Spatial Engineering Direct Cooperativity between Binding Sites for Uranium Sequestration.

Spatial Engineering Direct Cooperativity between Binding Sites for Uranium Sequestration.
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DOI:
10.1002/advs.202001573
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发表时间:
2021-01
期刊:
Advanced science (Weinheim, Baden-Wurttemberg, Germany)
影响因子:
--
通讯作者:
Ma S
Ma S
中科院分区:
其他
文献类型:
--
作者:
Sun Q;Song Y;Aguila B;Ivanov AS;Bryantsev VS;Ma S

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预组织是自然界使用的一个基本设计原则,它允许表达协同途径。在这里,一个完整的帐户的概念和实验的发展,从随机分布的功能,以一个收敛的安排,促进合作的结合,从而赋予特殊的亲和力对感兴趣的分析物。与使用铀封存作为模型应用的随机和隔离方式相比,以空间锁定方式相邻填充的螯合基团的所得材料显示高达两个数量级的改善。该吸附剂显示出优异的提取效率,能够在10分钟内将铀浓度从5ppm降低到小于1ppb,即使系统渗透有高浓度的竞争离子。其从海水中提取铀的能力进一步支持了其效率,其吸收能力为5.01 mg g−1,使其成为迄今为止描述的最高容量的海水铀提取材料之一。这里提出的概念揭示了一个新的范例,在设计有效的吸附剂材料,通过操纵的空间分布,以放大功能的合作。吸附剂材料中的特定螯合基团对感兴趣的分析物的亲和力通过在适当的布置下设计其空间分布而显著增加,从而驱动协同结合,从而改善性能。
Preorganization is a basic design principle used by nature that allows for synergistic pathways to be expressed. Herein, a full account of the conceptual and experimental development from randomly distributed functionalities to a convergent arrangement that facilitates cooperative binding is given, thus conferring exceptional affinity toward the analyte of interest. The resulting material with chelating groups populated adjacently in a spatially locked manner displays up to two orders of magnitude improvement compared to a random and isolated manner using uranium sequestration as a model application. This adsorbent shows exceptional extraction efficiencies, capable of reducing the uranium concentration from 5 ppm to less than 1 ppb within 10 min, even though the system is permeated with high concentrations of competing ions. The efficiency is further supported by its ability to extract uranium from seawater with an uptake capability of 5.01 mg g−1, placing it among the highest‐capacity seawater uranium extraction materials described to date. The concept presented here uncovers a new paradigm in the design of efficient sorbent materials by manipulating the spatial distribution to amplify the cooperation of functions. The affinity of a specific chelating group in sorbent materials toward analyte of interest is significantly increased through engineering their spatial distribution, at an appropriate arrangement, driving the cooperative binding and thereby improved performance.
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