Determinants of Fe2+ over M2+ (M = Mg, Mn, Zn) Selectivity in Non-Heme Iron Proteins,Inorganic Chemistry

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Determinants of Fe2+ over M2+ (M = Mg, Mn, Zn) Selectivity in Non-Heme Iron Proteins
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2016-12-05 00:00:00 , DOI: 10.1021/acs.inorgchem.6b01822
Todor Dudev ₁ , Valia Nikolova ₁

Affiliation

Iron cations are indispensable players in a number of vital biological processes such as respiration, cell division, nitrogen fixation, oxygen transport, nucleotide synthesis, oxidant protection, O₂ activation in the metabolism of various organic substrates, gene regulation, and protein structure stabilization. The basic mechanisms and factors governing the competition between Fe²⁺ and other metal species from the cellular fluids such as Mg²⁺, Mn²⁺, and Zn²⁺ are, however, not well understood, and several outstanding questions remain. (i) How does the Fe²⁺ binding site select the “right” cation and protect itself from attacks by other biogenic cations present in the surrounding milieu? (ii) Do the iron binding sites employ different selectivity strategies toward metal cations possessing different ligand affinities and cytosolic concentrations? (iii) What are the key determinants of metal selectivity in Fe²⁺ proteins? In this study, by employing density functional theory calculations combined with polarizable continuum model computations, we endeavor to address these questions by evaluating the thermodynamic outcome of the competition between Fe²⁺ and Mg²⁺/Mn²⁺/Zn²⁺ in model non-heme mononuclear metal binding sites of various compositions and charge states. The present calculations, which are in line with available experimental data, shed light on the mechanism of Fe²⁺–Mg²⁺/Mn²⁺/Zn²⁺ competition in non-heme iron proteins and disclose the key factors governing the process.

中文翻译：

非血红素铁蛋白中Fe ²⁺超过M ^2+的决定因素（M = Mg，Mn，Zn）

铁阳离子在许多重要的生物学过程中是必不可少的，例如呼吸，细胞分裂，固氮，氧运输，核苷酸合成，氧化剂保护，各种有机底物的代谢中的O ₂活化，基因调节和蛋白质结构稳定。然而，控制Fe ²⁺和其他金属物质从细胞液（如Mg 2 ⁺，Mn ²⁺和Zn ^2+）中竞争的基本机理和因素尚未得到很好的理解，仍然存在一些悬而未决的问题。（i）Fe ²⁺如何结合位点选择“正确的”阳离子，并保护自己免受周围环境中存在的其他生物阳离子的攻击？（ii）铁结合位点对具有不同配体亲和力和胞浆浓度的金属阳离子采用不同的选择性策略吗？（iii）Fe ²⁺蛋白质中金属选择性的关键决定因素是什么？在这项研究中，通过使用密度泛函理论计算与可极化连续体模型计算相结合，我们努力通过评估Fe ²⁺与Mg ²⁺ / Mn ²⁺ / Zn ²⁺之间竞争的热力学结果来解决这些问题。在各种组成和电荷状态的模型非血红素单核金属结合位点中。目前的计算结果与现有的实验数据相吻合，阐明了非血红素铁蛋白中Fe ²⁺ -Mg ²⁺ / Mn ²⁺ / Zn ²⁺竞争的机理，并揭示了控制该过程的关键因素。

更新日期：2016-12-05

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