Theory and application of polyelectrolyte complexation

聚电解质络合理论与应用

• 批准号: 0852353
• 负责人: Jianzhong Wu
• 金额: $ 32.02万
• 依托单位: University of California-Riverside
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2009
• 资助国家: 美国
• 起止时间: 2009-07-01 至 2014-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0852353&HistoricalAwards=false
• 关键词: Theory; application; polyelectrolyte; complexation

0852353WuInteraction between polyelectrolytes and oppositely charged substances results in various self assembled structures commonplace in industrial settings, health care, and biology. While there is a large body of experimental work on polyelectrolyte complexation, much lagged behind is development of a reliable theoretical tool to describe the underlying structure and thermophysical properties. The theoretical predictions are important not only for engineering applications but also for understanding fundamental biological processes that involve association of oppositely charged biomacromolecules. The proposed research seeks to develop predictive models useful for quantifying structure and thermodynamic stability of polyelectrolyte complexes from a molecular perspective. The theoretical models will be validated with results from molecular simulations and well characterized experimental systems. A case study is also proposed to apply the theoretical tools for understanding genome packaging in viral capsids.Intellectual merit: The theoretical techniques to be used in this research are built uponrecent work in the PI's group in development and application of classical density functional theory (DFT). DFT provides a unifying computational tool for describing the microscopic structure and interfacial behavior of complex molecular systems. Preliminary investigations have demonstrated that it is able to capture both the local packaging and long range electrostatic and intra chain correlations essential for a successful description of strongly charged polyelectrolyte systems. The planned research focuses on development of complementary molecular models for investigating the structure and phase transitions of polyelectrolyte complexes. If successful, accomplishments from this work may open new avenues for understanding diverse molecular self assembly processes and thereby will transform industrial design and practice of both synthetic and natural polyelectrolyte systems.Broader impacts: The generic nature of the theoretical techniques proposed in this work promises applications not only to polyelectrolyte systems but also to the broader fields of complex fluids. In particular, development of advanced computational methods may have unusual impacts in fundamental research toward understanding the molecular basis of viral replication cycle that often entails strong interactions of DNA/RNA chains with oppositely charged polypeptides or proteins. Such understanding is essential for identification of potential drug targets for treatment of virus induced contagious diseases and for formulation of efficient gene/biopharmaceuticals health care delivery systems.This project will provide opportunity for young scientists to gain interdisciplinary research experience and motivate their career interests in molecular modeling and engineering. In addition to supporting one senior graduate student toward his/her advanced degree, this project will recruit at least two undergraduate students from the University Honors Program (UHP) by offering research based thesis projects. Based on the introductory materials related to this research, the PI plans to prepare lectures and special seminars to introduce recent developments in viral self assembly and gene delivery. In addition to UHP, the introductory materials will also be used for the university FastStart summer academy program, designed for high-school students who aspire to biomedical and engineering careers

聚电解质和相反电荷物质之间的相互作用导致各种自组装结构在工业环境、医疗保健和生物中司空见惯。虽然有大量关于聚电解质络合的实验工作，但对于描述底层结构和热物理性质的可靠理论工具的开发却非常滞后。这些理论预测不仅对工程应用很重要，而且对于理解涉及相反电荷的生物大分子结合的基本生物过程也很重要。这项研究旨在从分子的角度开发可用于量化聚电解质络合物的结构和热力学稳定性的预测模型。理论模型将通过分子模拟和具有良好特性的实验系统的结果进行验证。还提出了一个案例研究，以应用理论工具来理解病毒衣壳中的基因组包装。智力优势：本研究中使用的理论技术是建立在PI小组最近在经典密度泛函理论(DFT)的发展和应用方面的工作基础上的。密度泛函理论为描述复杂分子体系的微观结构和界面行为提供了统一的计算工具。初步研究表明，它能够捕捉到对强电荷聚电解质体系的成功描述所必需的局部封装以及长程静电和链内关联。计划中的研究重点是开发互补的分子模型，以研究聚电解质络合物的结构和相变。如果成功，这项工作的成果可能会为理解不同的分子自组装过程开辟新的途径，从而将改变合成和天然聚电解质系统的工业设计和实践。广泛的影响：这项工作中提出的理论技术的一般性不仅适用于聚电解质系统，还将应用于更广泛的复杂流体领域。特别是，先进计算方法的发展可能会对基础研究产生不同寻常的影响，以了解病毒复制周期的分子基础，该分子基础通常需要DNA/RNA链与相反电荷的多肽或蛋白质发生强烈相互作用。这样的了解对于确定治疗病毒引起的传染病的潜在药物靶点和制定有效的基因/生物药物保健传递系统是至关重要的。这个项目将为年轻科学家提供机会，获得跨学科的研究经验，并激发他们对分子建模和工程的职业兴趣。除了支持一名高级研究生攻读他/她的高级学位外，该项目还将通过提供基于研究的论文项目，从大学荣誉计划(UHP)招收至少两名本科生。根据与这项研究相关的介绍性材料，PI计划准备讲座和专题研讨会，介绍病毒自我组装和基因传递的最新进展。除了UHP，这些介绍性材料还将用于大学快速启动暑期学院计划，该计划是为渴望生物医学和工程职业的高中生设计的