Hydrogenation of Carbon Dioxide Using Half-sandwich Cobalt, Rhodium, and Iridium complexes:DFT study

• 作 者: ChengHou;GuoWang;ZhihanZhang;ZhuofengKe;CunyuanZhao;
• 机 构: School of Chemistry and Chemical Engineering,Sun Yat-sen University,Guangzhou 510275
• 出 处: 第十二届全国量子化学会议
• 发表日期: 2014年期

　　We present a computational insight into the hydrogenation of CO2 catalyzed by a serious of classical catalysts,[Cp*M(6,6-R2-bpy)(OH2)]SO4(M = Co,Rh,Ir,bpy = 2,2-bipyridine,R = OH).Our research has revealed that the mechanism mainly consists of two step,the heterolytic cleavage of H2 and the hydride transfer to the CO2.The heterolytic cleavage is the rate determining step(RDS).The origin of metal effects mainly attributes to the backdonation ability.Two outer sphere different hydride transfer mode was compared and the results suggested that the functional group played a versatile role in the catalytic cycle.These findings are expected to provide useful guidelines for the rational design of highly efficient transition metal catalysts for Carbon Dioxide fixation.