Presidential Young Investigators Award

在有机溶剂中使用酶是一项相对较新的技术，它极大地扩展了传统的水基生物催化。然而，在有机合成和基于酶的分析等领域的大量应用仅仅为阐明控制有机介质中的酶催化的原理和参数提供了框架。在PYI奖的过程中，将追求两个长期的研究方向，包括：1)理解和控制决定非水介质中酶催化的参数；2)开发在有机合成中使用酶作为催化剂的方法。第一个目标是研究溶剂对酶结构和功能的作用。EPR自旋标记将被用来探测非水介质中催化过程中的酶活性部位和表面微环境。第二个目标对区域和立体选择性生物转化具有深远的影响。有待研究的具体反应包括合成用于生物降解聚合物的含糖聚酯，过氧化物酶生产的酚醛树脂，作为无甲醛塑料的替代品，以及低聚糖的选择性合成。酶是自然界的催化剂，在温和的条件下表现出强烈的反应特异性和快速的催化速度。传统上，酶被认为是水基催化剂。由于酶在活组织内的水(水)环境中发挥作用，几乎所有酶在生物催化中的应用都涉及到水溶液。不幸的是，对于大多数具有商业意义的反应(例如，制药、合成中间体、塑料生产等)，水不是合适的反应介质。合成化学家很早以前就意识到了这一点，大多数有机反应都是在有机(非水)溶剂中进行的。最近，一些研究小组已经证明，酶在有机溶剂中可以发挥作用。本次PYI奖的研究方向涉及有机介质中酶催化的基础和应用两个方面。从基本观点出发，我们将研究在溶剂中控制酶功能的因素。

The use of enzymes in organic solvents is a relatively new technology that significantly extends conventional aqueous- based biocatalysis. However, the multitude of applications in areas such as organic synthesis and enzyme-based analyses have provided only the framework for elucidating the principles and parameters that govern enzymatic catalysis in organic media. Two long-term research directions will be pursued during the course of the PYI award and include l) the understanding and control of the parameters that dictate enzymatic catalysis in non-aqueous media; and 2) the development of methodologies for the use of enzymes as catalysts in organic synthesis. The first goal involves studying the role of the solvent on enzyme structure and function. EPR spin labeling will be performed to probe enzymic active site and surface microenvironments during catalysis in non-aqueous media. The second goal has far reaching implications for regio-and stereoselective biotransformations. Specific reactions to be studied include the synthesis of sugar-containing polyesters for biodegradable polymers, peroxidase-produced phenolic resins as formaldehyde-free plastics replacements, and selective synthesis of oligosaccharides. Enzymes are nature's catalysts that exhibit keen reaction specificities and fast rates of catalysis under mild conditions. Traditionally, enzymes have been thought of as water-based catalysts. Because enzymes function in a water (aqueous) environment within living tissues, nearly all applications of enzymes in biocatalysis has involved aqueous solutions. Unfortunately, for most reactions of commercial interest (e.g., pharmaceutical manufacture, synthetic intermediates, plastics production, etc.), water is not a suitable reaction medium. Synthetic chemists had realized this long ago, and most organic reactions are routinely performed in organic (non-aqueous) solvents. Recently, a number of research groups have shown that enzymes can function in organic solvents. The research directions being targeted during the course of this PYI award involve both fundamental and applied aspects of enzymatic catalysis in organic media. From a fundamental standpoint, the factors that control enzyme function in solvents will be studied.