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(gc3568)Computational Design of Catalysts: The Control of Chemical Transformation


EMSL Project ID
3568

Abstract

The petroleum and chemical industries contribute ~$500 billion to the GNP of the U.S. These industries rely for their financial well being on their ability to produce new products by using energy-efficient, low-cost, and environmentally clean processes, with a minimal number of undesirable side products. Key ingredients in 90% of chemical manufacturing processes are catalysts. A catalyst?s role is to make a chemical reaction that produces a desired product proceed much more efficiently than it otherwise would by changing the kinetics of the process. Catalysis and catalytic processes account for nearly 20% of the U.S. GDP and nearly 20% of all industrial products. Chemical transformations in industry take a cheap feedstock (usually some type of hydrocarbon) and convert it into a higher value product by rearranging the carbon atoms and by adding functional groups to the compound. About 5 quads per year are used in the production of the top 50 chemicals in the U.S. and catalytic routes account for the production of 30 of these chemicals, consuming 3 quads. Improved catalysts can increase efficiency leading to reduced energy requirements, while increasing product selectivity and concomitantly decreasing wastes and emissions. A process yield improvement of only 10% would save 0.23 quads per year! In addition, production of the top 50 chemicals leads to almost 21 billion pounds of CO2 emitted to the atmosphere per year. Improved catalysts can help to reduce this carbon burden on the atmosphere. As new products become ever more sophisticated, the need to quickly develop new catalysts grows rapidly in importance. A fundamental understanding of chemical transformations is needed to enable scientists to address the grand challenge of the precise control of molecular processes by using catalysts. A desirable approach to catalyst design is to analyze at the molecular level exactly how catalysts function and to use this information to lead to the discovery of new systems and to optimize the design of others. Without this information, it is impossible to ?tune? the catalyst to have the desired effect. For example, even the most sophisticated experimental techniques are unable to provide the details of the chemical reactions occurring at the surface of a heterogeneous catalyst or information about how to tune a homogeneous catalyst to gain a factor of 2 to 4 in performance. Computational methods hold the key to catalyst design. Advanced characterization tools and in situ spectroscopies can provide identities and structures of reactive intermediates (and thus reaction mechanisms); time-resolved methods will provide kinetics and dynamics of elementary processes. These constitute critical benchmarks for validating computational methods. However, catalyst design will require quantitative information about transition states for critical reaction processes in catalysis. These are only accessible by computational methods. It is the marriage of theory and experiment that will lead us to quantitative design principles and methodologies. Computational chemistry is an enabling tool for addressing challenges in the optimal design of processes for controlling and enabling chemical transformations leading to processes that have high selectivity, have minimal environmental impact, and are optimal in their use of energy. We propose to use computational chemistry to address a variety of problems in catalyst science including oxidative dehydrogenation, organic oxidation chemistry and selectivity, hydrogenation of alkenes and isomerization of alkenes and alkanes, and reactions of carbohydrates. This will be done for both heterogeneous and homogeneous catalytic systems.

Project Details

Project type
Capability Research
Start Date
2003-09-30
End Date
2006-10-01
Status
Closed

Team

Principal Investigator

David Dixon
Institution
University of Alabama

Team Members

Faisal Mehmood
Institution
Air Force Research Laboratory

Minh Nguyen
Institution
University of Alabama

Myrna Hernandez Matus
Institution
University of Alabama

Falk Eichhorn
Institution
University of Wisconsin, Madison

Christopher Taylor
Institution
Los Alamos National Laboratory

Donghai Mei
Institution
Tiangong University

Si-dian Li
Institution
Xinzhou Teachers University

Vamsi Vadhri
Institution
University of Virginia

Shan Oh
Institution
University of Wisconsin, Madison

Yan Wang
Institution
Emory University

Ashish Mhadeshwar
Institution
University of Delaware

Zhi Wang
Institution
Emory University

Vencislav Parvanov
Institution
Emory University

Petia Bobadova-parvanova
Institution
Emory University

Aditya Bhan
Institution
University of California, Berkeley

Peter Ferrin
Institution
University of Wisconsin, Madison

Daniel Grant
Institution
University of Alabama

Amanda Holland
Institution
University of Alabama

Ryan House
Institution
University of Alabama

Xin Huang
Institution
Washington State University Tri-Cities

Raluca Craciun
Institution
University of Alabama

Bing Dai
Institution
Pacific Northwest National Laboratory

Qingfeng Ge
Institution
Southern Illinois University

Charnita Peoples
Institution
University of Alabama

Lesley Magee
Institution
University of Alabama

Lijun Xu
Institution
University of Virginia

Eric Knoll
Institution
Columbia University

David Rinaldo
Institution
Columbia University

Li Tian
Institution
Columbia University

Rahul Nabar
Institution
University of Wisconsin, Madison

Jian-zhi Hu
Institution
Pacific Northwest National Laboratory

Anand Nilekar
Institution
University of Wisconsin, Madison

Amit Gokhale
Institution
University of Wisconsin, Madison

Raj Chakrabarti
Institution
Massachusetts Institute of Technology

Shampa Kandoi
Institution
University of Wisconsin, Madison

John Kitchin
Institution
University of Delaware

Michael Enever
Institution
University of Delaware

Lei Zhang
Institution
Columbia University

Byungchan Kim
Institution
Columbia University

Sally Wasileski
Institution
University of Virginia

Michael Janik
Institution
Pennsylvania State University

Emmanouil Mavrikakis
Institution
University of Wisconsin, Madison

Lars Grabow
Institution
University of Wisconsin, Madison

Nedialka Iordanova
Institution
Pacific Northwest National Laboratory

David Fumento
Institution
Columbia University

Rafal Bachorz
Institution
Universitaet Karlsruhe

Kazuhiro Omiya
Institution
Emory University

David Quiñonero
Institution
Universitat de les Illes Balears

Peng Zhang
Institution
Emory University

Antara Dutta
Institution
Emory University

Jianjun Liu
Institution
Emory University

Henryk Witek
Institution
Emory University

Qingfang Wang
Institution
Emory University

Guishan Zheng
Institution
University of Illinois at Urbana-Champaign

Maciej Haranczyk
Institution
Lawrence Berkeley National Laboratory

Annabella Selloni
Institution
Princeton University

John Jaffe
Institution
Pacific Northwest National Laboratory

John White
Institution
University of Texas at Austin

Dennis Bennett
Institution
University of Wisconsin, Milwaukee

Justin Ehresmann
Institution
University of Southern California

Stephen Dimagno
Institution
University of Nebraska - Lincoln

Mark Barteau
Institution
University of Michigan

Enrique Iglesia
Institution
University of California, Berkeley

Maciej Gutowski
Institution
Heriot-Watt University

Sung Mo
Institution
Emory University

Andri Arnaldsson
Institution
University of Washington

Zhiyong Zhou
Institution
Columbia University

Jason Gonzales
Institution
Emory University

Charles Campbell
Institution
University of Washington

Kiran Boggavarapu
Institution
Virginia Commonwealth University

Edoardo Apra
Institution
Environmental Molecular Sciences Laboratory

Keiji Morokuma
Institution
Emory University

Mark White
Institution
Mississippi State University

Hannes Jonsson
Institution
University of Iceland

Tom Waters
Institution
Washington State University Tri-Cities

James Franz
Institution
Pacific Northwest National Laboratory

Jun Li
Institution
Tsinghua University

James Haw
Institution
University of Southern California

James Gole
Institution
Georgia Institute of Technology

Stephan Irle
Institution
Emory University

Matthew Neurock
Institution
University of Minnesota

Richard Friesner
Institution
Columbia University

Djamaladdin Musaev
Institution
Emory University