High pressure synthesis of p-type Fe-substituted CoSb3 skutterudites

Liu, Yadi; Li, Xiaohui; Zhang, Qian; Chen, Chen; Li, Jianghua; Zhang, Long; Tian, Yongjun; Xu, Bin

doi:10.1007/s10854-016-4582-6

Cited by 11 publications

(5 citation statements)

References 35 publications

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“…Figure b shows a relative comparison of the reported ZT values for p-type CoSb 3 -based skutterudites, ,,− ,, which suggests that this value of ZT realized in the present study is far higher than those previously reported for p-type CoSb 3 unfilled skutterudites. ,,− ,, To govern the usefulness of the material, the average ZT has also been calculated and the comparison chart with previous reports is shown in Supporting Information (Section 4).…”

Section: Resultssupporting

confidence: 51%

“…19−24 A ZT ∼ 0.2 at 700 K was reported in Fe doped p-type CoSb 3 prepared through encapsulated induction melting, 22 and the nanostructured Fe doped CoSb 3 synthesized by a chemical route resulted in a ZT ∼ 0.25 at 800 K. 20 Further, an enhanced ZT ∼ 0.53 at 823 K was reported by partial substitution of Fe on the Co-site in CoSb 3 , using a microwave assisted synthesis. 25 Moreover, the co-substitutions of Mn and Sn in CoSb 3 yielded a ZT ∼ 0.54 at 723 K, 26 which was the highest reported thus far in p-type doped-CoSb 3 unfilled skutterudites, although much higher values have been reported for their n-type counterparts. 10 Feng et al 24 have recently introduced graphene into the CoSb 3 matrix via a nanocomposite approach and realized an enhanced ZT ∼ 0.61 at 800 K.…”

Section: ■ Introductionmentioning

confidence: 88%

“…The highest reported ZT for pristine CoSb 3 synthesized through nanostructuring and hot pressed compaction is 0.17 at 610 K, , which is quite low due to its unoptimized carrier concentration; however, different approaches have been reported to enhance its ZT, which include doping, nanostructuring, and more recently employing a composite approach. − A ZT ∼ 0.2 at 700 K was reported in Fe doped p-type CoSb 3 prepared through encapsulated induction melting, and the nanostructured Fe doped CoSb 3 synthesized by a chemical route resulted in a ZT ∼ 0.25 at 800 K . Further, an enhanced ZT ∼ 0.53 at 823 K was reported by partial substitution of Fe on the Co-site in CoSb 3 , using a microwave assisted synthesis . Moreover, the co-substitutions of Mn and Sn in CoSb 3 yielded a ZT ∼ 0.54 at 723 K, which was the highest reported thus far in p-type doped-CoSb 3 unfilled skutterudites, although much higher values have been reported for their n-type counterparts .…”

Section: Introductionmentioning

confidence: 99%

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Collective Effect of Fe and Se To Improve the Thermoelectric Performance of Unfilled p-Type CoSb₃ Skutterudites

Bhardwaj

Gahtori

Johari

et al. 2019

ACS Appl. Energy Mater.

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Filled skutterudites constitute an important class of efficient and stable thermoelectric materials for power generation; however, their commercialization has been hampered due to the usage of expensive rare-earth elements as “fillers” and the nonavailability of the efficient and compatible p-type counterpart. In view of this, we report a state-of-the-art thermoelectric figure of merit (ZT) in rare-earth-free p-type unfilled CoSb3 skutterudite co-doped with Fe and Se, synthesized using a facile process of arc-melting and spark plasma sintering, which is both fast and scalable. The doping of Fe and Se have been chosen in accordance with the first-principles-based density functional theory (DFT) calculations which suggested that Fe leads to p-type conduction in CoSb3, while Se strengthens the thermoelectric properties. The experimental results also suggest that the optimized partial substitutional doping of Fe at the Co-site and Se at the Sb-site in CoSb3 leads to a favorable tuning of the electrical and thermal transport properties, which resulted in a high ZT ∼ 0.7 at 870 K in an optimized skutterudite composition of Fe0.25Co0.75Sb2.965Se0.035, which is the highest value reported thus far for unfilled CoSb3-based p-type skutterudites. The resulting ZT of Fe0.25Co0.75Sb2.965Se0.035 is higher by 2 orders of magnitude than that for its pristine counterpart. In addition, the theoretically estimated transport properties of pristine and doped CoSb3, calculated employing the density functional theory (DFT) and Boltzmann transport equations, were found to be in good qualitative agreement with those measured experimentally.

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Section: Resultssupporting

confidence: 51%

Section: ■ Introductionmentioning

confidence: 88%

Section: Introductionmentioning

confidence: 99%

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Collective Effect of Fe and Se To Improve the Thermoelectric Performance of Unfilled p-Type CoSb₃ Skutterudites

Bhardwaj

Gahtori

Johari

et al. 2019

ACS Appl. Energy Mater.

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“…Part of this discrepancy is due to the fact that our DFT calculations provide a description of the materials that is strictly only valid at a temperature of 0 K and pressure of 0 GPa, whereas most experiments are performed at room temperature and pressure. 23,73,74 Another reason for this discrepancy is due to the fact that the reported experimental values are those of partially-filled skutterudites, whereas our compounds are fully-filled.…”

Section: Is Close Tomentioning

confidence: 69%

Thermoelectric Performance of n-type Filled Skutterudites RECo₄Sb₁₂ Using Rare Earths as Filler Atoms (RE=Nd,Sm,Eu,Yb)

BENAOUAD

Meskine²,

Benbedra³

et al. 2023

ECS J. Solid State Sci. Technol.

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In this work, we perform first-principles calculations based on density functional theory and the semi-classical Boltzmann method to study the structural, mechanical, electronic, and thermoelectric properties of rare earths filled skutterudites RECo4Sb12 (RE= Nd,Sm,Eu,Yb). It is found that these compounds are n-type semiconductors with high effective mass and narrow bandgap. The main focus here is to investigate the effect of filler rare earth elements on the thermoelectric response of binary skutterudite CoSb3. In doing so, we compute for each compound the Seebeck coefficient, electrical conductivity, electronic thermal conductivity, and figure of merit in the temperature range from 400 K to 1000 K. The relaxation time and lattice thermal conductivity are calculated as well. Our results reveal that low thermal conductivity and high Seebeck coefficient can be achieved at the same time in RE-filled skutterudites RECo4Sb12, thereby improving their thermoelectric performance which makes them attractive thermoelectric materials at high temperatures.

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“…For example, as a way to increase the filling factors of skutterudites, techniques such as high-pressure sintering (HPS) or high pressure-high temperature (HPHT) using diamond anvil cells (DACs) are shown to be good alternatives. [302,[326][327][328][329][330][331][332][333][334] In some occasions, these methods are also used in combination with non-equilibrium syntheses such as melt spinning R y Co 4 Sb 12 (R = Nd, Sm, Gd, Tb, and Dy with zTs up to 1.3) or super-cooling reaching the same zT for R y Co 4 Sb 12 (R = Ce, Ca, Nd, Sm, Gd, Yb, Dy).…”

Section: Iic Skutteruditesmentioning

confidence: 99%

Thermoelectrics: From history, a window to the future

Beretta

Neophytou

Hodges

et al. 2019

Materials Science and Engineering: R: Reports

428

316

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Thermoelectricity offers a sustainable path to recover and convert waste heat into readily available electric energy, and has been studied for more than two centuries. From the controversy between Galvani and Volta on the Animal Electricity, dating back to the end of the XVIII century and anticipating Seebeck's observations, the understanding of the physical mechanisms evolved along with the development of the technology. In the XIX century Ørsted clarified some of the earliest observations of the thermoelectric phenomenon and proposed the first thermoelectric pile, while it was only after the studies on thermodynamics by Thomson, and Rayleigh's suggestion to exploit the Seebeck effect for power generation, that a diverse set of thermoelectric generators was developed.From such pioneering endeavors, technology evolved from massive, and sometimes unreliable, thermopiles to very reliable devices for sophisticated niche applications in the XX century, when Radioisotope Thermoelectric Generators for space missions and nuclear batteries for cardiac pacemakers were introduced. While some of the materials adopted to realize the first thermoelectric generators are still investigated nowadays, novel concepts and improved understanding of materials growth, processing, and characterization developed during the last 30 years has provided new avenues for the enhancement of the thermoelectric conversion efficiency, for example through nanostructuration, and favored the development of new classes of thermoelectric materials. With

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High pressure synthesis of p-type Fe-substituted CoSb3 skutterudites

Cited by 11 publications

References 35 publications

Collective Effect of Fe and Se To Improve the Thermoelectric Performance of Unfilled p-Type CoSb₃ Skutterudites

Collective Effect of Fe and Se To Improve the Thermoelectric Performance of Unfilled p-Type CoSb₃ Skutterudites

Thermoelectric Performance of n-type Filled Skutterudites RECo₄Sb₁₂ Using Rare Earths as Filler Atoms (RE=Nd,Sm,Eu,Yb)

Thermoelectrics: From history, a window to the future

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High pressure synthesis of p-type Fe-substituted CoSb3 skutterudites

Cited by 11 publications

References 35 publications

Collective Effect of Fe and Se To Improve the Thermoelectric Performance of Unfilled p-Type CoSb3 Skutterudites

Collective Effect of Fe and Se To Improve the Thermoelectric Performance of Unfilled p-Type CoSb3 Skutterudites

Thermoelectric Performance of n-type Filled Skutterudites RECo4Sb12 Using Rare Earths as Filler Atoms (RE=Nd,Sm,Eu,Yb)

Thermoelectrics: From history, a window to the future

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Product

Resources

About

Collective Effect of Fe and Se To Improve the Thermoelectric Performance of Unfilled p-Type CoSb₃ Skutterudites

Collective Effect of Fe and Se To Improve the Thermoelectric Performance of Unfilled p-Type CoSb₃ Skutterudites

Thermoelectric Performance of n-type Filled Skutterudites RECo₄Sb₁₂ Using Rare Earths as Filler Atoms (RE=Nd,Sm,Eu,Yb)