High Thermoelectric Figure of Merit by Resonant Dopant in Half-Heusler Alloys

Half-Heusler alloys have been one of the benchmark high temperature thermoelectric materials owing to their thermal stability and promising figure of merit ZT. Simonson et al. early showed that small amounts of vanadium doped in Hf0.75Zr0.25NiSn enhanced the Seebeck coefficient and correlated the change with the increased density of states near the Fermi level. We herein report a systematic study on the role of vanadium (V), niobium (Nb), and tantalum (Ta) as prospective resonant dopants in enhancing the ZT of n-type half-Heusler alloys based on Hf0.6Zr0.4NiSn0.995Sb0.005. The V doping was found to increase the Seebeck coefficient in the temperature range 300-1000 K, consistent with a resonant doping scheme. In contrast, Nb and Ta act as normal n-type dopants, as evident by the systematic decrease in electrical resistivity and Seebeck coefficient. The combination of enhanced Seebeck coefficient due to the presence of V resonant states and the reduced thermal conductivity has led to a state-of-the-art ZT of 1.3 near 850 K in n-type (Hf0.6Zr0.4)0.99V0.01NiSn0.995Sb0.005 alloys.Comment: Submitted to AIP Advance

Effect of disorder on the thermal transport and elastic properties in thermoelectric Zn4Sb3

Zn4Sb3 undergoes a phase transition from alpha to beta phase at T1[approximate]250 K. The high temperature beta-Zn4Sb3 phase has been widely investigated as a potential state-of-the-art thermoelectric (TE) material, due to its remarkably low thermal conductivity. We have performed electronic and thermal transport measurements exploring the structural phase transition at 250 K. The alpha to beta phase transition manifests itself by anomalies in the resistivity, thermopower, and specific heat at 250 K as well as by a reduction in the thermal conductivity as Zn4Sb3 changes phase from the ordered alpha to the disordered beta-phase. Moreover, measurements of the elastic constants using resonant ultrasound spectroscopy (RUS) reveal a dramatic softening at the order-disorder transition upon warming. These measurements provide further evidence that the remarkable thermoelectric properties of beta-Zn4Sb3 are tied to the disorder in the crystal structure

Thermoelectric and Seebeck coefficients of granular metals

In this work we present a detailed study and derivation of the thermopower and thermoelectric coefficient of nano-granular metals at large tunneling conductance between the grains, g_T>> 1. An important criterion for the performance of a thermoelectric device is the thermodynamic figure of merit which is derived using the kinetic coefficients of granular metals. All results are valid at intermediate temperatures, E_c>>T/g_T>\delta, where \delta is the mean energy level spacing for a single grain and E_c its charging energy. We show that the electron-electron interaction leads to an increase of the thermopower with decreasing grain size and discuss our results in the light of future generation thermoelectric materials for low temperature applications. The behavior of the figure of merit depending on system parameters like grain size, tunneling conductance, and temperature is presented.Comment: 27 pages, 10 figures, revtex

Effect of disorder on the thermal transport and elastic properties in thermoelectric Zn\u3csub\u3e4\u3c/sub\u3eSb\u3csub\u3e3\u3c/sub\u3e

Zn4Sb3 undergoes a phase transition from α to β phase at T1≈250 K. The high temperature β-Zn4Sb3 phase has been widely investigated as a potential state-of-the-art thermoelectric (TE) material, due to its remarkably low thermal conductivity. We have performed electronic and thermal transport measurements exploring the structural phase transition at 250 K. The α to β phase transition manifests itself by anomalies in the resistivity, thermopower, and specific heat at 250 K as well as by a reduction in the thermal conductivity as Zn4Sb3 changes phase from the ordered α to the disordered β-phase. Moreover, measurements of the elastic constants using resonant ultrasound spectroscopy (RUS) reveal a dramatic softening at the order-disorder transition upon warming. These measurements provide further evidence that the remarkable thermoelectric properties of β-Zn4Sb3 are tied to the disorder in the crystal structure

Preferential scattering by interfacial charged defects for enhanced thermoelectric performance in few-layered n-type Bi2Te3

Over the past two decades several nano-structuring methods have helped improve the figure of merit (ZT) in the state-of-the art bulk thermoelectric materials. While these methods could enhance the thermoelectric performance of p-type Bi2Te3, it was frustrating to researchers that they proved ineffective for n-type Bi2Te3 due to the inevitable deterioration of its thermoelectric properties in the basal plane. Here, we describe a novel chemical-exfoliation spark-plasma-sintering (CE-SPS) nano-structuring process, which transforms the microstructure of n-type Bi2Te3 in an extraordinary manner without compromising its basal plane properties. The CE-SPS processing leads to preferential scattering of electrons at charged grain boundaries, and thereby increases the electrical conductivity despite the presence of numerous grain boundaries, and mitigates the bipolar effect via band occupancy optimization leading to an upshift (by ~ 100 K) and stabilization of the ZT peak over a broad temperature range of ~ 150 K

Solvent contribution to the stability of a physical gel characterized by quasi-elastic neutron scattering

The dynamics of a physical gel, namely the Low Molecular Mass Organic Gelator {\textit Methyl-4,6-O-benzylidene-$\alpha$ -D-mannopyranoside ($\alpha$-manno)} in water and toluene are probed by neutron scattering. Using high gelator concentrations, we were able to determine, on a timescale from a few ps to 1 ns, the number of solvent molecules that are immobilised by the rigid network formed by the gelators. We found that only few toluene molecules per gelator participate to the network which is formed by hydrogen bonding between the gelators' sugar moieties. In water, however, the interactions leading to the gel formations are weaker, involving dipolar, hydrophobic or $\pi-\pi$ interactions and hydrogen bonds are formed between the gelators and the surrounding water. Therefore, around 10 to 14 water molecules per gelator are immobilised by the presence of the network. This study shows that neutron scattering can give valuable information about the behaviour of solvent confined in a molecular gel.Comment: Langmuir (2015