David C. Lacy
Office: 657 Natural Sciences Complex
Phone: (716) 645-4114
Fax: (716) 645-6963
E-mail: DCLacy at buffalo edu
Education and Training:
B.S., Colorado State University, CO (2007)
Ph.D., University of California-Irvine, CA (2012)
NIH Postdoctoral Fellow, California Institute of Technology, CA (2012 – 2015)
Solar Energy Conversion
Using first-row transition metal molecular compounds and a bio-inspired approach, we will tackle three major chemical problems associated with solar energy conversion/storage…
- Water oxidation with earth-abundant molecular catalysts.
One strategy to meet future energy needs is to split water into O2 and H2 photo-electrochemically. While many details surrounding the mechanism of photosynthetic water oxidation have been experimentally elucidated, the O–O bond forming step in photosynthesis remains invisible to experiment. To help address questions regarding this step, the Lacy lab is working with organometallic manganese compounds that offer the potential of oxidizing water and, by close examination of intermediate species, expose the O–O bond forming process.
- Oxidation of strong C–H bonds (such as those in methane) using molecular oxygen.
Hydroxylation of hydrocarbons is an important chemical transformation in a broad range of fields spanning solar fuels and pharmaceuticals. A difficult initial step in this transformation is the required homolytic cleavage of very strong C–H bonds. This process is accomplished in the enzyme methane monooxygenase (MMO) in which methane is converted to methanol and water via supposed homolytic C–H bond cleavage pathways mediated by high-valent transition metal species and molecular oxygen. Reproducing this transformation is difficult with synthetic first-row transition metal complexes, such as iron and manganese, and is a challenge we are undertaking.
- Reduction of CO2 to useful products at low overpotentials.
An amazing feat accomplished by CO2 reductases and related enzymes is their ability to equilibrate carbon dioxide and a reduced carbon-containing product (such as carbon monoxide or formate) at low overpotentials. This is in stark contrast to synthetic molecular catalysts that irreversibly operate at staggeringly large overpotentials. The Lacy lab is interested in addressing this disparity using finely tuned enzyme model complexes in tandem with known CO2 reduction systems.
- Hill, E. A.; Weitz, A. C.; Onderko, E.; Romero-Rivera, A.; Guo, Y.; Swart, M.; Bominaar, E. L.; Green, M. T.; Hendrich, M. P.; Lacy, D. C.; Borovik, A. S. “Reactivity of an Fe(IV)-Oxo Complex with Protons and Oxidants” J. Am. Chem. Soc. (2016), 138, 13143.
- Lacy, David C.; Roberts, G. M.; Peters, J. C. “The Cobalt Hydride that Never Was: Revisiting Schrauzer’s Hydridocobaloxime” J. Am. Chem. Soc. (2015), 137, 4860.
- Zhang, M.; El-Roz, M.; Mendoza-Cortez, J. L.; Lacy, D. C.; Peters, J. C.; Head-Gordon, M.; Frei, H. “Visible Light Sensitized CO2 Activation by the Tetraaza [CoIIN4H(MeCN)]2+ Complex Investigated by FT-IR Spectroscopy and DFT Calculations” J. Phys. Chem. C (2015), 119, 4645.
- Lacy, David C.; McCrory, C. C. L.; Peters, J. C. “Studies of Cobalt-Mediated Electrocatalytic CO2 Reduction Using a Redox-Active Ligand” Inorg. Chem. (2014), 53, 4980.
- Lacy, David C.; Mukherjee, J.; Lucas, R. L.; Day, V. W.; Borovik, A. S. “Metal Complexes with Varying Intramolecular Hydrogen Bonding Networks” Polyhedron (2013), 52, 261.
- Lacy, David C.; Park, Y. J.; Ziller, J. W.; Borovik, A. S. “Assembly and Properties of Heterobimetallic CoII/III/CaII Complexes with Aquo and Hyrdroxo Ligands” J. Am. Chem. Soc. (2012), 134, 17526.
- Gupta, R.; Lacy, D. C.; Borovik, A. S.; Hendrich P. “Electron Paramagnetic Resonance and Mössbauer Spectroscopy and DFT Analysis of a High-Spin Fe(IV)-Oxo Complex” J. Am. Chem. Soc. (2012), 134, 9774.
- Lacy, David C.; Gupta, R.; Stone, K. L.; Greaves, J.; Ziller, J. W.; Hendrich, M. P.; Borovik, A. S. “Formation, Structure, and EPR Detection of a High Spin Fe(IV)-Oxo Species Derived from Either an Fe(III)-Oxo or Fe(III)-OH Complex” J. Am. Chem. Soc. (2010), 132, 12188.