Droplet-Based EPR Spectroscopy for Real-Time Monitoring of Liquid-Phase Catalytic Reactions
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Date
2025-07-19
Publication Type
Journal Article
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yes
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Abstract
In situ monitoring is essential for catalytic process design, offering real-time insights into active structures and reactive intermediates. Electron paramagnetic resonance (EPR) spectroscopy excels at probing geometric and electronic properties of paramagnetic species during reactions. Yet, state-of-the-art liquid-phase EPR methods, like flat cells, require custom resonators, consume large amounts of reagents, and are unsuited for tracking initial kinetics or use with solid catalysts. To overcome these limitations, a droplet-based microfluidics platform is introduced for real-time EPR monitoring of liquid-phase catalytic reactions. By encapsulating solid and dissolved species within nanoliter droplets, this approach enables precise control over mass transport, reduces reagent consumption, and maintains uniform residence times irrespective of acquisition duration, permitting precise analysis of each spectral component under identical conditions. The platform's compatibility with standard resonators facilitates straightforward integration into any EPR spectrometer. Its versatility is demonstrated by monitoring dynamic ligand exchange processes, key for activating homogeneous catalysts, and tracking redox and radical kinetics in ascorbic acid oxidation by Cu(II) catalysts. Importantly, this method captures both supported and dissolved transition metal species, offering comprehensive insights into catalyst deactivation via metal leaching. This microfluidic approach sets a new standard for liquid-phase in situ EPR measurements, advancing studies of homogeneous and heterogeneous catalytic systems.
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published
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Journal / series
Volume
9 (7)
Pages / Article No.
2401771
Publisher
Wiley-VCH
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Software
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Subject
Droplet-based microfluidics; in situ electron paramagnetic resonance spectroscopy; kinetic analysis; liquid-phase catalytic reactions; real-time monitoring
Organisational unit
03810 - Jeschke, Gunnar / Jeschke, Gunnar
03871 - Pérez-Ramírez, Javier / Pérez-Ramírez, Javier
03914 - deMello, Andrew / deMello, Andrew
Notes
Funding
180544 - NCCR Catalysis (phase I) (SNF)