DedicatedtoProfessor Norihiro Tokitoh on the occasiono fh is 60th birthdayTo explore the coordination chemistry of dibenzopentalene dianion, reactions of two dilithium dibenzopentalenides having different silyl substituents with Cr(CO) 3 (CH 3 CN) 3 were investigated. The products were unexpected anionic complexes,T he proton at the 9-position is derived from Cr(CO) 3 (CH 3 CN) 3 ,a se videnced by the use of Cr(CO) 3 (CD 3 CN) 3 .T he X-ray diffraction analysis revealed that the chromiumi sc oordinated by an anionic fivemembered ring of the pentalene skeleton, and the lithium atom is coordinated by oxygen atoms of the carbonyl groups. The complexes form ad imer or ac age-liket etramer via carbonyl-lithium interactions,d epending on the bulk of the silyl groups.T he cubic tetramer appears to retain its cage structure in nonpolarsolvents such as benzene.Benzene and cyclopentadienyl anion (Cp À )s erve as 6p-electron-donating ligandsf or transition metals to form h 6 -arene and h 5