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铁结合对五价铀稳定性的影响。

The effect of iron binding on uranyl(v) stability.

作者信息

Faizova Radmila, White Sarah, Scopelliti Rosario, Mazzanti Marinella

机构信息

Institut des Sciences et Ingénierie Chimiques , Ecole Polytechnique Fédérale de Lausanne (EPFL) , CH-1015 Lausanne , Switzerland . Email:

出版信息

Chem Sci. 2018 Aug 14;9(38):7520-7527. doi: 10.1039/c8sc02099j. eCollection 2018 Oct 14.

DOI:10.1039/c8sc02099j
PMID:30319752
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC6179087/
Abstract

Here we report the effect of UO ···Fe cation-cation interactions on the redox properties of uranyl(v) complexes and on their stability with respect to proton induced disproportionation. The tripodal heptadentate Schiff base trensal ligand allowed the synthesis and characterization of the uranyl(vi) complexes [UO(trensal)K], and [UO(Htrensal)], and of uranyl(v) complexes presenting UO ···K or UO ···Fe cation-cation interactions ([UO(trensal)K]K, , [UO(trensal)] [K(2.2.2crypt)][K(2.2.2crypt)], , [UO(trensal)Fe(py)], ). The uranyl(v) complexes show similar stability in pyridine solution, but the presence of Fe bound to the uranyl(v) oxygen leads to increased stability with respect to proton induced disproportionation through the formation of a stable Fe-UO -U intermediate ([UO(trensal)Fe(py)U(trensal)]I, ) upon addition of 2 eq. of PyHCl to . The addition of 2 eq. of PyHCl to results in the immediate formation of U(iv) and UO compounds. The presence of an additional UO bound Fe in [(UO(trensal)Fe(py))Fe(py)]I, , does not lead to increased stability. Redox reactivity and cyclic voltammetry studies also show an increased range of stability of the uranyl(v) species in the presence of Fe with respect both to oxidation and reduction reactions, while the presence of a proton in complex results in a smaller stability range for the uranyl(v) species. Cyclic voltammetry studies also show that the presence of a Fe cation bound through one trensal arm in the trinuclear complex [{UO(trensal)}Fe], does not lead to increased redox stability of the uranyl(v) showing the important role of UO ···Fe cation-cation interactions in increasing the stability of uranyl(v). These results provide an important insight into the role that iron binding may play in stabilizing uranyl(v) compounds in the environmental mineral-mediated reduction of uranium(vi).

摘要

在此，我们报告了UO···Fe阳离子-阳离子相互作用对铀酰（V）配合物氧化还原性质及其在质子诱导歧化反应方面稳定性的影响。三脚架七齿席夫碱trensal配体使得合成并表征了铀酰（VI）配合物[UO(trensal)K]、[UO(Htrensal)]，以及呈现UO···K或UO···Fe阳离子-阳离子相互作用的铀酰（V）配合物（[UO(trensal)K]K、[UO(trensal)][K(2.2.2crypt)][K(2.2.2crypt)]、[UO(trensal)Fe(py)]）。铀酰（V）配合物在吡啶溶液中表现出相似的稳定性，但与铀酰（V）氧原子结合的铁的存在通过在加入2当量PyHCl到[UO(trensal)Fe(py)]时形成稳定的Fe-UO-U中间体（[UO(trensal)Fe(py)U(trensal)]I），导致其在质子诱导歧化反应方面的稳定性增加。向[UO(trensal)K]加入2当量PyHCl会立即形成U(IV)和UO化合物。在[(UO(trensal)Fe(py))Fe(py)]I中额外存在一个与UO结合的铁，并不会导致稳定性增加。氧化还原反应活性和循环伏安法研究还表明，在铁存在的情况下，铀酰（V）物种在氧化和还原反应方面的稳定性范围都有所增加，而配合物中质子的存在导致铀酰（V）物种的稳定性范围变小。循环伏安法研究还表明，在三核配合物[{UO(trensal)}Fe]中通过一个trensal臂结合的铁阳离子的存在，不会导致铀酰（V）的氧化还原稳定性增加，这表明UO···Fe阳离子-阳离子相互作用在提高铀酰（V）稳定性方面的重要作用。这些结果为铁结合在环境矿物介导的铀（VI）还原过程中稳定铀酰（V）化合物可能发挥的作用提供了重要见解。

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