Synthesis, structure, and transport properties of Ba8Cu16 – xAuxP30 clathrate solid solution

Wang, Jian; Voyles, Jackson; Grzybowski, Scott; Kovnir, Kirill

doi:10.1063/1.5134080

Title: Synthesis, structure, and transport properties of Ba₈Cu_{16 – x}Au_xP₃₀ clathrate solid solution

Journal Article · 02 February 2020 · Journal of Applied Physics

DOI: https://doi.org/10.1063/1.5134080 · OSTI ID:1599456

^[1]; Voyles, Jackson ^[2]; Grzybowski, Scott ^[2];

^[1]

Iowa State Univ., Ames, IA (United States); Ames Lab., Ames, IA (United States)
Iowa State Univ., Ames, IA (United States)

In this work, a new clathrate solid solution Ba₈Cu_{16 –}_xAu_xP₃₀ (x = 4, 8, 12) was synthesized by a high-temperature solid-state annealing method. The crystal structures of Ba₈Cu_{16 –}_xAu_xP₃₀ were determined by single crystal x-ray diffraction. This clathrate solid solution crystallizes in the orthorhombic superstructure of clathrate-I type with 23 crystallographically independent framework sites, eight of them are occupied by Au/Cu and 15 are exclusively occupied by P atoms. The distribution of Au and Cu atoms over these eight framework sites is not random with a clear preference for Au to occupy the largest (Au/Cu)P₄ tetrahedra in the framework. The thermal stability and thermoelectric properties of the Ba₈Cu_{16 –}_xAu_xP₃₀ solid solution were evaluated. Low thermal conductivity was achieved for Ba₈Cu_{16 –}_xAu_xP₃₀ due to the combination of the host–guest crystal structure with rattling Ba atoms with the presence of heavy Au atoms and substitutional Cu/Au disorder in the clathrate framework.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division

Grant/Contract Number:: AC02-06CH11357; SC0008931

OSTI ID:: 1599456

Journal Information:: Journal of Applied Physics, Journal Name: Journal of Applied Physics Journal Issue: 5 Vol. 127; ISSN 0021-8979

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: ENGLISH

References (50)

Thermoelectric Materials Owens-Baird, Bryan; Heinrich, Shannon; Kovnir, Kirill Encyclopedia of Inorganic and Bioinorganic Chemistry https://doi.org/10.1002/9781119951438.eibc2497	book	June 2017
High Thermoelectric Performance in PbTe Due to Large Nanoscale Ag2Te Precipitates and La Doping Pei, Yanzhong; Lensch-Falk, Jessica; Toberer, Eric S. Advanced Functional Materials, Vol. 21, Issue 2 https://doi.org/10.1002/adfm.201000878	journal	November 2010
High Thermoelectric Figure of Merit and Nanostructuring in Bulk p-type Na_1−xPb_mSb_yTe_m+2 Poudeu, Pierre F. P.; D'Angelo, Jonathan; Downey, Adam D. Angewandte Chemie, Vol. 118, Issue 23, p. 3919-3923 https://doi.org/10.1002/ange.200600865	journal	June 2006
Breaking the Tetra-Coordinated Framework Rule: New Clathrate Ba ₈ M ₂₄ P _{28+ δ} ( M =Cu/Zn) Dolyniuk, Juli-Anna; Zaikina, Julia V.; Kaseman, Derrick C. Angewandte Chemie, Vol. 129, Issue 9 https://doi.org/10.1002/ange.201611510	journal	January 2017
High Thermoelectric Figure of Merit and Nanostructuring in Bulk p-type Na1−xPbmSbyTem+2 Poudeu, Pierre F. P.; D'Angelo, Jonathan; Downey, Adam D. Angewandte Chemie International Edition, Vol. 45, Issue 23 https://doi.org/10.1002/anie.200600865	journal	June 2006
Breaking the Tetra-Coordinated Framework Rule: New Clathrate Ba ₈ M ₂₄ P _{28+ δ} ( M =Cu/Zn) Dolyniuk, Juli-Anna; Zaikina, Julia V.; Kaseman, Derrick C. Angewandte Chemie International Edition, Vol. 56, Issue 9 https://doi.org/10.1002/anie.201611510	journal	January 2017
Guest–Framework Interaction in Type I Inorganic Clathrates with Promising Thermoelectric Properties: On the Ionic versus Neutral Nature of the Alkaline-Earth Metal Guest A in A8Ga16Ge30 (A=Sr, Ba) Gatti, Carlo; Bertini, Luca; Blake, Nick P. Chemistry - A European Journal, Vol. 9, Issue 18 https://doi.org/10.1002/chem.200304837	journal	September 2003
Guest—Framework Interaction in Type I Inorganic Clathrates with Promising Thermoelectric Properties: On the Ionic versus Neutral Nature of the Alkaline-Earth Metal Guest A in A8Ga16Ge30 (A: Sr, Ba) Gatti, Carlo; Bertini, Luca; Blake, Nick P. ChemInform, Vol. 34, Issue 50 https://doi.org/10.1002/chin.200350002	journal	December 2003
Ba8Cu16P30 - eine neue tern�re Variante des Clathrat I-Strukturtyps D�nner, J.; Mewis, A. Zeitschrift f�r anorganische und allgemeine Chemie, Vol. 621, Issue 2 https://doi.org/10.1002/zaac.19956210205	journal	February 1995
The Smaller the Better: Hosting Trivalent Rare-Earth Guests in Cu–P Clathrate Cages Wang, Jian; He, Yuping; Mordvinova, Natalia E. Chem, Vol. 4, Issue 6 https://doi.org/10.1016/j.chempr.2018.04.001	journal	June 2018
Inhomogeneity and anisotropy of chemical bonding and thermoelectric properties of materials Grin, Yuri Journal of Solid State Chemistry, Vol. 274 https://doi.org/10.1016/j.jssc.2018.12.055	journal	June 2019
Clathrate thermoelectrics Dolyniuk, Juli-Anna; Owens-Baird, Bryan; Wang, Jian Materials Science and Engineering: R: Reports, Vol. 108 https://doi.org/10.1016/j.mser.2016.08.001	journal	October 2016
Unconventional Clathrates with Transition Metal–Phosphorus Frameworks Wang, Jian; Dolyniuk, Juli-Anna; Kovnir, Kirill Accounts of Chemical Research, Vol. 51, Issue 1 https://doi.org/10.1021/acs.accounts.7b00469	journal	December 2017
Twisted Kelvin Cells and Truncated Octahedral Cages in the Crystal Structures of Unconventional Clathrates, AM ₂ P ₄ (A = Sr, Ba; M = Cu, Ni) Dolyniuk, Juli-Anna; Wang, Jian; Lee, Kathleen Chemistry of Materials, Vol. 27, Issue 12 https://doi.org/10.1021/acs.chemmater.5b01592	journal	June 2015
Chemical Bonding and Transport Properties in Clathrates-I with Cu–Zn–P Frameworks Dolyniuk, Juli-Anna; Wang, Jian; Marple, Maxwell A. T. Chemistry of Materials, Vol. 30, Issue 10 https://doi.org/10.1021/acs.chemmater.8b00966	journal	April 2018
Introducing a Magnetic Guest to a Tetrel-Free Clathrate: Synthesis, Structure, and Properties of Eu _x Ba _{8– x} Cu ₁₆ P ₃₀ (0 ≤ x ≤ 1.5) Kovnir, Kirill; Stockert, Ulrike; Budnyk, Sergij Inorganic Chemistry, Vol. 50, Issue 20 https://doi.org/10.1021/ic201474h	journal	October 2011
Neutron Diffraction Study of the Type I Clathrate Ba ₈ Al _x Si _{46– x} : Site Occupancies, Cage Volumes, and the Interaction between the Guest and the Host Framework Roudebush, John H.; de la Cruz, Clarina; Chakoumakos, Bryan C. Inorganic Chemistry, Vol. 51, Issue 3 https://doi.org/10.1021/ic202095e	journal	December 2011
LiPbSb 3 S 6 : A Semiconducting Sulfosalt with Very Low Thermal Conductivity Agha, Eva C.; Malliakas, Christos D.; Im, Jino Inorganic Chemistry, Vol. 53, Issue 2 https://doi.org/10.1021/ic402262z	journal	December 2013
Spinodal Decomposition and Nucleation and Growth as a Means to Bulk Nanostructured Thermoelectrics: Enhanced Performance in Pb _1- _x Sn _x Te−PbS Androulakis, John; Lin, Chia-Her; Kong, Hun-Jin Journal of the American Chemical Society, Vol. 129, Issue 31 https://doi.org/10.1021/ja071875h	journal	August 2007
Probing the Lower Limit of Lattice Thermal Conductivity in an Ordered Extended Solid: Gd ₁₁₇ Co ₅₆ Sn ₁₁₂ , a Phonon Glass–Electron Crystal System Schmitt, Devin C.; Haldolaarachchige, Neel; Xiong, Yimin Journal of the American Chemical Society, Vol. 134, Issue 13 https://doi.org/10.1021/ja300240g	journal	March 2012
Ca _{1– x} RE _x Ag _{1– y} Sb (RE = La, Ce, Pr, Nd, Sm; 0 ≤ x ≤1; 0 ≤ y ≤1): Interesting Structural Transformation and Enhanced High-Temperature Thermoelectric Performance Wang, Jian; Liu, Xiao-Cun; Xia, Sheng-Qing Journal of the American Chemical Society, Vol. 135, Issue 32 https://doi.org/10.1021/ja403653m	journal	July 2013
Clathrate Ba ₈ Au ₁₆ P ₃₀ : The “Gold Standard” for Lattice Thermal Conductivity Fulmer, James; Lebedev, Oleg I.; Roddatis, Vladimir V. Journal of the American Chemical Society, Vol. 135, Issue 33 https://doi.org/10.1021/ja4052679	journal	August 2013
Intricate Short-Range Ordering and Strongly Anisotropic Transport Properties of Li _{1– x} Sn _{2+ x} As ₂ Lee, Kathleen; Kaseman, Derrick; Sen, Sabyasachi Journal of the American Chemical Society, Vol. 137, Issue 10 https://doi.org/10.1021/jacs.5b00237	journal	March 2015
Elusive β-Zn ₈ Sb ₇ : A New Zinc Antimonide Thermoelectric Wang, Jian; Kovnir, Kirill Journal of the American Chemical Society, Vol. 137, Issue 39 https://doi.org/10.1021/jacs.5b08214	journal	September 2015
Convergence of electronic bands for high performance bulk thermoelectrics Pei, Yanzhong; Shi, Xiaoya; LaLonde, Aaron Nature, Vol. 473, Issue 7345, p. 66-69 https://doi.org/10.1038/nature09996	journal	May 2011
Ultralow thermal conductivity and high thermoelectric figure of merit in SnSe crystals Zhao, Li-Dong; Lo, Shih-Han; Zhang, Yongsheng Nature, Vol. 508, Issue 7496, p. 373-377 https://doi.org/10.1038/nature13184	journal	April 2014
Strained endotaxial nanostructures with high thermoelectric figure of merit Biswas, Kanishka; He, Jiaqing; Zhang, Qichun Nature Chemistry, Vol. 3, Issue 2 https://doi.org/10.1038/nchem.955	journal	January 2011
Complex thermoelectric materials Snyder, G. Jeffrey; Toberer, Eric S. Nature Materials, Vol. 7, Issue 2, p. 105-114 https://doi.org/10.1038/nmat2090	journal	February 2008
Better thermoelectrics through glass-like crystals Beekman, Matt; Morelli, Donald T.; Nolas, George S. Nature Materials, Vol. 14, Issue 12 https://doi.org/10.1038/nmat4461	journal	November 2015
Ultra-low thermal conductivity of two-dimensional phononic crystals in the incoherent regime Xie, Guofeng; Ju, Zhifang; Zhou, Kuikui npj Computational Materials, Vol. 4, Issue 1 https://doi.org/10.1038/s41524-018-0076-9	journal	April 2018
Geometric tuning of thermal conductivity in three-dimensional anisotropic phononic crystals Wei, Zhiyong; Wehmeyer, Geoff; Dames, Chris Nanoscale, Vol. 8, Issue 37 https://doi.org/10.1039/C6NR04199J	journal	January 2016
Controlling superstructural ordering in the clathrate-I Ba ₈ M ₁₆ P ₃₀ (M = Cu, Zn) through the formation of metal–metal bonds Dolyniuk, J.; Whitfield, P. S.; Lee, K. Chemical Science, Vol. 8, Issue 5 https://doi.org/10.1039/C7SC00354D	journal	January 2017
High-efficiency thermoelectric Ba ₈ Cu ₁₄ Ge ₆ P ₂₆ : bridging the gap between tetrel-based and tetrel-free clathrates Wang, Jian; Lebedev, Oleg I.; Lee, Kathleen Chemical Science, Vol. 8, Issue 12 https://doi.org/10.1039/C7SC03482B	journal	January 2017
Theoretical chemistry of gold. III Pyykkö, Pekka Chemical Society Reviews, Vol. 37, Issue 9 https://doi.org/10.1039/b708613j	journal	January 2008
Thermoelectric properties of a clathrate compound Ba8Cu16P30 Huo, Dexuan; Sasakawa, Tetsuya; Muro, Yuji Applied Physics Letters, Vol. 82, Issue 16 https://doi.org/10.1063/1.1568819	journal	April 2003
Ag9TlTe5: A high-performance thermoelectric bulk material with extremely low thermal conductivity Kurosaki, Ken; Kosuga, Atsuko; Muta, Hiroaki Applied Physics Letters, Vol. 87, Issue 6 https://doi.org/10.1063/1.2009828	journal	August 2005
Chemical trends of the rattling phonon modes in alloyed germanium clathrates Dong, Jianjun; Sankey, Otto F.; Ramachandran, Ganesh K. Journal of Applied Physics, Vol. 87, Issue 11 https://doi.org/10.1063/1.373447	journal	June 2000
A practical field guide to thermoelectrics: Fundamentals, synthesis, and characterization Zevalkink, Alex; Smiadak, David M.; Blackburn, Jeff L. Applied Physics Reviews, Vol. 5, Issue 2 https://doi.org/10.1063/1.5021094	journal	June 2018
Thermoelectric enhancement in PbTe with K or Na codoping from tuning the interaction of the light- and heavy-hole valence bands Androulakis, John; Todorov, Iliya; Chung, Duck-Young Physical Review B, Vol. 82, Issue 11 https://doi.org/10.1103/PhysRevB.82.115209	journal	September 2010
Intrinsically Minimal Thermal Conductivity in Cubic I−V−VI2 Semiconductors Morelli, D. T.; Jovovic, V.; Heremans, J. P. Physical Review Letters, Vol. 101, Issue 3, Article No. 035901 https://doi.org/10.1103/PhysRevLett.101.035901	journal	July 2008
Phonon-glass electron-crystal thermoelectric clathrates: Experiments and theory Takabatake, Toshiro; Suekuni, Koichiro; Nakayama, Tsuneyoshi Reviews of Modern Physics, Vol. 86, Issue 2 https://doi.org/10.1103/RevModPhys.86.669	journal	June 2014
A short history of SHELX Sheldrick, George M. Acta Crystallographica Section A Foundations of Crystallography, Vol. 64, Issue 1, p. 112-122 https://doi.org/10.1107/S0108767307043930	journal	December 2007
Thermal Barrier Coatings for Gas-Turbine Engine Applications Padture, N. P. Science, Vol. 296, Issue 5566 https://doi.org/10.1126/science.1068609	journal	April 2002
Cooling, Heating, Generating Power, and Recovering Waste Heat with Thermoelectric Systems Bell, L. E. Science, Vol. 321, Issue 5895, p. 1457-1461 https://doi.org/10.1126/science.1158899	journal	September 2008
Enhancement of Thermoelectric Efficiency in PbTe by Distortion of the Electronic Density of States Heremans, J. P.; Jovovic, V.; Toberer, E. S. Science, Vol. 321, Issue 5888, p. 554-557 https://doi.org/10.1126/science.1159725	journal	July 2008
Thermoelectrics Run Hot and Cold Tritt, T. M. Science, Vol. 272, Issue 5266 https://doi.org/10.1126/science.272.5266.1276	journal	May 1996
Thermoelectric Cooling and Power Generation DiSalvo, F. J. Science, Vol. 285, Issue 5428, p. 703-706 https://doi.org/10.1126/science.285.5428.703	journal	July 1999
Complex thermoelectric materials Snyder, G. Jeffrey; Toberer, Eric S. Materials for Sustainable Energy https://doi.org/10.1142/9789814317665_0016	book	October 2010
Thermoelectric enhancement in PbTe with K, Na co-doping from tuning the interaction of the light and heavy hole valence bands Androulakis, John; Todorov, Iliya; Chung, Duck-Young arXiv https://doi.org/10.48550/arxiv.1007.1637	text	January 2010
Phonon-glass electron-crystal thermoelectric clathrates: Experiments and theory Takabatake, Toshiro; Suekuni, Koichiro; Nakayama, Tsuneyoshi arXiv https://doi.org/10.48550/arxiv.1402.5756	text	January 2014

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