Total Synthesis Toolkit for Constructing Multi-Catalytic Colloidal Hybrid Nanoparticles

宾夕法尼亚州立大学的Raymond Schaak教授得到了大分子、超分子和纳米化学（MSN）项目的支持，致力于开发一种用于多催化反应过程的复杂胶体混合纳米颗粒合理构建的总合成框架。本研究建立在最近建立的纳米颗粒类似物的正交反应性、位点特异性反应性、化学选择性、区域特异性、取代基效应和偶联化学的基础上。反应工具包将扩展到包括新型纳米颗粒转化，线性与径向生长模式，以及克服混合纳米颗粒的保护-去保护策略。成核和反应性的自然倾向。最终，这些合成工具以及对它们如何发生的理解将扩展我们如何构建异常复杂的混合纳米粒子以及如何将纳米粒子放置在多域粒子上的任何所需位置的知识。这些复杂的胶体杂化纳米颗粒将被用作多催化剂系统，在单锅反应中偶联几个顺序的催化转化。化学家们通过逐步合理地修饰和连接较小的分子构建块来合成大分子。这一过程与现有的无机纳米结构设计能力形成鲜明对比，它以机械考虑和经验指导为指导，并由广泛的化学转化库促进。胶体混合纳米粒子包含多个不同的纳米粒子域，通过固态界面融合在一起，可以被认为是“人工分子”。这项研究的一个主要目标是开发新的合成工具，以及对它们如何工作的机制见解，这将有助于弥合复杂分子的合成能力与混合纳米粒子系统的合成能力之间的差距，后者要落后得多。这些胶体混合纳米颗粒具有作为模块化系统的潜力，可以在一个锅中有效地进行多种催化反应。一个不同的学生群体，包括一组本科生研究人员，将接触到一个独特的跨学科项目，并将积极参与各种推广工作。将开发一个新的基于探究的本科实验模块，将有机合成概念应用于混合纳米粒子系统，并将开发向学生介绍科学伦理和化学与社会界面的作业，并将其整合到大一化学课程中。

Professor Raymond Schaak at the Pennsylvania State University is supported by the Macromolecular, Supramolecular, and Nanochemistry (MSN) program in work to develop a total synthesis framework for the rational construction of complex colloidal hybrid nanoparticles for use in multi-catalytic reaction processes. This research builds on recently established nanoparticle analogues of orthogonal reactivity, site-specific reactivity, chemoselectivity, regiospecificity, substituent effects, and coupling chemistry. The reaction toolkit will be expanded to include new classes of nanoparticle transformations, linear vs. radial growth modes, and protection-deprotection strategies for overcoming the hybrid nanoparticles? natural tendencies toward nucleation and reactivity. Ultimately, these synthetic tools and an understanding of how they occur will expand our knowledge of how to construct exceptionally complex hybrid nanoparticles and how to place nanoparticles at any desired location on a multi-domain particle. These complex colloidal hybrid nanoparticles will be explored for use as multi-catalyst systems that couple several sequential catalytic transformations in a single-pot reaction.Chemists approach the synthesis of large molecules by rationally modifying and linking together smaller molecular building blocks in a stepwise manner. This process, which contrasts sharply with existing design capabilities for inorganic nanostructures, is guided by mechanistic considerations and empirical guidelines and is facilitated by an extensive library of chemical transformations. Colloidal hybrid nanoparticles, which contain multiple distinct nanoparticle domains fused together through solid-state interfaces, can be considered as "artificial molecules." A primary goal of this research is to develop new synthetic tools, along with mechanistic insights into how they work, that will help to bridge the gap between the synthetic capabilities that exist for complex molecules vs. those available for hybrid nanoparticle systems, which are much less advanced. These colloidal hybrid nanoparticles have the potential to function as modular systems for efficiently carrying out multiple catalytic reactions in a single pot. A diverse group of students, including a team of undergraduate researchers, will be exposed to a unique cross-disciplinary project and will actively participate in a variety of outreach efforts. A new inquiry-based undergraduate laboratory module to apply organic synthesis concepts to hybrid nanoparticle systems will be developed, and assignments introducing students to scientific ethics and the interface of chemistry and society will be developed and integrated into freshman chemistry courses.