Structural Investigation of Molecularly Engineering Polymers Prepared by Enzymatic Polymerization

酶聚合制备分子工程聚合物的结构研究

• 批准号: 9986644
• 负责人: Ashok Cholli
• 金额: $ 29.4万
• 依托单位: University of Massachusetts Lowell
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2000
• 资助国家: 美国
• 起止时间: 2000-02-01 至 2004-01-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=9986644&HistoricalAwards=false
• 关键词: Structural; Investigation; Molecularly; Engineering; Polymers

The key objective of the proposed research is to understand the basic mechanisms of the oxidative enzymatic polymerization of electroactive polymers using multi-nuclei solution and solid state NMR spectroscopy. This approach involves a simple, one-pot, environmentally compatible reaction that leads to the synthesis of a new class of water soluble, electrically and photonically active polymers. This nobel biocatalytic approach provides, obviates the experimental difficulties previously encountered with traditional chemical reactions and now affords exciting new opportunities to understand these fundamental oxidative mechanisms. NMR spectroscopy will be used extensively in this program both as a probe to understand these oxidative coupling mechanisms and as a tool to optimize the reactions such that the electrical and optical properties of the resulting polymers may be enhanced. The main focus of this effort will involve two sub areas of investigation using both multi-nuclei solution and solid-state NMR techniques: (a) Oxidative coupling mechanisms for phenols and substituted phenols, and (b) Reaction mechanisms of enzymatic polymerization for polyaniline and the role of polyanionic or polycationic templates on enzymatic polymerization. This study will significantly advance the basic understanding of the mechanisms and nature of enzymatic oxidative coupling and as a result allow for the controlled optimization of the reactions. It is expected that this new insight will led to the ability to molecularly engineer a wide variety of novel electroactive polymers that should find wide commercial application.This biocatalytic approach to polymer synthesis is environmentally friendly and offers an effective alternative approach to the synthesis of electroactive polymers. The processing of these enzymatically-synthesized polymers can also be carried out in an environmentally benign manner given their water solubility. Advancement of research in this area thus will help to reduce the use of hazardous chemicals both during the synthetic steps and processing. A deeper understanding of the molecular basis of the enzymatic synthesis may lead to potential technological innovations beneficial to the society.

本研究的主要目标是了解使用多核溶液和固态核磁共振波谱进行电活性聚合物氧化酶聚合的基本机制。 这种方法涉及简单、一锅、环境兼容的反应，从而合成一类新型水溶性、电活性和光活性聚合物。 这种诺贝尔生物催化方法消除了以前传统化学反应遇到的实验困难，现在为了解这些基本氧化机制提供了令人兴奋的新机会。 核磁共振波谱将在该计划中广泛使用，既作为了解这些氧化偶联机制的探针，又作为优化反应的工具，从而增强所得聚合物的电学和光学性能。 这项工作的主要重点将涉及使用多核溶液和固态核磁共振技术进行研究的两个子领域：（a）苯酚和取代苯酚的氧化偶联机制，以及（b）聚苯胺酶聚合的反应机制以及聚阴离子或聚阳离子模板在酶聚合中的作用。 这项研究将显着促进对酶促氧化偶联的机制和性质的基本理解，从而实现反应的受控优化。 预计这一新见解将带来分子工程各种新型电活性聚合物的能力，这些聚合物应该具有广泛的商业应用。这种聚合物合成的生物催化方法是环境友好的，并为电活性聚合物的合成提供了一种有效的替代方法。 鉴于其水溶性，这些酶合成聚合物的加工也可以以环境友好的方式进行。 因此，该领域研究的进步将有助于减少合成步骤和加工过程中危险化学品的使用。 对酶合成的分子基础的更深入了解可能会带来有益于社会的潜在技术创新。