Mechanistic investigation of CO2 hydrogenation by Ru(ii) and Ir(iii) aqua complexes under acidic conditions: two catalytic systems differing in the nature of the rate determining step
作者:Seiji Ogo、Ryota Kabe、Hideki Hayashi、Ryosuke Harada、Shunichi Fukuzumi
DOI:10.1039/b607993h
日期:——
bpy (5) and 4,4′-OMe-bpy (6)} act as catalysts for hydrogenation of CO2 into HCOOH at pH 3.0 in H2O. The active hydride catalysts cannot be observed in the hydrogenation of CO2 with the ruthenium complexes, whereas the active hydride catalysts, [Cp*IrIII(L)(H)]+ L = bpy (7) and 4,4′-OMe-bpy (8)}, have successfully been isolated after the hydrogenation of CO2 with the iridium complexes. The key to the
钌水性络合物[(η 6 -C 6我6)的Ru II(L)(OH 2)] 2+ L =py(1)和4,4'-OMe-bpy(2),py = 2,2'-联吡啶,4,4'-OMe-bpy = 4,4'-二甲氧基-2,2'-联吡啶}和铱水性络合物的[Cp *铱III(L)(OH 2)] 2+ 的Cp * =η 5 -C 5我5,L =py(5)和4,4'-OMe-bpy(6)}充当催化剂 为了 氢化在pH 3.0中将CO 2转化为HCOOH高氧2。活跃的氢化物 催化剂用钌配合物在CO 2加氢中无法观察到氢化物 催化剂,[Cp * Ir III(L)(H)] + L =py(7)和4,4'-OMe-bpy(8)}已成功地用铱络合物将CO 2氢化后分离出来。主动隔离成功的关键氢化物 催化剂是活性炭形成过程中CO 2催化加氢过程中决定速率的步骤的变化氢化物 催化剂[(η 6 -C 6我6)的Ru II(L)(H)]