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首页> 外文期刊>Chemistry: A European journal >Supramolecular bidentate ligands by metal-directed in situ formation of antiparallel beta-sheet structures and application in asymmetric catalysis
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Supramolecular bidentate ligands by metal-directed in situ formation of antiparallel beta-sheet structures and application in asymmetric catalysis

机译：超分子双齿配体的金属定向原位形成反平行β-折叠结构及其在不对称催化中的应用

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摘要

The principles of protein structure design, molecular recognition, and supramolecular and combinatorial chemistry have been applied to develop a convergent metal-ion-assisted self-assembly approach that is a very simple and effective method for the de novo design and the construction of topologically predetermined antiparallel beta-sheet structures and self-assembled catalysts. A new concept of in situ generation of bidentate P-ligands for transition-metal catalysis, in which two complementary, monodentate, peptide-based ligands are brought together by employing peptide secondary structure motif as constructing tool to direct the self-assembly process, is achieved through formation of stable beta-sheet motifs and subsequent control of selectivity. The supramolecular structures were studied by H-1, P-31, and C-13 NMR spectroscopy, ESI mass spectrometry, X-ray structure analysis, and theoretical calculations. Our initial catalysis results confirm the close relationship between the self-assembled sheet conformations and the catalytic activity of these metallopeptides in the asymmetric rhodium-catalyzed hydroformylation. Good catalyst activity and moderate enantioselectivity were observed for the selected combination of catalyst and substrate, but most importantly the concept of this new methodology was successfully proven. This work presents a perspective interface between protein design and supramolecular catalysis for the design of beta-sheet mimetics and screening of libraries of self-organizing supramolecular catalysts.
机译：蛋白质结构设计，分子识别以及超分子和组合化学原理已用于开发会聚的金属离子辅助自组装方法，该方法是从头设计和拓扑预定结构的非常简单有效的方法。反平行的β-折叠结构和自组装催化剂。一种原位生成双齿P-配体用于过渡金属催化的新概念，其中通过利用肽二级结构基序作为构建工具来指导自组装过程，将两个互补的，基于单齿，基于肽的配体结合在一起。通过形成稳定的β-折叠基序并随后控制选择性来实现。通过H-1，P-31和C-13 NMR光谱，ESI质谱，X射线结构分析和理论计算研究了超分子结构。我们的初步催化结果证实了自组装的片状构象与这些金属肽在不对称铑催化的加氢甲酰化反应中的紧密关系。对于所选的催化剂和底物组合，观察到良好的催化剂活性和适度的对映选择性，但最重要的是，这种新方法的概念已得到成功证明。这项工作提出了蛋白质设计和超分子催化之间的透视接口，用于设计β-折叠模拟物和筛选自组织超分子催化剂的文库。

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