Synthesis and Isolation of [Fe@Ge10]3−: A Pentagonal Prismatic Zintl Ion Cage Encapsulating an Interstitial Iron Atom

Author:

Zhou Binbin1,Denning Mark S.1,Kays Deborah L.1,Goicoechea Jose M.1

Affiliation:

1. Department of Chemistry, Chemistry Research Laboratory, University of Oxford, Mansfield Road, Oxford OX1 3TA, U.K., and School of Chemistry, University of Nottingham, University Park, Nottingham NG7 2RD, U.K.

Publisher

American Chemical Society (ACS)

Subject

Colloid and Surface Chemistry,Biochemistry,General Chemistry,Catalysis

Reference39 articles.

1. Monomeric, two-coordinate Mn, Fe and Co(ii) complexes featuring 2,6-(2,4,6-trimethylphenyl)phenyl ligands

2. All operations were carried out under an inert atmosphere employing standard Schlenk-line or glovebox techniques. Ethylenediamine (99%, Aldrich) was distilled over sodium metal while toluene (99.9%. Rathburn Chemicals, Ltd.) and THF (99.9%. Rathburn Chemicals, Ltd.) were purified through an MBraun MB SPS-800 solvent system. All solvents were stored in gas-tight ampoules under argon. The intermetallic precursor, K4Ge9, was synthesized from a stoichiometric mixture of the elements (K: 99.95%, Aldrich; Ge: 99.999% Strem) according to a previously reported synthetic procedure. [K(2,2,2-crypt)]3[Fe@Ge10]·2en: K4Ge9(62 mg, 0.077 mmol), FeAr2(26 mg, 0.038 mmol), and 2,2,2-crypt (50 mg, 0.133 mmol) were weighed out into a test tube inside a nitrogen-filled glovebox. The solids were dissolved in ethylenediamine (2 mL) and trace amounts of THF were added to aid in the dissolution of FeAr2. The reaction mixture was allowed to stir for 1 h, yielding a dark brown solution which was subsequently filtered and layered with toluene to allow for crystallization. Small greenish black rodlike crystals of [K(2,2,2-crypt)]3[Fe@Ge10]·2en suitable for single-crystal X-ray diffraction were obtained after 3 days alongside crystals of other known [Ge9]n−clusters. ES-MS:m/z781.2 [Fe@Ge10]−, 822.2 {K[Fe@Ge10]}−, 1198.7 {[K(2,2,2-crypt)][Fe@Ge10]}−. ES+ MS:m/z2443.9 {[K(2,2,2-crypt)]4[Fe@Ge10]}+.

3. Single crystal X-ray diffraction data were collected at 150 K on an Enraf-Nonius Kappa-CCD diffractometer equipped with an Oxford Cryosystems low-temperature device. The crystal was mounted on a glass fiber using N-Paratone oil and quickly placed under the nitrogen flow of the cryostream. Data were collected using graphite-monochromated Mo Kα radiation (λ = 0.710 73 Å); equivalent reflections were merged, and the images were processed with the DENZO and SCALEPACK programs. Corrections for Lorentz polarization effects and absorption were performed, and the structures were solved by direct methods using SIR92. The structures were refined onF2using SHELXL. Crystallographic data for [K(2,2,2-crypt)]3[Fe@Ge10]·2en: triclinic,P1̅,a= 14.4014(1),b= 15.7227(1),c= 21.6608(2), α = 93.2587(3),β= 100.4043(3),γ= 107.2794(4),V= 4574.29(6),Z= 2, R1/wR2 4.38/11.88% for the observed data (I≥ 2σ(I)), R1/wR2 5.72, 12.56% for all the data.

4. A Carbon-Free Sandwich Complex [(P 5 ) 2 Ti] 2−

5. Chemistry of Deltahedral Zintl Ions

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