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

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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.