School of Chemical Engineering
Forney Hall of Chemical Engineering
480 Stadium Mall Drive
West Lafayette, IN 47907-2100
The properties of interfaces determine many of the macroscopic characteristics of a broad range of important engineering materials, from heterogeneous catalysts to batteries, and in recent years, first principles calculations have emerged as powerful tools for elucidating these properties at the atomic scale. These ab initio calculations are capable of determining structural and energetic properties of interfaces that are difficult, if not impossible, to access experimentally, and in some cases, the calculations have been used to identify new materials with superior properties.
In the Greeley group, we combine first principles calculations of interfaces with classical thermodynamic and kinetic theories to predict macroscopic catalytic and materials properties. We apply these general techniques to several specific classes of interfaces, with an ultimate goal of understanding and designing materials from first principles. Specific areas of interest include:
1) Heterogeneous catalysis. One of our primary focus areas is the complex chemistry of biomass conversion to hydrogen and to liquid fuels on metal surfaces; in particular, we seek to develop accelerated strategies for modeling these reaction networks with first principles calculations. An additional interest is in determining how the interactions between nanoparticle catalysts and oxide supports can, in some cases, lead to novel reactivity patterns that are not observable on either the nanoparticle or the support in isolation.
2) Electrocatalysis. We apply surface science-based techniques, which have been extensively studied at gas-solid interfaces, to probe the fundamental mechanistic details electrocatalytic processes that occur in fuel cells and electrolyzers. We also focus on developing models of the stability of metal/liquid interfaces in electrocatalytic environments; our goal, in this work, is to determine the durability of fuel cells during extended periods of operation.
3) Energy storage in batteries. Although battery technology has been deployed commercially for many years, the fundamental science and engineering of electrode/electrolyte interfaces in batteries is still poorly understood. Our work in this area focuses on the study of lithiation of next-generation anode materials for lithium ion batteries, with an ultimate goal of both predicting higher capacity battery materials and understanding the processes that degrade these materials over long cycle periods.
We are a part of the Purdue Catalysis Center, which fosters interaction among faculty and students in catalysis research groups by collaborating on research projects, sharing resources and facilities, and holding weekly joint group meetings.
- Tej Choksi
- Hee-Joon Chun
- Xiangkui Gu
- William Parker (visiting scholar from Argonne National Laboratory)
- Rees Rankin
- Handan Yildirim
- Zhenhua Zeng
- Zhijian Zhao
Awards and Honors
"The road from animal electricity to green energy: combining experiment and theory in electrocatalysis," J. Greeley and N. Markovic, Energy and Environmental Science, DOI:10.1039/C2EE21754F.
"First Principles Simulations of the Electrochemical Lithiation and Delithiation of Faceted Crystalline Silicon," M. K. Y. Chan, C. Wolverton, and J. Greeley, Journal of the American Chemical Society, 134, (2012) 14362.
"Trends in Selective Hydrogen Peroxide Production on Transition Metal Surfaces from First Principles," R. Rankin and J. Greeley, ACS Catalysis, 2, (2012) 2664.
"Decomposition Pathways of Glycerol via C-H, O-H, and C-C Bond Scission on Pt(111): A Density Functional Theory Study," B. Liu and J. Greeley, J. Phys. Chem. C, 115, (2011) 19702.
"Alloys of platinum and early transition metals as oxygen reduction electrocatalysts," J. Greeley, I. E. L. Stephens, A. S. Bondarenko, T. P. Johansson, H. A. Hansen, T. F. Jaramillo, J. Rossmeisl, I. Chorkendorff, and J. K. Norskov, Nature Chemistry, 1, (2009) 552.