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Journal ArticleDOI

Ultrahigh Power Factor and Electron Mobility in n-Type Bi2Te3-x%Cu Stabilized under Excess Te Condition.

16 Aug 2019-ACS Applied Materials & Interfaces (American Chemical Society)-Vol. 11, Iss: 34, pp 30999-31008
TL;DR: An ultrahigh carrier mobility and power factor of nearly unchanged by increasing the Cu content in contrast to the general understanding of inverse relationship between electrical conductivity and Seebeck coefficient is reported, which synergistically lead to a record high power factor among all polycrystalline n-type Bi2Te3-based materials.
Abstract: The thermoelectric (TE) community has mainly focused on improving the figure of merit (ZT) of materials. However, the output power of TE devices directly depends on the power factor (PF) rather than ZT. Effective strategies of enhancing PF have been elusive for Bi2Te3-based compounds, which are efficient thermoelectrics operating near ambient temperature. Here, we report ultrahigh carrier mobility of ∼467 cm2 V-1 s-1 and power factor of ∼45 μW cm-1 K-2 in a new n-type Bi2Te3 system with nominal composition CuxBi2Te3.17 (x = 0.02, 0.04, and 0.06). It is obtained by reacting Bi2Te3 with surplus Cu and Te and subsequently pressing powder products by spark plasma sintering (SPS). The SPS discharges excess Te but stabilizes the high extent of Cu in the structure, giving unique SPS CuxBi2Te3.17 samples. The analyzed composition is close to "CuxBi2Te3". Their charge transport properties are highly unusual. Hall carrier concentration and mobility simultaneously increase with the higher mole fraction of Cu contrary to the typical carrier scattering mechanism. As a consequence, the electrical conductivity is considerably enhanced with Cu incorporation. The Seebeck coefficient is nearly unchanged by the increasing Cu content in contrast to the general understanding of inverse relationship between electrical conductivity and Seebeck coefficient. These effects synergistically lead to a record high power factor among all polycrystalline n-type Bi2Te3-based materials.
Citations
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Journal ArticleDOI
01 Dec 2019-Nature
TL;DR: A high intrinsic thermoelectric figure of merit is found for a metastable thin-film Fe2V0.8W0.2Al Heusler alloy, which may arise from a large differential density of states at the Fermi level and a Weyl-like electron dispersion close to the Fermani level, which indicates a high mobility of charge carriers owing to linear crossing in the electronic bands.
Abstract: Thermoelectric materials transform a thermal gradient into electricity. The efficiency of this process relies on three material-dependent parameters: the Seebeck coefficient, the electrical resistivity and the thermal conductivity, summarized in the thermoelectric figure of merit. A large figure of merit is beneficial for potential applications such as thermoelectric generators. Here we report the thermal and electronic properties of thin-film Heusler alloys based on Fe2V0.8W0.2Al prepared by magnetron sputtering. Density functional theory calculations suggest that the thin films are metastable states, and measurements of the power factor—the ratio of the Seebeck coefficient squared divided by the electrical resistivity—suggest a high intrinsic figure of merit for these thin films. This may arise from a large differential density of states at the Fermi level and a Weyl-like electron dispersion close to the Fermi level, which indicates a high mobility of charge carriers owing to linear crossing in the electronic bands. A high intrinsic thermoelectric figure of merit is found for a metastable thin-film Fe2V0.8W0.2Al Heusler alloy.

205 citations

Journal ArticleDOI
TL;DR: In this paper, an APT-based investigation of the local chemical decoration states of various types of lattice defects in thermoelectric materials is presented, which can be used to better understand the interplay between thermodynamic properties and microstructural features, extending the concept of defect engineering to the field of segregation engineering.

64 citations

Journal ArticleDOI
TL;DR: This work developed high performance n-type Bi2-xSbxTe3, a composition long thought to only make good p-type thermoelectrics, to replace the mainstream n- type Bi2Te3-xSex near room temperature.
Abstract: For decades, the V2VI3 compounds, specifically p-type Bi2-xSbxTe3 and n-type Bi2Te3-xSex, have remained the cornerstone of commercial thermoelectric solid-state cooling and power generation near room temperature. However, a long-standing problem in V2VI3 thermoelectrics is that n-type Bi2Te3-xSex is inferior in performance to p-type Bi2-xSbxTe3 near room temperature, restricting the device efficiency. In this work, we developed high-performance n-type Bi2-xSbxTe3, a composition long thought to only make good p-type thermoelectrics, to replace the mainstream n-type Bi2Te3-xSex. The success arises from the synergy of the following mechanisms: (i) the donorlike effect, which produces excessive conduction electrons in Bi2Te3, is compensated by the antisite defects regulated by Sb alloying; (ii) the conduction band degeneracy increases from 2 for Bi2Te3 and Bi2Te3-xSex to 6 for Bi2-xSbxTe3, favoring high Seebeck coefficients; and (iii) the larger mass fluctuation yet smaller electronegativity difference and smaller atomic radius difference between Bi and Sb effectively suppresses the lattice thermal conductivity and retains decent carrier mobility. A state-of-the-art zT of 1.0 near room temperature was attained in hot deformed Bi1.5Sb0.5Te3, which is higher than those for most known n-type thermoelectric materials, including commercial Bi2Te3-xSex ingots and the popular Mg3Sb2. Technically, building both the n-leg and p-leg of a thermoelectric module using similar chemical compositions has key advantages in the mechanical strength and the durability of devices. These results attested to the promise of n-type Bi2-xSbxTe3 as a replacement of the mainstream n-type Bi2Te3-xSex near room temperature.

29 citations

Journal ArticleDOI
TL;DR: In this paper , the state-of-the-art fabrication techniques for the on-chip integration of 2D materials are reviewed, which are categorized into material synthesis, onchip transfer, film patterning and property tuning/modification.
Abstract: With compact footprint, low energy consumption, high scalability, and mass producibility, chip‐scale integrated devices are an indispensable part of modern technological change and development. Recent advances in 2D layered materials with their unique structures and distinctive properties have motivated their on‐chip integration, yielding a variety of functional devices with superior performance and new features. To realize integrated devices incorporating 2D materials, it requires a diverse range of device fabrication techniques, which are of fundamental importance to achieve good performance and high reproducibility. This paper reviews the state‐of‐art fabrication techniques for the on‐chip integration of 2D materials. First, an overview of the material properties and on‐chip applications of 2D materials is provided. Second, different approaches used for integrating 2D materials on chips are comprehensively reviewed, which are categorized into material synthesis, on‐chip transfer, film patterning, and property tuning/modification. Third, the methods for integrating 2D van der Waals heterostructures are also discussed and summarized. Finally, the current challenges and future perspectives are highlighted.

28 citations

Journal ArticleDOI
TL;DR: In this paper, a new n-type Bi2Te3-based nanocomposite embedded with in-situ formed SnBi and Te nanoinclusions is constructed, and its thermoelectric performance is enhanced substantially as compared to pristine BTS.
Abstract: Although n-type Bi2Te3-based alloys are state-of-the-art thermoelectric material, their efficiency is still too low to satisfy its wide applications. Hence, it is imperative to improve the thermoelectric performance of n-type Bi2Te2.7Se0.3 (BTS). Here, we show that through a facile method of Sn addition in BTS a new SnxBi2Te2.7Se0.3 based nanocomposite embedded with in-situ formed SnBi and Te nanoinclusions ((SnBi + Te)/SnxBi2Te2.7Se0.3) is constructed, and its thermoelectric performance is enhanced substantially as compared to pristine BTS. Specifically, addition of 0.2 wt% of Sn in BTS causes 38% increase in power factor (PF) and 40% reduction in lattice thermal conductivity. The increased PF mainly comes from elevated Seebeck coefficient due to intensified energy dependent electron scattering caused by the interface potentials; while the reduced thermal conductivity originates from enhanced phonon scattering by the embedded nanoinclusions. Consequently, both high maximum figure of merit ZT (ZTmax = 1.11 at ~370 K) and large average ZT (ZTave = 1.03 at T = 300 K–500 K) are achieved for this sample, which are respectively 76% and 80% higher than those of BTS studied here.

26 citations

References
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Journal ArticleDOI
TL;DR: The effective ionic radii of Shannon & Prewitt [Acta Cryst. (1969), B25, 925-945] are revised to include more unusual oxidation states and coordinations as mentioned in this paper.
Abstract: The effective ionic radii of Shannon & Prewitt [Acta Cryst. (1969), B25, 925-945] are revised to include more unusual oxidation states and coordinations. Revisions are based on new structural data, empirical bond strength-bond length relationships, and plots of (1) radii vs volume, (2) radii vs coordination number, and (3) radii vs oxidation state. Factors which affect radii additivity are polyhedral distortion, partial occupancy of cation sites, covalence, and metallic character. Mean Nb5+-O and Mo6+-O octahedral distances are linearly dependent on distortion. A decrease in cation occupancy increases mean Li+-O, Na+-O, and Ag+-O distances in a predictable manner. Covalence strongly shortens Fe2+-X, Co2+-X, Ni2+-X, Mn2+-X, Cu+-X, Ag+-X, and M-H- bonds as the electronegativity of X or M decreases. Smaller effects are seen for Zn2+-X, Cd2+-X, In2+-X, pb2+-X, and TI+-X. Bonds with delocalized electrons and therefore metallic character, e.g. Sm-S, V-S, and Re-O, are significantly shorter than similar bonds with localized electrons.

51,997 citations

Journal ArticleDOI
TL;DR: Solar energy is by far the largest exploitable resource, providing more energy in 1 hour to the earth than all of the energy consumed by humans in an entire year, and if solar energy is to be a major primary energy source, it must be stored and dispatched on demand to the end user.
Abstract: Global energy consumption is projected to increase, even in the face of substantial declines in energy intensity, at least 2-fold by midcentury relative to the present because of population and economic growth. This demand could be met, in principle, from fossil energy resources, particularly coal. However, the cumulative nature of CO2 emissions in the atmosphere demands that holding atmospheric CO2 levels to even twice their preanthropogenic values by midcentury will require invention, development, and deployment of schemes for carbon-neutral energy production on a scale commensurate with, or larger than, the entire present-day energy supply from all sources combined. Among renewable energy resources, solar energy is by far the largest exploitable resource, providing more energy in 1 hour to the earth than all of the energy consumed by humans in an entire year. In view of the intermittency of insolation, if solar energy is to be a major primary energy source, it must be stored and dispatched on demand to the end user. An especially attractive approach is to store solar-converted energy in the form of chemical bonds, i.e., in a photosynthetic process at a year-round average efficiency significantly higher than current plants or algae, to reduce land-area requirements. Scientific challenges involved with this process include schemes to capture and convert solar energy and then store the energy in the form of chemical bonds, producing oxygen from water and a reduced fuel such as hydrogen, methane, methanol, or other hydrocarbon species.

7,076 citations

Journal ArticleDOI
02 May 2008-Science
TL;DR: Electrical transport measurements, coupled with microstructure studies and modeling, show that the ZT improvement is the result of low thermal conductivity caused by the increased phonon scattering by grain boundaries and defects, which makes these materials useful for cooling and power generation.
Abstract: The dimensionless thermoelectric figure of merit (ZT) in bismuth antimony telluride (BiSbTe) bulk alloys has remained around 1 for more than 50 years. We show that a peak ZT of 1.4 at 100°C can be achieved in a p-type nanocrystalline BiSbTe bulk alloy. These nanocrystalline bulk materials were made by hot pressing nanopowders that were ball-milled from crystalline ingots under inert conditions. Electrical transport measurements, coupled with microstructure studies and modeling, show that the ZT improvement is the result of low thermal conductivity caused by the increased phonon scattering by grain boundaries and defects. More importantly, ZT is about 1.2 at room temperature and 0.8 at 250°C, which makes these materials useful for cooling and power generation. Cooling devices that use these materials have produced high-temperature differences of 86°, 106°, and 119°C with hot-side temperatures set at 50°, 100°, and 150°C, respectively. This discovery sets the stage for use of a new nanocomposite approach in developing high-performance low-cost bulk thermoelectric materials.

4,695 citations

Journal ArticleDOI
20 Sep 2012-Nature
TL;DR: It is shown that heat-carrying phonons with long mean free paths can be scattered by controlling and fine-tuning the mesoscale architecture of nanostructured thermoelectric materials, and an increase in ZT beyond the threshold of 2 highlights the role of, and need for, multiscale hierarchical architecture in controlling phonon scattering in bulk thermoeLECTrics.
Abstract: Controlling the structure of thermoelectric materials on all length scales (atomic, nanoscale and mesoscale) relevant for phonon scattering makes it possible to increase the dimensionless figure of merit to more than two, which could allow for the recovery of a significant fraction of waste heat with which to produce electricity.

3,670 citations