NIRT: Functional Nanoparticle Formation by Block Copolymer Directed Assembly

作者声明：Robert Prud‘homme，et al.机构：普林斯顿大学提案编号：0506966标题：NIRT：由BLOCKCOPOLYMER Directed Assembly形成的功能纳米颗粒(NIRT)本提案是响应纳米科学与工程倡议(NSF 04-043，NIRT类别)而收到的。基于他们新发现的通过嵌段共聚控制快速沉淀法生产纳米颗粒的工艺，PI计划对动力学、热力学和聚合物材料科学有一个全面的、基本的了解，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、Kevin reystis和Panagiotopoulos[普林斯顿]、Macosko[UMinn]和Fox[ISU])，他们在NIRT项目之前就有很好的合作记录。他们的纳米粒子形成方法被称为“纳米沉淀”，包括三个组成部分：(1)快速和定制的微观混合，(2)高过饱和度产生快速成核和生长，以及(3)稳定新型嵌段共聚物，通过自组装来动态阻止增长，从而产生可调的和极窄的粒子尺寸分布。我们的目标是在基础上，也就是分子水平上了解纳米颗粒系统是如何形成的，并将这些知识应用于设计新型纳米材料。理解需要通过模拟来模拟多个尺度上的复杂相互作用：宏观尺度上的湍流微观混合、微观尺度上的嵌段共聚物组装以及微观尺度上的成核和生长。在模拟的启发下，需要同时进行实验工作，以提供关于组装动力学和颗粒尺寸分布的基本数据，以验证模拟。纳米粒子的形成依赖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观混合时间；(2)粒子的成核和生长时间；(3)反应耦合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。这项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和多尺度建模计划。微观层面的模拟提供了对形成机制的洞察和对中尺度模拟的投入，在中尺度上，输送和化学的相互作用控制着组装。宏观建模集成了更精细尺度的模拟结果，并提供了设计工具，使纳米颗粒的形成可以被操纵，以产生在医学、印刷和制造中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，超出当前模拟策略的范围，这些领域无法解决超过几十个分子的多种长度尺度或系统尺寸。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，扩展到需要尺寸可控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接受研究项目的培训，这些项目本身就是跨学科的，并融入了现实世界的应用。

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.