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1.
Adv Mater ; : e2408320, 2024 Sep 17.
Artigo em Inglês | MEDLINE | ID: mdl-39285801

RESUMO

Achieving both formability and functionality in thermoelectric materials remains a significant challenge due to their inherent brittleness. Previous approaches, such as polymer infiltration, often compromise thermoelectric efficiency, underscoring the need for flexible, all-inorganic alternatives. This study demonstrates that the extreme brittleness of thermoelectric bismuth telluride (Bi2Te3) bulk compounds can be overcome by harnessing the nanoscale flexibility of Bi2Te3 nanoribbons and twisting them into a yarn structure. The resulting Bi2Te3 yarn, with a Seebeck coefficient of -126.6 µV K-1, exhibits remarkable deformability, enduring extreme bending curvatures (down to 0.5 mm-1) and tensile strains of ≈5% through over 1000 cycles without significant resistance change. This breakthrough allows the yarn to be seamlessly integrated into various applications-wound around metallic pipes, embedded within life jackets, or woven into garments-demonstrating unprecedented adaptability and durability. Moreover, a simple 4-pair thermoelectric generator comprising Bi2Te3 yarns and metallic wires generates a maximum output voltage of 67.4 mV, substantiating the effectiveness of thermoelectric yarns in waste heat harvesting. These advances not only challenge the traditional limitations posed by the brittleness of thermoelectric materials but also open new avenues for their application in wearable and structural electronics.

2.
Adv Sci (Weinh) ; 11(24): e2308075, 2024 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-38626376

RESUMO

Manipulating thermal properties of materials can be interpreted as the control of how vibrations of atoms (known as phonons) scatter in a crystal lattice. Compared to a perfect crystal, crystalline solids with defects are expected to have shorter phonon mean free paths caused by point defect scattering, leading to lower lattice thermal conductivities than those without defects. While this is true in many cases, alloying can increase the phonon mean free path in the Cd-doped AgSnSbSe3 system to increase the lattice thermal conductivity from 0.65 to 1.05 W m-1 K-1 by replacing 18% of the Sb sites with Cd. It is found that the presence of lone pair electrons leads to the off-centering of cations from the centrosymmetric position of a cubic lattice. X-ray pair distribution function analysis reveals that this structural distortion is relieved when the electronic configuration of the dopant element cannot produce lone pair electrons. Furthermore, a decrease in the Grüneisen parameter with doping is experimentally confirmed, establishing a relationship between the stereochemical activity of lone pair electrons and the lattice anharmonicity. The observed "harmonic" behavior with doping suggests that lone pair electrons must be preserved to effectively suppress phonon transport in these systems.

3.
Nat Commun ; 15(1): 1996, 2024 Mar 14.
Artigo em Inglês | MEDLINE | ID: mdl-38485943

RESUMO

Thermoelectric technology has potential for converting waste heat into electricity. Although traditional thermoelectric materials exhibit extremely high thermoelectric performances, their scarcity and toxicity limit their applications. Zinc oxide (ZnO) emerges as a promising alternative owing to its high thermal stability and relatively high Seebeck coefficient, while also being earth-abundant and nontoxic. However, its high thermal conductivity (>40 W m-1K-1) remains a challenge. In this study, we use a multi-step strategy to achieve a significantly high dimensionless figure-of-merit (zT) value of approximately 0.486 at 580 K (estimated value) by interfacing graphene quantum dots with 3D nanostructured ZnO. Here, we show the fabrication of graphene quantum dots interfaced 3D ZnO, yielding the highest zT value ever reported for ZnO counterparts; specifically, our experimental results indicate that the fabricated 3D GQD@ZnO exhibited a significantly low thermal conductivity of 0.785 W m-1K-1 (estimated value) and a remarkably high Seebeck coefficient of - 556 µV K-1 at 580 K.

4.
Adv Sci (Weinh) ; 11(35): e2402147, 2024 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-39041948

RESUMO

Manipulating the grain boundary and chiral structure of enantiomorphic inorganic thermoelectric materials facilitates a new degree of freedom for enhancing thermoelectric energy conversion. Chiral twist mechanisms evolve by the screw dislocation phenomenon in the nanostructures; however, contributions of such chiral transport have been neglected for bulk crystals. Tellurium (Te) has a chiral trigonal crystal structure, high band degeneracy, and lattice anharmonicity for high thermoelectric performance. Here, Sb-doped Te crystals are grown to minimize the severe grain boundary effects on carrier transport and investigate the interface of chiral Te matrix and embedded achiral Sb2Te3 precipitates, which induce unusual lattice twists. The low grain boundary scattering and conformational grain restructuring provide electrical-favorable semicoherent interfaces. This maintains high electrical conductivity leading to a twofold increase in power factor compared to polycrystal samples. The embedded Sb2Te3 precipitates concurrently enable moderate phonon scattering leading to a remarkable decrease in lattice thermal conductivity and a high dimensionless figure of merit (zT) of 1.1 at 623 K. The crystal growth and chiral atomic reorientation unravel the emerging benefits of interface engineering as a crucial contributor to effectively enhancing carrier transport and minimizing phonon propagation in thermoelectric materials.

5.
Heliyon ; 9(11): e21117, 2023 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-37928035

RESUMO

Thermoelectric materials are attracting considerable attention to alleviate the global energy crisis by enabling the direct conversion of heat into electricity. As a class of I-V-VI2 semiconductors, AgBiSe2 is expected to be the potential thermoelectric material to replace conventional PbTe-based compounds due to its non-toxic and abundant nature of its constituent elements. This review article summarizes the fundamental properties of AgBiSe2, thermoelectric properties, the effect of different dopants on its transport properties and entropy engineering for cubic phase stabilization with the detailed description of related techniques used to analyze the properties of AgBiSe2. The current thermoelectric figure-of-merit and approaches to further improve performance and operational stability are also discussed.

6.
RSC Adv ; 12(16): 9698-9703, 2022 Mar 25.
Artigo em Inglês | MEDLINE | ID: mdl-35424952

RESUMO

Transition metal compounds based on silver (Ag) and palladium (Pd) are extensively used as catalysts in the petrochemical industries. The catalytic activities of Ag and Pd decrease over time and hence need to be discarded. The recovery of elements like Ag from waste catalyst is essential because of its limited availability and cost, and it is environmentally beneficial with regards to recycling. In this study, Pd and Ag were leached from waste catalyst providing an alternative source suitable for a Ag paste electrode. Through an efficient reduction process, AgCl particles were obtained which serve as a precursor to synthesize Ag using ammonia as the solvent. The obtained Ag was fabricated to Ag paste by using mixed dispersion and solvent. The electrical resistivity of the Ag paste was recorded as 6.14 µΩ cm at 417 °C in a hydrogen atmosphere.

7.
Adv Mater ; 34(38): e2204132, 2022 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-35944565

RESUMO

Cation disordering is commonly found in multinary cubic compounds, but its effect on electronic properties has been neglected because of difficulties in determining the ordered structure and defect energetics. An absence of rational understanding of the point defects present has led to poor reproducibility and uncontrolled conduction type. AgBiSe2 is a representative compound that suffers from poor reproducibility of thermoelectric properties, while the origins of its intrinsic n-type conductivity remain speculative. Here, it is demonstrated that cation disordering is facilitated by BiAg charged antisite defects in cubic AgBiSe2 which also act as a principal donor defect that greatly controls the electronic properties. Using density functional theory calculations and in situ Raman spectroscopy, how saturation annealing with selenium vapor can stabilize p-type conductivity in cubic AgBiSe2 alloyed with SnSe at high temperatures is elucidated. With stable and controlled hole concentration, a peak is observed in the weighted mobility and the density-of-states effective mass in AgBiSnSe3 , implying an increased valley degeneracy in this system. These findings corroborate the importance of considering the defect energetics for exploring the dopability of ternary thermoelectric chalcogenides and engineering electronic bands by controlling self-doping.

8.
Nat Commun ; 13(1): 3741, 2022 06 29.
Artigo em Inglês | MEDLINE | ID: mdl-35768427

RESUMO

Heat is a fundamental feedstock, where more than 80% of global energy comes from fossil-based heating process. However, it is mostly wasted due to a lack of proper techniques of utilizing the low-quality waste heat (<100 °C). Here we report thermoelectrobiocatalytic chemical conversion systems for heat-fueled, enzyme-catalyzed oxyfunctionalization reactions. Thermoelectric bismuth telluride (Bi2Te3) directly converts low-temperature waste heat into chemical energy in the form of H2O2 near room temperature. The streamlined reaction scheme (e.g., water, heat, enzyme, and thermoelectric material) promotes enantio- and chemo-selective hydroxylation and epoxidation of representative substrates (e.g., ethylbenzene, propylbenzene, tetralin, cyclohexane, cis-ß-methylstyrene), achieving a maximum total turnover number of rAaeUPO (TTNrAaeUPO) over 32000. Direct conversion of vehicle exhaust heat into the enantiopure enzymatic product with a rate of 231.4 µM h-1 during urban driving envisions the practical feasibility of thermoelectrobiocatalysis.


Assuntos
Temperatura Alta , Peróxido de Hidrogênio , Hidrocarbonetos , Hidroxilação , Emissões de Veículos
9.
ACS Appl Mater Interfaces ; 14(1): 1270-1279, 2022 Jan 12.
Artigo em Inglês | MEDLINE | ID: mdl-34979804

RESUMO

Charge carrier transport and corresponding thermoelectric properties are often affected by several parameters, necessitating a thorough comparative study for a profound understanding of the detailed conduction mechanism. Here, as a model system, we compare the electronic transport properties of two layered semiconductors, Sb2Si2Te6 and Bi2Si2Te6. Both materials have similar grain sizes and morphologies, yet their conduction characteristics are significantly different. We found that phase boundary scattering can be one of the main factors for Bi2Si2Te6 to experience significant charge carrier scattering, whereas Sb2Si2Te6 is relatively unaffected by the phenomenon. Furthermore, extensive point defect scattering in Sb2Si2Te6 significantly reduces its lattice thermal conductivity and results in high zT values across a broad temperature range. These findings provide novel insights into electron transport within these materials and should lead to strategies for further improving their thermoelectric performance.

10.
Adv Sci (Weinh) ; 8(20): e2100895, 2021 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-34390224

RESUMO

Thermoelectric properties are frequently manipulated by introducing point defects into a matrix. However, these properties often change in unfavorable directions owing to the spontaneous formation of vacancies at high temperatures. Although it is crucial to maintain high thermoelectric performance over a broad temperature range, the suppression of vacancies is challenging since their formation is thermodynamically preferred. In this study, using PbTe as a model system, it is demonstrated that a high thermoelectric dimensionless figure of merit, zT ≈ 2.1 at 723 K, can be achieved by suppressing the vacancy formation via dopant balancing. Hole-killer Te vacancies are suppressed by Ag doping because of the increased electron chemical potential. As a result, the re-dissolution of Na2 Te above 623 K can significantly increase the hole concentration and suppress the drop in the power factor. Furthermore, point defect scattering in material systems significantly reduces lattice thermal conductivity. The synergy between defect and carrier engineering offers a pathway for achieving a high thermoelectric performance by alleviating the power factor drop and can be utilized to enhance thermoelectric properties of thermoelectric materials.

11.
Sci Rep ; 7(1): 4496, 2017 07 03.
Artigo em Inglês | MEDLINE | ID: mdl-28674398

RESUMO

We report the enhanced thermoelectric properties of Ce-doped AgSbTe2 (AgSb1-xCexTe2) compounds. As the Ce contents increased, the proportion of heterophase Ag2Te in the AgSbTe2 gradually decreased, along with the size of the crystals. The electrical resistivity and Seebeck coefficient were dramatically affected by Ce doping and the lattice thermal conductivity was reduced. The presence of nanostructured Ag2Te heterophases resulted in a greatly enhanced dimensionless figure of merit, ZT of 1.5 at 673 K. These findings highlight the importance of the heterophase and doping control, which determines both electrical and thermal properties.

13.
Korean J Anesthesiol ; 68(4): 373-8, 2015 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-26257850

RESUMO

BACKGROUND: This study was performed to compare the incidence of emergence agitation (EA) between inhalation and intravenous anesthesia induction in children after sevoflurane anesthesia. METHODS: In this prospective and double-blind study, 100 children aged 3 to 7 years were enrolled. Subjects were randomly assigned to the sevoflurane (Group S) or thiopental (Group T) anesthesia induction groups. Anesthesia was induced using 8% sevoflurane and 4-6 mg/kg thiopental in Groups S and T, respectively. Anesthesia was maintained with nitrous oxide and sevoflurane. The children were evaluated at 5 and 20 min after arrival in the postanesthesia care unit (PACU) with a four-point agitation scale and the Pediatric Anesthesia Emergence Delirium scale. The incidence of EA and administration of the rescue agent were recorded. RESULTS: The incidence of EA was significantly lower in Group T compared to Group S at 5 min after PACU arrival (3/49 patients, 6% vs. 12/47 patients, 26%, P = 0.019). However, there was no difference between the two groups at 20 min after PACU arrival (23/49 vs. 19/47 patients in Group T vs. Group S, P = 0.425). The overall incidence of EA was 60% (28/47 patients) in Group S and 41% (20/49 patients) in Group T (P = 0.102). The number of children who received propofol as a rescue agent was significantly lower in Group T (Group S: 14/47 vs. Group T: 5/49, P = 0.031). CONCLUSIONS: Intravenous anesthesia induction with thiopental reduced the incidence of EA in the early PACU period compared to inhalation induction with sevoflurane in 3- to 7-year-old children undergoing sevoflurane anesthesia.

14.
J Nanosci Nanotechnol ; 15(10): 8299-304, 2015 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-26726507

RESUMO

Bi2Te3 thermoelectric thin films were deposited on the flexible polyimide substrates by RF magnetron co-sputtering of a Bi and a Te targets. The influence of the substrate temperature and RF power on the microstructure, chemical composition, and the thermoelectric properties of the sputtered films was investigated by using scanning electron microscopy, X-ray diffraction, energy dispersive X-ray spectroscopy, and in-plane resistivity/Seebeck coefficient measurement. It was shown that the thermoelectric properties of the films depend sensitively on the Bi/Te chemical composition ratio and the substrate temperature, and the layered structure was clearly observed from the cross section of the (00L)-oriented, nearly stoichiometric Bi2Te3 films when the substrate temperature is higher than 250 °C. As-deposited Bi2Te3 films deposited at 300 °C show the highest power factor of 0.97 mW/K(2)m and the Seebeck coefficient of -193 µV/K at 32 °C, which also have (00L) preferred orientation and the layered structure. The durability of the Bi2Te3 films on polyimide against repeated bending was also tested by monitoring the film resistance, and it was concluded that the Bi2Te3 films are applicable reliably on the curved surfaces with the radius of curvature larger than 5 mm.

15.
Nanoscale ; 7(1): 365, 2015 Jan 07.
Artigo em Inglês | MEDLINE | ID: mdl-25424730

RESUMO

Correction for 'Three-dimensional hierarchical Te-Si nanostructures' by Jae-Hong Lim et al., Nanoscale, 2014, 6, 11697-11702.

16.
Sci Rep ; 4: 5450, 2014 Jun 26.
Artigo em Inglês | MEDLINE | ID: mdl-24965478

RESUMO

Resistivity is an intrinsic feature that specifies the electrical properties of a material and depends on electron-phonon scattering near room temperature. Reducing the resistivity of a metal to its potentially lowest value requires eliminating grain boundaries and impurities, but to date few studies have focused on reducing the intrinsic resistivity of a pure metal itself. We could reduce the intrinsic resistivity of single-crystal Ag, which has an almost perfect structure, by impurity doping it with Cu. This paper presents our results: resistivity was reduced to 1.35 µΩ · cm at room temperature after 3 mol% Cu-doping of single-crystal Ag. Various mechanisms were examined in an attempt to explain the abnormal behavior.

17.
Nanoscale ; 6(20): 11697-702, 2014 Oct 21.
Artigo em Inglês | MEDLINE | ID: mdl-24988904

RESUMO

Three-dimensional hybrid nanostructures (i.e., Te "nanobranches" on a Si "nanotrunk" or Te "nanoleaves" on a Si "nanotrunk") were synthesized by combining the gold-assisted chemical etching of Si to form Si "nanotrunks" and the galvanic displacement of Si to form Te "nanobranches" or "nanoleaves." By adjusting the composition of the electrolyte used for the galvanic displacement reaction, the shape of the Te nanostructures could be changed from nanoleaves to nanobranches. The Si nanotrunks with Te nanobranches showed stronger luminescent emission in the visible region, with their Raman spectrum having a higher wave number, owing to their grain size being larger. This suggested that the optical and photoelectrochemical properties of Te-Si hybrid nanostructures depend on their shape and size. Using this approach, it should be possible to fabricate various hierarchical nanostructures for use in photoelectronic and photoelectrochemical devices.

18.
Sci Rep ; 4: 6230, 2014 Aug 29.
Artigo em Inglês | MEDLINE | ID: mdl-25169804

RESUMO

Copper (Cu) thin films have been widely used as electrodes and interconnection wires in integrated electronic circuits, and more recently as substrates for the synthesis of graphene. However, the ultra-high vacuum processes required for high-quality Cu film fabrication, such as molecular beam epitaxy (MBE), restricts mass production with low cost. In this work, we demonstrated high-quality Cu thin films using a single-crystal Cu target and radio-frequency (RF) sputtering technique; the resulting film quality was comparable to that produced using MBE, even under unfavorable conditions for pure Cu film growth. The Cu thin film was epitaxially grown on an Al2O3 (sapphire) (0001) substrate, and had high crystalline orientation along the (111) direction. Despite the 10(-3) Pa vacuum conditions, the resulting thin film was oxygen free due to the high chemical stability of the sputtered specimen from a single-crystal target; moreover, the deposited film had >5× higher adhesion force than that produced using a polycrystalline target. This fabrication method enabled Cu films to be obtained using a simple, manufacturing-friendly process on a large-area substrate, making our findings relevant for industrial applications.

19.
ACS Nano ; 7(10): 9106-14, 2013 Oct 22.
Artigo em Inglês | MEDLINE | ID: mdl-24016184

RESUMO

We demonstrate gate-controlled spin-orbit interaction (SOI) in InAs high-electron mobility transistor (HEMT) structures transferred epitaxially onto Si substrates. Successful epitaxial transfer of the multilayered structure after separation from an original substrate ensures that the InAs HEMT maintains a robust bonding interface and crystalline quality with a high electron mobility of 46200 cm(2)/(V s) at 77 K. Furthermore, Shubnikov-de Haas (SdH) oscillation analysis reveals that a Rashba SOI parameter (α) can be manipulated using a gate electric field for the purpose of spin field-effect transistor operation. An important finding is that the α value increases by about 30% in the InAs HEMT structure that has been transferred when compared to the as-grown structure. First-principles calculations indicate that the main causes of the large improvement in α are the bonding of the InAs HEMT active layers to a SiO2 insulating layer with a large band gap and the strain relaxation of the InAs channel layer during epitaxial transfer. The experimental results presented in this study offer a technological platform for the integration of III-V heterostructures onto Si substrates, permitting the spintronic devices to merge with standard Si circuitry and technology.

20.
Sci Rep ; 3: 2123, 2013.
Artigo em Inglês | MEDLINE | ID: mdl-23820973

RESUMO

The optimal hybridization of photovoltaic (PV) and thermoelectric (TE) devices has long been considered ideal for the efficient harnessing solar energy. Our hybrid approach uses full spectrum solar energy via lossless coupling between PV and TE devices while collecting waste energy from thermalization and transmission losses from PV devices. Achieving lossless coupling makes the power output from the hybrid device equal to the sum of the maximum power outputs produced separately from individual PV and TE devices. TE devices need to have low internal resistances enough to convey photo-generated currents without sacrificing the PV fill factor. Concomitantly, a large number of p-n legs are preferred to drive a high Seebeck voltage in TE. Our simple method of attaching a TE device to a PV device has greatly improved the conversion efficiency and power output of the PV device (~30% at a 15°C temperature gradient across a TE device).

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