Catalytic Activity Enhancement on Alcohol Dehydrogenation via Directing Reaction Pathways from Single- to Double-Atom Catalysis.
J Am Chem Soc
; 144(11): 4913-4924, 2022 03 23.
Article
en En
| MEDLINE
| ID: mdl-35261231
ABSTRACT
To further improve the intrinsic reactivity of single-atom catalysts (SACs), the controllable modification of a single site by coordinating with a second neighboring metal atom, developing double-atom catalysts (DACs), affords new opportunities. Here we report a catalyst that features two bonded Fe-Co double atoms, which is well represented by an FeCoN6(OH) ensemble with 100% metal dispersion, that work together to switch the reaction mechanism in alcohol dehydrogenation under oxidant-free conditions. Compared with Fe-SAC and Co-SAC, FeCo-DAC displays higher activity performance, yielding the desired products in up to 98% yields. Moreover, a broad diversity of benzyl alcohols and aliphatic alcohols convert into the corresponding dehydrogenated products with excellent yields and high selectivity. The kinetic reaction results show that lower activation energy is obtained by FeCo-DAC than that by Fe-SAC and Co-SAC. Moreover, computational studies demonstrate that the reaction path by DACs is different from that by SACs, providing a rationale for the observed enhancements.
Texto completo:
1
Base de datos:
MEDLINE
Asunto principal:
Etanol
/
Metales
Idioma:
En
Revista:
J Am Chem Soc
Año:
2022
Tipo del documento:
Article