Functionalized Organotin-Chalcogenide Complexes That Exhibit Defect Heterocubane Scaffolds: Formation, Synthesis, and Characterization

被引：34

作者：

Eussner, Jens P. ^{[1
,2
]}

Barth, Beatrix E. K. ^{[1
,2
]}

Leusmann, Eliza ^{[1
,2
]}

You, Zhiliang ^{[1
,2
]}

Rinn, Niklas ^{[1
,2
]}

Dehnen, Stefanie ^{[1
,2
]}

机构：

[1] Univ Marburg, Fachbereich Chem, D-35043 Marburg, Germany

[2] Univ Marburg, WZMW, D-35043 Marburg, Germany

来源：

CHEMISTRY-A EUROPEAN JOURNAL | 2013年 / 19卷 / 41期

关键词：

chalcogens; NMR spectroscopy; organic-inorganic hybrid composites; tin; X-ray diffraction; RAY STRUCTURAL-ANALYSIS; BASIS-SETS; BOND FORMATION; REACTIVITY; CHEMISTRY; SALTS; TRANSFORMATION; MOLECULES; FRAMEWORK; REDUCTION;

D O I：

10.1002/chem.201301521

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

The synthesis of new functionalized organotin-chalcogenide complexes was achieved by systematic optimization of the reaction conditions. The structures of compounds [((RSn)-Sn-1,2)(3)S4Cl] (1, 2), [(((RSn)-Sn-2)(2)SnS4)(2)(-S)(2)] (3), [((RSn)-Sn-1,2)(3)Se-4][SnCl3] (4, 5), and [Li(thf)(n)][((RSn)-Sn-3)((HRSn)-Sn-3)(2)Se4Cl] (6), in which R-1=CMe2CH2C(O)Me, R-2=CMe2CH2C(NNH2)Me, and R-3=CH2CH2COO, are based on defect heterocubane scaffolds, as shown by X-ray diffraction, (SnNMR)-Sn-119 spectroscopy, and ESI mass spectrometry analyses. Compounds 4, 5, and 6 constitute the first examples of defect heterocubane-type metal-chalcogenide complexes that are comprised of selenide ligands. Comprehensive DFT calculations prompted us to search for the formal intermediates [((RSnCl2)-Sn-1)(2)(-S)] (7) and [((RSnCl)-Sn-1)(2)(-S)(2)] (8), which were isolated and helped to understand the stepwise formation of compounds 1-6.

引用

页码：13792 / 13802

页数：11

共 67 条

[1] Contracted all-electron Gaussian basis sets for atoms Rb to Xe [J].

Ahlrichs, R ;

May, K .

PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2000, 2 (05) :943-945

[2]

[Anonymous], ANGEW CHEM

[3]

[Anonymous], ANGEW CHEM

[4] Relativistic DFT calculation of 119Sn chemical shifts and coupling constants in tin compounds [J].

Bagno, A ;

Casella, G ;

Saielli, G .

JOURNAL OF CHEMICAL THEORY AND COMPUTATION, 2006, 2 (01) :37-46

[5] DENSITY-FUNCTIONAL EXCHANGE-ENERGY APPROXIMATION WITH CORRECT ASYMPTOTIC-BEHAVIOR [J].

BECKE, AD .

PHYSICAL REVIEW A, 1988, 38 (06) :3098-3100

[6] Hypercoordinated organotin compounds containing sulfur and chlorine.: Molecular structures of [(Ph3P)2N]+[S(SnR2Cl)2Cl]- (R =Me, t-Bu) [J].

Beckmann, J ;

Dakternieks, D ;

Duthie, A ;

Jones, C ;

Jurkschat, K ;

Tiekink, ERT .

JOURNAL OF ORGANOMETALLIC CHEMISTRY, 2001, 636 (1-2) :138-143

[7] MOLECULAR AND CRYSTAL-STRUCTURES OF TETRA(METHYLGERMANIUM) HEXASULFIDE [J].

BENNO, RH ;

FRITCHIE, CJ .

JOURNAL OF THE CHEMICAL SOCIETY-DALTON TRANSACTIONS, 1973, (05) :543-546

[8] THIASTANNACYCLOHEXANES (R2SNS)3 AND ADAMANTANES (RSN)4S6 - SYNTHESES, PROPERTIES, AND STRUCTURES [J].

BERWE, H ;

HAAS, A .

CHEMISCHE BERICHTE-RECUEIL, 1987, 120 (07) :1175-1182

[9] Mixed Organotin(IV) Chalcogenides: From Molecules to Sn-S-Se Semiconducting Thin Films Deposited by Spin-Coating [J].

Bouska, Marek ;

Strizik, Lukas ;

Dostal, Libor ;

Ruzicka, Ales ;

Lycka, Antonin ;

Benes, Ludvik ;

Vlcek, Milan ;

Prikryl, Jan ;

Knotek, Petr ;

Wagner, Tomas ;

Jambor, Roman .

CHEMISTRY-A EUROPEAN JOURNAL, 2013, 19 (06) :1877-1881

[10] Intramolecularly Coordinated Organotin Tellurides: Stable or Unstable? [J].

Bouska, Marek ;

Dostal, Libor ;

Padelkova, Zdenka ;

Lycka, Antonin ;

Herres-Pawlis, Sonja ;

Jurkschat, Klaus ;

Jambor, Roman .

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2012, 51 (14) :3478-3482

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