Decoupling Carrier-Phonon Scattering Boosts the Thermoelectric Performance of n-Type GeTe-Based Materials.

The coupled relationship between carrier and phonon scattering severely limits the thermoelectric performance of n-type GeTe materials. Here, we provide an efficient strategy to enlarge grains and induce vacancy clusters for decoupling carrier-phonon scattering through the annealing optimization of n-type GeTe-based materials. Specifically, boundary migration is used to enlarge grains by optimizing the annealing time, while vacancy clusters are induced through the aggregation of Ge vacancies during annealing. Such enlarged grains can weaken carrier scattering, while vacancy clusters can strengthen phonon scattering, leading to decoupled carrier-phonon scattering. As a result, a ratio between carrier mobility and lattice thermal conductivity of ∼492.8 cm3 V-1 s-1 W-1 K and a peak ZT of ∼0.4 at 473 K are achieved in Ge0.67Pb0.13Bi0.2Te. This work reveals the critical roles of enlarged grains and induced vacancy clusters in decoupling carrier-phonon scattering and demonstrates the viability of fabricating high-performance n-type GeTe materials via annealing optimization.

Lattice Distortions and Multiple Valence Band Convergence Contributing to High Thermoelectric Performance in MnTe.

Here, a new route is proposed for the minimization of lattice thermal conductivity in MnTe through considerable increasing phonon scattering by introducing dense lattice distortions. Dense lattice distortions can be induced by Cu and Ag dopants possessing large differences in atom radius with host elements, which causes strong phonon scattering and results in extremely low lattice thermal conductivity. Density functional theory (DFT) calculations reveal that Cu and Ag codoping enables multiple valence band convergence and produces a high density of state values in the electronic structure of MnTe, contributing to the large Seebeck coefficient. Cu and Ag codoping not only optimizes the Seebeck coefficient but also substantially increases the carrier concentration and electrical conductivity, resulting in the significant enhancement of power factor. The maximum power factor reaches 11.36 µW cm-1 K-2 in Mn0.98 Cu0.04 Ag0.04 Te. Consequently, an outstanding ZT of 1.3 is achieved for Mn0.98 Cu0.04 Ag0.04 Te by these synergistic effects. This study provides guidelines for developing high-performance thermoelectric materials through the rational design of effective dopants.

Ultrafast and Cost-Effective Fabrication of High-Performance Carbon-Based Flexible Thermoelectric Hybrid Films and Their Devices.

Due to their cost-effectiveness and industry-scale feasibility, carbon-based composites have been considered to be promising thermoelectric materials for low-grade power generation. However, current fabrications for carbon-based composites are time-consuming, and their thermoelectric properties are still low. Herein, we develop an ultrafast and cost-effective hot-pressing method to fabricate a novel carbon-based hybrid film, which consists of ionic liquid/phenolic resin/carbon fiber/expanded graphite. This method only costs no more than 15 min. We found that the expanded graphite as the major component enables high flexibility and the introduction of phenolic resin and carbon fiber enhances the shear resistance and toughness of the film, while the ion-induced carrier migration contributes to a high power factor of 38.7 µW m-1 K-2 at 500 K in the carbon-based hybrid film. After the comparison based on the ratios between the power factor with fabrication time and cost among the current conventional carbon-based thermoelectric composites, our hybrid films show the best cost-effective property. Besides, a flexible thermoelectric device, assembled by the as-designed hybrid films, shows a maximum output power density of 79.3 nW cm-2 at a temperature difference of 20 K. This work paves a new way to fabricate cost-effective and high-performance carbon-based thermoelectric hybrids with promising application potential.