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Asymmetric Cyclometalated RuII Polypyridyl-Type Complexes with Π-Extended Carbanionic Donor Sets
Friedrich Schiller Univ Jena, Lab Organ & Macromol Chem IOMC, Humboldtstr 10, D-07743 Jena, Germany.;Friedrich Schiller Univ Jena, Ctr Energy & Environm Chem Jena CEEC Jena, Philosophenweg 7a, D-07743 Jena, Germany..
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström. Yale Univ, Dept Chem, POB 208107,225 Prospect St, New Haven, CT 06520 USA..
Friedrich Schiller Univ Jena, Lab Inorgan & Analyt Chem, Lessingstr 8, D-07743 Jena, Germany..
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Chemistry - Ångström, Molecular Biomimetics. (Molekylär Oorganisk Kemi)ORCID iD: 0000-0002-1691-729X
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2017 (English)In: Inorganic Chemistry, ISSN 0020-1669, E-ISSN 1520-510X, Vol. 56, no 14, 7720-7730 p.Article in journal (Refereed) Published
Abstract [en]

A series of novel cyclometalated Ru-II complexes were investigated featuring the tridentate dqp ligand platform (dqp is 2,6-di(quinolin-8-yl)pyridine), in order to utilize the octahedral coordination mode around the Ru center to modulate the electrochemical and photophysical properties. The heteroleptic complexes feature C-1 symmetry due to symmetry breaking by the peripheral five- or six-membered carbanionic chelate (phenyl, naphthyl, or anthracenyl units). The chelation mode is controlled by the steric effects and C-H activation selectivity of the ligand, which prompted the development of a general synthesis protocol. The optimized conditions to achieve high overall yields (55-75%) involve NaHCO3 as the base and an simplified purification protocol: i.e., facile chromatographic separation using commercially available amino-functionalized silica applying nonaqueous salt-free conditions to omit the necessity of counterion exchange. The structural, photophysical, and electrochemical properties were studied in depth, and the results were corroborated by density functional theory (DFT) calculations. Steady state and time-resolved spectroscopy revealed red-shifted absorption (up to 750 run) and weak IR emission (800-1000 nm) combined with prolonged emission lifetimes (up to 20 ns) in comparison to classical tpy-based (tpy is 2,2':6',2 ''-terpyridine) complexes. An enhanced stability was observed by blocking the reactive positions of the carbanionic ligand framework, while the reactive positions may be exploited for further functionalization.

Place, publisher, year, edition, pages
2017. Vol. 56, no 14, 7720-7730 p.
National Category
Inorganic Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-332419DOI: 10.1021/acs.inorgchem.7b00392ISI: 000405972200018OAI: oai:DiVA.org:uu-332419DiVA: diva2:1154471
Funder
Swedish Energy AgencyKnut and Alice Wallenberg Foundation
Note

Title in WoS: Asymmetric Cyclometalated Ru-II Polypyridyl-Type Complexes with pi-Extended Carbanionic Donor Sets

Available from: 2017-11-02 Created: 2017-11-02 Last updated: 2017-11-02Bibliographically approved

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Parada, Giovanny A.Ott, Sascha

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