Hydrogen Generation Catalyzed by Fluorinated Diglyoxime–Iron Complexes at Low Overpotentials
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https://figshare.com/articles/dataset/Hydrogen_Generation_Catalyzed_by_Fluorinated_Diglyoxime_Iron_Complexes_at_Low_Overpotentials/2520085
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资源简介：
FeII complexes containing the fluorinated
ligand 1,2-bis(perfluorophenyl)ethane-1,2-dionedioxime
(dArFgH2; H = dissociable proton) exhibit relatively
positive FeII/I reduction potentials. The air-stable difluoroborated
species [(dArFgBF2)2Fe(py)2] (2) electrocatalyzes H2 generation at −0.9
V vs SCE with icat/ip ≈ 4, corresponding to a turnover frequency (TOF) of
∼20 s–1 [Faradaic yield (FY) = 82 ±
13%]. The corresponding monofluoroborated, proton-bridged
complex [(dArFg2H-BF2)Fe(py)2] (3) exhibits an improved TOF of ∼200
s–1 (icat/ip ≈ 8; FY = 68 ± 14%) at −0.8 V with
an overpotential of 300 mV. Simulations of the electrocatalytic cyclic
voltammograms of 2 suggest rate-limiting protonation
of an Fe“0” intermediate (kRLS ≈ 200 M–1 s–1) that undergoes hydride protonation to form H2. Complex 3 likely reacts via protonation of an FeI intermediate
that subsequently forms H2 via a bimetallic mechanism (kRLS ≈ 2000 M–1 s–1). 3 catalyzes production at relatively
positive potentials compared with other iron complexes.
创建时间：
2012-05-23
