Organo-f element Chemistry: Integrated Synthetic, Mechanistic, and Catalytic and Thermochemical Studies

美国国家科学基金会化学部的化学催化项目支持西北大学的托宾·马克斯教授领导四个紧密相连的研究项目，将研究与教育相结合，专注于新的和不寻常的催化转化的基础和面向技术的方面，主要涉及丰富的稀土元素、榄系元素和相关的早期过渡金属元素。我们的目标是使用实验成键能量信息来了解不寻常的成键模式，了解已知的化学计量和催化转化，并预测元素周期表这一部分中的新转化。该项目旨在通过以下研究阐明发明新的、高效、有用、原子效率高和环境可接受的“绿色”催化工艺的原理：1)催化金属-杂元素化学--氢化和氢功能化；2)催化材料合成；3)多核催化；4)离子液体中的亲电稀土催化--氢化及其微观反转。在研究中，学生从事新催化剂的合成和提纯，表征其分子结构和动力学，将这些催化剂应用于探索性反应活性研究、分子模拟和电子结构计算，并严格阐明反应动力学和机理。学生还将熟悉聚合反应方法，并深入了解聚合物的微观结构、流变学、分子量和热特性。发现、理解、改进和应用涉及含有金属-碳和金属杂原子的分子和碎片的化学转化对美国化学工业至关重要。这些转变包括高效、原子经济的催化工艺，用于大规模生产燃料、塑料、药品和其他重要的经济化学品。此外，建立广泛的化学知识库和这一领域技术熟练的国家研究人员专家队伍，对于开发更具选择性、对环境无害和具有经济竞争力的技术至关重要。国家还需要为核工业培训基础重元素化学的研究人员。该项目专注于有机金属/催化/材料化学，目的是影响、表征、理解和向社区传播不同寻常的和潜在有用的新的化学计量和催化反应原理，以及对成键和成键能量学的新见解。这些研究/教育活动有意让青年科学家参与知识创造的方方面面。参与这个具有挑战性的多方面/多学科项目，包括与工业科学家的互动，将为具有不同背景的研究生、本科生和博士后学生在工业、政府实验室和学术界从事富有成效的职业生涯做好准备。

The Chemical Catalysis Program in the Chemistry Division at the National Science Foundation supports Professor Tobin Marks of Northwestern University to lead four closely interlinked research thrusts, integrating research and education, and focusing on fundamental and technologically-oriented aspects of new and unusual catalytic transformations, primarily involving abundant lanthanide, actinide, and related early transition metal elements. The goal is to use experimental bonding energetic information to understand unusual bonding modes, to understand known stoichiometric and catalytic transformations, and to predict new ones in this part of the Periodic Table. The project seeks to elucidate principals for inventing new, efficient, useful, atom-efficient, and environmentally acceptable "green" catalytic processes by investigating: 1) catalytic metal-heteroelement chemistry--hydroelementation and hydro-functionalization; 2) catalytic materials synthesis; 3) multinuclear catalysis; 4) electrophilic lanthanide catalysis in ionic liquids--hydroelementation and its microscopic reverse. In carrying out research, students engage in the synthesis and purification of new catalysts, characterizing their molecular structures and dynamics, implementing these catalysts in exploratory reactivity studies, molecular modeling and electronic structure computation, and rigorous elucidation of reaction kinetics and mechanism. Students also become familiar with polymerization reaction methodologies and with in-depth polymer microstructure, rheology, molecular weight, and thermal characterization. Discovering, understanding, improving, and applying chemical transformations involving metal-carbon and metal-heteroatom containing molecules and fragments are of central importance to the U.S. chemical industry. These transformations include efficient, atom-economical catalytic processes for the production of fuels, plastics, pharmaceuticals, and other economically important chemicals on a huge scale. Furthermore, creating a broad chemical knowledge base and a technically skilled national cadre of researchers expert in this field is crucial to developing ever more selective, environmentally benign, and economically competitive technologies. There is also a national need for researchers trained in basic heavy element chemistry for the nuclear industry. This project focuses on organometallic/catalytic/materials chemistry with the goal being to effect, characterize, understand, and disseminate to the community, unusual and potentially useful new stoichiometric and catalytic reactivity principals, as well as new insights into bonding and bonding energetics. These research/education activities deliberately involve young scientists in all aspects of this knowledge creation. Participation in this challenging, multifaceted/multidisciplinary project, including interactions with industrial scientists, will prepare graduate, undergraduate, and postdoctoral students, having diverse backgrounds, for productive careers in industry, government laboratories, and academe.