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The reaction between {CeCp*2H}2 with CO2 in thf resulted in a new cerium(III) carbonate species, {Ce(Cp*)2(thf)}2(μ-η2:η1-CO3). Investigations into the mechanism suggest the intermediacy of a bridging oxo-complex, {CeCp*2(thf) x }2(μ-O), which could either be formed from the ring opening and oxygen abstraction from an oxygenated solvent such as thf or via insertion of CO2 and elimination of formaldehyde from the resulting methylenediolate intermediate.