Abstract: A process for the dehydrogenation of alkyl-containing compounds comprises reacting an alkyl-containing compound and a Group VI nitrosyl complex characterized as a transition metal complex having the composition Cp?M(NO)(R1)(R2), wherein Cp? is selected from certain substituted and unsubstituted ?5-cyclopentadienyl groups; M is W or Mo; and R1 and R2 are independently selected from CH2C(CH3)3; CH2Si(CH3)3; CH2(C6H5); CH3; hydrogen; and ?3-allyl; provided that if R1 is hydrogen, R2 is ?3-allyl; under conditions such that the alkyl-containing compound is converted to an olefin, and in particular embodiments, a terminal olefin. The dehydrogenation can be carried out using a neat and/or undried alkyl-containing compound and/or may be conducted under air, and does not require a sacrificial olefin to drive the reaction, thereby increasing convenience and decreasing cost in comparison with some other dehydrogenation processes.