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Journal Article

In situ Detection of Cobaloxime Intermediates During Photocatalysis Using Hollow-Core Photonic Crystal Fiber Microreactors

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Frosz,  Michael
Fibre Fabrication and Glass Studio, Technology Development and Service Units, Max Planck Institute for the Science of Light, Max Planck Society;

External Resource

https://onlinelibrary.wiley.com/doi/10.1002/anie.202214788
(Publisher version)

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Citation

Lawson, T., Gentleman, A. S., Pinnell, J., Eisenschmidt, A., Antón-García, D., Frosz, M., et al. (2023). In situ Detection of Cobaloxime Intermediates During Photocatalysis Using Hollow-Core Photonic Crystal Fiber Microreactors. Angewandte Chemie, International Edition in English, 62(9): e202214788. doi:10.1002/anie.202214788.


Cite as: https://hdl.handle.net/21.11116/0000-000D-0E20-0
Abstract
Hollow-core photonic crystal fibers (HC-PCFs) provide a novel approach for in situ UV/Vis spectroscopy with enhanced detection sensitivity. Here, we demonstrate that longer optical path lengths than afforded by conventional cuvette-based UV/Vis spectroscopy can be used to detect and identify the CoI and CoII states in hydrogen-evolving cobaloxime catalysts, with spectral identification aided by comparison with DFT-simulated spectra. Our findings show that there are two types of signals observed for these molecular catalysts; a transient signal and a steady-state signal, with the former being assigned to the CoI state and the latter being assigned to the CoII state. These observations lend support to a unimolecular pathway, rather than a bimolecular pathway, for hydrogen evolution. This study highlights the utility of fiber-based microreactors for understanding these and a much wider range of homogeneous photocatalytic systems in the future.