Determining C-H Activation Reaction Mechanisms of Nonheme Iron Catalysts with Ultrafast Multi-Dimensional Multiple-Mode Vibrational Spectroscopy

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With this award, the Chemical Measurement and Imaging Program of the Division of Chemistry is funding Professor Junrong Zheng of Rice University to elucidate details of the C-H activation mechanism catalyzed by Fe-containing organic molecules, by studying signatures of the reaction intermediates. The structures of key intermediates are being investigated by a broadband multiple-dimensional multiple-mode vibrational spectroscopy method being developed for these purposes in the Zheng group. An outreach program developed by Professor Zheng is allowing local high school students the opportunity to participate in this research and that projects associated with fundamental molecular events underneath daily phenomena are being designed for high school students to inspire their interest in fundamental physical sciences. Graduate and undergraduate students are being actively mentored and involved in all aspects of the research and education plan. Animated cartoons will be developed to demonstrate basic chemical and physical principles for kids.This project focuses on the structural determinations of the intermediate oxidants of the nonheme catalyst Fe(S,S-PDP), resolving the disagreement about its C-H activation mechanism. The intermediates can be paramagnetic and transient in liquids and difficult to be resolved by traditional techniques. To meet the challenge, novel ultrafast vibrational spectroscopic methods are being developed to resolve the in situ structures of these transient species with an ultrafast temporal resolution. Organic syntheses of various reagents and catalysts and theoretical calculations are being conducted to reach a comprehensive understanding of the reactions. The broader impacts of this work include bringing a deeper understanding of many C-H activation reactions catalyzed by heme and nonheme molecules, and developing a novel method that can resolve many molecular structures in both inorganic and organic chemistry that are difficult for traditional techniques.