Rare three-valence-band convergence leading to ultrahigh thermoelectric performance in all-scale hierarchical cubic SnTe

Literature Information

Publication Date 2023-11-09
DOI 10.1039/D3EE02482B
Impact Factor 38.532
Authors

Fan Li, Xin Liu, Shu-Rong Li, Xiao-Fan Zhang, Ni Ma, Xin-Jing Li, Xin-Yun Lin, Haijun Wu


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Abstract

Band convergence is an important approach for improving the thermoelectric performance, as it can significantly increase the Seebeck coefficient without obviously sacrificing the electrical conductivity. Herein, we report a rare three-valence-band convergence achieved in doped p-type cubic SnTe to enhance the power factor and obtain a record-high ZT. Ternary MnCdTe2 alloying activates the lower-energy-lying Λ valence band (with a large degeneracy of Nv = 8), and additional Ge doping promotes energy alignment between the Λ and L bands, leading to a rare three-valence-band (i.e., L, Σ and Λ) convergence that pronouncedly enhances the power factor (PF = 29.3 μW cm−1 K−2 at 900 K). Ge doping also greatly enhances the solid solubility of MnCdTe2 in the SnTe matrix and effectively tunes the precipitate size, producing all-scale hierarchical structures, which generate a full spectrum of phonon scattering, especially low-frequency acoustic–optical scattering, leading to an ultralow lattice thermal conductivity (κL = 0.26 W m−1 K−1 at 670 K). Collectively, this gives a record-high ZT of 1.97 at 900 K and an average ZTave of 0.8 in the temperature range of 300 to 900 K for 8% MnCdTe2-doped SnTe with 3.2% Ge. Furthermore, a single-leg TE module based on (SnTe)0.92(MnCd0.6Ge0.4Te2)0.08 outputs a power density of 800 mW cm−2 for a ΔT of 446 K, which is competitive with those of devices based on state-of-the-art mid-temperature materials (600–900 K) within the same ΔT, demonstrating great potential for future applications.

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Source Journal

Energy & Environmental Science

Energy & Environmental Science
CiteScore: 32.34
Self-citation Rate: 3.4%
Articles per Year: 481

Energy & Environmental Science is an international journal dedicated to publishing exceptionally important and high quality, agenda-setting research tackling the key global and societal challenges of ensuring the provision of energy and protecting our environment for the future. The scope is intentionally broad and the journal recognises the complexity of issues and challenges relating to energy conversion and storage, alternative fuel technologies and environmental science. For work to be published it must be linked to the energy-environment nexus and be of significant general interest to our community-spanning readership. All scales of studies and analysis, from impactful fundamental advances, to interdisciplinary research across the (bio)chemical, (bio/geo)physical sciences and chemical engineering disciplines are welcomed. Topics include, but are not limited to, the following: Solar energy conversion and photovoltaics Solar fuels and artificial photosynthesis Fuel cells Hydrogen storage and (bio) hydrogen production Materials for energy systems Capture, storage and fate of CO2, including chemicals and fuels from CO2 Catalysis for a variety of feedstocks (for example, oil, gas, coal, biomass and synthesis gas) Biofuels and biorefineries Materials in extreme environments Environmental impacts of energy technologies Global atmospheric chemistry and climate change as related to energy systems Water-energy nexus Energy systems and networks Globally applicable principles of energy policy and techno-economics

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