Epitaxial Growth of Guanidyl-Functionalized Magnetic Metal–Organic Frameworks with Multiaffinity Sites for Selective Capture of Global Phosphopeptides

作者：Ning Zhang, Ting Huang, Peisi Xie, Zhu Yang, Lan Zhang, Xiaoping Wu, Zongwei Cai · 发表于：ACS Applied Materials & Interfaces · 年份：2022 · DOI：10.1021/acsami.2c10353 · 被引用次数：27 · 研究领域：Metal-Organic Frameworks: Synthesis and Applications、Advanced Nanomaterials in Catalysis、Molecular Sensors and Ion Detection

The flexible and controlled synthesis of metal–organic framework (MOF)-derived hybrid nanostructures is of great significance in fine tuning of their enrichment performance in large-scale and in-depth phosphoproteome analysis. Herein, a magnetic guanidyl-functionalized MOF hybrid coating with multiaffinity sites, denoted as Fe 3 O 4 @G-ZIF-8, was fast fabricated via a one-pot epitaxial growth strategy for the first time and applied for selective and highly efficient enrichment of global phosphopeptides. The intrinsic unsaturated metal sites of ZIF-8 endow the surface-mounted MOF coatings with immobilized metal ion affinity chromatography interaction with multiphosphorylated peptides. The oriented anchoring of bifunctional guanidineacetic acid on the magnetic MOF nanospheres provides additional affinity sites (guanidyl groups) for specific recognition of phosphopeptides by “salt bridge” interaction, as well as active site carboxyl groups for the coordination with the metal ions. The as-prepared Fe 3 O 4 @G-ZIF-8 exhibits large surface area (382.5 m 2 g –1 ), good superparamagnetic property (41.6 emu g –1 ) and stability, and size-exclusion effect (1.73 nm), which can serve as a specific adsorbent for global phosphopeptide analysis with satisfactory selectivity, great detection sensitivity (1 fmol), and rapid magnetic separation. Moreover, the successful application of Fe 3 O 4 @G-ZIF-8 for selective capture of both multi- and mono-phosphopeptides from human saliva and serum de...