Key Laboratory of Medicinal Molecule Science and Pharmaceutics Engineering, Ministry of Industry and Information Technology, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, Beijing, 102488, China.
College of Chemistry, Fuzhou University, Fuzhou, 350108, China.
Angew Chem Int Ed Engl. 2024 Aug 12;63(33):e202406946. doi: 10.1002/anie.202406946. Epub 2024 Jul 9.
Control of phosphate capture and release is vital in environmental, biological, and pharmaceutical contexts. However, the binding of trivalent phosphate (PO ) in water is exceptionally difficult due to its high hydration energy. Based on the anion coordination chemistry of phosphate, in this study, four charge-neutral tripodal hexaurea receptors (L-L), which were equipped with morpholine and polyethylene glycol terminal groups to enhance their solubility in water, were synthesized to enable the pH-triggered phosphate binding and release in aqueous solutions. Encouragingly, the receptors were found to bind PO anion in a 1 : 1 ratio via hydrogen bonds in 100 % water solutions, with L exhibiting the highest binding constant (1.2×10 M). These represent the first neutral anion ligands to bind phosphate in 100 % water and demonstrate the potential for phosphate capture and release in water through pH-triggered mechanisms, mimicking native phosphate binding proteins. Furthermore, L can also bind multiple bioavailable phosphate species, which may serve as model systems for probing and modulating phosphate homeostasis in biological and biomedical researches.
控制磷酸盐的捕获和释放对于环境、生物和制药领域至关重要。然而,由于三价磷酸盐(PO )的高水合能,其在水中的结合非常困难。基于磷酸盐的阴离子配位化学,本研究合成了四个电荷中性的三脚六元瓜环受体(L-L),它们配备了吗啉和聚乙二醇末端基团以提高其在水中的溶解度,从而能够在水溶液中实现 pH 触发的磷酸盐结合和释放。令人鼓舞的是,这些受体被发现能够通过氢键在 100%的水溶液中以 1:1 的比例结合 PO 阴离子,其中 L 表现出最高的结合常数(1.2×10 M)。这代表了第一个在 100%水中结合磷酸盐的中性阴离子配体,并展示了通过 pH 触发机制在水中捕获和释放磷酸盐的潜力,模拟了天然磷酸盐结合蛋白。此外,L 还可以结合多种生物可用的磷酸盐物种,这可能作为在生物和生物医学研究中探测和调节磷酸盐动态平衡的模型系统。