SusChEM: IUPAC: Harnessing the Unquenched Reactivity of Novel Frustrated Lewis Pairs for Transition Metal-Free Hydrogenation Catalysis

在这个由化学部门化学催化项目资助的项目中，德克萨斯理工大学的Clemens Krempner教授研究了使用受挫刘易斯对（FLPs）作为不饱和有机物质催化氢化过程中昂贵、不丰富和有毒的贵金属的替代品。FLPs是位阻刘易斯酸碱对，由于它们不能形成经典的刘易斯酸碱配合物而具有未淬灭的反应活性。路易斯酸和碱的新组合，能够可逆地切割二氢，确定了结合计算/实验的方法。有吸引力的弱路易斯酸包括硼和硼酸酯，因为这些化合物很容易从廉价的起始材料合成或以低成本商业上可用。磷腈和胍被用作基础组分。通过模块化FLP合成、详细的催化测试以及对新型催化剂和潜在催化机制的计算研究，催化剂开发的进展得到了扩大。该项目由李淑华教授（中国南京大学）和于尔根·克兰克尔迈耶教授（德国亚琛工业大学）合作完成。总之，这三个小组结合他们各自的专业领域，生产亚胺，酮和烯烃的过渡金属无氢化-在制药工业的重要底物。这项工作的广泛影响包括对博士后、研究生和本科生的领导力培训，以及思想和专业知识的国际交流。

In this project, funded by the Chemical Catalysis Program of the Chemistry Division, Professor Clemens Krempner of Texas Tech University examines the use of frustrated Lewis pairs (FLPs) as replacements for expensive, less abundant, and toxic precious metals used in the catalytic hydrogenation of unsaturated organic species. FLPs are sterically-encumbered Lewis acid-base pairs of unquenched reactivity due to their inability to form classical Lewis-acid-base complexes. Novel combinations of Lewis acids and bases, capable of reversibly cleaving dihydrogen, are identified by a combined computational / experimental approach. Attractive weak Lewis acids include boronic and boric esters, as these compounds are readily synthesized from inexpensive starting materials or are commercially available at low cost. Phosphazenes and guanidines are used as the base components. Progress in catalyst development is amplified by the combination of modular FLP synthesis, detailed catalytic testing, and computational investigations on novel catalysts and the underlying catalytic mechanisms. This project is performed in collaboration with Professor Shuhua Li (Nanjing University, Nanjing, China) and Professor Juergen Klankermayer (RWTH Aachen, Aachen, Germany). Together, these three groups combine their separate areas of expertise to produce transition metal-free hydrogenation of imines, ketones and olefins - important substrates in the pharmaceutical industry. The broader impacts of this work include leadership training for postdoctoral fellows and graduate and undergraduate students and an international exchange of ideas and expertise.