Dynamically Adaptive Catalytic Capsules on Solid Supports

固体支持物上的动态自适应催化胶囊

• 批准号: EP/I005447/1
• 负责人: Jonathan Nitschke
• 金额: $ 137.61万
• 依托单位: University of Cambridge
• 依托单位国家: 英国
• 项目类别: Fellowship
• 财政年份: 2010
• 资助国家: 英国
• 起止时间: 2010 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FI005447%2F1
• 关键词: Dynamically; Adaptive; Catalytic; Capsules; Solid

The chemist's quest to transform matter has benefitted from tremendous advances in recent years, with new methods and techniques in chemical synthesis appearing at an accelerating pace. The majority of transformations in the synthetic chemist's toolbox require large inputs of energy, organic solvents, and protecting groups that serve as chemical masking tape, fulfilling their purpose and then being discarded. It would be of benefit to reduce the amounts of all three inputs for both ecological and economic reasons.Biological systems carry out chemistry in water efficiently and economically, using assembly lines of enzymes to piece molecules together. Biological receptors and catalysts differ from synthetic versions in that their functions have been honed through the selective pressures of evolution as opposed to design from first principles, allowing their function to be tuned in ways that the cleverest designer might find hard to predict. All living matter bears witness to the incredible chemical and systemic complexity that can be achieved through the 'blind' design of natural selection.The goal of this project is to create a new class of molecular containers capable of evolving to bind different guests with high affinity. This adaptation will find use in the creation of guest-specific sensors and enzyme-like catalysts, as cages are tailor-made to lower the activation energy for specific reactions. The ability to quickly make designer catalysts for different reactions, coupled with the ability to operate in water, could render these catalytic capsules industrially useful as green nano-reactors. Immobilisation of templated capsules on solid supports will allow for the creation of flow reactors (nano assembly lines) and sensors tailored to specific substrates and analytes.

化学家对物质转化的探索得益于近年来的巨大进步，化学合成的新方法和技术正在加速出现。合成化学家工具箱中的大多数转化需要大量的能量、有机溶剂和保护基团的输入，这些保护基团充当化学掩蔽胶带，实现它们的目的，然后被丢弃。从生态和经济的角度来看，减少这三种投入物的数量是有益的。生物系统利用酶的装配线将分子组装在一起，有效而经济地在水中进行化学反应。生物受体和催化剂与合成版本的不同之处在于，它们的功能是通过进化的选择压力而磨练出来的，而不是根据第一原理设计的，这使得它们的功能能够以最聪明的设计师可能难以预测的方式进行调整。所有的生命物质都见证了通过自然选择的“盲目”设计可以实现的令人难以置信的化学和系统复杂性。这个项目的目标是创造一种新型的分子容器，能够进化到以高亲和力结合不同的客人。这种适应将用于创造特定的客人传感器和酶样催化剂，因为笼子是量身定制的，以降低特定反应的活化能。快速制造用于不同反应的设计催化剂的能力，加上在水中操作的能力，可以使这些催化胶囊在工业上用作绿色纳米反应器。将模板化胶囊固定在固体支持物上将允许创建流动反应器（纳米组装线）和针对特定底物和分析物定制的传感器。

项目成果

Selective endo and exo binding of mono- and ditopic ligands to a rhomboidal diporphyrin prism.

• DOI: 10.1002/anie.201501359
• 发表时间: 2015-06
• 期刊: Angewandte Chemie
• 作者: G. Jayamurugan;D. Roberts;Tanya K. Ronson;J. Nitschke

Generation of a dynamic system of three-dimensional tetrahedral polycatenanes.

• DOI: 10.1002/anie.201209708
• 发表时间: 2013-05-27
• 期刊: Angewandte Chemie (International ed. in English)
• 作者: Black SP;Stefankiewicz AR;Smulders MM;Sattler D;Schalley CA;Nitschke JR;Sanders JK
• 通讯作者: Sanders JK