Gautier-Luneau Isabelle, Merle Claire, Phanon Delphine, Lebrun Colette, Biaso Frédéric, Serratrice Guy, Pierre Jean-Louis
Laboratoire de Chimie Biomimétique, LEDSS, ICMG, UMR CNRS 5616, Université Joseph Fourier, BP 53, 38041 Grenoble Cedex 9, France.
Chemistry. 2005 Mar 18;11(7):2207-19. doi: 10.1002/chem.200401087.
Despite the crucial role of "iron(III) citrate systems" in the iron metabolism of living organisms (bacteria as well as plants or mammals), the coordination chemistry of ferric citrate remains poorly defined. Variations in the experimental conditions used for the preparation of so-called ferric citrates (iron salt, Fe:cit molar ratio, base, pH, temperature, solvent) lead to several different species, which are in equilibrium in solution. To date, six different anionic complexes have been structurally characterized in the solid state, by ourselves or others. In the work described herein, we have established the experimental conditions leading to each of them. Five were obtained from aqueous solution. With the exception of a nonanuclear species (of which fragments have been detected), all were identified in aqueous solution on the basis of electrospray ionization mass spectrometry. In addition, the spectra revealed a new trinuclear species, which could not be crystallized. Kinetic studies of iron uptake from citrate species by iron chelators confirmed the results indicated by the ESI-MS studies. These studies also allowed the relative molar fraction of mononuclear versus polynuclear complexes to be determined, which depends on the Fe:cit molar ratio.
尽管“柠檬酸铁(III)体系”在生物体(细菌、植物或哺乳动物)的铁代谢中起着关键作用,但柠檬酸铁的配位化学仍未得到很好的定义。用于制备所谓柠檬酸铁(铁盐、铁与柠檬酸的摩尔比、碱、pH值、温度、溶剂)的实验条件的变化会导致几种不同的物种,它们在溶液中处于平衡状态。迄今为止,我们自己或其他人已经在固态中对六种不同的阴离子配合物进行了结构表征。在本文所述的工作中,我们确定了导致每种配合物产生的实验条件。其中五种是从水溶液中获得的。除了一种九核物种(已检测到其片段)外,所有物种都是基于电喷雾电离质谱在水溶液中鉴定出来的。此外,光谱还揭示了一种无法结晶的新的三核物种。铁螯合剂从柠檬酸物种中摄取铁的动力学研究证实了电喷雾电离质谱研究所得出的结果。这些研究还能够确定单核与多核配合物的相对摩尔分数,这取决于铁与柠檬酸的摩尔比。