On the Extended Series of Quaternary Zintl Phases Ca13REMnSb11 (RE = La–Nd, Sm, Gd–Dy)

Prakash, Jai; Stoyko, Stanislav; Voss, Leonard; Bobev, Svilen

doi:10.1002/ejic.201600306

Title: On the Extended Series of Quaternary Zintl Phases Ca13REMnSb11 (RE = La–Nd, Sm, Gd–Dy)

Abstract

Eight new compounds with a general formula Ca _14– _x RE _x MnSb ₁₁ ( RE = La–Nd, Sm, Gd–Dy; x ≈ 1) were synthesized by the molten flux method and their structures were established via single‐crystal X‐ray diffraction. The overarching goal of this study was to investigate the effect of electron doping, via substitution of RE ³⁺ at Ca ²⁺ sites, on the crystal structure and physical properties of Ca ₁₄ MnSb ₁₁ , which is a candidate for thermoelectric applications. All studied phases are isostructural, and crystallize in the tetragonal body‐centered space group I 4 ₁ / acd (Ca ₁₄ AlSb ₁₁ structure type, Pearson index tI 208). The structure is made up of MnSb ₄ ^10– tetrahedra, randomly mixed Ca ²⁺ and RE ³⁺ cations, Sb ^3– anions, and linear Sb ₃ ^7– polyanions. Comprehensive structural work confirms high rare‐earth metal content with Ca ²⁺ / RE ³⁺ randomly mixed on all four cation sites, with the caveat that the larger RE atoms (La–Nd) prefer to occupy the Ca2 site, while the smaller RE atoms (Sm, Gd, Tb, and Dy) preferably occupy the Ca1 site. Nearly phase‐pure polycrystalline samples have been synthesized using solid‐state reactions, and havemore »« less

Authors:

Prakash, Jai ^[1]; Stoyko, Stanislav ^[1]; Voss, Leonard ^[1];

^[1]

Department of Chemistry and Biochemistry University of Delaware 19716 Newark DE USA

Publication Date:: Wed May 18 00:00:00 EDT 2016

Sponsoring Org.:: USDOE

OSTI Identifier:: 1400459

Resource Type:: Publisher's Accepted Manuscript

Journal Name:: European Journal of Inorganic Chemistry

Additional Journal Information:: Journal Name: European Journal of Inorganic Chemistry Journal Volume: 2016 Journal Issue: 18; Journal ID: ISSN 1434-1948

Publisher:: Wiley Blackwell (John Wiley & Sons)

Country of Publication:: Germany

Language:: English

Citation Formats


                    Prakash, Jai, Stoyko, Stanislav, Voss, Leonard, and Bobev, Svilen. On the Extended Series of Quaternary Zintl Phases Ca13REMnSb11 (RE = La–Nd, Sm, Gd–Dy).  Germany: N. p., 2016. 
Web.  doi:10.1002/ejic.201600306.

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                    Prakash, Jai, Stoyko, Stanislav, Voss, Leonard, & Bobev, Svilen. On the Extended Series of Quaternary Zintl Phases Ca13REMnSb11 (RE = La–Nd, Sm, Gd–Dy).  Germany.  https://doi.org/10.1002/ejic.201600306

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                    Prakash, Jai, Stoyko, Stanislav, Voss, Leonard, and Bobev, Svilen. Wed .  
"On the Extended Series of Quaternary Zintl Phases Ca13REMnSb11 (RE = La–Nd, Sm, Gd–Dy)".  Germany.  https://doi.org/10.1002/ejic.201600306.

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@article{osti_1400459,

  title        = {On the Extended Series of Quaternary Zintl Phases Ca13REMnSb11 (RE = La–Nd, Sm, Gd–Dy)},

  author       = {Prakash, Jai and Stoyko, Stanislav and Voss, Leonard and Bobev, Svilen},

  abstractNote = {Eight new compounds with a general formula Ca 14– x RE x MnSb 11 ( RE = La–Nd, Sm, Gd–Dy; x ≈ 1) were synthesized by the molten flux method and their structures were established via single‐crystal X‐ray diffraction. The overarching goal of this study was to investigate the effect of electron doping, via substitution of RE 3+ at Ca 2+ sites, on the crystal structure and physical properties of Ca 14 MnSb 11 , which is a candidate for thermoelectric applications. All studied phases are isostructural, and crystallize in the tetragonal body‐centered space group I 4 1 / acd (Ca 14 AlSb 11 structure type, Pearson index tI 208). The structure is made up of MnSb 4 10– tetrahedra, randomly mixed Ca 2+ and RE 3+ cations, Sb 3– anions, and linear Sb 3 7– polyanions. Comprehensive structural work confirms high rare‐earth metal content with Ca 2+ / RE 3+ randomly mixed on all four cation sites, with the caveat that the larger RE atoms (La–Nd) prefer to occupy the Ca2 site, while the smaller RE atoms (Sm, Gd, Tb, and Dy) preferably occupy the Ca1 site. Nearly phase‐pure polycrystalline samples have been synthesized using solid‐state reactions, and have been used for physical property measurements. The resistivities of the bulk Ca 14– x RE x MnSb 11 ( RE = La–Nd, Sm, Gd; x ≈ 1) samples reveal semiconducting behavior, consistent with the notion of electron doping in the parent p ‐type Ca 14 MnSb 11 material. Magnetic susceptibilities suggest complex magnetic ordering at temperatures below ca. 50 K, likely originating from coupling between two or more magnetic sub‐lattices.},

  doi          = {10.1002/ejic.201600306},

  journal      = {European Journal of Inorganic Chemistry},

  number       = 18,

  volume       = 2016,

  place        = {Germany},

  year         = {Wed May 18 00:00:00 EDT 2016},

  month        = {Wed May 18 00:00:00 EDT 2016}

}

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Title: On the Extended Series of Quaternary Zintl Phases Ca13REMnSb11 (RE = La–Nd, Sm, Gd–Dy)

Abstract

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Optical Study of Interactions in a $d$ -Electron Kondo Lattice with Ferromagnetism
journal, July 2005

Structure, Magnetism, and Magnetoresistance of the Compounds Eu ₁₄ MnAs ₁₁ and Eu ₁₄ MnP ₁₁
journal, April 2001

Super-Paramagnetic Blocking Phenomena and Room-Temperature Ferromagnetism in Wide Band-Gap Dilute Magnetic Semiconductor (Ga, Mn)N
journal, July 2007

High-temperature thermoelectric studies of A11Sb10 (A=Yb, Ca)
journal, April 2007

High Temperature Thermoelectric Properties of Yb ₁₄ MnSb ₁₁ Prepared from Reaction of MnSb with the Elements
journal, August 2015

The Crystal Structure and Magnetic Properties of a New Ferrimagnetic Semiconductor: Ca ₂₁ Mn ₄ Sb ₁₈
journal, March 2003

Structure, Heat Capacity, and High-Temperature Thermal Properties of Yb ₁₄ Mn _{1− x} Al _x Sb ₁₁
journal, April 2009

Exploring the Limits of the Zintl Concept for the A14MPn11 Structure Type with M = Zn, Cd
journal, January 1995

A short history of SHELX
journal, December 2007

Structure, Magnetism, and Colossal Magnetoresistance (CMR) of the Ternary Transition Metal Solid Solution Ca ₁₄ _- _x Eu _x MnSb ₁₁ (0 < x < 14)
journal, August 2002

Effect of Ca Doping on the Thermoelectric Performance of Yb14MnSb11
journal, August 2010

XMCD Characterization of the Ferromagnetic State of Yb ₁₄ MnSb ₁₁
journal, August 2002

A Novel Ferromagnet: Ca _l4 MnBi ₁₁
journal, April 1990

Revised effective ionic radii and systematic studies of interatomic distances in halides and chalcogenides
journal, September 1976

X-ray photoelectron spectroscopy studies of Yb14MnSb11 and Yb14ZnSb11
journal, January 2005

Bonding, moment formation, and magnetic interactions in ${Ca}_{14} {MnBi}_{11}$ and ${Ba}_{14} {MnBi}_{11}$
journal, March 2002

Darstellung und Struktur der Verbindung Ca14AlSb11
journal, December 1984

Effects of Sc and Y substitution on the structure and thermoelectric properties of Yb14MnSb11
journal, October 2016

Traversing the Metal-Insulator Transition in a Zintl Phase: Rational Enhancement of Thermoelectric Efficiency in Yb ₁₄ Mn _{1− x} Al _x Sb ₁₁
journal, September 2008

Effective Field Theories of Magnetism
journal, August 1966

Indirect exchange interaction in semiconductors
journal, July 1980

Zintl Phases: Transitions between Metallic and Ionic Bonding
journal, September 1973

Structure, Magnetism, and Magnetoresistance of the Rare-Earth Transition Metal Compounds Eu ₁₃ AMnSb ₁₁ (A = Ca, Sr, Ba, and Yb)
journal, May 2002

Structural analysis of the phase separation in magnetic semiconductor (Zn, Cr)Te
journal, August 2012

Colossal Magnetoresistance in the Transition-Metal Zintl Compound Eu ₁₄ MnSb ₁₁
journal, December 1997

Preparation and thermoelectric properties of polycrystalline nonstoichiometric Yb14MnSb11 Zintl compounds
journal, June 2010

Improved Thermoelectric Performance in Yb ₁₄ Mn _{1− x} Zn _x Sb ₁₁ by the Reduction of Spin-Disorder Scattering
journal, May 2008

Interplay between Size and Electronic Effects in Determining the Homogeneity Range of the A ₉ Zn ₄₊ _x Pn ₉ and A ₉ Cd ₄₊ _x Pn ₉ Phases (0 ≤ x ≤ 0.5), A = Ca, Sr, Yb, Eu; Pn = Sb, Bi
journal, August 2007

Zintl-Phasen: Übergangsformen zwischen Metall- und Ionenbindung
journal, September 1973

STRUCTURE TIDY – a computer program to standardize crystal structure data
journal, April 1987

Yb14−xTmxMnSb11 (0<x<0.5): Structure and magnetic properties
journal, March 2014

Non-stoichiometric compositions arising from synergistic electronic and size effects. Synthesis, crystal chemistry and electronic properties of A ₁₄ Cd _1+x Pn ₁₁ compounds (0 ≤ x ≤ 0.3; A = Sr, Eu; Pn = As, Sb)
journal, January 2015

High thermoelectric efficiency in lanthanum doped Yb14MnSb11
journal, August 2008

The Zintl-Klemm Concept - A Historical Survey: The Zintl-Klemm Concept - A Historical Survey
journal, November 2014

Yb ₁₄ MnSb ₁₁ : New High Efficiency Thermoelectric Material for Power Generation
journal, April 2006

Magnetic and structural effects of partial Ce substitution in Y b ₁₄ MnSb ₁₁
journal, April 2015

Structure and properties of the transition-metal Zintl compounds A14MnPn11 (A = Ca, Sr, Ba; Pn = As, Sb)
journal, January 1994

Yb ₁₄ MgSb ₁₁ and Ca ₁₄ MgSb ₁₁ —New Mg-Containing Zintl Compounds and Their Structures, Bonding, and Thermoelectric Properties
journal, December 2014

Improved Thermoelectric Properties in Lu-doped Yb$_{14}$MnSb$_{11}$ Zintl Compounds
journal, February 2012

Kondo lattice behavior in the ordered dilute magnetic semiconductor ${Yb}_{14 - x} {La}_{x} {MnSb}_{11}$
journal, November 2005