A high-performance thermoelectric oxyselenide BiCuSeO ceramic with ZT > 1.1 at 823 K and higher average ZT value (ZTave ≈0.8) is obtained. The heavy doping element and nanostructures can effectively tune its electronic structure, hole concentration, and thermal conductivity, resulting in substantially enhanced mobility, power factor, and thus ZT value. This work provides a path to high-performance thermoelectric ceramics.
A significant enhancement of thermoelectric performance in layered oxyselenides BiCuSeO was achieved. The electrical conductivity and Seebeck coefficient of BiCu(1-x)SeO (x = 0-0.1) indicate that the carriers were introduced in the (Cu(2)Se(2))(2-) layer by Cu deficiencies. The maximum of electrical conductivity is 3 × 10(3) S m(-1) for Bicu(0.975)Seo at 650 °C, much larger than 470 S m(-1) for pristine BiCuSeO. Featured with very low thermal conductivity (∼0.5 W m(-1) K(-1)) and a large Seebeck coefficient (+273 μV K(-1)), ZT at 650 °C is significantly increased from 0.50 for pristine BiCuSeO to 0.81 for BiCu(0.975)SeO by introducing Cu deficiencies, which makes it a promising candidate for medium temperature thermoelectric applications.
The n-type polycrystalline Bi 2 O 2 Se 1Àx Cl x (0≤x≤0.04) samples were fabricated through solid-state reaction followed by spark plasma sintering. The carrier concentration was markedly increased to 1.38910 20 cm À3 by 1.5% Cl doping. The maximum electrical conductivity is 213.0 S/cm for x=0.015 at 823 K, which is much larger than 6.2 S/cm for pristine Bi 2 O 2 Se. Furthermore, the considerable enhancement of the electrical conductivity outweighs the moderate reduction of the Seebeck coefficient by Cl doping, thus contributing to a high power factor of 244.40 lÁWK À2 Ám À1 at 823 K. Coupled with the intrinsically suppressed thermal conductivity originating from the low velocity of sound and Young's modulus, a ZT of 0.23 at 823 K for Bi 2 O 2 Se 0.985 Cl 0.015 was achieved, which is almost threefold the value attained in pristine Bi 2 O 2 Se. It reveals that Se-site doping can be an effective strategy for improving the thermoelectric performance of the layered Bi 2 O 2 Se bulks. K E Y W O R D S doping, electrical conductivity, layered crystal structures, thermoelectric properties, Young's modulus Engineering,
The low power factor (PF) of BiCuSeO oxyselenide inhibits further improvement on thermoelectric figure of merit in the moderate temperature range. In this Letter, we show that the electron transport properties of doped BiCuSeO oxyselenide can be accurately described in acoustic phonon scattering assumption within the framework of single parabolic band model. It is further found that the doping elements alter the electron transport properties by tuning the effective mass and deformation potential. Based on these understandings, we argue that the higher power factor can be achieved by choosing the doping element based on reducing deformation potential coefficient and decreasing effective mass.
Lithium metal battery (LMB) possessing a high theoretical capacity is a promising candidate of advanced energy storage devices. However, its safety and stability are challenged by lithium dendrites and the leakage of liquid electrolyte. Here, a self-enhancing gel polymer electrolyte (GPE) is created by in situ polymerizing 1,3-dioxolane (DOL) in the nanofibrous skeleton for enabling safe LMB. The nanofiber membrane possesses a better affinity with poly-DOL (PDOL) than commercial separator for constructing homogeneous GPE with enhanced ion conductivity. Furthermore, polydopamine is introduced on nanofiber membrane to form hydrogen bonding with PDOL and bis((trifluoromethyl)sulfonyl)imide anion, dramatically improving the mechanical strength, ionic conductivity, and transference number of GPE. Besides, molecular dynamic simulation is used to reveal the intrinsic factors of high ionic conductivity and reinforcing effect in the meantime. Consequently, the LiFePO 4 //Li batteries using self-enhancing GPE show extraordinary cyclic stability over 800 cycles under high current density of 2 C, with a capacity decay of 0.021% per cycle, effectively suppressing the growth of lithium dendrites. This ingenious strategy is expected to manufacture advanced performance and high safety LMBs and compatible with the current battery production.
Oxide-based ceramics could be promising thermoelectric materials because of their thermal and chemical stability at high temperature. However, their mediocre electrical conductivity or high thermal conductivity is still a challenge for the use in commercial devices. Here, we report significantly suppressed thermal conductivity in SrTiO3-based thermoelectric ceramics via high-entropy strategy for the first time, and optimized electrical conductivity by defect engineering. In high-entropy (Ca0.2Sr0.2Ba0.2Pb0.2La0.2)TiO3 bulks, the minimum thermal conductivity can be 1.17 W/(m·K) at 923 K, which should be ascribed to the large lattice distortion and the huge mass fluctuation effect. The power factor can reach about 295 μW/(m·K2) by inducing oxygen vacancies. Finally, the ZT value of 0.2 can be realized at 873 K in this bulk sample. This approach proposed a new concept of high entropy into thermoelectric oxides, which could be generalized for designing high-performance thermoelectric oxides with low thermal conductivity.
BiCuSeO oxyselenides have been successfully fabricated by self-propagating high-temperature synthesis (SHS). Compared with the SHS process of the binary or ternary alloys, thermal analysis indicates the ignition temperature of quaternary layered BiCuSeO oxyselenides approaches the second lower melting point of the compound. The ZT value of SHS-synthesized BiCuSeO is almost 1.5 times larger than that of the solid state reaction (SSR) product at 873K. This is attributed to the existing amorphous region, nano-pores, and optimized grain size. Furthermore, with the partial substitution of Pb 2+ for Bi 3+ , ZT was enhanced through the optimization of charge carrier concentration and band gap narrowing. This achieved a ZT of 0.91 at 873K for Bi1-xPbxCuSeO (x=0.04). Combining with the Debye-Callaway model
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