Biomimetic and Polymeric Catalysis in Water

这一奖项由化学部化学结构、动力学和机制计划颁发，支持哥伦比亚大学罗纳德·布雷斯洛教授研究大分子内部催化作用的努力。这些酶模拟物有许多优点，包括在反应物种周围组织定义明确的三维结构的能力。布雷斯洛教授和他的团队准备了含有咪唑侧链的聚合物，这种聚合物比之前研究得最好的多胺更有效。该小组还研究新的聚合物，包括一些尺寸和形状定义非常严格的聚合物。这些新聚合物被用作生物反应的模拟物，在对生命至关重要的过程中使用硫胺素焦磷酸作为辅酶。在第二个项目中，布雷斯洛教授和他的团队开发了氨基酸、核苷和糖是如何在益生菌地球上形成的证据。这项工作解决了手性结构的形成，这是科学中尚未解开的巨大谜团之一。现代化学的一个主要目标是能够可靠地预测未知化合物的性质。布雷斯洛教授的研究小组和哥伦比亚大学化学系的合作者开发了计算方法，以定量预测形成惯用手的反应的表现程度。他们的方法预测了未知的化学成分，这些化学成分可能会导致制造药物化合物的有用的合成过程。这项研究计划展示了反应如何利用疏水结合在水中进行，同时避免了水与催化基团和底物结合时可能引起的问题。人造酶系统扩大了化学领域，包括多种成分自发结合到催化剂上的过程，就像天然酶一样。水是一种环境友好的溶剂，作为绿色化学的一个组成部分引起了人们的极大兴趣。

This award by the Chemical Structure, Dynamics and Mechanisms Program of the Chemistry Division supports the efforts of Professor Ronald Breslow of Columbia University to study catalysis within the interiors of macromolecules. There are many advantages to these enzyme mimics, including the ability to organize well-defined three-dimensional structures around the reacting species. Professor Breslow and his group prepare polymers containing imidazole sidechains that are even more effective than the best previously-studied polyamines. The group also studies new polymers, including some with very highly defined sizes and shapes. These new polymers are used as mimics for biological reactions that use thiamine pyrophosphate as a coenzyme in processes that are central to life. The catalysts are used for cleaving RNA.In a second project, Professor Breslow and his group develops evidence about how amino acids, nucleosides, and sugars form on prebiotic earth. This work addressed the formation of chiral structures, one of the great unsolved mysteries in science. A major goal of modern chemistry is to be able to predict the properties of unknown compounds reliably. Professor Breslow's research group and collaborators from Columbia University's Chemistry Department develop computational methods to quantitatively predict the extent to which reactions that establish handedness perform. Their methods predict unknown chemistries that could lead to useful synthetic processes for manufacturing medicinal compounds. This research program show how reactions perform in water taking advantage of hydrophobic binding while avoiding the problems that water can cause when it binds to catalytic groups and substrates. The artificial enzyme systems expand the field of chemistry to include processes in which multiple components are spontaneously bound to a catalyst, as happens with natural enzymes. Water is an environmentally benign solvent and is of great interest as a component of Green Chemistry.