Flexible Cu0.005Bi0.5Sb1.495Te3 Thin Films: Magnetron Sputtering Preparation and Thermoelectric Properties

doi:10.15541/jim20250134

Abstract

Abstract:

Bismuth telluride-based materials have been extensively studied due to their outstanding thermoelectric performance at room temperature. However, bismuth telluride is inherently brittle, which poses a significant challenge in developing flexible bismuth telluride-based materials with high thermoelectric performance remains in thermoelectric research. In this study, a non(00l) layered flexible p-type thermoelectric thin film was fabricated by depositing Cu_0.005Bi_0.5Sb_1.495Te₃onto polyimide (PI) substrates using magnetron sputtering technology, with a systematic investigation of the effect of sputtering pressure on thermoelectric properties. The results show that at 0.7 Pa sputtering pressure, its mobility is enhanced due to the large grain size and high crystallinity, its carrier concentration is optimized to 5.78×10¹⁹ cm⁻³, and its room-temperature power factor (PF) reaches 1660 μW·m⁻¹·K⁻². In addition, the film exhibits excellent mechanical flexibility, showing less than 10% variation in resistivity at a bending radius of 5 mm and less than 5% variation in Seebeck coefficient after 600 cycles of bending. Furthermore, a flexible thermoelectric device comprising four p-type thermoelectric legs (5 mm×25 mm×767 nm) was designed and fabricated based on this film. The device demonstrates promising performance, generating an output voltage of 18.5 mV, with a power density reaching 44.80 μW·cm⁻² under a temperature difference of 30 K. Touch-sensitive linguistic output design of the device demonstrates promising potential for language assistance applications. This work provides valuable insights into the magnetron sputtering preparation of high-performance flexible bismuth telluride-based thermoelectric materials and the optimization of their properties.

Key words: Cu_0.005Bi_0.5Sb_1.495Te₃, magnetron sputtering, thin film, flexible thermoelectric device

CLC Number:

TQ125

GE Zesheng, LIU Miao, TANG Zhe, ZHOU Yan, WAN Shun, ZONG Peng’an. Flexible Cu_0.005Bi_0.5Sb_1.495Te₃ Thin Films: Magnetron Sputtering Preparation and Thermoelectric Properties[J]. Journal of Inorganic Materials, 2025, 40(11): 1237-1244.

Figures/Tables 14

Fig. 1 XRD patterns of CBST-x (x=0.5, 0.7, 1.0, 1.5) thin films (a) XRD patterns; (b) Localized enlargements of (015) crystal plane diffraction peaks

Fig. 2 Surface microstructures of CBST-x (x=0.5, 0.7, 1.0, 1.5) thin films (a-d) Surface SEM images of (a) CBST-0.5, (b) CBST-0.7, (c) CBST-1.0, and (d) CBST-1.5; (e) TEM and (f) HRTEM images with SAED pattern of CBST-0.7

Fig. 3 Cross-sectional microstructures of CBST-x (x=0.5, 0.7, 1.0, 1.5) thin films (a) CBST-0.5; (b) CBST-0.7; (c) CBST-1.0; (d) CBST-1.5

Fig. 4 XPS spectra of CBST-0.7 thin film (a) Cu2p; (b) Bi4f; (c) Sb3d; (d) Te3d

Fig. 5 Thermoelectric properties, flexibility and integrated device output properties of CBST thin films (a-c) Variation of (a) n and μ, (b) S and σ, (c) PF of CBST-x (x=0.5, 0.7, 1.0, 1.5) thin films; (d) S, (e) σ, and (f) PF of CBST-0.7 thin film (300-550 K); (g, h) Flexibility characterization of CBST-0.7 thin film: (g) Resistivity change under different bending radii (5-10 mm),(h) Seebeck coefficient changes with bending cycles (100-600 cycles); (i) Relationship between Voc, Poc and current of TEG composed of 4 single p-type thermoelectric legs with optimal performance at different temperatures (10-30 K)

Fig. 6 Single p-type TEG and touch sensing language output design (a) Touching single-p-type TEG with different numbers of finger; (b) Voc generated by the TEG upon touching by one to four fingers; (c, d) TEG converts the resulting voltage signal into words (c) “RACE” and (d) “CARE”

Table S1 EDS detected atomic percentages of CBST films prepared at different working pressures (0.5-1.5 Pa)

Sample	Cu/%	Bi/%	Sb/%	Te/%	(Bi+Sb)/Te	Formula
CBST-0.5	0.14	10.53	31.25	58.08	41.78/58.08	Cu_0.0066Bi_0.50Sb_1.48Te_2.76
CBST-0.7	0.12	10.52	29.90	59.46	40.43/59.46	Cu_0.0057Bi_0.50Sb_1.42Te_2.83
CBST-1.0	0.11	9.73	29.87	60.29	39.60/60.29	Cu_0.0056Bi_0.50Sb_1.53Te_3.09
CBST-1.5	0.09	10.05	28.52	61.34	38.57/61.34	Cu_0.0045Bi_0.50Sb_1.42Te_3.05

Fig. S1 Different crystal face orientation factor F of CBST- x(x=0.5, 0.7, 1.0, 1.5) thin films

Fig. S2 Distributions of elements in CBST-0.7 thin film (a) Cu; (b) Bi; (c) Sb; (d) Te

Table S2 XRD analysis results of CBST thin films prepared at different working pressures

Sample	2θ/(°)	FWHM, β/rad	Grain size, D/nm	Dislocation density, δ/ (×10¹⁵, m⁻²)	Strain, ε/ (×10⁻³, line⁻²·m⁻⁴)
CBST-0.5	28.26	0.00435	32.511	0.946	1.054
CBST-0.7	28.18	0.00317	44.602	0.503	0.768
CBST-1.0	28.14	0.00332	42.556	0.552	0.805
CBST-1.5	27.98	0.00467	30.261	1.092	1.132

Table S3 Comparison of room-temperature PF of the CBST film prepared in this work and literature

Material	Crystal orientation	PF/(μW·m⁻¹·K⁻²)
Bi₂Te₃^[16]	(00l)	3000
Bi_0.4Sb_1.6Te₃^[40]	(00l)	2000
Bi₂Te₃^[42]	(00l)	1610
Sb₂Te₃^[43]	(015)	1210
Sb₂Te₃^[44]	(015)	1220
W-Bi_0.5Sb_1.5Te₃^[19]	(015)	1375
Cu_0.005Bi_0.5Sb_1.495Te₃(This Work)	(015)	1660

Table S4 Comparison of the output performance of the thermoelectric device in this work and literature

Material	Device type	N (leg numbers)	ΔT/K	V_oc/mV	P_max/nW	Average V_oc/mV	P_max density/(μW·cm⁻²)
Bi₂Te₃/CFF (carbon fiber fabric)^[27]	Single p-type	5	32	6.0	90.6	1.2	0.72
Bi₂Te₃/Ni Foam^[46]	Single n-type	5	30	3.7	22.7	0.8	0.71
Bi₂Te₃-Sb₂Te₃^[47]	π-type	26	24	48.9	693.5	1.9	−
Bi₂Te₃-Sb₂Te₃^[48]	π-type	200	40	430.0	32.0	2.2	94.81
Bi_0.5Sb_1.5Te₃-Bi₂Te_2.7Se_0.3^[49]	π-type	13	68	70.0	11000.0	5.4	140.00
This work	Single p-type	4	30	18.5	6.9	4.6	44.80

Fig. S3 Low-magnification TEM image and element distributions of CBST-0.7 thin film

Fig. S4 TEG structure diagram, physical diagram and power generation circuit diagram (a) Schematic and photograph of the single-p-type TEG composed of four thin-film legs with optimized performance; (b) Circuit schematic of the TEG integrated with an external load resistor

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Flexible Cu_0.005Bi_0.5Sb_1.495Te₃ Thin Films: Magnetron Sputtering Preparation and Thermoelectric Properties

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