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首页> 外文期刊>Chemistry: A European journal >Evolution of Actinyl Peroxide Clusters U_(28) in Dilute Electrolyte Solution: Exploring the Transition from Simple Ions to Macroionic Assemblies
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Evolution of Actinyl Peroxide Clusters U_(28) in Dilute Electrolyte Solution: Exploring the Transition from Simple Ions to Macroionic Assemblies

机译：稀电解质溶液中of系过氧化物簇U_（28）的演化：探索从简单离子到大分子组装的转变。

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摘要

Actinyl peroxide clusters, a unique class of uranylcontaining nanoclusters discovered in recent years, are crucial intermediates between the (UO_2)~(2+) aqua-ion monomer and bulk uranyl minerals. Herein, two actinyl polyoxometalate nanoclusters of Cs_(15)[(Ta(O_2)_4)Cs_4K_(12)(UO_2(O_2)_(1.5))_(28)]?20H_2O (CsKU_(28)) and Na_6K_9[(Ta(O_2)_4)Rb_4Na_(12)(UO_2(O_2)_(1.5))_(28)]?20H_2O (RbNaU_(28)) were synthesized by incorporating a central Ta(O_2)_4~(3-) anion that templates a hollow shell of 28 uranyl peroxide polyhedra. When dissolved in aqueous solutions with additional electrolytes, those 1.8 nm-size macroanions self-assembled into spherical, hollow, blackberry-type supramolecular structures, as was characterized by laser-light scattering (LLS) and TEM techniques. These clusters are the smallest macroions reported to date that form blackberry structures in solution, therefore, can be treated as valuable models for investigating the transition from simple ions to macroions. Kinetic studies showed an unusually long lag phase in the initial self-assembly process, which is followed by a rapid formation of the blackberry structures in solution. The small cluster size and high surface-charge density are essential in regulating the supramolecular structure formation, as was shown from the high activation energy barrier of 51.2±2 kJmol~(-1). Different countercations were introduced into the system to investigate the effect of ion binding to the length of the lag phase. The current research provides yet another scale of self-assembly of uranyl peroxide complexes in aqueous media.
机译：in化过氧化物簇是近年来发现的一类独特的含铀酰的纳米簇，是（UO_2）〜（2+）水性离子单体与大量铀酰矿物之间的重要中间体。在此，两个Cs_（15）[（Ta（O_2）_4）Cs_4K_（12）（UO_2（O_2）_（1.5））_（28）]？20H_2O（CsKU_（28））和Na_6K_9 [（通过掺入中心Ta（O_2）_4〜（3-）阴离子合成Ta（O_2）_4）Rb_4Na_（12）（UO_2（O_2）_（1.5））_（28）]？20H_2O（RbNaU_（28））该模板以28个过氧化铀酰多面体的空心壳为模板。当溶解在具有附加电解质的水溶液中时，那些1.8 nm尺寸的大阴离子会自组装成球形，中空的黑莓型超分子结构，这是通过激光散射（LLS）和TEM技术表征的。这些簇是迄今为止报道的在溶液中形成黑莓结构的最小的宏观离子，因此，可以作为研究从简单离子到宏观离子过渡的有价值的模型。动力学研究表明，在初始自组装过程中出现了异常长的滞后阶段，随后在溶液中迅速形成了黑莓结构。如51.2±2 kJmol〜（-1）的高活化能垒所示，小分子簇大小和高表面电荷密度对于调节超分子结构的形成至关重要。将不同的抗衡阳离子引入系统中，以研究离子键合对滞后相长度的影响。当前的研究提供了水性介质中过氧化铀酰复合物自组装的另一种规模。

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