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

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.

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 Creators:
Lawson, Takashi1, Author
Gentleman, Alexander S. 1, Author
Pinnell, Jonathan1, Author
Eisenschmidt, Annika1, Author
Antón-García, Daniel1, Author
Frosz, Michael2, Author           
Reisner, Erwin1, Author
Euser, Tijmen G.1, Author
Affiliations:
1External, ou_persistent22              
2Fibre Fabrication and Glass Studio, Technology Development and Service Units, Max Planck Institute for the Science of Light, Max Planck Society, ou_2364724              

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 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.

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Language(s): eng - English
 Dates: 2023-02-20
 Publication Status: Issued
 Pages: 8
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1002/anie.202214788
 Degree: -

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Title: Angewandte Chemie, International Edition in English
  Abbreviation : Angew. Chem., Int. Ed. Engl.
Source Genre: Journal
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Publ. Info: Weinheim : Wiley-VCH
Pages: 8 Volume / Issue: 62 (9) Sequence Number: e202214788 Start / End Page: - Identifier: ISSN: 0570-0833
CoNE: https://pure.mpg.de/cone/journals/resource/0570-0833