Insights into the different mechanistic stages of light-induced hydrogen evolution of a 5,5 '-bisphenanthroline linked RuPt complex

Laemmle, Martin and Pilz, T. David and Kutta, Roger Jan and Muessler, Marius and Mengele, Alexander K. and Goerls, Helmar and Heinemann, Frank W. and Rau, Sven (2022) Insights into the different mechanistic stages of light-induced hydrogen evolution of a 5,5 '-bisphenanthroline linked RuPt complex. DALTON TRANSACTIONS, 51 (40). pp. 15282-15291. ISSN 1477-9226, 1477-9234

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Abstract

Herein, the synthesis in conjunction with the structural, electrochemical, and photophysical characterization of a 5,5'-bisphenanthroline (phenphen) linked heterodinuclear RuPt complex (Ru(phenphen)Pt) and its light-driven hydrogen formation activity are reported. A single crystal X-ray diffraction (SC-XRD) analysis identified a perpendicular orientation of the two directly linked 1,10-phenanthroline moieties. The disruption of pi-conjugation blocks intramolecular electron transfer as evidenced by a comparative time-resolved optical spectroscopy study of Ru(phenphen)Pt and the reference complexes Ru(phenphen) and Ru(phenphen)Ru. However, reductive quenching is observed in the presence of an external electron donor such as triethylamine. Irradiating Ru(phenphen)Pt with visible light (470 nm) leads to H-2 formation. We discuss a potential mechanism that mainly proceeds via Pt colloids and provide indications that initial hydrogen generation may also proceed via a molecular pathway. As previous reports on related heterodinuclear RuPt-based photocatalysts revealed purely molecular hydrogen evolution, the present work thus highlights the role of the bridging ligand in stabilizing the catalytic center and consequently determining the mechanism of light-induced hydrogen evolution in these systems.

Item Type: Article
Uncontrolled Keywords: SUPRAMOLECULAR PHOTOCATALYST; WATER REDUCTION; METAL-COMPLEXES; RU(II); GENERATION; PLATINUM; LIGANDS; FUTURE; OXYGEN; PD
Subjects: 500 Science > 540 Chemistry & allied sciences
Divisions: Chemistry and Pharmacy > Institut für Physikalische und Theoretische Chemie > Chair of Physical Chemistry I
Depositing User: Dr. Gernot Deinzer
Date Deposited: 20 Feb 2024 07:14
Last Modified: 20 Feb 2024 07:14
URI: https://pred.uni-regensburg.de/id/eprint/58161

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