Fabrication and Thermoelectric Performance of Ce0.9Fe3CoSb12 Thin Films via Magnetron Sputtering for Flexible Thermoelectric and Sensing Applications

doi:10.15541/jim20250137

Abstract

Abstract:

Skutterudite-based CoSb₃ materials have attracted significant attention in thermoelectric applications due to their environmental friendliness, thermal stability and excellent thermoelectric properties. While considerable progress has been made in the development of n-type skutterudite thermoelectric thin films, research on high-performance p-type filled skutterudite flexible thin films remains limited, particularly in the context of flexible device integration. In this work, p-type Ce_0.9Fe₃CoSb₁₂ thin films were deposited on glass substrates via radio frequency magnetron sputtering, and influence of sputtering power (100-120 W) on the film composition, microstructure, and thermoelectric properties was systematically investigated. The results reveal that increasing the sputtering power leads to a gradual decrease in the Ce/Fe atomic ratio and a corresponding increase in the hole concentration, which enhances the electrical conductivity (σ) but reduces the Seebeck coefficient (S). The film deposited at 110 W exhibits the highest thermoelectric performance, achieving a power factor (PF) of 76.7 μW·m^-1∙K^-2 at room temperature and 103.5 μW·m^-1∙K^-2 at 500 K. Building upon these findings, flexible Ce_0.9Fe₃CoSb₁₂ films were further fabricated on polyimide (PI) substrates with substrate heating applied during deposition to improve interfacial adhesion. A flexible thin-film thermoelectric generator was successfully integrated, and its potential application in temperature sensing was evaluated. The device demonstrates excellent mechanical flexibility and reliable thermal sensing performance, highlighting its promise for use in flexible thermoelectric sensor technologies.

Key words: thermoelectric, CoSb₃, thin film, magnetron sputtering, thermoelectric sensor

CLC Number:

TB34

GE Yeming, TANG Zhe, LIU Miao, LOU Size, LIU Zhenguo, ZHOU Yan, WAN Shun, ZONG Peng'an. Fabrication and Thermoelectric Performance of Ce_0.9Fe₃CoSb₁₂ Thin Films via Magnetron Sputtering for Flexible Thermoelectric and Sensing Applications[J]. Journal of Inorganic Materials, 2026, 41(1): 55-62.

Figures/Tables 8

Fig. 1 Diagrams of thin film and thermoelectric device fabrication (a) Schematic diagram of fabrication of Ce0.9Fe3CoSb12 thin film by magnetron sputtering; (b) Schematic diagram of thermoelectric device

Fig. 2 XRD patterns of Ce0.9Fe3CoSb12 thin films deposited at different sputtering powers (a) XRD patterns; (b) Localized enlargements of (013) crystal plane diffraction peak

Fig. 3 Microstructure analyses of Ce0.9Fe3CoSb12 thin films (a-d) SEM images of Ce0.9Fe3CoSb12 thin films deposited at different sputtering powers; (e) EDS elemental mappings and (f) HRTEM image of Ce0.9Fe3CoSb12 thin film deposited at 110 W

Fig. 4 Thermoelectric performance of Ce0.9Fe3CoSb12 thin films prepared at various sputtering powers (a-e) p, μ, σ, S, and PF of Ce0.9Fe3CoSb12 thin films prepared under different sputtering powers; (f) Comparison of PF of CoSb3-based films at room temperature[20-22,24,30 -31]; (g-i) Relationship between σ, S, and PF of the 110 W Ce0.9Fe3CoSb12 sample as a function of temperature

Fig. 5 Characterization of mechanical flexibility, thermoelectric output and touch sensing capability of the Ce0.9Fe3CoSb12 flexible thermoelectric device (a) Schematic diagram of Ce0.9Fe3CoSb12 flexible thin film placed on a bent tube during the bending test; (b) σ/σ0 varied with different curvature radii after 200 bending cycles on tubes; (c) σ/σ0 varied with bending cycles on a tube with a curvature radius of 6 mm; (d) Schematic diagram of the voltage-current circuit for device output performance testing; (e) Relationship between output voltage and output current under different ΔT; (f) Relationship between output power and output current under different ΔT; (g, h) Output voltage corresponding to different numbers of legs touched on the touch sensor; (i) Voltage signals converted into words by touch sensor, using "FISH" as an example

Fig. 6 Respiratory sensing output test (a) Integration of the respiratory sensor into a mask, with the backside positioned near the breathing inlet and the front side exposed to the ambient air; (b) Voltage signals detected by the sensor while worn in a resting state; (c-e) Voltage signals recorded during the transition from jumping to sitting while wearing the sensor

Table S1 Mass fractions of various elements in thin films deposited at different sputtering powers and chemical formulas of films calculated with Co molar ratio as the base

Sputtering power/W	Ce/%	Fe/%	Co/%	Sb/%	Formula
100	7.23	8.91	3.24	80.62	Ce_0.938Fe_2.9CoSb_12.04
110	6.88	9.21	3.14	80.77	Ce_0.92Fe_3.09CoSb_12.43
120	6.82	9.98	3.38	79.81	Ce_0.85Fe_3.14CoSb_11.43
130	6.83	9.03	3.04	81.09	Ce_0.942Fe_3.13CoSb_12.9

Fig. S1 Changes in conductivities of Ce0.9Fe3CoSb12 thin films on multiple bending cycles with substrate heating on and off

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Fabrication and Thermoelectric Performance of Ce_0.9Fe₃CoSb₁₂ Thin Films via Magnetron Sputtering for Flexible Thermoelectric and Sensing Applications

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