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首页> 外文期刊>Chemistry: A European journal >The Solution Structure and Self-Association Properties of the Cyclic Lipodepsipeptide Pseudodesmin A Support Its Pore-Forming Potential
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The Solution Structure and Self-Association Properties of the Cyclic Lipodepsipeptide Pseudodesmin A Support Its Pore-Forming Potential

机译：环状脂肽肽Pseudodesmin A的溶液结构和自缔合特性支持其孔形成潜力。

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摘要

Pseudodesmin A is it cyclic lipodepsipeptide (CLP) of the viscosin group with a moderate in vitro biological activity. For several CLPs, including members of this group, this activity has been related to the ability to form ion pores in cellular membranes. As their size does not allow individual CLPs to span the membrane bilayer, individual monomers must somehow assemble into a larger structure. NMR spectroscopy has been used to demonstrate that in chloroform and other apolar organic solvents, pseudodesmin A monomers assemble into a supramolecular structure. These self-assembled structures can become sufficiently large to span the membrane bilayer as demonstrated with translational diffusion NMR spectroscopic measurements. With the aim to obtain more insight into the structural nature of this assembly, the solution conformation of pseudodesmin A was first determined by using ROESY (rOe) restraints measured in acetonitrile, in which no self-association occurs. The structure, which is found to be mostly similar to the previously described crystal structure. is shown to be retained within the supramolecular complex. Intermolecular rOe contacts obtained in chloroform together with chemical shift perturbation data provides structural insight into the organization of the self-associated complex. Based upon this analysis, a model for the organization of pseudodesmin A monomers in the supramolecular assembly is proposed, which is in agreement with the formation of bilayer spanning hydrophilic pores and provides the basis for a structure-function relationship for this type of CLPs. Finally, it is demonstrated that the differences previously reported between the crystal and solution conformation of the white line inducing principle (WLIP), a close analogue of pseudodesmin A, are the result of the use of dimethyl sulfoxide as solvent, whose strong hydrogen-bonding capacity induces conformational exchange.
机译：Pseudodesmin A是粘性黏膜素基团的环状脂二肽（CLP），具有中等的体外生物学活性。对于包括该组成员在内的几个CLP，这种活性与在细胞膜上形成离子孔的能力有关。由于其尺寸不允许单个CLP跨膜双层，因此单个单体必须以某种方式组装成更大的结构。 NMR光谱已被用于证明在氯仿和其他非极性有机溶剂中，拟除蛋白A单体组装成超分子结构。这些自组装的结构可以变得足够大以跨越膜双层，如通过平移扩散NMR光谱测量所证明的。为了更深入地了解该组件的结构性质，首先使用乙腈中测量的ROESY（rOe）约束条件确定了假结蛋白A的溶液构象，在该约束条件下未发生自缔合。发现该结构与先前描述的晶体结构最相似。显示出保留在超分子复合物中。在氯仿中获得的分子间rOe接触以及化学位移扰动数据为自缔合物的组织提供了结构上的见识。基于此分析，提出了一种在超分子组装体中构建假desmin A单体的模型，该模型与跨亲水孔的双层形成一致，并为此类CLP的结构-功能关系提供了基础。最后，证明先前报道的白线诱导原理（WLIP）的晶体和溶液构象之间的差异是假结蛋白A的近似类似物，是使用二甲亚砜作为溶剂的结果，该溶剂具有很强的氢键作用能力诱导构象交换。

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