Straightforward route to the adamantane clusters [Sn4Q 10]4- (Q = S, Se, Te) and use in the assembly of open-framework chalcogenides (Me4N)2M[Sn 4Se10] (M = MnII, FeII, Co II, ZnII) including the first telluride member (Me 4N)2Mn[Ge4Te...

Konstantina Tsamourtzi, Jung Hwan Song, Thomas Bakas, Arthur J Freeman, Pantelis N. Trikalitis, Mercouri G Kanatzidis

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Abstract

Title full: Straightforward route to the adamantane clusters [Sn4Q 10]4- (Q = S, Se, Te) and use in the assembly of open-framework chalcogenides (Me4N)2M[Sn 4Se10] (M = MnII, FeII, Co II, ZnII) including the first telluride member (Me 4N)2Mn[Ge4Te10]. The reaction of K2Sn2Q5 (Q = S, Se, Te) with stoichiometric amounts of alkyl-ammonium bromides R4NBr (R = methyl or ethyl) in ethylenediamine (en) afforded the corresponding salts (R4N)4[Sn4Q10] (Q = S, Se, Te) in high yield. Although the compound K2Sn2Te5 is not known, this reaction is also applicable to solids with a nominal composition "K2Sn2Te5" which in the presence of R4NBr in en are quantitatively converted to the salts (R 4N)4[Sn4Te10] on a multigram scale. These salts contain the molecular adamantane clusters [Sn4Q 10]4- and can serve as soluble precursors in simple metathesis reactions with transition metal salts to synthesize the large family of open-framework compounds (Me4N)2M[Sn4Se 10] (M = Mn2+, Fe2+, Co2+, Zn 2+). Full structural characterization of these materials as well as their magnetic and optical properties is reported. Depending on the transition metal in (Me4N)2M[Sn4Se10], the energy band gaps of these compounds lie in the range of 1.27-2.23 eV. (Me 4N)2Mn[Ge4Te10] is the first telluride analogue to be reported in this family. This material is a narrow band gap semiconductor with an optical absorption energy of 0.69 eV. Ab initio electronic band structure calculations validate the semiconductor nature of these chalcogenides and indicate a nearly direct band gap.

Original languageEnglish
Pages (from-to)11920-11929
Number of pages10
JournalInorganic Chemistry
Volume47
Issue number24
DOIs
Publication statusPublished - 2008

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Adamantane
Chalcogenides
ethylenediamine
tellurides
chalcogenides
Salts
assembly
routes
salts
Band structure
Transition metals
Energy gap
transition metals
ammonium bromides
molecular clusters
metathesis
Light absorption
energy bands
narrowband
Magnetic properties

ASJC Scopus subject areas

  • Inorganic Chemistry
  • Physical and Theoretical Chemistry

Cite this

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title = "Straightforward route to the adamantane clusters [Sn4Q 10]4- (Q = S, Se, Te) and use in the assembly of open-framework chalcogenides (Me4N)2M[Sn 4Se10] (M = MnII, FeII, Co II, ZnII) including the first telluride member (Me 4N)2Mn[Ge4Te...",
abstract = "Title full: Straightforward route to the adamantane clusters [Sn4Q 10]4- (Q = S, Se, Te) and use in the assembly of open-framework chalcogenides (Me4N)2M[Sn 4Se10] (M = MnII, FeII, Co II, ZnII) including the first telluride member (Me 4N)2Mn[Ge4Te10]. The reaction of K2Sn2Q5 (Q = S, Se, Te) with stoichiometric amounts of alkyl-ammonium bromides R4NBr (R = methyl or ethyl) in ethylenediamine (en) afforded the corresponding salts (R4N)4[Sn4Q10] (Q = S, Se, Te) in high yield. Although the compound K2Sn2Te5 is not known, this reaction is also applicable to solids with a nominal composition {"}K2Sn2Te5{"} which in the presence of R4NBr in en are quantitatively converted to the salts (R 4N)4[Sn4Te10] on a multigram scale. These salts contain the molecular adamantane clusters [Sn4Q 10]4- and can serve as soluble precursors in simple metathesis reactions with transition metal salts to synthesize the large family of open-framework compounds (Me4N)2M[Sn4Se 10] (M = Mn2+, Fe2+, Co2+, Zn 2+). Full structural characterization of these materials as well as their magnetic and optical properties is reported. Depending on the transition metal in (Me4N)2M[Sn4Se10], the energy band gaps of these compounds lie in the range of 1.27-2.23 eV. (Me 4N)2Mn[Ge4Te10] is the first telluride analogue to be reported in this family. This material is a narrow band gap semiconductor with an optical absorption energy of 0.69 eV. Ab initio electronic band structure calculations validate the semiconductor nature of these chalcogenides and indicate a nearly direct band gap.",
author = "Konstantina Tsamourtzi and Song, {Jung Hwan} and Thomas Bakas and Freeman, {Arthur J} and Trikalitis, {Pantelis N.} and Kanatzidis, {Mercouri G}",
year = "2008",
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language = "English",
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pages = "11920--11929",
journal = "Inorganic Chemistry",
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publisher = "American Chemical Society",
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T1 - Straightforward route to the adamantane clusters [Sn4Q 10]4- (Q = S, Se, Te) and use in the assembly of open-framework chalcogenides (Me4N)2M[Sn 4Se10] (M = MnII, FeII, Co II, ZnII) including the first telluride member (Me 4N)2Mn[Ge4Te...

AU - Tsamourtzi, Konstantina

AU - Song, Jung Hwan

AU - Bakas, Thomas

AU - Freeman, Arthur J

AU - Trikalitis, Pantelis N.

AU - Kanatzidis, Mercouri G

PY - 2008

Y1 - 2008

N2 - Title full: Straightforward route to the adamantane clusters [Sn4Q 10]4- (Q = S, Se, Te) and use in the assembly of open-framework chalcogenides (Me4N)2M[Sn 4Se10] (M = MnII, FeII, Co II, ZnII) including the first telluride member (Me 4N)2Mn[Ge4Te10]. The reaction of K2Sn2Q5 (Q = S, Se, Te) with stoichiometric amounts of alkyl-ammonium bromides R4NBr (R = methyl or ethyl) in ethylenediamine (en) afforded the corresponding salts (R4N)4[Sn4Q10] (Q = S, Se, Te) in high yield. Although the compound K2Sn2Te5 is not known, this reaction is also applicable to solids with a nominal composition "K2Sn2Te5" which in the presence of R4NBr in en are quantitatively converted to the salts (R 4N)4[Sn4Te10] on a multigram scale. These salts contain the molecular adamantane clusters [Sn4Q 10]4- and can serve as soluble precursors in simple metathesis reactions with transition metal salts to synthesize the large family of open-framework compounds (Me4N)2M[Sn4Se 10] (M = Mn2+, Fe2+, Co2+, Zn 2+). Full structural characterization of these materials as well as their magnetic and optical properties is reported. Depending on the transition metal in (Me4N)2M[Sn4Se10], the energy band gaps of these compounds lie in the range of 1.27-2.23 eV. (Me 4N)2Mn[Ge4Te10] is the first telluride analogue to be reported in this family. This material is a narrow band gap semiconductor with an optical absorption energy of 0.69 eV. Ab initio electronic band structure calculations validate the semiconductor nature of these chalcogenides and indicate a nearly direct band gap.

AB - Title full: Straightforward route to the adamantane clusters [Sn4Q 10]4- (Q = S, Se, Te) and use in the assembly of open-framework chalcogenides (Me4N)2M[Sn 4Se10] (M = MnII, FeII, Co II, ZnII) including the first telluride member (Me 4N)2Mn[Ge4Te10]. The reaction of K2Sn2Q5 (Q = S, Se, Te) with stoichiometric amounts of alkyl-ammonium bromides R4NBr (R = methyl or ethyl) in ethylenediamine (en) afforded the corresponding salts (R4N)4[Sn4Q10] (Q = S, Se, Te) in high yield. Although the compound K2Sn2Te5 is not known, this reaction is also applicable to solids with a nominal composition "K2Sn2Te5" which in the presence of R4NBr in en are quantitatively converted to the salts (R 4N)4[Sn4Te10] on a multigram scale. These salts contain the molecular adamantane clusters [Sn4Q 10]4- and can serve as soluble precursors in simple metathesis reactions with transition metal salts to synthesize the large family of open-framework compounds (Me4N)2M[Sn4Se 10] (M = Mn2+, Fe2+, Co2+, Zn 2+). Full structural characterization of these materials as well as their magnetic and optical properties is reported. Depending on the transition metal in (Me4N)2M[Sn4Se10], the energy band gaps of these compounds lie in the range of 1.27-2.23 eV. (Me 4N)2Mn[Ge4Te10] is the first telluride analogue to be reported in this family. This material is a narrow band gap semiconductor with an optical absorption energy of 0.69 eV. Ab initio electronic band structure calculations validate the semiconductor nature of these chalcogenides and indicate a nearly direct band gap.

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