To date, only {a very|a really|an extremely|an incredibly} {limited|restricted} {number of|quantity of|variety of} complexes {based|primarily based} on low-valent {main|primary|principal|major|key|most important} group or f-block {elements|components} have {allowed|permitted} the reductive coupling of CO molecules to afford multicarbon oxygenates. Herein, we described the reactivity {of the|from the|in the|on the|with the|of your} divalent thulium {complex|complicated} [Tm(Cpttt)2] (Cpttt = 1,{2|two},4-tris(tert-butyl)cyclopentadienyl) towards CO, {leading|top|major} to selective CO reductive dimerization and trimerization into ethynediolate (C2) and ketenecarboxylate (C3) complexes, respectively. Quantum chemical (DFT) calculations {were|had been|have been} performed to shed light {on the|around the} elementary {steps|actions|measures|methods} of CO homologation and {support|assistance|help} a stepwise chain {growth|development} {from the|in the} C2 {to the|towards the|for the} C3 {product|item|solution} upon addition of {extra|additional|added|further} CO. The attempted decoordination {of the|from the|in the|on the|with the|of your} ethynediolate frag-ment by {treatment|therapy|remedy} with Me3SiI led to dimerization and rearrangement into a {3|three},4-dihydroxyfuran-2-one {complex|complicated}. Investiga-tion {of the|from the|in the|on the|with the|of your} reactivity {of the|from the|in the|on the|with the|of your} C2 and C3 complexes towards other electrophiles led to {unusual|uncommon} functionalization reactions: {while|whilst|although|even though|when|though} the reaction {of the|from the|in the|on the|with the|of your} ketenecarboxylate C3 {complex|complicated} with electrophiles yielded new multicarbon oxygenated complexes, the addition of CO2 {to the|towards the|for the} ethynediolate C2 {complex|complicated} resulted {in the|within the|inside the} formation of {a very|a really|an extremely|an incredibly} reactive intermediate, {allowing|permitting|enabling} C–H activation {of the|from the|in the|on the|with the|of your} toluene solvent. This original intermolecular reactivity corresponds to an unprecedented functionalization of CO-derived ligands, {which is|that is|which can be} induced by CO2. Formula of Potassium Phenoxide Formula of 6-Bromo-3-methoxy-1H-indazole PMID:23775868
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