Size-Driven Stability of Lanthanide Thiophosphates Grown from an Iodide Flux

Klepov, Vladislav V.; Breton, Logan S.; Pace, Kristen A.; Kocevski, Vancho; Besmann, Theodore M.; zur Loye, Hans-Conrad

doi:10.1021/acs.inorgchem.9b00806

Title: Size-Driven Stability of Lanthanide Thiophosphates Grown from an Iodide Flux

Journal Article · Tue Apr 23 00:00:00 EDT 2019 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.9b00806· OSTI ID:1527338

^[1]; Breton, Logan S. ^[1]; Pace, Kristen A. ^[1];

^[2]; Besmann, Theodore M. ^[2];

^[1]

Univ. of South Carolina, Columbia, SC (United States). Dept. of Chemistry and Biochemistry
Univ. of South Carolina, Columbia, SC (United States). Dept. of Mechanical Engineering

To determine the influence of the lanthanide size on the structures and properties of thiophosphates, a thiophosphate series containing different lanthanides was synthesized via high temperature flux crystal growth and their structures and physical properties analyzed and compared. Layered thiohypophosphates NaLnP2S6 (Ln = La, Ce, Pr) and thiopyrophosphates CsLnP2S7 (Ln = Pr, Nd, Sm, Gd, Tb, Dy, Ho, Er, Yb, Y) were grown out of an iodide flux using consistent reaction conditions across both series. Under the mildly reducing iodide flux reaction conditions a rather rare example of phosphorus reduction from the +5 to the +4 oxidation state was observed. Both resultant structure types are based on lanthanide thiophosphate sheets with the alkali cations located between them. Magnetic susceptibility measurements were conducted and revealed Curie-Weiss behavior of the samples, with a Van Vleck contribution in the CsSmP2S7 sample. UV-Vis data was found to be in good agreement with the literature, indicating little influence of the sulfide environment on the localized 4f orbitals.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Hierarchical Waste Form Materials (CHWM); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Univ. of South Carolina, Columbia, SC (United States)

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

Grant/Contract Number:: SC0018739; SC0016575; SC0016574

OSTI ID:: 1527338

Alternate ID(s):: OSTI ID: 1605400; OSTI ID: 1775438

Journal Information:: Inorganic Chemistry, Vol. 58, Issue 9; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 15 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Fluxes
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Lanthanides
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CSD 1891155: Experimental Crystal Structure Determination Klepov, Vladislav V.; Breton, Logan S.; Pace, Kristen A. https://doi.org/10.25505/fiz.icsd.cc21gx0g The current record is supplemented by this dataset	dataset	January 2019
CSD 1891156: Experimental Crystal Structure Determination Klepov, Vladislav V.; Breton, Logan S.; Pace, Kristen A. https://doi.org/10.25505/fiz.icsd.cc21gx1h The current record is supplemented by this dataset	dataset	January 2019
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CSD 1891159: Experimental Crystal Structure Determination Klepov, Vladislav V.; Breton, Logan S.; Pace, Kristen A. https://doi.org/10.25505/fiz.icsd.cc21gx4l The current record is supplemented by this dataset	dataset	January 2019
CSD 1891160: Experimental Crystal Structure Determination Klepov, Vladislav V.; Breton, Logan S.; Pace, Kristen A. https://doi.org/10.25505/fiz.icsd.cc21gx5m The current record is supplemented by this dataset	dataset	January 2019
CSD 1891161: Experimental Crystal Structure Determination Klepov, Vladislav V.; Breton, Logan S.; Pace, Kristen A. https://doi.org/10.25505/fiz.icsd.cc21gx6n The current record is supplemented by this dataset	dataset	January 2019
CSD 1891162: Experimental Crystal Structure Determination Klepov, Vladislav V.; Breton, Logan S.; Pace, Kristen A. https://doi.org/10.25505/fiz.icsd.cc21gx7p The current record is supplemented by this dataset	dataset	January 2019
CSD 1891163: Experimental Crystal Structure Determination Klepov, Vladislav V.; Breton, Logan S.; Pace, Kristen A. https://doi.org/10.25505/fiz.icsd.cc21gx8q The current record is supplemented by this dataset	dataset	January 2019
CSD 1891164: Experimental Crystal Structure Determination Klepov, Vladislav V.; Breton, Logan S.; Pace, Kristen A. https://doi.org/10.25505/fiz.icsd.cc21gx9r The current record is supplemented by this dataset	dataset	January 2019
CSD 1891165: Experimental Crystal Structure Determination Klepov, Vladislav V.; Breton, Logan S.; Pace, Kristen A. https://doi.org/10.25505/fiz.icsd.cc21gxbs The current record is supplemented by this dataset	dataset	January 2019
CSD 1891166: Experimental Crystal Structure Determination Klepov, Vladislav V.; Breton, Logan S.; Pace, Kristen A. https://doi.org/10.25505/fiz.icsd.cc21gxct The current record is supplemented by this dataset	dataset	January 2019

Title: Size-Driven Stability of Lanthanide Thiophosphates Grown from an Iodide Flux

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