Self-Assembled Multicomponent Ligands for Allosteric Catalysis

许多化学转化依赖于催化剂来提高反应速度或有利于形成所需的产品而不是所需的产品。通过采用高效的催化工艺，可以显著降低化学品、聚合物和材料的制造成本。然而，设计新型催化剂的一个重大挑战是，许多催化剂具有复杂的结构，很难合成。化学系的大分子、超分子和纳米化学计划支持俄勒冈大学的Michael Pluth教授开发新的方法，通过简单亚基的自组装来制备复杂结构的催化剂，并研究如何调节这些催化剂的活性。这项研究旨在为催化剂如何按需激活或失活提供新的见解。作为这项研究的科学目标的补充，该项目通过为研究生提供研究培训，帮助为工业界和学术界培养一支劳动力队伍。它还通过促进本科生的研究经验和扩大与当地初中和高中的外展活动来促进STEM教育。普卢斯的研究小组设计并合成了配体，这种配体可以在与“客体”分子结合后自组装成活性催化剂。他的研究旨在提供关于客体分子如何在结合时将信息传递给催化剂的新的基础知识，并使超分子催化的变构调节成为可能。特别令人感兴趣的是研究客体和宿主之间的手性转移，以揭示通过非共价相互作用对手性诱导的新见解。为了证明客体和催化剂之间的手性转移，他的研究小组使用手性客体作为手性辅助因子来实现对映选择性自组装催化剂，并研究了结合对铂和铑催化的氢甲酰化反应的速度和选择性的影响。

Many chemical transformations rely on catalysts to enhance the rate of a reaction or to favor formation of a desired product over an undesired product. The manufacturing costs of chemicals, polymers, and materials can be significantly reduced by employing efficient catalytic processes. A significant challenge in designing new catalysts, however, is that many catalysts have complicated structures and are difficult to synthesize. The Macromolecular, Supramolecular and Nanochemistry Program of the Division of Chemistry supports Professor Michael Pluth of the University of Oregon to develop novel approaches to preparing catalysts of complex structures via self-assembly of simple subunits and to investigate how the activities of these catalysts can be modulated. This research aims to provide new insights into how catalysts can be activated or deactivated on-demand. Complementing the scientific goals of this research, the project helps to prepare a workforce for industry and academia by providing research training to graduate students. It also promotes STEM education by facilitating research experiences for undergraduate students and by expanding outreach activities with local middle- and high schools.Prof. Pluth's research group designs and synthesizes ligands that can self-assemble into active catalysts after binding a "guest" molecule. His research aims to provide new basic knowledge on how guest molecules can transmit information to the catalyst upon binding and enable allosteric regulation of supramolecular catalysis. Of particular interest is the investigation of chirality transfer between guest and host to uncover new insights into chiral induction through non-covalent interactions. To demonstrate chirality transfer between guest and the catalyst, his research group uses chiral guests as chiral co-factors to enable enantioselective self-assembled catalysts and studies the impact of binding on the rate and selectivity of platinum- and rhodium-catalyzed hydroformylation reactions.