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Novel [FeFe]-hydrogenase mimics: unexpected course of the reaction of ferrocenyl α-thienyl thioketone with Fe3(CO)12

Novel [FeFe]-hydrogenase mimics: unexpected course of the reaction of ferrocenyl α-thienyl thioketone with Fe3(CO)12
Novel [FeFe]-hydrogenase mimics: unexpected course of the reaction of ferrocenyl α-thienyl thioketone with Fe3(CO)12

The influence of the substitution pattern in ferrocenyl α-thienyl thioketone used as a proli-gand in complexation reactions with Fe3 (CO)12 was investigated. As a result, two new sulfur–iron complexes, considered [FeFe]-hydrogenase mimics, were obtained and characterized by spectroscopic techniques (1H,13C{1H} NMR, IR, MS), as well as by elemental analysis and X-ray single crystal diffraction methods. The electrochemical properties of both complexes were studied and compared using cyclic voltammetry in the absence and in presence of acetic acid as a proton source. The performed measurements demonstrated that both complexes can catalyze the reduction of protons to molecular hydrogen H2 . Moreover, the obtained results showed that the presence of the ferrocene moiety at the backbone of the linker of both complexes improved the stability of the reduced species.

cyclic voltammetry, Quantum Chemistry, enzyme, sulfur–iron clusters
Daraosheh, Ahmad Q.
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Abul-Futouh, Hassan
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Murakami, Natsuki
ba90351a-aceb-4a5e-ba6e-3e039ca1571d
Ziems, Karl Michael
6d346238-2471-47c7-b89f-590059caf037
Görls, Helmar
38b5f774-70a8-45ed-8b27-a397bf4d18be
Kupfer, Stephan
4186aa37-4fda-4cd5-9b59-fd9c7aba924a
Gräfe, Stefanie
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Ishii, Akihiko
8fb29c12-f5cd-4a6e-86f3-97c83bdf2fa6
Celeda, Małgorzata
ce3f4032-f23f-4780-9b07-31c73f133721
Mlostoń, Grzegorz
2c51175a-af50-4d75-83aa-a29711c7f149
Weigand, Wolfgang
d98b6c6d-6fcf-4ac2-9739-3218eac778c2
Daraosheh, Ahmad Q.
f843c2be-8a4c-41db-b025-a4fc9cdec01b
Abul-Futouh, Hassan
15f779e6-156b-4595-a97c-648a6171d7f8
Murakami, Natsuki
ba90351a-aceb-4a5e-ba6e-3e039ca1571d
Ziems, Karl Michael
6d346238-2471-47c7-b89f-590059caf037
Görls, Helmar
38b5f774-70a8-45ed-8b27-a397bf4d18be
Kupfer, Stephan
4186aa37-4fda-4cd5-9b59-fd9c7aba924a
Gräfe, Stefanie
32b99c66-1736-44b1-9a25-aafd5991dbae
Ishii, Akihiko
8fb29c12-f5cd-4a6e-86f3-97c83bdf2fa6
Celeda, Małgorzata
ce3f4032-f23f-4780-9b07-31c73f133721
Mlostoń, Grzegorz
2c51175a-af50-4d75-83aa-a29711c7f149
Weigand, Wolfgang
d98b6c6d-6fcf-4ac2-9739-3218eac778c2

Daraosheh, Ahmad Q., Abul-Futouh, Hassan, Murakami, Natsuki, Ziems, Karl Michael, Görls, Helmar, Kupfer, Stephan, Gräfe, Stefanie, Ishii, Akihiko, Celeda, Małgorzata, Mlostoń, Grzegorz and Weigand, Wolfgang (2022) Novel [FeFe]-hydrogenase mimics: unexpected course of the reaction of ferrocenyl α-thienyl thioketone with Fe3(CO)12 †. Materials, 15 (8), [2867]. (doi:10.3390/ma15082867).

Record type: Article

Abstract

The influence of the substitution pattern in ferrocenyl α-thienyl thioketone used as a proli-gand in complexation reactions with Fe3 (CO)12 was investigated. As a result, two new sulfur–iron complexes, considered [FeFe]-hydrogenase mimics, were obtained and characterized by spectroscopic techniques (1H,13C{1H} NMR, IR, MS), as well as by elemental analysis and X-ray single crystal diffraction methods. The electrochemical properties of both complexes were studied and compared using cyclic voltammetry in the absence and in presence of acetic acid as a proton source. The performed measurements demonstrated that both complexes can catalyze the reduction of protons to molecular hydrogen H2 . Moreover, the obtained results showed that the presence of the ferrocene moiety at the backbone of the linker of both complexes improved the stability of the reduced species.

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More information

Accepted/In Press date: 11 April 2022
e-pub ahead of print date: 14 April 2022
Additional Information: Publisher Copyright: © 2022 by the authors. Licensee MDPI, Basel, Switzerland.
Keywords: cyclic voltammetry, Quantum Chemistry, enzyme, sulfur–iron clusters

Identifiers

Local EPrints ID: 498207
URI: http://eprints.soton.ac.uk/id/eprint/498207
PURE UUID: d06e598a-525a-429a-8d72-96654e194d80
ORCID for Karl Michael Ziems: ORCID iD orcid.org/0000-0001-5369-7778

Catalogue record

Date deposited: 12 Feb 2025 17:45
Last modified: 13 Feb 2025 03:16

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Contributors

Author: Ahmad Q. Daraosheh
Author: Hassan Abul-Futouh
Author: Natsuki Murakami
Author: Karl Michael Ziems ORCID iD
Author: Helmar Görls
Author: Stephan Kupfer
Author: Stefanie Gräfe
Author: Akihiko Ishii
Author: Małgorzata Celeda
Author: Grzegorz Mlostoń
Author: Wolfgang Weigand

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