From the reaction of C5H5Fe(CO)(CNCH3)2+ and C6F5Li we have isolated, in order of chromatographic elution, C5H5Fe-(CNCH3)2C6F5, C5H5Fe(CO)(CHCH3)C(C6F5)=NCH3 (first isomer), and C5H5Fe(CO)(CNCH3)C(C6F5)=NCH3 (second isomer). The latter two compounds each contain an N-methylpentafluorobenzimido group; these are formally derivatives of acylmetal compounds. Isomer B has a lower stability and converts to isomer A; the latter slowly loses CO to give C5H5Fe-(CNCH3)2C6F5. From the reaction of C5H5Fe(CO)2CNCH3+ and C6F5Li four direct products are characterized including exo-1-C6F5C5H5Fe(CO)2(CNCH3), [C5H5Fe(CO)2]2, C5H5Fe(CO)(CNCH3)C6F5 and C5H5Fe(CO)2C(C6F5)=NCH3. A secondary product, exo-1-CCl3C5H5Fe(CO)2(CNCH3), arose unexpectedly when the crude reaction mixture was treated with chloroform; its precursor could not be determined however. We have also characterized the compound C5H5Fe(CO)-(CNCH3)I, which was believed to arise from reaction of C5H5Fe(CO)2CNCH3+ and I-. © 1969, American Chemical Society. All rights reserved.