Arsine, Stibine and Phosphine Derivatives of [Fe2(CO)6(μ-bdt)] (bdt = Benzenedithiolate) : Syntheses, Structures and Spectroscopic and Electrocatalytic Studies
(2025) In Inorganics 13(2).- Abstract
The reactivity of the benzenedithiolate (bdt)-bridged complex [Fe2(CO)6(µ-bdt)] with arsine, stibine and phosphine ligands has been studied. The new mono- and disubstituted complexes [Fe2(CO)5(EPh3)(µ-bdt)] (E = As, 1; E = Sb 3) and [Fe2(CO)4(EPh3)2(µ-bdt)] (E = As, 2; E = Sb, 4) and the previously reported [Fe2(CO)4(PPh2H)2(µ-bdt)] (5) have been prepared by Me3NO-initiated carbonyl substitution reactions of [Fe2(CO)6(µ-bdt)] with appropriate ligands at 80 °C. Spectroscopic and single-crystal X-ray diffraction studies reveal that in all cases the introduced... (More)
The reactivity of the benzenedithiolate (bdt)-bridged complex [Fe2(CO)6(µ-bdt)] with arsine, stibine and phosphine ligands has been studied. The new mono- and disubstituted complexes [Fe2(CO)5(EPh3)(µ-bdt)] (E = As, 1; E = Sb 3) and [Fe2(CO)4(EPh3)2(µ-bdt)] (E = As, 2; E = Sb, 4) and the previously reported [Fe2(CO)4(PPh2H)2(µ-bdt)] (5) have been prepared by Me3NO-initiated carbonyl substitution reactions of [Fe2(CO)6(µ-bdt)] with appropriate ligands at 80 °C. Spectroscopic and single-crystal X-ray diffraction studies reveal that in all cases the introduced ligands occupy apical coordination site(s) lying trans to the iron–iron bond. Their electrochemistry has been probed by cyclic voltammetry and selected complexes have been tested as proton reduction catalysts. Monosubstituted complexes 1 and 3 show two irreversible reductions at ca. −1.7 V and −2.0 V, respectively, relative to Fc+/Fc, while the disubstituted complexes 2 and 5 show a single irreversible reduction at ca. −2.2 V and −1.84 V, respectively. Complexes 1, 3 and 5 can catalyse electrocatalytic proton reduction in the presence of either p-toluene sulfonic acid (TsOH) or trifluoroacetic acid (CF3CO2H).
(Less)
- author
- Rahaman, Ahibur LU ; Kulsume, Ummey ; Alam, Fakir R. ; Haukka, Matti ; Ghosh, Shishir ; Hogarth, Graeme ; Nordlander, Ebbe LU and Kabir, Shariff E.
- organization
- publishing date
- 2025-02
- type
- Contribution to journal
- publication status
- published
- subject
- keywords
- CO substitution, diiron-dithiolate complex, proton reduction, triphenylarsine, triphenylstibine
- in
- Inorganics
- volume
- 13
- issue
- 2
- article number
- 63
- publisher
- MDPI AG
- external identifiers
-
- scopus:85218710748
- ISSN
- 2304-6740
- DOI
- 10.3390/inorganics13020063
- language
- English
- LU publication?
- yes
- id
- 7eb416ac-f538-47a3-9610-1d794687d7bc
- date added to LUP
- 2025-06-25 10:17:03
- date last changed
- 2025-06-25 10:17:33
@article{7eb416ac-f538-47a3-9610-1d794687d7bc, abstract = {{<p>The reactivity of the benzenedithiolate (bdt)-bridged complex [Fe<sub>2</sub>(CO)<sub>6</sub>(µ-bdt)] with arsine, stibine and phosphine ligands has been studied. The new mono- and disubstituted complexes [Fe<sub>2</sub>(CO)<sub>5</sub>(EPh<sub>3</sub>)(µ-bdt)] (E = As, 1; E = Sb 3) and [Fe<sub>2</sub>(CO)<sub>4</sub>(EPh<sub>3</sub>)<sub>2</sub>(µ-bdt)] (E = As, 2; E = Sb, 4) and the previously reported [Fe<sub>2</sub>(CO)<sub>4</sub>(PPh<sub>2</sub>H)<sub>2</sub>(µ-bdt)] (5) have been prepared by Me<sub>3</sub>NO-initiated carbonyl substitution reactions of [Fe<sub>2</sub>(CO)<sub>6</sub>(µ-bdt)] with appropriate ligands at 80 °C. Spectroscopic and single-crystal X-ray diffraction studies reveal that in all cases the introduced ligands occupy apical coordination site(s) lying trans to the iron–iron bond. Their electrochemistry has been probed by cyclic voltammetry and selected complexes have been tested as proton reduction catalysts. Monosubstituted complexes 1 and 3 show two irreversible reductions at ca. −1.7 V and −2.0 V, respectively, relative to Fc<sup>+</sup>/Fc, while the disubstituted complexes 2 and 5 show a single irreversible reduction at ca. −2.2 V and −1.84 V, respectively. Complexes 1, 3 and 5 can catalyse electrocatalytic proton reduction in the presence of either p-toluene sulfonic acid (TsOH) or trifluoroacetic acid (CF<sub>3</sub>CO<sub>2</sub>H).</p>}}, author = {{Rahaman, Ahibur and Kulsume, Ummey and Alam, Fakir R. and Haukka, Matti and Ghosh, Shishir and Hogarth, Graeme and Nordlander, Ebbe and Kabir, Shariff E.}}, issn = {{2304-6740}}, keywords = {{CO substitution; diiron-dithiolate complex; proton reduction; triphenylarsine; triphenylstibine}}, language = {{eng}}, number = {{2}}, publisher = {{MDPI AG}}, series = {{Inorganics}}, title = {{Arsine, Stibine and Phosphine Derivatives of [Fe<sub>2</sub>(CO)<sub>6</sub>(μ-bdt)] (bdt = Benzenedithiolate) : Syntheses, Structures and Spectroscopic and Electrocatalytic Studies}}, url = {{http://dx.doi.org/10.3390/inorganics13020063}}, doi = {{10.3390/inorganics13020063}}, volume = {{13}}, year = {{2025}}, }