NIRT: Functional Nanoparticle Formation by Block Copolymer Directed Assembly

摘要：Robert Prud'homme，等。提案编号：0506966标题：“NIRT：通过嵌段共聚物定向组装形成功能纳米颗粒”该提案是根据纳米尺度科学与工程计划（NSF 04-043， NIRT类别）收到的。基于他们新发现的通过嵌段共聚物控制的快速沉淀生产纳米颗粒的工艺，pi计划开发对动力学，热力学和聚合物材料科学的全面，基本的理解，从而能够精确控制和设计具有独特光学，机械，化学和生物特性的纳米颗粒。这个多学科团队由三个机构的pi组成（Prud'homme, Kevrekidis, and Panagiotopoulos [Princeton]， Macosko [UMinn]和Fox [ISU]），他们在这个NIRT项目之前就有很强的合作记录。他们的纳米颗粒形成方法，被称为“纳米沉淀”，有三个组成部分：(1)快速和定制的微混合，(2)高过饱和以产生快速成核和生长，(3)稳定新型嵌段共聚物，通过自组装动态阻止生长，产生可调的和极窄的粒径分布。我们的目标是在一个基本的，即分子水平上理解纳米粒子系统是如何形成的，并将这些知识应用于设计新型纳米材料。理解需要从模拟中输入，以模拟跨多个尺度的复杂相互作用：宏观尺度上的湍流微混合，微观尺度上的嵌段共聚物组装和成核和生长。通过模拟，需要同时进行实验工作，以提供组装动力学和粒度分布的基本数据，以验证模拟。通过“纳米沉淀”形成纳米颗粒主要取决于四个时间尺度的控制：(1)在新型反应器中产生过饱和的微混合时间；(2)颗粒成核和生长时间；(3)反应偶联形成嵌段共聚物的时间尺度；(4)嵌段共聚物自组装对空间稳定时间的影响。研究是围绕这些时间尺度组织的，每个方面都需要一个综合的实验研究计划和多尺度建模。微观层面的模拟提供了对形成机制的洞察，并为中尺度的建模提供了输入，在中尺度上，传输和化学的相互作用控制着组装。宏观尺度建模集成了精细尺度的仿真结果，并提供了设计工具，使纳米颗粒的形成可以被操纵，以生产具有医学、印刷和制造业应用的新型功能纳米材料。智力优势：pi希望开发多尺度模拟工具，开辟新的研究领域，超越当前模拟策略的范围，这些策略无法解决超过几十个分子的多个长度尺度或系统尺寸。更广泛的影响：理解和控制纳米颗粒形成过程的进展将超越药物输送和喷墨打印的直接应用，扩展到需要控制尺寸的功能纳米颗粒的广泛应用。研究生研究人员和本科生参与者将在研究项目中接受培训，这些项目本质上是跨学科的，并融入了实际应用。

ABSTRACTPI: Robert Prud'homme, et al. Institution: Princeton University Proposal Number: 0506966Title: "NIRT: FUNCTIONAL NANOPARTICLE FORMATION BY BLOCKCOPOLYMER DIRECTED ASSEMBLY"This proposal was received in response to the Nanoscale Science and Engineering initiative, NSF 04-043, category NIRT. Based on their newly discovered process to produce nanoparticles by block copolymer-controlled rapid precipitation, the PIs plan to develop a comprehensive, fundamental understanding of the kinetics, thermodynamics, and polymer material science that enables the precise control and design of nano-sized particles with unique optical, mechanical, chemical and biological properties. This multidisciplinary team consists of PIs at three institutions (Prud'homme, Kevrekidis, and Panagiotopoulos [Princeton], Macosko [UMinn], and Fox [ISU]), who have a strong record of collaboration that pre-dates this NIRT project.Their approach to nanoparticle formation, termed "NanoPrecipitation", has three components: (1) rapid and tailored micromixing, (2) high supersaturation to produce rapid nucleation and growth, and (3) stabilizing novel block copolymer that kinetically arrest growth by self-assembly to produce tunable and extremely narrow particle size distributions. The goals are to understand at a basic, that is molecular, level how a nanoparticulate system is formed and to apply this knowledge to engineer novel nano materials. Understanding requires input from simulations to model complex interactions across multiple scales: turbulent micromixing at a macroscopic scale, block copolymer assembly and nucleation and growth at a microscale. A simultaneous experimental effort, informed by the simulations, is required to provide basic data on assembly kinetics and particle size distributions to validate the simulations. Nanoparticle formation by "NanoPrecipitation" depends critically on control of four time scales: (1) micromixing time in novel reactors to produce supersaturation; (2) particle nucleation and growth time; (3) the time scale for reactive coupling to form block copolymers, and (4) block copolymer self-assembly to effect steric stabilization time. The research is organized around these timescales, with each aspect requiring an integrated program of experimental research and multi-scale modeling. Simulations at the microscopic level provide insight into formation mechanisms and inputs into the modeling at the mesoscale where the interplay of transport and chemistry controls assembly. Macroscale modeling integrates simulation results from the finer scales, and provides the design tools so that nanoparticle formation can be manipulated to produce novel functional nano materials with applications in medicine, printing and manufacturing.Intellectual merit: The PIs hope to develop multi-scale simulation tools that open new research areas beyond the reach of current simulation strategies which are incapable of addressing multiple length scales or system sizes beyond a few tens of molecules.Broader Impacts: Advances in understanding and controlling the process of nanoparticle formation will extend beyond the direct applications in drug delivery and inkjet printing to a wide range of applications requiring functional nanoparticles of controlled size. Graduate researchers and undergraduate participants will be trained in research projects that are inherently interdisciplinary and infused with real-world applications.