Abstract
This work explores the solid-liquid interface of a rhenium-tricarbonyl complex embedded in a layer of zirconium oxide deposited by atomic layer deposition (ALD). Time-resolved and steady state infrared spectroscopy were applied to reveal the correlations between the thickness of the ALD layer and the spectroscopic response of the system. We observed a transition of the molecular environment from flexible to rigid, as well as limitations to ligand exchange and excited state quenching on the embedded complexes, when the ALD layer is roughly of the same height as the molecules.
Highlights
Inspired by research on the conversion of light energy to chemical energy[1] and heterogeneous photochemical water reduction systems, which are often based on immobilized molecular photosensitizers and catalysts,[2,3] this work aims to investigate the solid/liquid interface of these types of systems
This work explores the solid–liquid interface of a rhenium-tricarbonyl complex embedded in a layer of zirconium oxide deposited by atomic layer deposition (ALD)
We explored different IR spectroscopic methods to probe the degree to which ReP-Cl was covered by the ALD layer: FTIR, transient Vis-pump-IR-probe and 2D-IR spectroscopy
Summary
Inspired by research on the conversion of light energy to chemical energy[1] and heterogeneous photochemical water reduction systems, which are often based on immobilized molecular photosensitizers and catalysts,[2,3] this work aims to investigate the solid/liquid interface of these types of systems They are often comprised of transition metal complexes as photoactive and/or catalytic compounds, which are bound to (transition) metal oxide scaffolds.[4,5,6,7,8] Additional stabilizing layers, deposited by ALD or other methods,[9,10,11,12] have been explored to protect adsorbed molecules against desorption by limiting solvent exposure of the binding site. ALD can be applied to stabilize photoelectrodes against corrosion, and has been used on top of sensitizer- and/or catalyst-functionalized semiconductor surfaces in dye-sensitized solar cells and photoelectrochemical cells.[15,16] As such, ALD seems to be the best method to control the thickness and nature of the deposited cover layer described previously.[13,14,17]
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