Exploring the Electrochemistry of Iron Dithiolene and Its Potential for Electrochemical Homogeneous Carbon Dioxide Reduction

Armstrong, Craig G. and Potter, Mark and Malcomson, Thomas and Hogue, Ross W. and Armstrong, Sapphire McNeil and Kerridge, Andrew and Toghill, Kathryn (2022) Exploring the Electrochemistry of Iron Dithiolene and Its Potential for Electrochemical Homogeneous Carbon Dioxide Reduction. ChemElectroChem, 9 (17): e202200610. e202200610. ISSN 2196-0216

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Abstract

In this work, the dithiolene complex iron(III) bis-maleonitriledithiolene [Fe(mnt) 2 ] is characterised and evaluated as a homogeneous CO 2 reduction catalyst. Electrochemically the Fe(mnt) 2 is reduced twice to the trianionic Fe(mnt) 2 3- state, which is correspondingly found to be active towards CO 2 . Interestingly, the first reduction event appears to comprise overlapping reversible couples, attributed to the presence of both a dimeric and monomeric form of the dithiolene complex. In acetonitrile Fe(mnt) 2 demonstrates a catalytic response to CO 2 yielding typical two-electron reduction products; H 2 , CO and CHOOH. The product distribution and yield were governed by the proton source. Operating with H 2 O as the proton source gave only H 2 and CO as products, whereas using 2,2,2-trifluoroethanol gave 38% CHOOH faradaic efficiency with H 2 and CO as minor products.

Item Type:
Journal Article
Journal or Publication Title:
ChemElectroChem
Uncontrolled Keywords:
Research Output Funding/yes_externally_funded
Subjects:
?? carbon dioxide reductioniron dithiolenehomogeneous catalysisdensity funtional theorymechanistic insightsyes - externally fundedelectrochemistrycatalysissdg 7 - affordable and clean energysdg 13 - climate action ??
ID Code:
174037
Deposited By:
Deposited On:
04 Aug 2022 13:45
Refereed?:
Yes
Published?:
Published
Last Modified:
15 Jul 2024 22:52