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Postsynthetic Functionalization of Zr4+-Immobilized Core–Shell Structured Magnetic Covalent Organic Frameworks for Selective Enrichment of Phosphopeptides
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2019-03-20 00:00:00 , DOI: 10.1021/acsami.9b03330 Chaohong Gao 1 , Jing Bai 1 , Yanting He 1 , Qiong Zheng 1 , Wende Ma 1 , Zhixian Lei 1 , Mingyue Zhang 1 , Jie Wu 1 , Fengfu Fu 1 , Zian Lin 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2019-03-20 00:00:00 , DOI: 10.1021/acsami.9b03330 Chaohong Gao 1 , Jing Bai 1 , Yanting He 1 , Qiong Zheng 1 , Wende Ma 1 , Zhixian Lei 1 , Mingyue Zhang 1 , Jie Wu 1 , Fengfu Fu 1 , Zian Lin 1
Affiliation
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Chemical modification of covalent organic frameworks (COFs) is indispensable for integrating functionalities of greater complexity and accessing advanced COF materials suitable for more potential applications. Reported here is a novel strategy for fabricating controllable core–shell structured Zr4+-immobilized magnetic COFs ([email protected]@Zr4+) composed of a high-magnetic-response magnetic colloid nanocrystal cluster (MCNC) core, Zr4+ ion-functionalized two-dimensional COFs as the shell by sequential postsynthetic functionalization and, for the first time, the application of the [email protected]@Zr4+ composites for efficient and selective enrichment of phosphopeptides. The as-prepared [email protected]@Zr4+ composites possess regular porosity with large surface areas, high Zr4+ loading amount, strong magnetic responsiveness, and good thermal/chemical stability, which can serve as an ideal adsorbent for selective enrichment of phosphopeptides and simultaneous size exclusion of biomacromolecules, such as proteins. The high detection sensitivity (10 fmol) together with the excellent recovery of phosphopeptides is also obtained. These outstanding features suggest that the [email protected]@Zr4+ composites are of great benefit for pretreatment prior to mass spectrometry analysis of phosphopeptides. In addition, the performance of the developed approach in selective enrichment of phosphopeptides from the tryptic digests of defatted milk and directly specific capture of endogenous phosphopeptides from human serum gives powerful proof for its high selectivity and effectiveness in identifying the low-abundance phosphopeptides from complicated biological samples. This study not only provides a strategy for versatile functionalization of magnetic COFs but also opens a new avenue in their use in phosphoproteome analysis.
中文翻译：
合成后功能化的Zr 4+固定化的核壳结构磁性共价有机骨架，可选择性富集磷酸肽
共价有机骨架（COF）的化学修饰对于整合功能更复杂的功能以及获得适用于更多潜在应用的高级COF材料是必不可少的。这里报道的是一种新颖的策略，用于制备可控的核-壳结构的Zr 4+固定的磁性COF（[电子邮件保护] @Zr 4+），该COF由高磁响应磁性胶体纳米晶体簇（MCNC）核，Zr 4+组成。离子官能化的二维COFs通过顺序合成后的官能化作用作为壳，并且首次应用[电子邮件保护] @Zr 4+复合材料有效和选择性地富集磷酸肽。准备好的[受电子邮件保护] @Zr 4+复合材料具有规则的孔隙率，大表面积，高Zr 4+负载量，强磁响应性和良好的热/化学稳定性，可作为理想的吸附剂，用于选择性富集磷酸肽并同时排除生物大分子（如蛋白质）的尺寸。还获得了高检测灵敏度（10 fmol）以及出色的磷酸肽回收率。这些出色的功能表明[电子邮件保护] @Zr 4+在磷酸肽的质谱分析之前，这种复合材料对于预处理非常有用。此外，从脱脂牛奶的胰蛋白酶消化物中选择性富集磷酸肽并从人血清中直接特异性捕获内源性磷酸肽的方法的开发性能，为从复杂的生物中鉴定低丰度磷酸肽的高选择性和有效性提供了有力的证据。样品。这项研究不仅为磁性COF的通用功能化提供了策略，而且为它们在磷酸化蛋白质组分析中的使用开辟了一条新途径。
更新日期：2019-03-20
中文翻译：
合成后功能化的Zr 4+固定化的核壳结构磁性共价有机骨架，可选择性富集磷酸肽
共价有机骨架（COF）的化学修饰对于整合功能更复杂的功能以及获得适用于更多潜在应用的高级COF材料是必不可少的。这里报道的是一种新颖的策略，用于制备可控的核-壳结构的Zr 4+固定的磁性COF（[电子邮件保护] @Zr 4+），该COF由高磁响应磁性胶体纳米晶体簇（MCNC）核，Zr 4+组成。离子官能化的二维COFs通过顺序合成后的官能化作用作为壳，并且首次应用[电子邮件保护] @Zr 4+复合材料有效和选择性地富集磷酸肽。准备好的[受电子邮件保护] @Zr 4+复合材料具有规则的孔隙率，大表面积，高Zr 4+负载量，强磁响应性和良好的热/化学稳定性，可作为理想的吸附剂，用于选择性富集磷酸肽并同时排除生物大分子（如蛋白质）的尺寸。还获得了高检测灵敏度（10 fmol）以及出色的磷酸肽回收率。这些出色的功能表明[电子邮件保护] @Zr 4+在磷酸肽的质谱分析之前，这种复合材料对于预处理非常有用。此外，从脱脂牛奶的胰蛋白酶消化物中选择性富集磷酸肽并从人血清中直接特异性捕获内源性磷酸肽的方法的开发性能，为从复杂的生物中鉴定低丰度磷酸肽的高选择性和有效性提供了有力的证据。样品。这项研究不仅为磁性COF的通用功能化提供了策略，而且为它们在磷酸化蛋白质组分析中的使用开辟了一条新途径。
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