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Bis(4′-(4-pyridyl)-2,2′:6′,2′′-terpyridine)ruthenium(II) complexes and their N-alkylated derivatives in catalytic light-driven water oxidation

Lv, H. and Rudd, J. A. and Zhuk, P. F. and Lee, J. Y. and Constable, E. C. and Housecroft, C. E. and Hill, C. L. and Musaev, D. G. and Geletii, Y. V.. (2013) Bis(4′-(4-pyridyl)-2,2′:6′,2′′-terpyridine)ruthenium(II) complexes and their N-alkylated derivatives in catalytic light-driven water oxidation. RSC Advances, 3. pp. 20647-20654.

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Official URL: http://edoc.unibas.ch/dok/A6184004

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Abstract

Hydrogen sulfate salts of [Ru(1)2]2+ where 1 = 4′-(4-pyridyl)-2,2′:6′,2′′-terpyridine and four N-alkylated derivatives [Ru(L)2]4+ were used as photosensitizers (λmax ∼510 nm) for water oxidation in light driven reactions with peroxydisulfate as a sacrificial electron acceptor and Na10[Co4(H2O)2(α-PW9O34)2] (Co4POM) as the catalyst in sodium borate buffers at pH 8.0 and 9.0. The N-substituents investigated were benzyl (L+ = 2+), ethyl (L+ = 3+), allyl (L+ = 4+) and 4-cyanobenzyl (L+ = 5+). The O2 yield in the presence of [Ru(L)2]4+ (L+ = 2+–4+) was comparable to that obtained in the presence [Ru(bpy)3]2+ (bpy = 2,2′-bipyridine) using light sources with λmax ≈ 490 nm. The ruthenium(III) complexes [Ru(1)2]3+ and [Ru(L)2]5+ (L+ = 2+–5+) are rather unstable in acidic conditions and could not be isolated. The most efficient photosensitizers [Ru(L)2]5+ (L+ = 2+ and 4+) were the least stable under weakly basic conditions (pH 9.0) with a half-life τ1/2 ∼ 10 ms. The stability of the complexes under photocatalytic turnover conditions is probably controlled by the rate at which ligand L+ is oxidized by Co4POM in its highest oxidation state.
Faculties and Departments:05 Faculty of Science > Departement Chemie > Former Organization Units Chemistry > Anorganische Chemie (Housecroft)
UniBasel Contributors:Housecroft, Catherine Elizabeth and Constable, Edwin Charles and Rudd, Jennifer Amy
Item Type:Article, refereed
Article Subtype:Research Article
Publisher:Royal Society of Chemistry
e-ISSN:2046-2069
Note:Publication type according to Uni Basel Research Database: Journal article
Identification Number:
Last Modified:03 May 2017 13:58
Deposited On:06 Dec 2013 09:35

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