Substituent Effect of the Bridging Ligand in the Trinuclear
Ru Complexes on Photocatalytic Oxygenation of a Sulfide and Alkenes
Posted on 2017-10-23 - 17:07
To examine the effect
of tuning the electron transfer ability between
photosensitizers and reaction centers on the activity of visible-light-driven
catalysts, a series of trinuclear Ru photocatalysts containing two
Ru(II) photosensitizers and a Ru(II) reaction center bridged by a
substituted bipyrimidine was prepared. The introduction of electron-donating
or electron-withdrawing groups on the ligands was found to affect
the photophysical and electrochemical properties of these catalysts.
Density functional theory calculations of the mononuclear Ru complexes
with nonsubstituted and substituted bipyrimidine ligands, which correspond
to the reaction center of the trinuclear complexes, revealed how the
electronic effect of the substituents affect the frontier orbital
energies. For photocatalytic oxygenation of a sulfide and terminal
alkenes, the catalyst with a 5,5′-dibromo-2,2′-bipyrimidine
ligand showed higher activity than the catalyst with 5,5′-dimethyl-2,2′-bipyrimidine
and nonsubstituted bipyrimidine ligands, as expected according to
the electronic effects of these ligands. In contrast, the catalyst
with the nonsubstituted bipyrimidine ligand showed the highest activity
toward inner alkenes, which may be due to steric effects.
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Phungsripheng, Siwas; Akita, Munetaka; Inagaki, Akiko (2017). Substituent Effect of the Bridging Ligand in the Trinuclear
Ru Complexes on Photocatalytic Oxygenation of a Sulfide and Alkenes. ACS Publications. Collection. https://doi.org/10.1021/acs.inorgchem.7b01764
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AUTHORS (3)
SP
Siwas Phungsripheng
MA
Munetaka Akita
AI
Akiko Inagaki
KEYWORDS
electron-withdrawing groupsSubstituent Effectnonsubstituted bipyrimidine ligandstheory calculationstrinuclear Ru photocatalystsvisible-light-driven catalyststerminal alkenesbipyrimidine ligandsnonsubstituted bipyrimidine ligandTrinuclear Ru Complexesreaction centerselectron transfer abilityPhotocatalytic OxygenationRu complexeselectrochemical propertiesBridging Ligandtrinuclear complexessteric effectsphotocatalytic oxygenationreaction center