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The mechanisms of CO2 functionalization promoted by a silylamido N-heterocyclic carbene(NHC) uranium complex M(LD)N″2,where M = U/Ce,LD = OCMe2CH2(1-C{NCH2CH2N-R}),R = 2,6-iPr2-C6H3(abbreviated as Dipp),and N″= N(SiMe3)2,were investigated theoretically.