Computational Environmental Catalysis @ Notre Dame
Overview
The goal of research in the Schneider group is to develop molecular-level understanding, and ultimately to direct molecular-level design, of chemical reactivity at surfaces and interfaces.
This heterogeneous chemistry is a key element of virtually every aspect of the energy enterprise, and is fundamental to environmental processes on the earth and in the atmosphere. Examples range from the preparation of clean fuels from crude oil or coal, to the transformation of chemical to electrical energy in fuel cells, to the remediation of exhaust from fossil fuel combustion, to even the sequestration of CO2 via mineralization. While the processes and technologies of interest are very different when viewed macroscopically, at the molecular level unifying chemical and physical phenomena emerge.
First-principles simulations based on density functional theory (DFT) allow this reactivity to be probed at the molecular scale, providing insight and guidance for the development of improved catalytic materials and processes. Understanding gained at the molecular level allows us to better control-and ultimately to tailor-chemical systems to perform functions more cleanly, efficiently, and durably. The problems we address cut across the traditional boundaries of chemical engineering, chemistry, physics, environmental science, and materials science, and our work both draws on and impacts all of these fields.
Collaborations with research groups in academia and at the National Laboratories are important for validating and applying our results, and interactions with industry are critical for guidance and ensuring relevance to practical catalysis and environmental chemistry.
Key research areas of current interest
Gas adsorption at metal oxide surfaces
We characterize the adsorption properites of water, NOx and other environmentally significant molecules at metal oxide surfaces |
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Nanoscale heterogeneous catalysis
We use first principles thermodynamics models to probe the structure and composition of supported catalyst particles under realistic reaction conditions
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Catalysis at metal and metal oxide surfaces
We develop atomistically detailed models of oxidative catalytic reactivity at transition metal and metal oxide surfaces
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Selective catalytic reduction of nitrogen oxides
The selective catalytic reduction of nitrogen oxides from high efficiency combustion processes presents special catalytic challenges that we simulate at the atomic scale |
The people doing the work
The Tools
Our research program is built on state-of-the-art first-principles molecular simulation tools based primarily on density functional theory (DFT). These quantum mechanical calculations take advantage of some of the latest and most powerful computers available (including the CBE SaND cluster) to produce accurate predictions of chemical structure, energetics, and reactivity for systems that were impossible to simulate even just a few years ago. Statistical thermodynamics and kinetics methods provide the coupling to the macroscopic world. The simulations are informed with simple but powerful concepts of chemical structure and bonding-key to both the effective use of the tools and extraction of useful physical insight. We partner closely with experimentalists both to validate results and to provide an avenue for their rapid application.
Primary simulation tools
Plane-wave/pseudopotential DFT: The Vienna ab-initio Simulation Package (VASP)
Local-orbital DFT: Amsterdam Density Functional code (ADF)
The big computer: Simulations @ Notre Dame cluster (SaND)
Sources of Support
DOE Basis Energy Sciences
NSF Chemical, Bioengineering, Environmental, and Transport Systems
NSF Chemistry
DOE National Energy Technology Laboratory
The WaterCAMPWS
Ford Motor Company
ExxonMobil Research and Engineering
University of Notre Dame