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1.
Inorg Chem ; 60(15): 11364-11373, 2021 Aug 02.
Artigo em Inglês | MEDLINE | ID: mdl-34269565

RESUMO

Copper-based sulfides are promising materials for thermoelectric applications, which can convert waste heat into electricity. This study reports the enhanced thermoelectric performance of Cu26V2Ge6S32 colusite via substitution of antimony (Sb) for germanium (Ge) and introduction of copper (Cu) as an interstitial atom. The crystal structure of the solid solutions and Cu-rich compounds were analyzed by powder X-ray diffraction and scanning transmission electron microscopy. Both chemical approaches decrease the hole carrier concentration, which leads to a reduction in the electronic thermal conductivity while keeping the thermoelectric power factor at a high value. Furthermore, the interstitial Cu atoms act as phonon scatterers, thereby decreasing the lattice thermal conductivity. The combined effects increase the dimensionless thermoelectric figure of merit ZT from 0.3 (Cu26V2Ge6S32) to 0.8 (Cu29V2Ge5SbS32) at 673 K.

2.
Phys Chem Chem Phys ; 22(4): 2081-2086, 2020 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-31904070

RESUMO

Famatinite Cu3SbS4 has attracted attention for its potential application in thermoelectric (TE) contexts. In this work, we report the impacts of co-substituting Ge and P for Sb on TE properties. Melting and heat treatment methods were adopted to synthesize samples of Cu3Sb1-x-yGexPyS4 (x≤ 0.4, y≤ 0.3). In this system, Ge functioned as an acceptor for doping a hole to the valence band, which led to enhancement of the TE power factor. Contrastingly, P barely altered the electronic structure. Furthermore, both Ge and P acted as point defects, which effectively decreased lattice thermal conductivity. The combined effects of the co-substitution gave rise to an enhanced dimensionless figure of merit, ZT, of 0.67 at 673 K.

3.
Inorg Chem ; 58(2): 1425-1432, 2019 Jan 22.
Artigo em Inglês | MEDLINE | ID: mdl-30620579

RESUMO

We report the preparations, thermoelectric and magnetic properties, and electronic structures of Cu-Ti-S systems, namely, cubic thiospinel c-Cu1- xTi2S4 ( x ≤ 0.375), a derivative cubic and Ti-rich phase c-Cu1- xTi2.25S4 ( x = 0.5, 0.625), and a rhombohedral phase r-CuTi2S4. All samples have the target compositions except for r-CuTi2S4, whose actual composition is Cu1.14Ti1.80S4. All of the phases have n-type metallic character and exhibit Pauli paramagnetism, as proven by experiments and first-principles calculations. The Cu and Ti deficiencies in c-Cu1- xTi2S4 and r-CuTi2S4, respectively, decrease the electron-carrier concentration, whereas the "excess" of Ti ions in c-Cu1- xTi2.25S4 largely increases it. For r-CuTi2S4, the reduced carrier concentration increases the electrical resistivity and Seebeck coefficient, leading to the highest thermoelectric power factor of 0.5 mW K-2 m-1 at 670 K. For all of the Cu-Ti-S phases, the thermal conductivity at 670 K is 3.5-5 W K-1 m-1, where the lattice part of the conductivity is as low as 1 W K-1 m-1 at 670 K. As a result, r-CuTi2S4 shows the highest dimensionless thermoelectric figure of merit ZT of 0.2. The present systematic study on the Cu-Ti-S systems provides insights into the structural design of thermoelectric materials based on Cu-M-S (M = transition-metal elements).

4.
J Nanosci Nanotechnol ; 13(7): 4799-824, 2013 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-23901503

RESUMO

In this review, we present the synthesis and characterization of Pt, Pd, Pt based bimetallic and multi-metallic nanoparticles with mixture, alloy and core-shell structure for nano-catalysis, energy conversion, and fuel cells. Here, Pt and Pd nanoparticles with modified nanostructures can be controllably synthesized via chemistry and physics for their uses as electro-catalysts. The cheap base metal catalysts can be studied in the relationship of crystal structure, size, morphology, shape, and composition for new catalysts with low cost. Thus, Pt based alloy and core-shell catalysts can be prepared with the thin Pt and Pt-Pd shell, which are proposed in low and high temperature proton exchange membrane fuel cells (PEMFCs), and direct methanol fuel cells (DMFCs). We also present the survey of the preparation of Pt and Pd based catalysts for the better catalytic activity, high durability, and stability. The structural transformations, quantum-size effects, and characterization of Pt and Pd based catalysts in the size ranges of 30 nm (1-30 nm) are presented in electro-catalysis. In the size range of 10 nm (1-10 nm), the pure Pt catalyst shows very large surface area for electro-catalysis. To achieve homogeneous size distribution, the shaped synthesis of the polyhedral Pt nanoparticles is presented. The new concept of shaping specific shapes and morphologies in the entire nano-scale from nano to micro, such as polyhedral, cube, octahedra, tetrahedra, bar, rod, and others of the nanoparticles is proposed, especially for noble and cheap metals. The uniform Pt based nanosystems of surface structure, internal structure, shape, and morphology in the nanosized ranges are very crucial to next fuel cells. Finally, the modifications of Pt and Pd based catalysts of alloy, core-shell, and mixture structures lead to find high catalytic activity, durability, and stability for nano-catalysis, energy conversion, fuel cells, especially the next large-scale commercialization of next PEMFCs, and DMFCs.


Assuntos
Fontes de Energia Elétrica , Nanopartículas Metálicas/química , Metanol/química , Paládio/química , Platina/química , Polímeros/química , Catálise , Eletrólitos/química , Desenho de Equipamento , Análise de Falha de Equipamento
5.
Nanomaterials (Basel) ; 11(6)2021 Jun 11.
Artigo em Inglês | MEDLINE | ID: mdl-34208185

RESUMO

The temperature dependence thermal conductivity of the indium-gallium-zinc oxide (IGZO) thin films was investigated with the differential three-omega method for the clear demonstration of nanocrystallinity. The thin films were deposited on an alumina (α-Al2O3) substrate by direct current (DC) magnetron sputtering at different oxygen partial pressures ([PO2] = 0%, 10%, and 65%). Their thermal conductivities at room temperature were measured to be 1.65, 1.76, and 2.58 Wm-1K-1, respectively. The thermal conductivities decreased with an increase in the ambient measurement temperature. This thermal property is similar to that of crystalline materials. Electron microscopy observations revealed the presence of nanocrystals embedded in the amorphous matrix of the IGZO films. The typical size of the nanocrystals was approximately 2-5 nm with the lattice distance of about 0.24-0.26 nm. These experimental results indicate that the nanocrystalline microstructure controls the heat conduction in the IGZO films.

6.
J Colloid Interface Sci ; 359(2): 339-50, 2011 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-21524421

RESUMO

In this paper, we presented the preparation procedure of Pt nanoparticles with the well-controlled polyhedral morphology and size by a modified polyol method using AgNO(3) in accordance with the reduction of H(2)PtCl(6) in EG at high temperature around 160°C. The methods of UV-vis spectroscopy, X-ray diffraction (XRD), transmission electron microscopy (TEM), and high resolution (HR) TEM measurements were used to characterize their surface morphology, size, and crystal structure. We have observed that the polyhedral Pt nanoparticles of sharp edges and corners were produced in the preferential homogenous growth as well as the formation of porous and large Pt particles by self-aggregation and assembly originating from as-prepared polyhedral Pt nanoparticles. It is most impressive to find that the arrangement of Pt nanoparticles was observed in their surface attachments, self-aggregation, random and directed surface self-assembly by the bottom-up approach. Their high electrocatalytic activity for methanol oxidation was predicted. The findings and results showed that the polyhedral Pt nanoparticle-based catalysts exhibited the high electrocatalytic activity for their potential applications in developing the efficient Pt-based catalysts for direct methanol fuel cells.

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