Role of Spacers in Molecularly Linked RuRh Dyads: A Comparative Synthetic and Ultrafast Spectroscopic Investigation
Mohini Semwal, Martin Lämmle, Elias H. P. Brohmer, Steffen Volk, Linda Zedler, Stephan Kupfer, Alexander K. Mengele, Georgina E. Shillito, Sven Rau, Benjamin Dietzek-Ivanšić
TL;DR
This study explores how spacers in RuRh complexes affect their photocatalytic performance using synthetic and spectroscopic methods.
Contribution
The paper introduces a comparative analysis of Ru(II)-based dinuclear complexes to understand the role of spacers in photocatalysis.
Findings
Minor structural changes in the complexes significantly influence photocatalytic activity.
The spacer choice determines photophysical and photochemical properties.
Ultrafast spectroscopy and quantum calculations reveal electronic process dynamics.
Abstract
Supramolecular photocatalysts consisting of photosensitizer (PS), bridging ligand (BL), and catalytic center (CAT) have garnered significant attention in solar fuel applications. In this study, the photophysics and photocatalytic properties of two Ru(II)-based dinuclear complexes, specifically [(tbbpy)2Ru(p(Ph)np)Rh(Cp*)Cl]3+ (n = 0, 1; Ru(pp)Rh for n = 0 or Ru(p(Ph)p)Rh for n = 1; tbbpy = 4,4′-di-tert-butyl-2,2′-bipyridine, Cp* = pentamethylcyclopentadienyl, Ph = phenyl, p = 1,10-phenanthroline), are investigated. These complexes are studied as model complexes only differing by the distance between PS and CAT and thus allows a selective investigation of the influence of spacers in light-driven catalysis. A joint synthetic, spectroscopic, and theoretical approach, incorporating time-resolved absorption and emission spectroscopy, resonance Raman (rR) spectroscopy, density functional…
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Taxonomy
TopicsMagnetism in coordination complexes · Lanthanide and Transition Metal Complexes · Catalytic Processes in Materials Science