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First Principles Theory and Modeling of Interfacial Processes for Environment-Friendly Materials


EMSL Project ID
47584

Abstract

A fundamental knowledge of the chemical and physical properties at gas-solid or liquid-solid interfaces is essential for the design and discovery of breakthrough materials. Computational strategies using high performance computing provide the opportunity to design surfaces and interfaces with desired functionalities. This requires both an understanding of the processes that are occurring at the interfaces as well as relating desired properties to key calculated parameters such as reaction energies and barriers, which can be used in screening many potential candidates. This proposal is focused on the use of computations to both understand structure-function relationships as well as use of this insight to help design new materials for processes involving various types of catalysis and energy storage. The computational studies will be based on state-of-the-art electronic structure methods including density functional theory, a powerful tool for understanding and design of new catalysts. The proposed computational studies involve collaboration with world-class experimentalists at the Pacific Northwest National Laboratory and Argonne National Laboratory. The computations will be focused on three interrelated areas: (1) catalysis by subnanometer clusters, (2) photocatalysis on TiO2 surfaces, and (3) modeling of solid-liquid interfaces.

New catalysts are needed for making and breaking specific bonds for energy efficient and environmentally friendly catalysts. Recent studies have shown that supported subnanometer clusters exhibit novel catalytic properties for breaking C-H and O-H bonds. We will carry out systematic studies to explore the unusual catalytic properties of these clusters and to determine how they might be tailored to make and break specific bonds. These computations will play a key role in the design and discovery of environmentally friendly catalysts for industrial processes. Electrocatalysis provides a low-temperature, energy efficient alternative to heterogeneous catalysis that has potential uses for chemical transformations as well as the development of alternative energy sources. We will investigate the use of subnanometer clusters for carbon dioxide electroreduction, wherein CO2 is electrochemically reduced to CO and hydrogenated products in acidic solution. This reaction has the potential to both produce useful chemicals from an essentially limitless feedstock and reduce atmospheric greenhouse gas loadings. Efficient utilization of solar energy through photocatalysis would be a significant step towards easing current energy demands. TiO2 is a prototypical photocatalyst used for organic pollutant degradation and also for water splitting, H2 being an important fuel source. Despite the importance of TiO2, there are many fundamental issues that are not well understood, such as how photoexcited holes and electrons interact with surface adsorbates and lead to their catalytic decomposition. Molecular modeling methods provide an excellent way to study surface reactions and provide insights into the intermediates and reaction pathways. Finally, we will use computations to model the solid-electrolyte interfaces involved in energy storage systems as well as catalysis. In lithium ion batteries the SEI plays a key role in the performance and safety of li-ion batteries and have become one of the most important energy storage devices for portable electronics, electric and plug-in hybrid vehicles, owing to their high energy density and design flexibility. Computations will be used to study the structure and properties of important SEI components and how they are formed from electrolytes.

Project Details

Project type
Large-Scale EMSL Research
Start Date
2012-10-01
End Date
2014-09-30
Status
Closed

Team

Principal Investigator

Larry Curtiss
Institution
Argonne National Laboratory

Team Members

Denise Ford
Institution
Argonne National Laboratory

Cong Liu
Institution
Argonne National Laboratory

Ujjal Das
Institution
Argonne National Laboratory

Xin Tan
Institution
Argonne National Laboratory

Brandon Bukowski
Institution
Purdue University

Maria Chan
Institution
Argonne National Laboratory

Weronika Walkosz
Institution
Argonne National Laboratory

Rajeev Surendran Assary
Institution
Northwestern University

Juan Cristobal Garcia Sanchez
Institution
Worcester Polytechnic Institute

Junbo Chen
Institution
Worcester Polytechnic Institute

Christopher Seith
Institution
Worcester Polytechnic Institute

Glen Ferguson
Institution
Argonne National Laboratory

Kah Chun Lau
Institution
Argonne National Laboratory

Haiying He
Institution
Argonne National Laboratory

Rees Rankin
Institution
Argonne National Laboratory

Lei Cheng
Institution
Argonne National Laboratory

Jeffrey Greeley
Institution
Argonne National Laboratory

Hakim Iddir
Institution
Argonne National Laboratory

Nathaniel Deskins
Institution
Worcester Polytechnic Institute

Peter Zapol
Institution
Argonne National Laboratory

Michel Dupuis
Institution
University at Albany, State University of New York