Cross-reactive binding versus selective phosphate sensing in an imine macrocycle sensor
Cross-reactive binding versus selective phosphate sensing in an imine macrocycle sensor
复制标题
亚胺大环传感器中的交叉反应结合与选择性磷酸盐传感
DOI：
10.1016/j.chempr.2022.05.010
复制
发表时间：
2022
期刊：
影响因子：
23.5
通讯作者：
Anzenbacher, Pavel
中科院分区：
文献类型：
--
作者：
Radujević, Aco;Penavic, Andrej;Pavlović, Radoslav Z.;Badjić, Jovica D.;Anzenbacher, Pavel
我们展示了一种新的方法，适合于分析磷酸盐混合物的化学传感器。在这里，交叉反应性受体和环境敏感性荧光团的组合允许结合各种磷酸盐并获得分析物特异性荧光响应。我们已经研究了一个灵活的和交叉反应的亚胺吡咯大环，包括氢键供体和受体，一个能够自组织响应磷酸盐型阴离子。通过理论和核磁共振（NMR）研究阐明了这种交叉反应性结合。对环境敏感的丹磺酰荧光团进行修饰，其响应于具有不同程度的荧光放大的分析物的存在，导致将交叉反应性结合转化为可变的分析物响应，并使含氧阴离子能够区分。阴离子亲和力的变化趋势为H2 PO 4->AMP> H2 P2 O 72->ADP>ATP。我们发现，只有一个传感器可以区分各种磷酸盐，包括它们的混合物。通过应用机器学习算法，我们能够区分12种阴离子，并准确定量ATP，ADP，AMP，PPi，Pi及其混合物。
We demonstrate a new approach to chemosensors suited for analysis of phosphate mixtures. Here, a combination of a cross-reactive receptor and an environmentally sensitive fluorophore allows for binding various phosphates and obtaining analyte-specific fluorescence response. We have investigated a flexible and cross-reactive imine-pyrrole macrocycle comprising both hydrogen-bond donors and acceptors, one that is capable of self-organizing in response to phosphate-type anions. This cross-reactive binding was elucidated by theoretical and nuclear magnetic resonance (NMR) studies. Incorporating an environmentally sensitive dansyl fluorophore, which responds to the presence of analytes with a varying degree of fluorescence amplification, resulted in translating the cross-reactive binding into variable analyte response and enabled differentiation of oxyanions. The trend of anion affinities is H2PO4−>AMP>H2P2O72−>ADP>ATP. We show that only one sensor can differentiate among various phosphates including their mixtures. By applying machine learning algorithms, we were able to differentiate between 12 anions and accurately quantify ATP, ADP, AMP, PPi, Pi, and their mixtures.