The strategy outlined here differs fundamentally from previously described strategies for the formation of C–N bonds from N2.Typically, carbon electrophiles have been used to create C–N bonds,either from N2 (refs. 11,13,42–45) or nitrides that result from cleavage of N2(refs. 15–17,46). In the proposed reaction, silylation plays a key part bymaking the coordinated N2 sufficiently reactive to accept the migrating aryl group from the metal centre. The silylated amines that areformed can be used in further synthetic steps or can be deprotectedto the parent anilines using mild aqueous acid. In this method, theC–N bond comes from the migration of a hydrocarbyl from a metal toa N2-derived group, a strategy that has been used in few stoichiometricC–N bond formation reactions18,47. The ability of these iron complexesto generate a hydrocarbyl group on the iron through C–H activation,and then transfer it to an activated N2, provides a new tactic for couplinghydrocarbons to N atoms from atmospheric N2, combining the powersof these bond-cleaving reactions.
The strategy outlined here differs fundamentally from previously described strategies for the formation of C–N bonds from N2.<br>Typically, carbon electrophiles have been used to create C–N bonds,<br>either from N2 (refs. 11,13,42–45) or nitrides that result from cleavage of N2<br>(refs. 15–17,46). In the proposed reaction, silylation plays a key part by<br>making the coordinated N2 sufficiently reactive to accept the migrating aryl group from the metal centre. The silylated amines that are<br>formed can be used in further synthetic steps or can be deprotected<br>to the parent anilines using mild aqueous acid. In this method, the<br>C–N bond comes from the migration of a hydrocarbyl from a metal to<br>a N2-derived group, a strategy that has been used in few stoichiometric<br>C–N bond formation reactions18,47. The ability of these iron complexes<br>to generate a hydrocarbyl group on the iron through C–H activation,<br>and then transfer it to an activated N2, provides a new tactic for coupling<br>hydrocarbons to N atoms from atmospheric N2, combining the powers<br>of these bond-cleaving reactions.
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