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Chemical control of structure and guest uptake by a conformationally mobile porous material

机译：构象可移动的多孔材料的化学控制结构和客体吸收

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Metal-organic frameworks (MOFs) are crystalline synthetic porous materials formed by binding organic linkers to metal nodes: they can be either rigid(1,2) or flexible(3). Zeolites and rigid MOFs have widespread applications in sorption, separation and catalysis that arise from their ability to control the arrangement and chemistry of guest molecules in their pores via the shape and functionality of their internal surface, defined by their chemistry and structure(4,5). Their structures correspond to an energy landscape with a single, albeit highly functional, energy minimum. By contrast, proteins function by navigating between multiple metastable structures using bond rotations of the polypeptide(6,7), where each structure lies in one of the minima of a conformational energy landscape and can be selected according to the chemistry of the molecules that interact with the protein. These structural changes are realized through the mechanisms of conformational selection (where a higher-energy minimum characteristic of the protein is stabilized by small-molecule binding) and induced fit (where a small molecule imposes a structure on the protein that is not a minimum in the absence of that molecule)(8). Here we show that rotation about covalent bonds in a peptide linker can change a flexible MOF to afford nine distinct crystal structures, revealing a conformational energy landscape that is characterized by multiple structural minima. The uptake of small-molecule guests by the MOF can be chemically triggered by inducing peptide conformational change. This change transforms the material from a minimum on the landscape that is inactive for guest sorption to an active one. Chemical control of the conformation of a flexible organic linker offers a route to modifying the pore geometry and internal surface chemistry and thus the function of open-framework materials.
机译：金属有机骨架（MOF）是通过将有机连接基与金属结点结合而形成的结晶合成多孔材料：它们可以是刚性的（1,2）或柔性的（3）。沸石和刚性MOF在吸附，分离和催化中具有广泛的应用，这是由于它们能够通过其内表面的形状和功能来控制客体分子在其孔中的排列和化学性质的能力所致（4,5） ）。它们的结构对应于具有单个（尽管功能强大）最低能耗的能源格局。相比之下，蛋白质通过使用多肽的键旋转在多个亚稳结构之间导航来发挥功能（6,7），其中每个结构都位于构象能态的极小值中，可以根据相互作用的分子的化学性质进行选择与蛋白质。这些结构变化是通过构象选择（通过小分子结合稳定蛋白质的高能最小特征）和诱导适应（其中小分子在蛋白质上施加的结构不是最小的）实现的。没有那个分子）（8）。在这里，我们显示了围绕肽接头中共价键的旋转可以改变柔性MOF，以提供9个不同的晶体结构，从而揭示以多个结构极小为特征的构象能态。 MOF可以通过诱导肽构象变化来化学触发MOF对小分子客体的吸收。这一变化将材料从对客体吸附无效的地貌上的最小值转变为有效的物质。柔性有机连接基构型的化学控制为改变孔的几何形状和内部表面化学性质以及开放框架材料的功能提供了一条途径。

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