High thermoelectric efficiency in lanthanum doped Yb14MnSb11

Toberer, Eric S.; Brown, Shawna R.; Ikeda, Teruyuki; Kauzlarich, Susan M.; Snyder, G. Jeffrey

doi:10.1063/1.2970089

Cited by 119 publications

(127 citation statements)

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“…High thermoelectric efficiency has been demonstrated in a number of Zintl compounds (CsBi 4 Te 6 , Yb 14 MnSb 11 , Ca 3 AlSb 3 , AZn 2 Sb 2 ). [4][5][6][7][8][9][10][11] One promising new Zintl compound is Ca 5 Al 2 Sb 6 , which shows a peak zT of 0.6 at 1000 K with Na 1þ doping on the Ca 2þ site. 13 A prior investigation revealed Ca 5 Al 2 Sb 6 to be a narrow band-gap semiconductor (0.5 eV) with exceptionally low lattice thermal conductivity (0.6 W m À1 K À1 at 800 K).…”

Section: Introductionmentioning

confidence: 99%

Improved carrier concentration control in Zn-doped Ca5Al2Sb6

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Toberer

Bleith

et al. 2011

Journal of Applied Physics

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Ca 5 Al 2 Sb 6 is an inexpensive, Earth-abundant compound that exhibits promising thermoelectric efficiency at temperatures suitable for waste heat recovery. Inspired by our previous study of p-type Ca 5Àx Na x Al 2 Sb 6 , this work investigates doping with Zn 2þ on the Al 3þ site (Ca 5 Al 2Àx Zn x Sb 6 ). We find Zn to be an effective p-type dopant, in contrast to the low solubility limit and poor doping efficiency of Na. Seebeck coefficient measurements indicate that the hole band mass is unaffected by the dopant type in the high-zT temperature range. Band structure and density of states calculations are employed in order to understand the carrier concentration-dependent effective mass. Ca 5 Al 2Àx Zn x Sb 6 has a low lattice thermal conductivity that approaches the predicted minimum value at high temperature (1000 K) due to the complex crystal structure and high mass contrast.

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Section: Introductionmentioning

confidence: 99%

Improved carrier concentration control in Zn-doped Ca5Al2Sb6

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Toberer

Bleith

et al. 2011

Journal of Applied Physics

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“…While the carrier concentration of Yb 9 Mn 4.2 Sb 9 is very close to the optimal value, samples with Zn have carrier concentrations that are far too large. However, the possibility of reducing the carrier concentration of Zn-containing samples by doping with an n-type dopant, 16,18 higher zT than that of the Mn analogue could potentially be realized in future work.…”

Section: Varying Interstitial Zn Contentmentioning

confidence: 99%

“…5,6 They oen have very low lattice thermal conductivity due to their large unit cells, and it is possible to nely tune their electronic properties by doping, providing a route to improved zT. High thermoelectric efficiency has been demonstrated in a number of different Zintl compounds [7][8][9][10][11][12][13][14][15][16][17] including Yb 14 MnSb 11 (ref. 16 and 18) and YbCd 2Àx Zn x Sb 2 , both of which have zT values above unity at high temperatures.…”

Section: Introductionmentioning

confidence: 99%

Thermoelectric properties of the Yb₉Mn_4.2−xZn_xSb₉solid solutions

et al. 2014

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a Yb 9 Mn 4.2 Sb 9 has been shown to have extremely low thermal conductivity and a high thermoelectric figure of merit attributed to its complex crystal structure and disordered interstitial sites. Motivated by previous work which shows that isoelectronic substitution of Mn by Zn leads to higher mobility by reducing spin disorder scattering, this study investigates the thermoelectric properties of the solid solution, Yb 9 Mn 4.2Àx Zn x Sb 9 (x ¼ 0, 1, 2, 3 and 4.2). Measurements of the Hall mobility at high temperatures (up to 1000 K) show that the mobility can be increased by more than a factor of 3 by substituting Zn into Mn sites. This increase is explained by the reduction of the valence band effective mass with increasing Zn, leading to a slightly improved thermoelectric quality factor relative to Yb 9 Mn 4.2 Sb 9 . However, increasing the Zn-content also increases the p-type carrier concentration, leading to metallic behavior with low Seebeck coefficients and high electrical conductivity. Varying the filling of the interstitial site in Yb 9 Zn 4+y Sb 9 (y ¼ 0.2, 0.3, 0.4 and 0.5) was attempted, but the carrier concentration ($10 21 cm À3 at 300 K) and Seebeck coefficients remained constant, suggesting that the phase width of Yb 9 Zn 4+y Sb 9 is quite narrow.

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“…12 The previous work on the La and Tm solid solutions shows that only a limited amount of rare earth can be substituted in the system. 12,18,19 Ce was chosen to substitute for Yb because it will likely substitute as Ce 3+ , which has an unpaired 4 f 1 electron and commonly participates in Kondo interactions. Ce substitution is expected to increase the magnetic moment of the Yb 14 MnSb 11 , partially not only due to unpaired f electron associated with Ce 3+ but also by reducing the screening of Mn moments due to the additional electron introduced by Ce substitution occupying the tetrahedron's associated hole.…”

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Magnetic and structural effects of partial Ce substitution in Y b14MnSb11

Grebenkemper

Kauzlarich

2015

APL Materials

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Single crystals of Y b14−xCexMnSb11 were grown from tin metal as a flux solvent with a maximum Ce incorporation of 0.6. The phases with x ∼ 0.1–0.6 crystallize in the tetragonal Ca14AlSb11 structure type with I41/acd space group. In this structure type, there are 4 crystallographically unique Yb sites and the structure can be described according to the Zintl concept as containing 14Y b2+ + [MnSb4]9− + [Sb3]7− + 4Sb3−. For x > 0.3, Ce is incorporated on specific Yb sites in the structure as a function of x, initially at x = 0.3 on the Yb(2) site followed by Yb(4) at higher values of x. These sites have the largest volume as indicated by Hirshfeld surface analysis of chemical bonding. As Ce content is increased, the ferromagnetic ordering temperatures decrease and effective paramagnetic moments increase. The magnetic ordering temperatures decrease from the undoped TC of 50 K until x ∼ 0.4, where the lowest TC of 39 K is reached. As the additional electron introduced by Ce3+ fills the hole associated with [MnSb4]9−, the screening of the Mn moments is reduced. This leads to an increase in overall moment attributed to Mn in addition to the moment from the Ce3+ f electron. Increasing Ce content also leads to an increase in electrical resistivity, an expected effect from reducing the carrier concentration.

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High thermoelectric efficiency in lanthanum doped Yb14MnSb11

Cited by 119 publications

References 12 publications

Improved carrier concentration control in Zn-doped Ca5Al2Sb6

Improved carrier concentration control in Zn-doped Ca5Al2Sb6

Thermoelectric properties of the Yb₉Mn_4.2−xZn_xSb₉solid solutions

Magnetic and structural effects of partial Ce substitution in Y b14MnSb11

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High thermoelectric efficiency in lanthanum doped Yb14MnSb11

Cited by 119 publications

References 12 publications

Improved carrier concentration control in Zn-doped Ca5Al2Sb6

Improved carrier concentration control in Zn-doped Ca5Al2Sb6

Thermoelectric properties of the Yb9Mn4.2−xZnxSb9solid solutions

Magnetic and structural effects of partial Ce substitution in Y b14MnSb11

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Thermoelectric properties of the Yb₉Mn_4.2−xZn_xSb₉solid solutions