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Redox-Active Tetraruthenium Macrocycles Built from 1,4-Divinylphenylene-Bridged Diruthenium Complexes

Redox-Active Tetraruthenium Macrocycles Built from 1,4-Divinylphenylene-Bridged Diruthenium Complexes

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SCHEERER, Stefan, Michael LINSEIS, Evelyn WUTTKE, Sabrina WEICKERT, Malte DRESCHER, Oliver TRÖPPNER, Ivana IVANOVIĆ-BURMAZOVIĆ, Andreas IRMLER, Fabian PAULY, Rainer F. WINTER, 2016. Redox-Active Tetraruthenium Macrocycles Built from 1,4-Divinylphenylene-Bridged Diruthenium Complexes. In: Chemistry - A European Journal. 22(28), pp. 9574-9590. ISSN 0947-6539. eISSN 1521-3765

@article{Scheerer2016Redox-34888, title={Redox-Active Tetraruthenium Macrocycles Built from 1,4-Divinylphenylene-Bridged Diruthenium Complexes}, year={2016}, doi={10.1002/chem.201601384}, number={28}, volume={22}, issn={0947-6539}, journal={Chemistry - A European Journal}, pages={9574--9590}, author={Scheerer, Stefan and Linseis, Michael and Wuttke, Evelyn and Weickert, Sabrina and Drescher, Malte and Tröppner, Oliver and Ivanović-Burmazović, Ivana and Irmler, Andreas and Pauly, Fabian and Winter, Rainer F.} }

Linseis, Michael 2016-07-27T15:28:22Z Winter, Rainer F. 2016 Redox-Active Tetraruthenium Macrocycles Built from 1,4-Divinylphenylene-Bridged Diruthenium Complexes Scheerer, Stefan eng Ivanović-Burmazović, Ivana Irmler, Andreas Weickert, Sabrina Drescher, Malte Tröppner, Oliver 2016-07-27T15:28:22Z Irmler, Andreas Scheerer, Stefan Wuttke, Evelyn Pauly, Fabian Pauly, Fabian Metallamacrocylic tetraruthenium complexes were generated by treatment of 1,4-divinylphenylene-bridged diruthenium complexes with functionalized 1,3-benzene dicarboxylic acids and characterized by HR ESI-MS and multinuclear NMR spectroscopy. Every divinylphenylene diruthenium subunit is oxidized in two consecutive one-electron steps with half-wave potential splittings in the range of 250 to 330 mV. Additional, smaller redox-splittings between the +/2+ and 0/+ and the 3+/4+ and 2+/3+ redox processes, corresponding to the first and the second oxidations of every divinylphenylene diruthenium entity, are due to electrostatic effects. The lack of electronic coupling through bond or through space is explained by the nodal properties of the relevant molecular orbitals and the lateral side-by-side arrangement of the divinylphenylene linkers. The polyelectrochromic behavior of the divinylphenylene diruthenium precursors is retained and even amplified in these metallamacrocyclic structures. EPR studies down to T=4 K indicate that the dications 1-H<sup>2+</sup> and 1-OBu<sup>2+</sup> are paramagnetic. The dications and the tetracation of macrocycle 3-H display intense (dications) or weak (3-H<sup>4+</sup> ) EPR signals. Quantum chemical calculations indicate that the four most stable conformers of the macrocycles are largely devoid of strain. Bond parameters, energies as well as charge and spin density distributions of model macrocycle 5-H<sup>Me</sup> were calculated for the different charge and spin states. Ivanović-Burmazović, Ivana Weickert, Sabrina Linseis, Michael Winter, Rainer F. Drescher, Malte Wuttke, Evelyn Tröppner, Oliver

Dateiabrufe seit 27.07.2016 (Informationen über die Zugriffsstatistik)

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