Molecularly Imprinted Polymeric Receptors with Interfacial Hydrogen Bonds for Peptide Recognition in Water
Molecularly Imprinted Polymeric Receptors with Interfacial Hydrogen Bonds for Peptide Recognition in Water
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DOI：
10.1021/acsapm.0c00354
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发表时间：
2020-06
影响因子：
5
通讯作者：
M. Zangiabadi;Yan Zhao
中科院分区：
文献类型：
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作者：
M. Zangiabadi;Yan Zhao
蛋白质受体通过疏水和氢键相互作用结合其多肽配体，以获得高亲和力和选择性。然而，由于客体分子的复杂性和密切相关序列之间的细微结构差异，用同样的原理构建多肽的合成受体是具有挑战性的。多肽在表面核心双交联胶束中的分子印迹产生了与多肽疏水侧链互补的疏水口袋。N，N‘-亚甲基双丙烯酰胺(MBAM)等酰胺功能化双丙烯酰胺(MBAM)交联剂在表面活性剂/水界面上形成了一层氢键，增强了多肽在水中的分子识别，尤其是富含极性残基的亲水性多肽。获得了极强的印迹效应，模型三肽的印迹/非印迹比为3000%~10000。这些氢键可以区分密切相关的多肽序列，并能够在水溶液缓冲液中普遍、简单、一锅制得高选择性的受体，用于结合具有~lt；200 nm亲和力的复杂亲水性多肽。
Protein receptors bind their peptide ligands by a combination of hydrophobic and hydrogen-bonding interactions to achieve high affinity and selectivity. Construction of synthetic receptors for peptides by the same principle, however, is challenging because of the complexity of the guest molecules and subtle structural differences among closely related sequences. Molecular imprinting of peptides in surface–core doubly-cross-linked micelles yielded hydrophobic pockets complementary to the hydrophobic side chains of peptides. Amide-functionalized bis(acrylamide) cross-linkers such as N,N′-methylenebis(acrylamide) (MBAm) used in the core cross-linking installed a layer of hydrogen bonds at the surfactant/water interface and was found to enhance the molecular recognition of peptides in water, particularly hydrophilic ones rich in polar residues. An extremely strong imprinting effect was obtained, with the imprinted/nonimprinted ratio ranging from 3000 to 10000 for model tripeptides. These hydrogen bonds allowed distinction of closely related peptide sequences and enabled a general, simple, one-pot preparation of highly selective receptors for binding complex hydrophilic peptides with <200 nM affinity in aqueous buffer.