Amide complex 9 was synthesized in 87% yield by treating 5 with KN(TMS)2, and it was crystallized with and without 18-crown-6 to give structures of 9-crown (Figure ) and 9 (Scheme 4, middle, and Figure ), respectively. Crown-free 9 is unstable as a solid at room temperature and in solution even at -40 °C, as evidenced by the appearance of multiple new peaks between 11 and -43 ppm in its NMR spectrum after a few days (Figure ). Once this unknown impurity formed, we have been unable to remove it by recrystallization or washing. 9-Crown, however, is more stable. The crystallographic structures of 9 and 9-crown lack axial solvent coordination (despite 9 being crystallized from THF), and their color is the same in coordinating and non-coordinating solvents. These observations suggest that solvent coordination to the N(TMS)2 adduct is unfavorable, possibly because the TMS groups block the axial sites. The crystallographic structure of 9 displays a square planar molecular geometry at iron with τ4 = 0.09-0.11. Fe-N bond lengths in 9 are Fe1-N14 = 1.915(3) and Fe2-N18 = 1.899(3), which are distinguishable. Interestingly, the structure of 9 shows a potassium cation lying in the pincer plane, with a K1-S11 distance of 3.133(1) Å and K2-S15 distance of 3.126(1) Å. The Fe-S bond lengths on the side with potassium are 2.2459(9) Å (Fe1) and 2.2463(9) Å (Fe2), which are indistinguishable. The Fe-S bond length is, however, significantly shorter on the side of the molecule without the close S-K contact, with a difference of 0.0065(12) Å at Fe1 and 0.0080 (12) Å at Fe2. Metrical parameters for 9-crown are shown in Table . The 1 H NMR spectra of 9 and 9crown in THF-d8 have eight and nine, respectively, paramagnetically-shifted peaks between 19 and -68 ppm (Figures and), consistent with C2v symmetry. Their chemical shifts are nearly the same.