Spectroelectrochemical studies of a ruthenium complex containing the pH sensitive 4,4'-dihydroxy-2,2'-bipyridine ligand

Dalton Transactions : an International Journal of Inorganic Chemistry
Erin J ViereJared J Paul

Abstract

Attaining high oxidation states at the metal center of transition metal complexes is a key design principle for many catalytic processes. One way to support high oxidation state chemistry is to utilize ligands that are electron-donating in nature. Understanding the structural and electronic changes of metal complexes as higher oxidation states are reached is critical towards designing more robust catalysts that are able to turn over at high rates without decomposing. To this end, we report herein the changes in structural and electronic properties as [Ru(bpy)2(44'bpy(OH)2)]2+is oxidized to [Ru(bpy)2(44'bpy(OH)2)]3+(bpy = 2,2'-bipyridine; 44'bpy(OH)2= 4,4'-dihydroxy-2,2'-bipyridine). The 44'bpy(OH)2ligand is a pH-dependent ligand where deprotonation of the hydroxyl groups leads to significant electronic donation to the metal center. A Pourbaix Diagram of the complex reveals a pH independent reduction potential below pH = 2.0 for the Ru3+/2+process at 0.91 V vs. Ag/AgCl. Above pH = 2.0, pH dependence is observed with a decrease in reduction potential until pH = 6.8 where the complex is completely deprotonated, resulting in a reduction potential of 0.62 V vs. Ag/AgCl. Spectroelectrochemical studies as a function of pH reveal the d...Continue Reading

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Citations

Jul 7, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Christian K NillesAlexander R Parent

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Methods Mentioned

BETA
X-Ray

Software Mentioned

APEX2
TDDFT
OLEX2
M06
XL

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