Collman J P, Brauman J I, Halbert T R, Suslick K S
Proc Natl Acad Sci U S A. 1976 Oct;73(10):3333-7. doi: 10.1073/pnas.73.10.3333.
The O2 vibration of dioxygen adducts of Fe and Co model complexes of alpha,alpha,alpha,alpha-tetrapivalamidophenylporphyrin ("picket fence" porphyrin, TpivPP) with 1-methylimidazole and 1-tritylimidazole as axial bases are reported, obtained with difference techniques between 16O2, 18O2, 169-18O, and NO with a Fourier transform infrared spectrometer. Assignments of upsilono2 are (O2)Fe(TpivPP) 1-methylimidazole, 1159 cm-1 in Nujol; (O2)Fe(TpivPP) 1-tritylimidazole, 1163 in benzene; (O2)Co(TpivPP) 1-methylimidazole, 1150 in Nujol; (O2)Co(TpivPP) 1-tritylimidazole, 1153 in benzene. Comparisons with other known Fe, Co, Cr, and Ti dioxygen complexes are made, and it is concluded that the bent dioxygen ligand is best viewed as bound superoxide, O2-. The CO affinities of various hemoproteins and model systems are discussed. A correlation between the CO stretching frequency and its binding constant is described. The drastically lowered affinity of hemoproteins for CO compared with unencumbered models is attributed to steric hindrance in the distal binding site, which allows discrimination between the already bent FeIII-O2- and the normally linear FeII-CO systems. If the affinity of hemoproteins in living systems for CO relative to O2 were not decreased, then massive poisoning would result from endogenous CO.
报道了α,α,α,α-四新戊酰胺基苯基卟啉(“栅栏”卟啉,TpivPP)的铁和钴模型配合物与1-甲基咪唑和1-三苯甲基咪唑作为轴向碱的双氧加合物的O₂振动情况,使用傅里叶变换红外光谱仪通过16O₂、18O₂、¹⁶⁹-¹⁸O和NO之间的差值技术获得。υO₂的归属为:(O₂)Fe(TpivPP) 1-甲基咪唑,在石蜡油中为1159 cm⁻¹;(O₂)Fe(TpivPP) 1-三苯甲基咪唑,在苯中为1163;(O₂)Co(TpivPP) 1-甲基咪唑,在石蜡油中为1150;(O₂)Co(TpivPP) 1-三苯甲基咪唑,在苯中为1153。与其他已知的铁、钴、铬和钛双氧配合物进行了比较,得出的结论是弯曲的双氧配体最好被视为结合的超氧化物O₂⁻。讨论了各种血红蛋白和模型系统对CO的亲和力。描述了CO伸缩频率与其结合常数之间的相关性。与无阻碍的模型相比,血红蛋白对CO的亲和力大幅降低归因于远端结合位点的空间位阻,这使得能够区分已经弯曲的FeIII-O₂⁻和正常线性的FeII-CO系统。如果生物系统中的血红蛋白对CO相对于O₂的亲和力没有降低,那么内源性CO将导致大规模中毒。