CAS: New Nonheme Iron Complexes for NOx Reduction, Mechanism, and Catalysis

约翰霍普金斯大学的大卫·P·戈德堡和萨拉·托伊教授试图了解仿生铁复合物如何与氮氧化物（NOx）物种反应。生物学中的NOx物种及其与金属离子的相互作用涉及细胞应激、信号转导和酶功能。其他类似的氮氧化物（HNO）由于其独特的生物活性而引起了人们的极大兴趣，包括其作为信号分子，抗氧化剂以及作为心力衰竭和癌症的药理学试剂的可能作用。 氮氧化物反应性的生物机制的理解将通过检查合成，仿生系统。特别是，Goldberg和Thoi的研究提供了有关一氧化氮和其他含氮气体以及氨的途径的新的基础知识。 一个目的是研究酸对铁与氮氧化物相互作用的影响。该团队还研究了产生HNO的新方法，HNO是铁基反应中的一种拟议的关键中间体。催化研究需要使用电解来评估反应途径。参与该项目的学生接受科学方法的培训，为他们在教育，研究和工业中的职业做好准备。本研究项目是在Goldberg实验室，结合Thoi实验室的电化学和电催化研究，设计、合成并研究用于NOx活化的非血红素铁络合物，并进行机理研究。这种协同作用的方法导致新的信息，结构与功能的生物相关性和环境意义的复合物。生物学中的NOx物种及其与金属离子的相互作用涉及细胞应激、信号转导和酶功能。M/NOx物种的环境意义来自全球氮循环，其涉及相互转化N2、NH3和NOx物种的氧化和还原途径。 研究生接受实验化学科学的培训，重点是生物无机化学，电化学，合成，催化，化学仪器和机制。研究人员和他们的研究生参加了巴尔的摩市的小学和高中外展计划。该奖项反映了NSF的法定使命，并被认为值得通过使用基金会的智力价值和更广泛的影响审查标准进行评估来支持。

Professors David P. Goldberg and Sara Thoi of Johns Hopkins University seek to understand how biomimetic iron complexes react with nitrogen oxide (NOx) species. NOx species and their interactions with metal ions in biology have been implicated in cellular stress, signal transduction, and enzymatic functioning. Other, similar nitrogen oxides (HNO) is of significant interest because of its unique biological activity, including its possible roles as a signaling molecule, an antioxidant, and as a pharmacological agent for heartfailure and cancer. An understanding of the biological mechanisms of NOx reactivity will be advanced by examining the synthetic, biomimetic systems. In particular, the research of Goldberg and Thoi give new fundamental knowledge about pathways to and from nitric oxide and other nitrogen-containing gases as well as ammonia. One objective is to examine the effect of acids on the way iron interacts with nitrogen oxides. The team also examines new ways to generate HNO, a proposed, key intermediate in the iron-based reactions. The catalysis research entails the use of electrolysis to evaluate the reaction pathways. Students involved in this project are trained in the scientific method, preparing them for occupations in education, research, and industry. Outreach efforts to neighboring middle and high schools broaden participation in STEM-related fields, with the ultimate goal of enhancing the scientific workforce.This research project involves the design, synthesis, and mechanistic study of nonheme iron complexes for the activation of NOx species in the Goldberg laboratory, combined with electrochemical and electrocatalytic studies in the Thoi laboratory. This synergistic approach leads to new information on how structure relates to function for complexes of biological relevance and environmental significance. NOx species and their interactions with metal ions in biology have been implicated in cellular stress, signal transduction, and enzymatic functioning. The environmental significance of M/NOx species arises from the global nitrogen cycle, which involves both oxidative and reductive pathways that interconvert N2, NH3, and NOx species. Graduate students are trained in experimental chemical science, with a focus on bioinorganic chemistry, electrochemistry, synthesis, catalysis, chemical instrumentation, and mechanism. The investigators and their graduate students participate in both elementary and high school outreach programs in Baltimore City.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.