Nano-Mesoscopic Scale Microstructure Regulation for p-Type Skutterudite Thermoelectric Materials
LIU Zhiyuan1,2(), WANG Yonggui2, ZHAO Chengyu2, YANG Ting2, XIA Ailin1,2
1.Key Laboratory of Green Fabrication and Surface Technology of Advanced Metal Materials, Ministry of Education, Anhui University of Technology, Ma'anshan 243002, China 2.School of Materials Science and Engineering, Anhui University of Technology, Ma'anshan 243002, China
Cite this article:
LIU Zhiyuan, WANG Yonggui, ZHAO Chengyu, YANG Ting, XIA Ailin. Nano-Mesoscopic Scale Microstructure Regulation for p-Type Skutterudite Thermoelectric Materials. Acta Metall Sin, 2022, 58(8): 979-991.
Skutterudite thermoelectric materials are one of the most promising candidates for critical components in thermoelectric devices because of their excellent electrical transport properties. Thermoelectric devices require p- and n-type skutterudite materials with matching properties. However, the p-type skutterudite materials have considerably worse thermoelectric and mechanical properties than those of n-type. Thus, it is important to enhance the thermoelectric and mechanical properties of p-type skutterudite materials for the development of high-efficiency thermoelectric devices. This study summarizes the recent research progress on the nano-mesoscopic scale regulation of the microstructure for p-type skutterudite thermoelectric materials. The thermoelectric and mechanical properties of p-type skutterudite materials can be notably enhanced by adjusting the microstructure at the nano-mesoscopic scale; thus, providing scientific and technical supports for the thermoelectric device's application.
Fund: National Natural Science Foundation of China(51872006);National Undergraduate Training Programs for Innovation and Entrepreneurship(S202110360181)
About author: LIU Zhiyuan, associate professor, Tel: (0555)2311570, E-mail: zhiyuanliu826@ahut.edu.cn
Fig.2 p-type skutterudite materials with low-dimensional nanostructure (a) SEM image of the La0.5Ce0.5Fe3CoSb12 sample[40] (b) SEM image of p-type filled skutterudite Ce0.45Nd0.45Fe3.5Co0.5Sb12 powder after ball milling for 5 h[25] (c, d) SEM images of Nd0.9Fe3CoSb12 samples prepared by traditional solid-state reaction (c) and MS method (d)[41] (e) SEM image of the free side of spun ribbon of La x Ti0.1Ga0.1Fe3CoSb12 sample[60] (f) thermoelectric figure of merit(ZT) values of La x Ti0.1Ga0.1Fe3CoSb12 sample prepared by MS and annealing sample (T—temperature)[60]
Fig.3 SEM image of Co0.95Fe0.05Sb3 thin film (a)[49], power factor (S2σ) of Co1 - x Fe x Sb3 (0 ≤ x ≤ 0.1) samples (b)[49], SEM image of CoSb3 + 0.72%Ti thin film (c)[42], schematic illustration of Ti doped CoSb3 thin film growth process ((1) nano Ti layer, (2) CoSb3 growing on the Ti layer, (3) annealed film) (d)[42], various phonon scattering mechanisms by nano-strcucture and Ti based points defect (e)[42], and temperature dependences of Seebeck coefficient (f)[42] and ZT values (g)[42] of the CoSb3 thin films with different Ti contents (Samples with Ti contents of 0, 0.25%, 0.57%, 0.72%, 0.83%, and 1.05% were labeled as S0, S1, S2, S3, S4, and S5, respectively)
Fig.4 FESEM image of CeFe4Sb11.9Te0.1 sample with nanopore structure (Arrows indicate nanopores in grains) (a)[34], ZT values of CeFe4Sb12 - x Te x skutterudite materials (b)[34], FESEM image of CeFe3.8Zn0.2Sb12 sample with nanofilm structure (c)[43], and ZT values of CeFe4 - x Zn x Sb12 samples (d)[43]
Fig.5 SEM image of CeFe3CoSb12 + 5%MoO2 (mole fraction) nanocomposite (a)[44], ZT values of CeFe3CoSb12 and (CeFe3CoSb12)1 - x (MoO2) x composite (b)[44], SEM image of the fracture surface for MmFe4Sb12 + 16%Mm2O3 (mass fraction) nanocomposite (Nano-composite 2) (c)[74], and ZT values of MmFe4Sb12 + 16%Mm2O3 nanocomposites and reference samples (Reference sample: hot pressed MmFe4Sb12 sample for 2 h (HP-2 h); Macro-composite: MmFe4Sb12 + 16%Mm2O3 composite (HP-2 h); Nano-composite 1: MmFe4Sb12 + 16%Mm2O3 nanocomposite by ball milling (BM) and HP-2 h; Nano-composite 2: MmFe4Sb12 + 16%Mm2O3 nanocomposite by BM, HP-4 h and annealing for 110 h) (d)[74]
Fig.6 SEM image of cross-sectional areas of CoSb3/0.2%G (mass fraction) sample (a)[77], power factorof CoSb3/x%G (mass fraction) samples (b)[77], SEM image of the fractured surfaces of CoSb3/3%MoS2 (mass fraction) nanocomposite (c)[45], and ZT values of CoSb3/xMoS2 nanocomposites (d)[45]
Fig.7 SEM image of La0.8Ti0.1Ga0.1Fe3CoSb12/0.1Fe3Si sample (a)[33], ZT values of La0.8Ti0.1Ga0.1Fe3CoSb12/xFe3Si nanocomposites (b)[33], SEM image of Nd0.6Fe2Co2Sb11.6Sn0.4 sample (c)[46], ZT values of Nd0.6Fe2Co2Sb12 - x Sn x nanocomposites (d)[46], FESEM image of CeFe4Sb12 + 0.2Ce sample (e)[82], TEM images of CeFe4Sb12 + 0.1Ce sample (f, g)[82], and ZT values of CeFe4Sb12 + yCe nanocomposites (TM—traditional method) (h)[82]
Fig.8 SEM images of the fracture surfaces showing crack propagation (a)[84], crack branching and fiber pullout (b)[84], crack deflection and fiber pullout (c)[84] of CeFe4Sb12/3%Cf (volume fraction) sample, SEM image of the polished surface of CeFe4Sb12/3%Cf sample (d)[84]; SEM images showing the fractured surface (e)[85], expanded crack (f)[85] for the Ce0.85Fe3CoSb12/1.4%rGO (reduced graphene oxide, volume fraction) sample; schematic diagram of toughing mechanism by rGO (F—force) (g)[85] and three-point flexural strength (σ) and fracture toughness (KIC) of the Ce0.85Fe3CoSb12/y%rGO (volume fraction) composites (h)[85]
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