Sterically demanding macrocyclic Eu(iii) complexes for selective recognition of phosphate and real-time monitoring of enzymatically generated adenosine monophosphate.
Sterically demanding macrocyclic Eu(iii) complexes for selective recognition of phosphate and real-time monitoring of enzymatically generated adenosine monophosphate.
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DOI：
10.1039/d1sc05377a
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发表时间：
2022-03-24
期刊：
影响因子：
8.4
通讯作者：
Butler SJ
中科院分区：
文献类型：
--
作者：
Bodman SE;Breen C;Kirkland S;Wheeler S;Robertson E;Plasser F;Butler SJ
在生物相关的水溶液中结合和感应阴离子的分子受体的设计是超分子化学中的一个关键挑战。无机磷酸盐的识别是特别具有挑战性的，因为它的高水合能和pH依赖的形态。腺苷一磷酸（AMP）是一个有价值的，但难以捉摸的超分子检测的目标，因为它的结构相似的更负电荷的阴离子，ATP和ADP。我们报道了两个新的大环Eu（III）受体能够选择性地传感无机磷酸盐和AMP在水中。受体含有空间要求高的8-（苄氧基）喹啉侧臂，其与金属中心配位，产生适合磷酸盐和AMP的结合口袋，同时排除潜在干扰螯合阴离子，特别是ATP、碳酸氢盐和乳酸盐。我们的Eu（iii）受体的传感选择性遵循AMP > ADP > ATP的顺序，这代表了对大多数报道的核苷磷酸受体观察到的选择性顺序的逆转。我们利用独特的主客体诱导的发射强度和寿命的变化，用于检测人血清样品中的无机磷酸盐，并用于实时监测AMP的酶促生产。我们提出了两个新的铕为基础的阴离子受体，选择性地结合无机磷酸盐和AMP在水介质中。它们的传感选择性遵循AMP > ADP > ATP的顺序，代表了对大多数核苷磷酸受体观察到的选择性顺序的逆转。
The design of molecular receptors that bind and sense anions in biologically relevant aqueous solutions is a key challenge in supramolecular chemistry. The recognition of inorganic phosphate is particularly challenging because of its high hydration energy and pH dependent speciation. Adenosine monophosphate (AMP) represents a valuable but elusive target for supramolecular detection because of its structural similarity to the more negatively charged anions, ATP and ADP. We report two new macrocyclic Eu(iii) receptors capable of selectively sensing inorganic phosphate and AMP in water. The receptors contain a sterically demanding 8-(benzyloxy)quinoline pendant arm that coordinates to the metal centre, creating a binding pocket suitable for phosphate and AMP, whilst excluding potentially interfering chelating anions, in particular ATP, bicarbonate and lactate. The sensing selectivity of our Eu(iii) receptors follows the order AMP > ADP > ATP, which represents a reversal of the order of selectivity observed for most reported nucleoside phosphate receptors. We have exploited the unique host–guest induced changes in emission intensity and lifetime for the detection of inorganic phosphate in human serum samples, and for monitoring the enzymatic production of AMP in real-time. We present two new europium-based anion receptors that selectively bind to inorganic phosphate and AMP in aqueous media. Their sensing selectivity follows the order AMP > ADP > ATP, representing a reversal of the selectivity order observed for most nucleoside phosphate receptors.
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使用发光灯笼型复合物在阴离子结合和传感的进步。
影响因子：
8.4
作者：
Bodman SE;Butler SJ
通讯作者：
Butler SJ
影响因子：
2.9
作者：
FREIST, W
通讯作者：
FREIST, W
影响因子：
8.4
作者：
Hewitt SH;Macey G;Mailhot R;Elsegood MRJ;Duarte F;Kenwright AM;Butler SJ
通讯作者：
Butler SJ
影响因子：
4.6
作者：
Huang, Sheng-Yin;Qian, Michelle;Pierre, Valerie C.
通讯作者：
Pierre, Valerie C.
影响因子：
4.3
作者：
Kuchelmeister, Hannes Y.;Schmuck, Carsten
通讯作者：
Schmuck, Carsten