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Metal/Support Interactions Regulate Substrate Binding in Fe/Co/Se Cluster Catalysts
Benjamin S Mitchell1, Andrei Chirila1, Daniel Y Zhou1
1Department of Chemistry, University of Washington, Seattle, Washington 98195, United States.
Inorganic Chemistry
|May 25, 2023
Summary
This study explores iron/cobalt-selenide clusters for catalysis. Optimized substrate affinity in these molecular catalysts enables efficient coupling reactions by balancing activation and dissociation.
Area of Science:
- Inorganic Chemistry
- Catalysis
- Materials Science
Background:
- Fe/Co6Se8 molecular clusters are investigated for catalytic applications.
- Understanding substrate affinity is crucial for optimizing catalytic efficiency.
Purpose of the Study:
- To determine the stereoelectronic requirements for achieving optimal substrate affinity in Fe/Co6Se8 clusters.
- To explore the reactivity of iron-nitrenoid intermediates in catalytic coupling reactions.
- To elucidate the role of isocyanide in catalyst stability and reactivity.
Main Methods:
- In situ observation of catalytically competent iron-nitrenoid intermediates.
- Investigation of nitrene transfer and hydrogen-atom abstraction pathways.
- Analysis of the impact of distal structural modifications on catalytic performance.
Main Results:
- A "Goldilocks regime" of substrate affinity was achieved for the coupling of tosyl azide and tert-butyl isocyanide.
- Isocyanide was found to prevent catalyst degradation but can inhibit reactivity at high concentrations.
- Distal changes in the catalyst structure significantly influenced substrate affinity, electronic properties, and catalytic activity.
Conclusions:
- Dynamic interactions between the substrate, active site, and support are key to achieving high catalytic activity.
- Optimized substrate activation coupled with facile dissociation is crucial for efficient catalysis.
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