Metal

Alcohol

Catalysis

Reactivity (psychology)

Photochemistry

Embedded system

Computer science

Benzyl alcohol

Alternative medicine

Combinatorial chemistry

Organic chemistry

Dehydrogenation

Atom (system on chip)

Medicine

Chemistry

Selectivity

Pathology

Journal of the American Chemical Society

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.

Catalytic Activity Enhancement on Alcohol Dehydrogenation via Directing Reaction Pathways from Single- to Double-Atom Catalysis