On-surface Redox Assembly of Metal-organic Complexes

Indiana University, Bloomington IN

Investigators

Abstract

The ability to control the transformation of one molecule into another is an overarching objective in chemical research. There are many challenging, but highly relevant, chemical reactions that we do not yet know how to control and design. Many of these transformations occur at surfaces that facilitate the reactions and transformations of gas phase molecules. This research program is a joint effort between Dr. Steven Tait and Dr. Kenneth Caulton at Indiana University to develop control of surface reaction chemistry using metal-organic complexes. Dr. Tait's research group has expertise in the chemistry of surfaces and the characterization of those chemistries using spectroscopy and microscopy. Dr. Caulton's research group has expertise in the design of metal-organic complexes for chemical reactions. Together, this collaborative team is advancing our ability to control and design surface chemistries, such as the conversion of the greenhouse gas carbon dioxide to products that could be used to make plastics and other useful materials. There are many broader impacts of this project. The program offers an excellent educational opportunity for student researchers to work in an interdisciplinary science program. This research will train students for productive careers in science and technology. The project also involves efforts to increase diversity in chemical science research and to make the results from the research accessible to the public through programs at science museums and high schools. The latter programs involve discussion of how molecules interact and assemble. The science museum and high school program also provides hands-on activities illustrating how scientists characterize molecules, including about how they create images of the chemical structures at the molecular level. In this research program, Drs. Steven Tait and Kenneth Caulton and their research groups at Indiana University are supported by the Macromolecular, Supramolecular, and Nanochemistry (MSN) Program to study the on-surface chemistry and assembly between tailored, redox-active ligands and single-site transition metals. The long-range goal of this work is to develop the ability to program chemical selectivity in functionalized surfaces, guided by both the chosen metal and active electron storage at the ligand. The team integrates the skills of a surface physical chemistry group with an organometallic chemistry group to develop an understanding of on-surface redox chemistry to produce well-defined surface reaction sites. These sites are designed to be uniform due to stoichiometric control and to create a repetitive nanoscale structure of the same reactive site in an arrayed metal-organic surface structure. Applying these strategies of ligand design and metal-complex formation to surface functionalization offers potentially transformative impacts in the fields of catalysis, sensing, and carbon recycling technologies. This interdisciplinary project allows new advances in the science of surface functionalization and new insights into redox chemistry processes. It also provides an outstanding training environment for the young scientists on the project to participate actively in an interdisciplinary research effort. This team is actively engaged in activities to increase diversity in interdisciplinary chemistry research and in outreach programs for the public, capitalizing on the highly visual nature (scanning probe microscopy) of the work.