Total Synthesis Toolkit for Constructing Multi-Catalytic Colloidal Hybrid Nanoparticles

用于构建多催化胶体杂化纳米粒子的全合成工具包

• 批准号: 1213475
• 负责人: Raymond Schaak
• 金额: $ 25万
• 依托单位: Pennsylvania State Univ University Park
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2012
• 资助国家: 美国
• 起止时间: 2012-09-01 至 2014-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1213475&HistoricalAwards=false
• 关键词: Total; Synthesis; Toolkit; Constructing; Multi; Total; Synthesis; Toolkit; Constructing; Multi

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.

宾夕法尼亚州立大学的雷蒙德·沙克（Raymond Schaak）教授得到了大分子，超分子和纳米化学（MSN）计划的支持，目的是为合理构建复杂的胶体混合纳米粒子在多种诱导反应过程中的合理构建提供了一个全合成框架。 这项研究基于最近建立的正交反应性，位点特异性反应性，化学选择性，恢复性，取代效应和耦合化学的纳米颗粒类似物。 反应工具包将扩展到包括新的纳米颗粒转换，线性与径向生长模式以及克服混合纳米颗粒的保护驱除策略？对成核和反应性的自然倾向。 最终，这些合成工具以及对它们发生的理解将扩展我们对如何构建异常复杂的混合纳米颗粒以及如何将纳米颗粒放置在多域粒子上任何所需位置的知识。 这些复杂的胶体混合纳米颗粒将被探索用作多催化剂系统，这些系统将单块反应中的几个顺序催化转化融合在一起。化学主义者通过以逐步的方式将较小的分子构建块合理地修饰并将较小的分子构件链接在一起，以合成大分子的合成。 该过程与无机纳米结构的现有设计能力形成鲜明对比，它以机械考虑和经验指南为指导，并通过广泛的化学转化库来促进。 胶体杂化纳米颗粒包含通过固态界面融合在一起的多个不同的纳米颗粒结构域，可被视为“人造分子”。 这项研究的主要目的是开发新的合成工具，以及对它们工作方式的机理见解，这将有助于弥合复杂分子与可用于混合纳米粒子系统的合成能力之间的差距，而这些分子可用于混合纳米粒子系统，而这些系统的先进程度要少得多。 这些胶体杂化纳米颗粒具有有效地在单个锅中有效进行多种催化反应的模块化系统。 包括一组本科研究人员在内的一群学生将接触到一个独特的跨学科项目，并将积极参与各种外展工作。 将开发一个新的基于询问的本科实验室模块，以将有机合成概念应用于混合纳米粒子系统，并将向学生介绍科学伦理学，化学和社会的界面将被介绍并融入大一新生化学课程中。