On the Effects of Aliovalent Substitutions in Thermoelectric Zintl Pnictides. Varied Polyanionic Dimensionality and Complex Structural Transformations–The Case of Sr3ZnP3 vs Sr3AlxZn1–xP3

Baranets, Sviatoslav; Balvanz, Adam; Darone, Gregory M.; Bobev, Svilen

doi:10.1021/acs.chemmater.2c00527

Title: On the Effects of Aliovalent Substitutions in Thermoelectric Zintl Pnictides. Varied Polyanionic Dimensionality and Complex Structural Transformations–The Case of Sr₃ZnP₃ vs Sr₃Al_xZn_1–xP₃

Journal Article · Wed Apr 20 00:00:00 EDT 2022 · Chemistry of Materials

DOI:https://doi.org/10.1021/acs.chemmater.2c00527· OSTI ID:1876199

^[1]; Balvanz, Adam ^[2]; Darone, Gregory M. ^[3];

^[1]

Univ. of Delaware, Newark, DE (United States)
Univ. of Delaware, Newark, DE (United States); Northwestern Univ., Evanston, IL (United States)
Univ. of Delaware, Newark, DE (United States); The Charter School of Wilmington, DE (United States)

The structures and the transport properties of a novel family of Zintl phosphides and arsenides with the formula AE₃ZnPn₃ and the solid solutions AE₃Al_xZn_1–xPn₃, AE₃ZnAs_yP_1–y (AE = Sr, Eu; Pn = P, As) are reported. Crystals of nine new phases have been obtained via Pb-flux reactions and used for structural work by means of single-crystal X-ray diffraction methods. The derived orthorhombic structure is without a direct analog, and features unusual structural units, where the Zn atoms are in both distorted tetrahedral and trigonal-planar coordination of pnictogens. Electronic structure calculations reveal moderately wide bandgaps for Sr₃ZnP₃ and Sr₃ZnAs₃, on the order of 0.70 and 0.63 eV, respectively. Electrical transport measurements above room temperature indicate relatively high resistivity values above 500 K (ρ ≈ 4.8 Ω cm and above), but some of the samples exhibit very high Seebeck coefficients, as large as 300 μV/K at 560 K for Sr₃ZnAs₃. Aliovalent substitutions in AE₃ZnPn₃, achieved by the partial replacement of Zn²⁺ with Al³⁺ cations promote occupational and positional disorder, which causes structural transformation towards the disordered variant of the Sr₅Al₂Sb₆ structure type. Such substitutions also change the dimensionality of the polyanionic sub-lattice in the resulting quaternary AE₃Al_xZn_1–xPn₃ phases. Furthermore, preliminary transport property data on the latter reveal nine times lower electrical resistivity (ρ₅₀₀ ≈ 0.5 Ω cm) together with a significantly enhanced Seebeck coefficient, αmax ≈ 430 μV/K at 560 K.

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Research Organization:: Univ. of Delaware, Newark, DE (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0008885

OSTI ID:: 1876199

Journal Information:: Chemistry of Materials, Vol. 34, Issue 9; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Chemical structure
Crystal structure
Crystals
Diseases and disorders
Pnictides

CSD 2151580: Experimental Crystal Structure Determination Sviatoslav, Baranets,; Adam, Balvanz,; M., Darone, Gregory https://doi.org/10.25505/fiz.icsd.cc2b6wt8 The current record is supplemented by this dataset	dataset	January 2022
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Title: On the Effects of Aliovalent Substitutions in Thermoelectric Zintl Pnictides. Varied Polyanionic Dimensionality and Complex Structural Transformations–The Case of Sr3ZnP3 vs Sr3AlxZn1–xP3

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Title: On the Effects of Aliovalent Substitutions in Thermoelectric Zintl Pnictides. Varied Polyanionic Dimensionality and Complex Structural Transformations–The Case of Sr₃ZnP₃ vs Sr₃Al_xZn_1–xP₃