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

约翰·霍普金斯大学的大卫·P·戈德堡教授和萨拉·索伊教授试图了解仿生铁络合物如何与氮氧化物(NOx)物种发生反应。在生物学中，NOx种类及其与金属离子的相互作用与细胞应激、信号转导和酶功能密切相关。其他类似的氮氧化物(HNO)由于其独特的生物活性而引起人们的极大兴趣，包括它可能作为信号分子、抗氧化剂以及心力衰竭和癌症的药理学试剂的作用。通过检查合成的仿生系统，将促进对NOx反应的生物学机制的理解。特别是，Goldberg和Thoi的研究提供了关于一氧化氮和其他含氮气体以及氨的来回路径的新的基础知识。其中一个目标是研究酸对铁与氮氧化物相互作用方式的影响。该团队还研究了生成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法来评估反应路径。参与这个项目的学生接受了科学方法的培训，为他们在教育、研究和工业领域的职业做好准备。这项研究项目涉及到Goldberg实验室中用于激活NOx物种的非血红素铁配合物的设计、合成和机理研究，以及Thoi实验室中的电化学和电催化研究。这种协同作用的方法导致了关于具有生物相关性和环境意义的复合体的结构与功能如何相关的新信息。在生物学中，NOx种类及其与金属离子的相互作用与细胞应激、信号转导和酶功能密切相关。M/NOx物种的环境意义源于全球氮循环，全球氮循环包括氧化和还原途径，这些途径将氮气、NH3和NOx物种相互转化。研究生培养的是实验化学科学，重点是生物无机化学、电化学、合成、催化、化学仪器和机理。调查人员和他们的研究生都参加了巴尔的摩市的小学和高中外展项目。这一奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

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.