Molecular Catalyst Synthesis Strategies to Prepare Atomically Dispersed Fe-N‑C Heterogeneous Catalysts

We report a strategy to integrate atomically dispersed iron within a heterogeneous nitrogen-doped carbon (N-C) support, inspired by routes for metalation of molecular macrocyclic iron complexes. The N-C support, derived from pyrolysis of a ZIF-8 metal–organic framework, is metalated via solution-pha...

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Bibliographic Details
Published in:	Journal of the American Chemical Society 2022-10, Vol.144 (41), p.18797-18802
Main Authors:	Bates, Jason S., Khamespanah, Fatemeh, Cullen, David A., Al-Omari, Abdulhadi A., Hopkins, Melissa N., Martinez, Jesse J., Root, Thatcher W., Stahl, Shannon S.
Format:	Article
Language:	eng
Subjects:	Amines Carbon - chemistry catalysts INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY Iron - chemistry materials metalation metals Nitrogen - chemistry oxidation reactions
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Summary:	We report a strategy to integrate atomically dispersed iron within a heterogeneous nitrogen-doped carbon (N-C) support, inspired by routes for metalation of molecular macrocyclic iron complexes. The N-C support, derived from pyrolysis of a ZIF-8 metal–organic framework, is metalated via solution-phase reaction with FeCl2 and tributyl amine, as a Brønsted base, at 150 °C. Fe active sites are characterized by 57Fe Mössbauer spectroscopy and aberration-corrected scanning transmission electron microscopy. The site density can be increased by selective removal of Zn2+ ions from the N-C support prior to metalation, resembling the transmetalation strategy commonly employed for the preparation of molecular Fe-macrocycles. The utility of this approach is validated by the higher catalytic rates (per total Fe) of these materials relative to established Fe-N-C catalysts, benchmarked using an aerobic oxidation reaction.
ISSN:	0002-7863 1520-5126