The capture,storage,and release of CO_(2)is one of the most pressing issues in chemistry.Herein,we designed bis(formazanate)magnesium complexes as precursors,which were synthesized by straightforward transamination be...The capture,storage,and release of CO_(2)is one of the most pressing issues in chemistry.Herein,we designed bis(formazanate)magnesium complexes as precursors,which were synthesized by straightforward transamination between the neutral formazan[PhNNC(4-tBuPh)NNHPh](LH)and[Mg{N(SiMe_(3))_(2)}_(2)].Depending on the solvent,either the homoleptic complex[L_(2)Mg]or the thf-coordinated complex[L_(2)Mg(thf)]was isolated.Reaction of the solvent-free complex[L_(2)Mg]with CO_(2)led to stoichiometric insertion into one of the four Mg–Nbonds with concomitant rearrangement of the ligand scaffold which adopts a trinuclear cagelike structure.The insertion reaction is reversible depending on thermolysis or treatment with tetrahydrofuran,which is corroborated by density functional theory calculations.This showcases the first example of reversible uptake of CO_(2)by an s-block coordination compound.展开更多
基金D.J.thanks the China Scholarship Council(grant no.201906030178)for generous supportWe also acknowledge support by the state of Baden-Württemberg through bwHPC and DFG through grant no.INST 40/467-1 FUGG(JUSTUS cluster).
文摘The capture,storage,and release of CO_(2)is one of the most pressing issues in chemistry.Herein,we designed bis(formazanate)magnesium complexes as precursors,which were synthesized by straightforward transamination between the neutral formazan[PhNNC(4-tBuPh)NNHPh](LH)and[Mg{N(SiMe_(3))_(2)}_(2)].Depending on the solvent,either the homoleptic complex[L_(2)Mg]or the thf-coordinated complex[L_(2)Mg(thf)]was isolated.Reaction of the solvent-free complex[L_(2)Mg]with CO_(2)led to stoichiometric insertion into one of the four Mg–Nbonds with concomitant rearrangement of the ligand scaffold which adopts a trinuclear cagelike structure.The insertion reaction is reversible depending on thermolysis or treatment with tetrahydrofuran,which is corroborated by density functional theory calculations.This showcases the first example of reversible uptake of CO_(2)by an s-block coordination compound.
