Department of Chemistry and Biochemistry, University of California at San Diego , 9500 Gilman Drive, La Jolla, California 92093, United States.
J Am Chem Soc. 2017 Jun 21;139(24):8160-8166. doi: 10.1021/jacs.7b01202. Epub 2017 Jun 7.
Previously, we adopted the construction principles of metal-organic frameworks (MOFs) to design a 3D crystalline protein lattice in which pseudospherical ferritin nodes decorated on their C symmetric vertices with Zn coordination sites were connected via a ditopic benzene-dihydroxamate linker. In this work, we have systematically varied both the metal ions presented at the vertices of the ferritin nodes (Zn(II), Ni(II), and Co(II)) and the synthetic dihydroxamate linkers, which yielded an expanded library of 15 ferritin-MOFs with the expected body-centered (cubic or tetragonal) lattice arrangements. Crystallographic and small-angle X-ray scattering (SAXS) analyses indicate that lattice symmetries and dimensions of ferritin-MOFs can be dictated by both the metal and linker components. SAXS measurements on bulk crystalline samples reveal that some ferritin-MOFs can adopt multiple lattice conformations, suggesting dynamic behavior. This work establishes that the self-assembly of ferritin-MOFs is highly robust and that the synthetic modularity that underlies the structural diversity of conventional MOFs can also be applied to the self-assembly of protein-based crystalline materials.
此前，我们采用金属有机骨架（MOFs）的构建原则设计了一个 3D 晶态蛋白质晶格，其中在 C 对称顶点上用 Zn 配位位点装饰的伪球形铁蛋白节点通过二齿苯二羟肟酸连接体连接。在这项工作中，我们系统地改变了铁蛋白节点顶点上呈现的金属离子（Zn(II)、Ni(II)和 Co(II)）和合成的二羟肟酸连接体，得到了扩展的 15 种铁蛋白-MOFs 库，具有预期的体心（立方或四方）晶格排列。晶体学和小角 X 射线散射（SAXS）分析表明，铁蛋白-MOFs 的晶格对称性和尺寸可以由金属和连接体组件共同决定。对块状结晶样品的 SAXS 测量表明，一些铁蛋白-MOFs 可以采用多种晶格构象，表明存在动态行为。这项工作确立了铁蛋白-MOFs 的自组装具有高度的稳健性，并且构成传统 MOFs 结构多样性的合成模块性也可以应用于基于蛋白质的结晶材料的自组装。
