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Multiple Bond Metatheses Between Carbon Dioxide and the Isocyanide Ligands of Mononuclear Nickel(0) Tetrakis-Isocyanide Complexes: Catalysis By Alkali Metal Ions

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The reaction of the tetrakis-(aryl isocyanide) complex Ni(CNAr)4 (1, Ar=2,6-Me2C6H3) with carbon dioxide in the presence of Li+ leads to the formation of Ni(CO)2(CNAr)2 (2) and the arylisocyanate, ArN=C=O. The tetrakis-(methyl isocyanide) complex Ni(CNMe)4 (3) reacts similarly with carbon dioxide in the presence of Li+ to produce Ni(CO)2(CNMe)2(4). 13C-labeling studies indicate that the carbonyl ligands of Ni(CO)2(CNR)2 are produced by multiple bond metatheses between CO2 and CNR (R=2,6-Me2C6H3, Me) not by deoxygenation of CO2. The reaction of 1 with 13CO2 gave Ni(CO)2(CNAr)2 (2) and ArN=13C=O. The reaction of Ni(13CNMe)4(3*) with CO2 gave Ni(13CO)2(CNMe)2(4*). The reactions are catalytic and first order in [Li+] over the range [Li+]/[1]: 0.01-40. Kinetic studies indicate that the rate of reaction of 1 with CO2 is first order in [C02]. The reaction order in [1] is complex. At high [Li+] and high [CO2], the reaction rate is second order in [1] but the rate saturates and becomes nearly independent of [1] at low [Li+] and low [CO2].

Affiliations: 1: Industrial Catalysis Research Team, Korea Research Institute of Chemical Technology (KRICT), Taejon, 305-606, Korea; 2: Department of Chemistry, Purdue University, 1393 Brown Laboratory, West Lafayette, IN 47907, USA


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