Microreaction Engineering of Aqueous Phase Metal Catalyzed Reactions

摘要：哈特曼，瑞安·L。机构：亚拉巴马塔斯卡卢萨大学提案编号：1264630题目：水相金属催化反应的微反应工程知识产权使用水作为反应溶剂有可能影响特种化学品的可持续、连续流制造。成功地设计这样的方法需要克服一些挑战的能力，包括1）控制固体作为反应器表面上的非共价键合材料的形成（例如，规模沉积），2）利用对控制合成转化的基本机制的理解设计有效的催化剂，3）创新新型反应器，其有效地偶联构成精细化学品生产中的中间体的芳族化合物，以及4）将分析与实验室合成工具集成，用于在线反应发现和优化。这项研究将解决这四个挑战。PI计划工程和集成的微反应器与共焦拉曼显微镜，其中的固有动力学和机械知识的钯催化的C-H官能化反应与亲水配体将在没有运输限制。在精细化学品制造中使用亲水性配体，并因此使用水作为反应溶剂，为获得有用化合物的绿色途径提供了机会。PI将结合联合收割机反应器设计原理、分析化学和合成方法，旨在开发一个平台，可用于以水为反应溶剂连续合成精细化学中间体。使能技术将结合以下联合收割机概念：（i）微反应器技术，（ii）用于合成有机反应的亲水配体的设计，（iii）用于反应监测的非侵入性分析技术，以及（iv）涉及反应和分离的多步微化学合成。如果成功，所产生的知识将促进可持续化学工艺设计的新范式：使用水作为溶剂制造精细化学品。更广泛的影响本研究旨在建立对利用水作为溶剂的合成途径的反应器和工艺设计的基本理解。这种理解将以可持续的方式推进合成特种化学品的化学过程。本科生和研究生将受益于这项工作，通过反应工程课程的演变和本科研究机会，为代表性不足的群体。此外，学生K-12+将通过创建在线YouTube视频，通过南加州大学和亚拉巴马大学之间的本科生竞争，旨在先进的化学和反应堆设计概念，真实的世界工程问题和流行文化的接口。这项工作还将通过与凝聚态化学波尔多研究所（ICMCB）的合作，使研究生接触到国际研究经验。这些教育内容将加强亚拉巴马大学的本科工程教育，培养K-12学生对工程职业的早期兴趣，并为研究生提供获得国际曝光的独特机会。

ABSTRACTPI: Hartman, Ryan L.Institutions: University of Alabama TuscaloosaProposal Number: 1264630Title: Microreaction Engineering of Aqueous Phase Metal Catalyzed ReactionsIntellectual Merit The use of water as a reaction solvent has the potential to impact the sustainable, continuous flow manufacturing of specialty chemicals. Successfully engineering such processes require the ability to overcome some challenges, including 1) management of the formation of solids as non-covalently bonded materials on reactor surfaces (e.g., scale deposition), 2) design of efficient catalysts using understanding of the fundamental mechanisms that govern synthetic transformations, 3) innovation of novel reactors that efficiently couple the aromatics that make-up intermediates in fine chemical production, and 4) integration of analytics with laboratory synthesis tools for online reaction discovery and optimization. This research will address each of these four challenges. The PIs plan the engineering and integration of microreactors with confocal Raman microscopy, where the intrinsic kinetic and mechanistic knowledge of palladium-catalyzed C-H functionalization reactions with hydrophilic ligands will be made available in the absence of transport limitations. The use of hydrophilic ligands, and hence water as a reaction solvent, in fine chemical manufacturing presents the opportunity for greener pathways to useful compounds. The PIs will combine reactor design principles, analytical chemistry, and synthetic methodologies aimed at developing a platform, which can be used to continuously synthesize fine chemical intermediates with water as a reaction solvent. The enabling technology will combine concepts of (i) microreactor technology, (ii) the design of hydrophilic ligands for synthetic organic reactions, (iii) non-invasive analytical techniques for reaction monitoring, and (iv) multi-step microchemical synthesis involving reactions and separations. If successful, the knowledge generated will foster a new paradigm of sustainable chemical process design: the use of water as a solvent to manufacture fine chemicals.Broader Impacts This research seeks to establish fundamental understanding of reactor and process design of synthetic pathways that utilize water as a solvent. This understanding will advance chemical processes that synthesize specialty chemicals, in a sustainable way. Undergraduate and graduate students will benefit from this work through the evolution of the reaction engineering curricula and undergraduate research opportunities for underrepresented groups. Furthermore, students K-12+ will be engaged by the creation of online YouTube videos through an undergraduate competition between the University of Southern California and the University of Alabama aimed at the interfacing of advanced chemistry and reactor design concepts, real world engineering problems, and pop culture. The work will also expose graduate students to international research experiences through collaboration with the Institute of Condensed Matter Chemistry Bordeaux (ICMCB). These educational components will strengthen the undergraduate engineering education at the University of Alabama, foster early interest in engineering careers from K-12 students, and provide unique opportunities for graduate students to gain international exposure.