Ligand effects on the electrochemical behavior of [Fe2(CO)5(L){μ-(SCH2)2(Ph)P=O}] (L = PPh3, P(OEt)3) hydrogenase model complexes

Dalton Transactions : an International Journal of Inorganic Chemistry
Laith R AlmazahrehWolfgang Weigand

Abstract

In this paper we study the influence of substituting one CO ligand in [Fe2(CO)6{μ-(SCH2)2(Ph)P=O}] (1) by better σ-donor L ligands affording [Fe2(CO)5(L){μ-(SCH2)2(Ph)P=O}] {L = PPh3 (2) and P(OEt)3 (3)} in relation to the steric interactions and the voltammetric behavior. Cyclic voltammetric investigations under N2 and CO showed remarkable differences in the electrochemical behaviour of complexes 2 and 3: (i) Complex 2 tends to expel PPh3 upon reduction whereas complex 3 exhibits chemical reversibility and (ii) Under CO, complex 3 reacts with CO affording a new compound P, which shows a reversible wave at E1/2 ∼ -0.9 V (vs. ferrocenium/ferrocene couple). The presence of CO assists the formation of 1 after electrochemically induced loss of PPh3 during the voltammetric experiment of 2. Using DFT calculations we provide an explanation for the difference in stabilities between the Fe-PPh3 and Fe-P(OEt)3 bonds.

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Citations

Oct 13, 2015·Dalton Transactions : an International Journal of Inorganic Chemistry·Ralf TrautweinWolfgang Weigand
Oct 11, 2016·Chemistry : a European Journal·Hassan Abul-FutouhWolfgang Weigand
Feb 16, 2017·Dalton Transactions : an International Journal of Inorganic Chemistry·Hassan Abul-FutouhWolfgang Weigand
May 5, 2018·Chemical Communications : Chem Comm·F WittkampU-P Apfel
Apr 20, 2021·Journal of Computational Chemistry·Pirouz KianiWilliam J Pietro

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