Abstract：
Lysine is one of the most abundant residues on the surface of proteins and its site-selective functionalization is extremely challenging. The existing methods of functionalization rely on differential reactivities of lysine on a protein, making it impossible to label less reactive lysines selectively. We here report polymeric nanoparticles that mimic enzymes involved in the posttranslational modifications of proteins that distinguish the chemical and supramolecular contexts of a lysine and deliver the labeling reagent precisely to its ε amino group. The nanoparticles are prepared through molecular imprinting of cross-linkable surfactant micelles, plus an in situ, on-micelle derivatization of the peptide template prior to the imprinting. The procedures encode the polymeric nanoparticles with all the supramolecular information needed for sequence identification and precise labeling, allowing single-site functionalization of a predetermined lysine on the target protein in a mixture.
摘要：
赖氨酸是蛋白质表面上最丰富的残基之一，其位点选择性官能化极具挑战性。现有的功能化方法依赖于赖氨酸对蛋白质的差异反应性，使得不可能选择性地标记反应性较低的赖氨酸。我们在这里报道了模拟蛋白质翻译后修饰中涉及的酶的聚合物纳米颗粒，这些酶可以区分赖氨酸的化学和超分子环境，并将标记试剂精确地传递到其ε氨基。通过可交联表面活性剂胶束的分子印迹制备纳米粒子，加上一个原位，在压印之前肽模板的胶束上衍生化。这些程序对聚合物纳米颗粒进行编码，具有序列识别和精确标记所需的所有超分子信息，允许在混合物中的靶蛋白上的预定赖氨酸的单位点官能化。
