Catalytic
transformation of light alkanes could have considerable
practical value, yet remains one of the most challenging areas in
catalysis research due to the inertness of the C–H bond. Here,
we proposed an efficient ammodehydrogenation (ADeH) catalytic system
for the direct C–N linkage between light alkanes and ammonia
for CH3CN and H2 (CO
x
free) production. This breakthrough is achieved over bifunctional
metal-modified HZSM-5 catalysts, through the tandem dehydrogenation–amination–dehydrogenation
mechanism. We show that ethane ADeH over the Pt/HZSM-5 catalyst can
be realized under atmospheric pressure at temperatures as low as 350
°C. The specific rate of CH3CN is ∼60 μmol/(g
min), and the selectivity is up to 99% under such mild conditions.
The yield of CH3CN increases with increasing temperature;
however, the selectivity decreases due to the formation of HCN, C2H4, and CH4. Additionally, the Pt/HZSM-5
catalyst is coke-resistant during the ADeH owing to the strong interaction
between NH3 and the acid sites of the catalyst. We anticipate
that the proposed ADeH could be extended for the transformation of
various n/iso-alkanes with tunable selectivity to
alkene and nitriles.