Department of Chemistry & Biochemistry

Biography

2012-present

Professor, University of Notre Dame

2002-2012

Associate Professor, University of Notre Dame

1996-2002

Assistant Professor, University of Notre Dame

1994-1996

Postdoctoral Fellow, California Institute of Technology

1994

Ph.D. in Inorganic Chemistry, University of Washington

1988

B.S. in Chemistry, B.S. in Humanities and Science, Massachusetts Institute of Technology

Selected Awards

2016

ACS Division of Inorganic Chemistry Award for Undergraduate Research Mentor

2011

Fellow, American Chemical Society

2009

Rev. Edmund P. Joyce, C.S.C. Award for Excellence in Undergraduate Teaching

2008

Shilts/Leonard Award for Outstanding Teaching in the College of Science

2003, 2006

John Kaneb Award for Undergraduate Teaching

2005

University of Notre Dame Presidential Award

2004

Thomas P. Madden Award for Outstanding Teaching in the First-Year Program

1998-2002

NSF Career Award

1998-2001

Dupont Young Professor Award

1996

Camille and Henry Dreyfus Foundation New Faculty Award

1995

NIH NRSA Postdoctoral Fellowship

Research Interests

Developing Catalysis for Energy and the Environment

Enhancing our understanding of the mechanisms of chemical reactions is critical to improve processes that interconvert between chemical and electrical energy or to make chemical products in a selective and environmentally benign way. The Brown group is addressing this general problem by making new inorganic or organometallic complexes with the aim of achieving reactivity through novel mechanisms.

Traditionally, oxidation-reduction reactions mediated by metal-containing compounds involve changes in both the oxidation state and bonding that directly involve those metal centers. We are exploring an alternative mode of redox reactivity, what we term "nonclassical" redox reactions, where bond-making or bond-breaking events occur at a metal center but oxidations or reductions occur not at the metal center but at redox-active ligands attached to the metal. These processes generate novel species with unusual electronic structure, which may be capable of unusual reactivity. Furthermore, separating the locus of electron transfer from that of changes in bonding mimics the heterogeneous catalysis involved in fuel cells, suggesting that nonclassical homogeneous reactions may lead to conceptual insights or practical advances in systems for interconverting electrical and chemical energy.

In some cases, we have observed reactions where both the oxidation state changes and the bonding changes take place at the ligand rather than the metal. This has allowed us to observe reactions at coordinatively saturated or even encapsulated metal centers that would normally be considered poor choices as catalysts because of the unavailability of open sites at the metal. We are currently engaged in elucidating the effect of the metal-ligand bonding on this ligand-centered reactivity and using that information to design new catalysts with enhanced reactivity, selectivity, or durability.

Recent Publications

• Do, T. H. and Brown, S. N. "Mono- and Bis(Iminoxolene)Iridium Complexes: Synthesis and Covalency in Pi Bonding" 2022 Inorganic Chemistry, 61 (14), pp.5547-5562. DOI: 10.1021/acs.inorgchem.1c04005.
• Ranis, L. G.; Gianino, J.; Hoffman, J. M. and Brown, S. N. "Nonclassical Oxygen Atom Transfer Reactions of an Eight-Coordinate Dioxomolybdenum(Vi) Complex" 2021 Inorganic Chemistry Frontiers, 8 (11), pp.2865-2870. DOI: 10.1039/d1qi00308a.
• Erickson, A. N.; Gianino, J.; Markovitz, S. J. and Brown, S. N. "Amphiphilicity in Oxygen Atom Transfer Reactions of Oxobis(Iminoxolene)Osmium Complexes" 2021 Inorganic Chemistry, 60 (6), pp.4004-4014. DOI: 10.1021/acs.inorgchem.1c00068.
• Do, T. H. and Brown, S. N. "Synthesis, Dynamics and Redox Properties of Eight-Coordinate Zirconium Catecholate Complexes" 2020 Dalton Transactions, 49 (33), pp.11648-11656. DOI: 10.1039/d0dt02487b.
• Gianino, J.; Erickson, A. N.; Markovitz, S. J. and Brown, S. N. "High-Valent Osmium Iminoxolene Complexes" 2020 Dalton Transactions, 49 (25), pp.8504-8515. DOI: 10.1039/d0dt01735c.
• Gianino, J. and Brown, S. N. "Highly Covalent Metal-Ligand Pi Bonding in Chelated Bis- and Tris(Iminoxolene) Complexes of Osmium and Ruthenium" 2020 Dalton Transactions, 49 (21), pp.7015-7027. DOI: 10.1039/d0dt01287d.