College of Chemistry, Jilin University, Changchun 130012, China.
China-Japan Union Hospital of Jilin University, Changchun 130033, China.
Talanta. 2024 Jan 1;266(Pt 2):125068. doi: 10.1016/j.talanta.2023.125068. Epub 2023 Aug 9.
Hydrogen-bonded organic frameworks (HOFs) have emerged as a promising class of materials for applications of separation and enrichment. Utilizing multiple-ligands to construct HOFs is a promising avenue towards the development of structurally stable and functionally diverse frameworks, offering opportunities to create customized binding sites for selective recognition of biomolecules. In recent years, due to the crucial role that protein post-translational modifications (PTMs) play in maintaining protein function and regulating signaling pathways, and the growing recognition of the extensive cross-talk that can occur between PTMs, simultaneous analysis of different types of PTMs represents a requirement of a new generation of enrichment materials. Here, for the first attempt, we report a dual-ligand HOF constructed from borate anion and guanidinium cation for the simultaneous identification of glycopeptides and phosphopeptides, especially mono-phosphopeptides. According to theoretical calculations, the HOF functional sites display a synergistic "matching" effect with mono-phosphopeptides, resulting in a stronger enrichment effect for mono-phosphopeptides as compared to multi-phosphopeptides. Also, due to its high hydrophilicity and boronate affinity, this material can efficiently capture glycoproteins. HOF is set to become an active research direction in the development of highly efficient simultaneous protein enrichment materials, and offers a new approach for comprehensive PTMs analysis.
氢键有机框架（HOFs）作为一种有前途的材料，已被广泛应用于分离和富集领域。利用多配体构建 HOFs 是开发结构稳定且功能多样的框架的一种很有前途的途径，为选择性识别生物分子的定制结合位点创造了机会。近年来，由于蛋白质翻译后修饰（PTMs）在维持蛋白质功能和调节信号通路方面的关键作用，以及 PTMs 之间广泛发生的交叉对话的认识不断加深，同时分析不同类型的 PTMs 成为新一代富集材料的需求。在这里，我们首次报道了一种由硼酸阴离子和胍阳离子构建的双配体 HOF，用于同时鉴定糖肽和磷酸肽，特别是单磷酸肽。根据理论计算，HOF 的功能位点与单磷酸肽显示出协同的“匹配”效应，导致单磷酸肽的富集效果比多磷酸肽更强。此外，由于其高亲水性和硼酸亲和性，该材料可以有效地捕获糖蛋白。HOF 将成为开发高效同时蛋白质富集材料的活跃研究方向，并为全面的 PTMs 分析提供了新方法。
