Molecular Catalyst Synthesis Strategies to Prepare Atomically Dispersed Fe-N-C Heterogeneous Catalysts.
J Am Chem Soc
; 144(41): 18797-18802, 2022 10 19.
Article
in En
| MEDLINE
| ID: mdl-36215721
ABSTRACT
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.
Full text:
1
Collection:
01-internacional
Database:
MEDLINE
Main subject:
Carbon
/
Nitrogen
Language:
En
Journal:
J Am Chem Soc
Year:
2022
Document type:
Article
Affiliation country:
United States