021/acsami.5b07596
n-type Bi2Te3-xSex nanoplates with enhanced thermoelectric efficiency driven by wide-frequency phonon scatterings and synergistic carrier scatterings
Hong, Min, Chasapis, Thomas C., Chen, Zhi Gang, Yang, Lei, Kanatzidis, Mercouri G., Snyder, G. Jeffrey and Zou, Jin. 2016. "n-type Bi2Te3-xSex nanoplates with enhanced thermoelectric efficiency driven by wide-frequency phonon scatterings and synergistic carrier scatterings." ACS Nano. 10 (4), pp. 4719-4727. https://doi.org/10.1021/acsnano.6b01156
Enhanced thermoelectric performance of ultrathin Bi2Se3 nanosheets through thickness control
Hong, Min, Chen, Zhi-Gang, Yang, Lei, Han, Guang and Zou, Jin. 2015. "Enhanced thermoelectric performance of ultrathin Bi2Se3 nanosheets through thickness control." Advanced Electronic Materials. 1 (6). https://doi.org/10.1002/aelm.201500025
High-performance thermoelectric Cu2Se nanoplates through nanostructure engineering
Yang, Lei, Chen, Zhi-Gang, Han, Guang, Hong, Min, Zou, Yichao and Zou, Jin. 2015. "High-performance thermoelectric Cu2Se nanoplates through nanostructure engineering." Nano Energy. 16, pp. 367-374. https://doi.org/10.1016/j.nanoen.2015.07.012
Impacts of Cu deficiency on the thermoelectric properties of Cu2-XSe nanoplates
Yang, Lei, Chen, Zhi-Gang, Han, Guang, Hong, Min and Zou, Jin. 2016. "Impacts of Cu deficiency on the thermoelectric properties of Cu2-XSe nanoplates." Acta Materialia. 113, pp. 140-146. https://doi.org/10.1016/j.actamat.2016.04.050
n-type Bi-doped PbTe nanocubes with enhanced thermoelectric performance
Yang, Lei, Chen, Zhi-Gang, Hong, Min, Wang, Lihua, Kong, Deli, Huang, Liqing, Han, Guang, Zou, Yichao, Dargusch, Matthew and Zou, Jin. 2017. "n-type Bi-doped PbTe nanocubes with enhanced thermoelectric performance." Nano Energy. 31, pp. 105-112. https://doi.org/10.1016/j.nanoen.2016.11.027