{1,1'-(Dimethylsilylene)bis[methanechalcogenolato]}diiron complexes [2Fe2E(Si)] (E=S, Se, Te)-[FeFe] hydrogenase models

Ulf Peter Apfel, Helmar Görls, Greg A N Felton, Dennis H. Evans, Richard S Glass, Dennis L Lichtenberger, Wolfgang Weigand

Research output: Contribution to journalArticle

13 Citations (Scopus)

Abstract

(Bis-selenolato) and (bis-tellurolato)diiron complexes [2Fe2E(Si)] were prepared and compared with the known (bis-thiolato)diiron complex A to assess their ability to produce hydrogen from protons. Treatment of [Fe 3(CO)12] with 4,4-dimethyl-1,2,4-diselenasilolane (1) in boiling toluene afforded hexacarbonyl{μ-{[1,1'-(dimethylsilylene) bis[methaneselenolato-κSe: κSe]](2 -)}}diiron(Fe-Fe) (2). The analog bis-tellurolato complex hexacarbonyl{μ-{[1,1'-(dimethylsilylene) bis[methanetellurolato-κTe: κTe]](2 -)}}diiron(Fe-Fe) (3) was obtained by treatment of [Fe3(CO)12] with dimethylbis(tellurocyanatomethyl)dimethylsilane, which was prepared in situ. All compounds were characterized by NMR, IR spectroscopy, mass spectrometry, elemental analysis and single-crystal X-ray analysis. The electrocatalytic properties of the [2Fe2X(Si)] (X=S, Se, Te) model complexes A, 1, and 2 towards hydrogen formation were evaluated.

Original languageEnglish (US)
Pages (from-to)2168-2175
Number of pages8
JournalHelvetica Chimica Acta
Volume95
Issue number11
DOIs
StatePublished - Nov 2012

Fingerprint

Hydrogenase
Hydrogen
X ray analysis
Toluene
hydrogen
Carbon Monoxide
boiling
Boiling liquids
Mass spectrometry
toluene
Protons
Infrared spectroscopy
Mass Spectrometry
Magnetic Resonance Spectroscopy
mass spectroscopy
Nuclear magnetic resonance
X-Rays
Single crystals
analogs
nuclear magnetic resonance

Keywords

  • Electrocatalysis
  • Hydrogenase
  • Iron complexes
  • Selenium complexes
  • Tellurium complexes
  • X-Ray crystallography

ASJC Scopus subject areas

  • Biochemistry
  • Organic Chemistry
  • Catalysis
  • Drug Discovery
  • Physical and Theoretical Chemistry
  • Inorganic Chemistry

Cite this

{1,1'-(Dimethylsilylene)bis[methanechalcogenolato]}diiron complexes [2Fe2E(Si)] (E=S, Se, Te)-[FeFe] hydrogenase models. / Apfel, Ulf Peter; Görls, Helmar; Felton, Greg A N; Evans, Dennis H.; Glass, Richard S; Lichtenberger, Dennis L; Weigand, Wolfgang.

In: Helvetica Chimica Acta, Vol. 95, No. 11, 11.2012, p. 2168-2175.

Research output: Contribution to journalArticle

Apfel, Ulf Peter ; Görls, Helmar ; Felton, Greg A N ; Evans, Dennis H. ; Glass, Richard S ; Lichtenberger, Dennis L ; Weigand, Wolfgang. / {1,1'-(Dimethylsilylene)bis[methanechalcogenolato]}diiron complexes [2Fe2E(Si)] (E=S, Se, Te)-[FeFe] hydrogenase models. In: Helvetica Chimica Acta. 2012 ; Vol. 95, No. 11. pp. 2168-2175.
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T1 - {1,1'-(Dimethylsilylene)bis[methanechalcogenolato]}diiron complexes [2Fe2E(Si)] (E=S, Se, Te)-[FeFe] hydrogenase models

AU - Apfel, Ulf Peter

AU - Görls, Helmar

AU - Felton, Greg A N

AU - Evans, Dennis H.

AU - Glass, Richard S

AU - Lichtenberger, Dennis L

AU - Weigand, Wolfgang

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N2 - (Bis-selenolato) and (bis-tellurolato)diiron complexes [2Fe2E(Si)] were prepared and compared with the known (bis-thiolato)diiron complex A to assess their ability to produce hydrogen from protons. Treatment of [Fe 3(CO)12] with 4,4-dimethyl-1,2,4-diselenasilolane (1) in boiling toluene afforded hexacarbonyl{μ-{[1,1'-(dimethylsilylene) bis[methaneselenolato-κSe: κSe]](2 -)}}diiron(Fe-Fe) (2). The analog bis-tellurolato complex hexacarbonyl{μ-{[1,1'-(dimethylsilylene) bis[methanetellurolato-κTe: κTe]](2 -)}}diiron(Fe-Fe) (3) was obtained by treatment of [Fe3(CO)12] with dimethylbis(tellurocyanatomethyl)dimethylsilane, which was prepared in situ. All compounds were characterized by NMR, IR spectroscopy, mass spectrometry, elemental analysis and single-crystal X-ray analysis. The electrocatalytic properties of the [2Fe2X(Si)] (X=S, Se, Te) model complexes A, 1, and 2 towards hydrogen formation were evaluated.

AB - (Bis-selenolato) and (bis-tellurolato)diiron complexes [2Fe2E(Si)] were prepared and compared with the known (bis-thiolato)diiron complex A to assess their ability to produce hydrogen from protons. Treatment of [Fe 3(CO)12] with 4,4-dimethyl-1,2,4-diselenasilolane (1) in boiling toluene afforded hexacarbonyl{μ-{[1,1'-(dimethylsilylene) bis[methaneselenolato-κSe: κSe]](2 -)}}diiron(Fe-Fe) (2). The analog bis-tellurolato complex hexacarbonyl{μ-{[1,1'-(dimethylsilylene) bis[methanetellurolato-κTe: κTe]](2 -)}}diiron(Fe-Fe) (3) was obtained by treatment of [Fe3(CO)12] with dimethylbis(tellurocyanatomethyl)dimethylsilane, which was prepared in situ. All compounds were characterized by NMR, IR spectroscopy, mass spectrometry, elemental analysis and single-crystal X-ray analysis. The electrocatalytic properties of the [2Fe2X(Si)] (X=S, Se, Te) model complexes A, 1, and 2 towards hydrogen formation were evaluated.

KW - Electrocatalysis

KW - Hydrogenase

KW - Iron complexes

KW - Selenium complexes

KW - Tellurium complexes

KW - X-Ray crystallography

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