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Physicochemical Analysis of Ruthenium(II) Sensitizers of 1,2,3-Triazole-Derived Mesoionic Carbene and Cyclometalating Ligands

TitlePhysicochemical Analysis of Ruthenium(II) Sensitizers of 1,2,3-Triazole-Derived Mesoionic Carbene and Cyclometalating Ligands
Publication TypeJournal Article
Year of Publication2014
AuthorsSinn, S, Schulze, B, Friebe, C, Brown, DG, Jaeger, M, Altuntas, E, Kuebel, J, Guntner, O, Berlinguette, CP, Dietzek, B, Schubert, US
JournalINORGANIC CHEMISTRY
Volume53
Pagination2083-2095
Date PublishedFEB 17
ISSN0020-1669
Abstract

A series of heteroleptic bis(tridentate) ruthenium(II) complexes bearing ligands featuring 1,2,3-triazolide and 1,2,3-triazolylidene units are presented. The synthesis of the (CNN)-N-boolean AND-N-boolean AND-coordinated ruthenium(II) triazolide complex is achieved by direct C H activation, which is enabled by the use of a 1,5-disubstituted triazole. By postcomplexation alkylation, the ruthenium(II) 1,2,3-triazolide complex can be converted to the corresponding 1,2,3-triazolylidene complex. Additionally, a ruthenium(II) complex featuring a (CNC)-N-boolean AND-C-boolean AND-coordinating bis(1,2,3-triazolylidene)pyridine ligand is prepared via transmetalation from a silver(I) triazolylidene precursor. The electronic consequences of the carbanion and mesoionic carbene donors are studied both experimentally and computationally. The presented complexes exhibit a broad absorption in the visible region as well as long lifetimes of the charge-separated excited state suggesting their application in photoredox catalysis and photovoltaics. Testing of the dyes in a conventional dye-sensitized solar cell (DSSC) generates, however, only modest power conversion efficiencies (PCEs).

DOI10.1021/ic402702z