Anion-Selective Electrodes Based On a CH-Hydrogen Bonding Bis-macrocyclic Ionophore with a Clamshell Architecture

Anion-Selective Electrodes Based On a CH-Hydrogen Bonding Bis-macrocyclic Ionophore with a Clamshell Architecture
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DOI:
10.1021/acs.analchem.0c04801
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发表时间:
2021-03-26
影响因子:
7.4
通讯作者:
Bachas,Leonidas G.
Bachas,Leonidas G.
中科院分区:
化学1区
文献类型:
--
作者:
Zeynaloo,Elnaz;Zahran,Elsayed M.;Bachas,Leonidas G.

文献摘要

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ch -氢键为制造具有高度预组织和选择性阴离子识别的大环离子载体提供了新的构建块。在这项研究中,阴离子结合的离子载体在一个蛤壳(ClS)的形状被采用,它是由两个蓝星(CNstar)大环与预先组织的空腔与一个12碳链连接。这个离子载体允许通过ch -氢键进行阴离子络合。对含该离子载体的膜基离子选择电极的电位性能进行了评价。制备了不同的膜组成,以确定膜中离子载体和亲脂添加剂的最佳浓度。优化后的电极斜率为- 58.2 mV/decade,对碘化物具有抗hofmeister选择性,检测限为纳摩尔。采用电喷雾电离质谱法研究了ClS与不同阴离子的相对结合强度。观察到的离子-离子团络合物的质量峰与相应电极的电位选择模式一致。总的来说,电极的选择性可以通过使用离子载体来改变,在离子载体中,两个CNstar大环通过一个柔性的12碳链连接在一起,以控制结合事件的分子性。
CH-hydrogen bonding provides access to new building blocks for making macrocyclic ionophores with high degrees of preorganization and selective anion recognition. In this study, an anion-binding ionophore in the shape of a clamshell (ClS) was employed that is composed of two cyanostar (CNstar) macrocycles with preorganized cavities linked with a 12-carbon chain. This ionophore allows for anion complexation by CH-hydrogen bonding. The potentiometric performance of membrane-based ion-selective electrodes incorporating this ionophore was evaluated. Different membrane compositions were prepared to determine the optimum concentrations of the ionophore and lipophilic additive in the membrane. The optimized electrode had a slope of −58.2 mV/decade and demonstrated ananti-Hofmeister selectivity pattern toward iodide with a nanomolar detection limit. Electrospray ionization mass spectrometry was employed to study the relative association strengths of ClS with various anions. The observed mass peaks of the ion–ionophore complexes were found to be consistent with the potentiometric selectivity pattern of the corresponding electrodes. Overall, the selectivity of the electrode could be altered by using an ionophore in which the two CNstar macrocycles are linked together with a flexible 12-carbon chain to control the molecularity of the binding event.