The Exceptional Diversity of Homoleptic Uranium–Methyl Complexes

Homoleptic σ‐bonded uranium–alkyl complexes have been a synthetic target since the Manhattan Project. The current study describes the synthesis and characterization of several unprecedented uranium–methyl complexes. Amongst these complexes, the first example of a homoleptic uranium–alkyl dimer, Li(THF)₄]₂U₂(CH₃)₁₀], as well as a seven‐coordinate uranium–methyl monomer, {Li(OEt₂)Li(OEt₂)₂UMe₇Li}_n were both crystallographically identified. The diversity of complexes reported herein provides critical insight into the structural diversity, electronic structure and bonding in uranium–alkyl chemistry.