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首页> 外文期刊>Dalton transactions: An international journal of inorganic chemistry >Carrier-facilitated bulk liquid membrane transport of iron(III) hydroxamate complexes utilizing a labile recognition agent and amine recognition in the second coordination sphere
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Carrier-facilitated bulk liquid membrane transport of iron(III) hydroxamate complexes utilizing a labile recognition agent and amine recognition in the second coordination sphere

机译：在第二配位领域中利用不稳定的识别剂和胺识别剂，促进了载运的铁（III）异羟肟酸铁配合物的液膜运输

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摘要

Carrier-facilitated bulk liquid membrane transport from an aqueous source phase through ha chloroform membrane phase to an aqueous receiving phase was studied for various Fe(III) hydroxamate complexes (siderophore mimics) using second coordination sphere recognition. Iron transport systems were designed using a strategy whereby a tetradentate siderophore mimic sequesters iron (III), leaving two labile aquated coordination sites for ternary complex formation. This aquated complex reacts with a bi-functional host/guest molecule capable of acting as a host for the iron complex via ternary complex formation, while simultaneously serving as a guest for a membrane-bound host (carrier). The bi-functional molecules utilized contain a hydroxamate host for Fe(III) binding and a portonated primary amine that can be "recognized" by a liquid membrane-bound hydrophobic ionophore, which carries the hydrophilic Fe(III)-complex across the hydrophobic membrane to an aqueous receiving phase. Four protonated amine hydroxamic acids were investigated as bi-functional host/guest molecules: β-alanine hydroxamic acid (H_2L~(ala))~+, L-glutamic acid γ-monohydroxamic acid (H_3L~(glu))~+, glycine hydroxamic acid (H_2L~(gly))~+, and L-lysine hydroxamic acid (H_3L~(lys))~(2+). These four bidentate ligands were each coordinated to Fe(III) along with the tetradentate N,N'-dihydroxy-N,N'-dimethyldecanediamide (H_2L~8) to form ternary complexes [Fe(L~8)(H_xL~y)~z; x = 1 or 2; y = ala, glu, gly, or lys; z = 0, +1, or +2] that were transported through a chloroform bulk liquid membrane by the lipophilic host carrier cis-dicyclohexano-18-crown-6 (DC18C6). No carrier-dependent flux was observed for Fe(L~8)(HL~(glu)), probably due to intramolecular H-bonding. Flux values for the transport of Fe(L~8)(H_xL~y)~z(x = 1 or 2; y = ala, gly, or lys; z = +1, or +2) facilitated by the membrane carrier (DC18C6) were highest when y = gly and lowest when y = ala. Equilibrium constants pertaining to two-phase distribution or ion pairing, second coordination sphere host-guest formation, and overall extraction were determined and used to rationalize variations in flux values.
机译：使用第二配位球识别技术研究了各种Fe（III）异羟肟酸酯络合物（铁载体模拟物）的载流子促进型液膜从水相通过氯仿膜相转移到水相接收相。铁的运输系统是采用四齿铁载体模拟螯合铁（III）的策略设计的，留下了两个不稳定的水合配位位以形成三元复合物。该水合配合物与双功能主体/客体分子反应，该分子能够通过三元配合物形成充当铁配合物的主体，同时充当膜结合主体（载体）的客体。所利用的双功能分子包含用于Fe（III）结合的异羟肟酸酯主体和可以被液膜结合的疏水性离子载体“识别”的链状伯胺，其通过疏水膜携带亲水性Fe（III）络合物到水接收相。研究了四种质子化胺异羟肟酸作为双功能主体/客体分子：β-丙氨酸异羟肟酸（H_2L〜（ala））〜+，L-谷氨酸γ-单异羟肟酸（H_3L〜（glu））〜+，甘氨酸异羟肟酸（H_2L〜（gly））〜+和L-赖氨酸异羟肟酸（H_3L〜（lys））〜（2+）。这四个双齿配体与四齿的N，N'-二羟基-N，N'-二甲基癸二酰胺（H_2L〜8）配位成Fe（III）形成三元络合物[Fe（L〜8）（H_xL〜y） 〜z; x = 1或2; y = ala，glu，gly或lys; z = 0，+ 1或+2]被亲脂性宿主载体cis-dicyclohexano-18-18-crown-6（DC18C6）转运通过氯仿本体液膜。没有观察到Fe（L〜8）（HL〜（glu））的载流子依赖性通量，可能是由于分子内的H键。由膜载体促进的Fe（L〜8）（H_xL〜y）〜z（x = 1或2; y = ala，gly或lys; z = +1或+2）的运输通量值当y = gly时DC18C6最高，当y = ala时DC18C6最低。确定了与两相分布或离子对，第二配位球主客体形成以及总体提取有关的平衡常数，并将其用于合理化通量值的变化。

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