期刊
ACS APPLIED MATERIALS & INTERFACES
卷 14, 期 39, 页码 44527-44538出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.2c11369
关键词
composite thermoelectrics; acoustic impedance mismatch; Kapitza radius; interface thermal resistance; work function; Kelvin probe force microscope; density functional theory
资金
- Foundation for Polish Science [TEAM-TECH/2016-2/14]
- Faculty of Materials Science and Ceramics, AGH University of Science and Technology, Krakow, Poland
- UGC, India [1392/ (CSIR-UGC NET JUNE 2018)]
- SERB [CRG/2019/000647]
This study demonstrates the enhanced thermoelectric performance of a composite material by manipulating its composition and acoustic impedance mismatch. The increase in electrical conductivity and Seebeck coefficient results in a higher power factor, while the difference in elastic properties leads to a large interface thermal resistance and reduced phonon thermal conductivity. The simultaneous effect of enhanced electrical parameters and reduced thermal conductivity provides a promising strategy for achieving higher thermoelectric figure of merit. Through detailed analysis of electrical properties and thermal transport, this study provides insights for the design and optimization of thermoelectric materials.
The preparation of composite materials is a promising methodology for concurrent optimization of electrical and thermal transport properties for improved thermoelectric (TE) performance. This study demonstrates how the acoustic impedance mismatch (AIM) and the work function of components decouple the TE parameters to achieve enhanced TE performance of the (1-z)Ge0.87Mn0.05Sb0.08Te-(z)WC composite. The simultaneous increase in the electrical conductivity (sigma) and Seebeck coefficient (alpha) with WC (tungsten carbide) volume fraction (z) results in an enhanced power factor (alpha(2)sigma) in the composite. The rise in sigma is attributed to the creation of favorable current paths through the WC phase located between grains of Ge0.87Mn0.05Sb0.08Te, which leads to increased carrier mobility in the composite. Detailed analysis of the obtained electrical properties was performed via Kelvin probe force microscopy (work function measurement) and atomic force microscopy techniques (spatial current distribution map and current-voltage (I-V) characteristics), which are further supported by density functional theory (DFT) calculations. Furthermore, the difference in elastic properties (i.e., sound velocity) between Ge0.87Mn0.05Sb0.08Te and WC results in a high AIM, and hence, a large interface thermal resistance (R-int) between the phases is achieved. The correlation between R-int and the Kapitza radius depicts a reduced phonon thermal conductivity (kappa(ph)) of the composite, which is explained using the Bruggeman asymmetrical model. Moreover, the decrease in kappa(ph) is further validated by phonon dispersion calculations that indicate the decrease in phonon group velocity in the composite. The simultaneous effect of enhanced alpha(2)sigma and reduced kappa(ph) results in a maximum figure of merit (zT) of 1.93 at 773 K for (1-z)Ge0.87Mn0.05Sb0.08Te-(z)WC composite for z = 0.010. It results in an average thermoelectric figure of merit (zT(av)) of 1.02 for a temperature difference (delta T) of 473 K. This study shows promise to achieve higher zT(av) across a wide range of composite materials.
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