Enzyme-Inspired Catalysis in Multifunctional Metal-Organic Framework Materials

这个项目是解决催化剂的合成与设计灵感来自酶，自然界的首要催化剂。酶催化反应的速度比合成催化剂快一百万倍。此外，它们这样做具有无与伦比的选择性，只生产所需的产品。如果工业催化剂的性能和酶一样好，那么商业反应就可以在大大降低能源成本和废物产生的情况下进行。有了这个动机，Gadzikwa博士和她在堪萨斯州立大学的研究小组正在开发酶激发的催化剂，用于将石油原料有效地转化为制药工业的化学原料。这个项目的很大一部分工作是由新手研究人员进行的。因此，Gadzikwa实验室为本科生提供了宝贵的实验室研究经验。Gadzikwa博士正在通过让第一代和代表性不足的少数民族学生参与进来，加强代表性不足群体对科学的参与。通过在弗林特山探索中心为小学生提供便利的活动，通过KState Girls research Our World （GROW）项目为中学生提供便利的活动，以及通过KState年度化学与物理研讨会为高中生提供便利的活动，向公众进行宣传。手性胺是生物活性分子的常见成分，目前通过低效的三步工业过程获得。这些有价值的产品可以通过石油化工过程中大规模生产的未官能化内烯烃的氢胺化更有效地获得。不幸的是，这些所谓的无偏烯烃的反应过于缓慢和不加区分，无法在工业上进行。为了解决这些问题，Gadzikwa博士的实验室正在采用酶的策略，并将它们转移到金属有机框架（MOF）材料的固态支架上。这项工作的动机是假设酶的三个最显著的特征的结合- (i)在形状选择性的密闭空间中分离的催化位点，（ii）在腔内促进和指导反应的侧链，（iii）灵活性，允许腔体在反应途径中强烈结合所有物质，将产生固态催化剂，其活性和选择性最终使无偏置烯烃的反应在工业上可行。本项目涉及到MOF的合成和功能化，这两项工作都是为了适应本科生研究人员的繁忙日程。Gadzikwa实验室吸引了来自堪萨斯路易斯斯托克斯少数民族参与联盟（KS-LSAMP）和堪萨斯州立大学第一代大学生发展学者计划的学生。Gadzikwa实验室还寻求通过公共宣传扩大参与，定期参加向堪萨斯州K-12学生推广化学的活动。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

This project is addressing the synthesis of catalysts with designs inspired by enzymes, Nature's premier catalysts. Enzymes catalyze reactions up to a million times faster than synthetic catalysts. Moreover, they do so with unparalleled selectivity, producing only the desired product. If industrial catalysts performed as well as enzymes, then commercial reactions could be conducted with greatly reduced energy costs and waste generation. With this motivation, Dr. Gadzikwa and her research group at Kansas State University are developing enzyme-inspired catalysts for the efficient conversion of petroleum raw materials into chemical feedstocks for the pharmaceutical industry. A significant portion of the work in this project is being conducted by novice researchers. The Gadzikwa lab is thus providing valuable laboratory research experience for undergraduates. Dr Gadzikwa is enhancing the participation of underrepresented groups in science by engaging first-generation and underrepresented minority students. Outreach to the public is being made by facilitating activities for elementary school children at the Flint Hills Discovery Center, for middle-schoolers through the KState Girls Researching Our World (GROW) program, and for high school students at the KState Annual Chemistry & Physics Symposium.Chiral amines, frequently occurring constituents of biologically active molecules, are currently accessed via an inefficient 3-step industrial process. These valuable products could potentially be obtained more efficiently via the hydroamination of unfunctionalized internal alkenes, which are produced on a large scale via petrochemical processes. Unfortunately, the reactions of these so-called unbiased olefins are prohibitively too slow and indiscriminate to undertake industrially. To address these problems, Dr. Gadzikwa's lab is co-opting the strategies of enzymes and transferring them onto the solid-state scaffold of metal-organic framework (MOF) materials. This work is motivated by the hypothesis that the combination of three of the most distinguishing characteristics of enzymes - (i) catalytic sites isolated within shape-selective, confined spaces, (ii) side chains within the cavities that promote and direct the reaction, and (iii) flexibility that allows the cavity to strongly bind all species in the reaction pathway - will result in solid-state catalysts whose activities and selectivities will finally render the reactions of unbiased olefins industrially feasible. This project involves MOF synthesis and functionalization, both of which are amenable to the busy schedules of undergraduate researchers. The Gadzikwa lab draws students from the Kansas Louis Stokes Alliance for Minority Participation (KS-LSAMP) and the KState Developing Scholars Program for first generation university students. The Gadzikwa lab also seeks to broaden participation via public outreach, routinely participating in activities to promote Chemistry to Kansas' K-12 students.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.