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Science ; 365(6460): 1418-1424, 2019 09 27.
Artigo em Inglês | MEDLINE | ID: mdl-31604269


Thermoelectric technology allows conversion between heat and electricity. Many good thermoelectric materials contain rare or toxic elements, so developing low-cost and high-performance thermoelectric materials is warranted. Here, we report the temperature-dependent interplay of three separate electronic bands in hole-doped tin sulfide (SnS) crystals. This behavior leads to synergistic optimization between effective mass (m*) and carrier mobility (µ) and can be boosted through introducing selenium (Se). This enhanced the power factor from ~30 to ~53 microwatts per centimeter per square kelvin (µW cm-1 K-2 at 300 K), while lowering the thermal conductivity after Se alloying. As a result, we obtained a maximum figure of merit ZT (ZT max) of ~1.6 at 873 K and an average ZT (ZT ave) of ~1.25 at 300 to 873 K in SnS0.91Se0.09 crystals. Our strategy for band manipulation offers a different route for optimizing thermoelectric performance. The high-performance SnS crystals represent an important step toward low-cost, Earth-abundant, and environmentally friendly thermoelectrics.

Inorg Chem ; 57(10): 6051-6056, 2018 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-29722989


The quaternary compound Cu2ZnSnSe4 (CZTSe), as a typical candidate for both solar cells and thermoelectrics, is of great interest for energy harvesting applications. Materials with a high thermoelectric efficiency have a relatively low thermal conductivity, which is closely related to their chemical bonding and lattice dynamics. Therefore, it is essential to investigate the lattice dynamics of materials to further improve their thermoelectric efficiency. Here we report a lattice dynamic study in a cobalt-substituted CZTSe system using temperature-dependent X-ray absorption fine structure spectroscopy (TXAFS). The lattice contribution to the thermal conductivity is dominant, and its reduction is mainly ascribed to the increment of point defects after cobalt substitution. Furthermore, a lattice dynamic study shows that the Einstein temperature of atomic pairs is reduced after cobalt substitution, revealing that increasing local structure disorder and weakened bonding for each of the atomic pairs are achieved, which gives us a new perspective for understanding the behavior of lattice thermal conductivity.

Chemosphere ; 197: 362-366, 2018 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-29407806


In this study, fly ash samples were collected from bag houses in a Chinese municipal solid waste incinerator (MSWI) and secondary fly ash (SFA) samples were collected from a high-temperature tubular electric furnace by thermal treatment of MSWI fly ash at 1050, 1100, 1150, 1200, and 1250 °C.We determined the speciation and atomic coordinates of lead in SFA using X-ray absorption spectroscopy (XAS) techniques. The results obtained by X-ray absorption near edge structure (XANES) spectra revealed that the mass fraction of PbO in MSWI fly ash was 57.9% (wt %) while PbCl2 and PbS were the dominant species in SFA. Extended X-ray absorption fine structure (EXAFS) data analysis indicated the atomic coordinates of Pb were proportional to the weights of PbCl2 and PbS, in good agreement with the XANES spectra. These findings highlight lead evaporation processes in the MSWI fly ash during heat treatment and provide a method for consistent speciation analysis of environmental samples using XAS.

Poluentes Atmosféricos/análise , Incineração/métodos , Chumbo/análise , Resíduos Sólidos/análise , Carbono/química , Cinza de Carvão/química , Metais Pesados/análise , Material Particulado/química , Eliminação de Resíduos/métodos , Espectroscopia por Absorção de Raios X , Raios X
ACS Appl Mater Interfaces ; 8(24): 15196-204, 2016 Jun 22.
Artigo em Inglês | MEDLINE | ID: mdl-27135808


We report remarkably enhanced thermoelectric performance of Te doped Cu2Se in midtemperature range. Through ball-milling process followed by spark plasma sintering (SPS), nanoscale Cu2Te clusters were embeded in the matrix of Cu2Se, inducing a drastic enhancement of thermoelectric performance by reducing the thermal conductivity without degrading the power factor. A large ZT value of 1.9 was achieved at 873 K for Cu2Se1.9Te0.1, which is about 2 times larger than that of the pure Cu2Se. The nanoscale heat management by Cu2Te nanoclusters in superionic conductors opens up an avenue for thermoelectric materials research.

Phys Chem Chem Phys ; 18(21): 14580-7, 2016 06 07.
Artigo em Inglês | MEDLINE | ID: mdl-27181423


The misfit layered cobaltate thermoelectrics are good candidates for high temperature thermoelectric applications. Ca3Co4O9 is a typical compound of this family, which consists of rock salt Ca2CoO3 slabs alternating with hexagonal CoO2 slabs with a large lattice mismatch along the b axis. Each slab is 0.3-0.5 nm thick and shows an inherent structural heterogeneity at the nanoscale. The latter is a key parameter that affects the electrical transport and the heat flow in these misfit structured thermoelectrics. To clarify the physical origin of the thermoelectric performance of iron doped Ca3Co4O9 we combined X-ray near-edge absorption spectroscopy (XANES) and quantum modeling using density functional theory. In contrast to single-site doping, the iron doping first occurs at the Co1 site of the rock salt slab at low doping while at higher doping it prefers the Ca1 site of the rock salt slab. Doping at the Ca1 site modifies the electronic structure tuning the nanoscale structural heterogeneity. This mechanism may open a new route to optimizing the thermoelectric performance of misfit layered thermoelectrics.