Wenjie Xie

Enhanced thermoelectric performance of β-Zn4Sb3 based nanocomposites through combined effects of density of states resonance and carrier energy filtering

It is a major challenge to elevate the thermoelectric figure of merit ZT of materials through enhancing their power factor (PF) and reducing the thermal conductivity at the same time. Experience has shown that engineering of the electronic density of states (eDOS) and the energy filtering mechanism (EFM) are two different effective approaches to improve the PF. However, the successful combination of these two methods is elusive. Here we show that the PF of β-Zn4Sb3 can greatly benefit from both effects. Simultaneous resonant distortion in eDOS via Pb-doping and energy filtering via introduction of interface potentials result in a ~40% increase of PF and an approximately twofold reduction of the lattice thermal conductivity due to interface scattering. Accordingly, the ZT of β-Pb0.02Zn3.98Sb3 with 3 vol.% of Cu3SbSe4 nanoinclusions reaches a value of 1.4 at 648 K. The combination of eDOS engineering and EFM would potentially facilitate the development of high-performance thermoelectric materials.

Theoretical and experimental investigations of the thermoelectric properties of Bi2S3

Electronic and transport properties of Bi2S3 with various dopants are studied using density functional theory and experimental characterizations. First, principle calculations of thermoelectric properties are used to evaluate the thermoelectric potential of the orthorhombic Bi2S3 structure. The computational screening of extrinsic defects is used to select the most favorable n-type dopants. Among all the dopants considered, hafnium and chlorine are identified as prospective dopants, whereas, e.g., germanium is found to be unfavorable. This is confirmed by experiment. Seebeck coefficient (S) and electrical conductivity (σ) measurements are performed at room temperature on pellets obtained by spark plasma sintering. An increase of power factors (S2·σ) from around 50 up to 500 μW K−2 m−1 is observed for differently doped compounds. In several series of samples, we observed an optimum of power factor above 500 μW K−2 m−1 at room temperature for a chlorine equivalence of 0.25 mol. % BiCl3. The obtained results...

High thermoelectric performance of tellurium doped paracostibite

Paracostibite (CoSbS) has recently been identified as a promising thermoelectric (TE) material, yet its full potential remains to be attained. We present herein an integrated method based on high throughput DFT computations validated with experiments that has allowed us to identify tellurium on antimony sites as a much more effective dopant than the formerly used nickel on cobalt sites. By carrying out a systematic adjustment optimization of the experimental parameters, we achieve a power factor as high as 2.7 mW m−1 K−2 at 543 K, which is maintained up to 730 K. This is, to the best of our knowledge, the largest value reported for polycrystalline metal sulfides.

Compatibility approach for the improvement of oxide thermoelectric converters for industrial heat recovery applications

New ceramic Ca3Co3.9O9+δ  /CaMn0.97W0.03O3−δ thermoelectric generators with different cross section areas Ap and An of the p- and the n-type leg are fabricated, characterized, and tested at high temperatures in long-term tests. The variation of the measured power output and the efficiency with changing Ap/An ratio is discussed and compared with calculations based on the measured material properties. The highest conversion efficiencies are reached for ratios close to the one predicted by the compatibility approach, whereas an improper choice of Ap/An leads to a strong reduction of the efficiency. A volume power density of 1.4 W/cm3 and an efficiency of 1.08% are found for the most promising generator (temperature difference ΔT= 734 K and Ap/An= 1.12). The results reveal the major importance of the Ap/An ratio for the conversion efficiency and subsequently cost and weight reduction issues, both crucial for a large scale application of thermoelectric converters. Additionally, the oxide generators proved to b...

Recent Developments in β-Zn4Sb3 Based Thermoelectric Compounds

Thermoelectricity has been recognized as an environmentally friendly energy conversion technology due to its ability to directly achieve conversion between heat and electricity for a long time. β- has attracted considerable interest as promising thermoelectric material in the moderate temperature range (500 K–900 K), which is the temperature range of most industrial waste heat sources. In this paper, first we present the structure of β- and the traditional doping strategy used to enhance its performance. Next, we review the details of some new methods utilized for improving the thermoelectric properties of β- and its thermal stability as well as reliability. Finally, the review finishes with highlighting some promising strategies for future research directions in the material.

A self-forming nanocomposite concept for ZnO-based thermoelectrics

Zinc oxide (ZnO) has a very broad and versatile range of applications provided by its high abundance and optical and electrical properties, which can be further tuned by donor substitution. Al-doped ZnO is probably the most thoroughly investigated material with regard to thermoelectric properties. Fairly reasonable electrical properties of donor-doped zinc oxide are usually combined with high thermal conductivity limiting potential applications. Here we report a new self-forming nanocomposite concept for ZnO-based thermoelectrics, where a controllable interplay between the exsolution of the nanophases and modification of the host matrix suppresses the thermal transport while imparting enhanced electrical performance. The thermoelectric performance of the best-obtained composite, described by the dimensionless figure-of-merit ZT, at 920–1200 K is almost twice that of the pure matrix composition and reaches up to 0.11. The proposed approach invokes controlled interactions between composite components as a novel tool for decoupling the electrical and thermal transport parameters and shows clear prospects for an implementation in other thermoelectric oxide systems. The results indicate that the proposed concept may also constitute a promising pathway to achieve stable electrical performance at high temperatures, which currently represents one of the major challenges towards achieving ZnO-based thermoelectrics.

Thermopower Enhancement from Engineering the Na0.7CoO2 Interacting Fermiology via Fe Doping

The sodium cobaltate system Co is a prominent representant of strongly correlated materials with promising thermoelectric response. In a combined theoretical and experimental study we show that, by doping the Co site of the compound at with iron, a further increase of the Seebeck coefficient is achieved. The Fe defects give rise to effective hole doping in the high-thermopower region of larger sodium content . Originally filled hole pockets in the angular-resolved spectral function of the material shift to low energy when introducing Fe, leading to a multisheet interacting Fermi surface. Because of the higher sensitivity of correlated materials to doping, introducing adequate substitutional defects is thus a promising route to manipulate their thermopower.