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Structure and Catalytic Activity of Supported Early Transition Metal Oxide Clusters


EMSL Project ID
24793

Abstract

This proposal is a continuation of research under EMSL User Proposal #22091. Current commercial heterogeneous catalysts are structurally and chemically complex and measurements on them can seldom be interpreted with atomic-level precision. This is especially so for supported transition metal oxide (TMO) catalysts, materials that find applications in a wide-array of industrially important hydrocarbon transformations. In our proposed research we focus on the preparation and detailed atomic/molecular level understanding of chemical reactivity of TMO clusters supported on other single crystal oxides surfaces. In our prior research we have successfully produced monodispersed (WO3)3 clusters on TiO2(110), characterized their structure using scanning tunneling microscopy, and have begun to explore their catalytic activity using molecular beams and temperature programmed desorption. Our future work will focus on: (1) Oxidation of alcohols on this model (WO3)3 / TiO2 110) System; (2) Preparation and Characterization of analogous Mo Based Model TMO System; and (3) The Effect of Support Oxide on TMO Structure and Reactivity.
The primary focus of the proposed work is on advancing the understanding of molecular and nano-scale systems and inventing novel approaches and experimental methods to resolve the complexities inherently limiting the understanding of heterogeneous catalytic systems. Such detailed molecular-level studies are germane to DOE programs in catalysis, environmental restoration, waste processing, and contaminant fate and transport and are also relevant to improved energy technologies, and understanding and mitigating the environmental impacts of energy use. These goals are consistent with the "Science of Interfacial Phenomena" EMSL science theme area which is seeking user proposals that "contribute to the atomic- and molecular-level understanding and control of the dynamic, reactive, and transport properties of interfaces having possible environmental and energy implications."

Project Details

Project type
Large-Scale EMSL Research
Start Date
2007-05-31
End Date
2010-09-30
Status
Closed

Team

Principal Investigator

Zdenek Dohnalek
Institution
Pacific Northwest National Laboratory

Team Members

Danda Acharya
Institution
Pacific Northwest National Laboratory

Xiao Lin
Institution
Pacific Northwest National Laboratory

Zhenjun Li
Institution
Pacific Northwest National Laboratory

Roger Rousseau
Institution
Pacific Northwest National Laboratory

Jinlong Gong
Institution
University of Texas at Austin

Yu Kwon Kim
Institution
Ajou University

Shao-chun Li
Institution
Tulane University

Nathaniel Deskins
Institution
Worcester Polytechnic Institute

Bojana Ginovska
Institution
Pacific Northwest National Laboratory

Zhenrong Zhang
Institution
Baylor University

John White
Institution
University of Texas at Austin

Bruce Kay
Institution
Pacific Northwest National Laboratory

Related Publications

Kim J, BD Kay, and Z Dohnalek. 2010. "Formaldehyde Polymerization on (WO3)3/TiO2(110) Model Catalyst." Journal of Physical Chemistry C 114(40):17017-17022.
Kim YK, BD Kay, JM White, and Z Dohnalek. 2008. "2-Propanol Dehydration on TiO2(110): The Effect of Bridge-Bonded Oxygen Vacancy Blocking." Surface Science 602(2):511-516. doi:10.1016/j.susc.2007.10.049
Kim YK, RJ Rousseau, BD Kay, JM White, and Z Dohnalek. 2008. "Catalytic Dehydration of 2-Propanol on (WO3)3 Clusters on TiO2(110)." Journal of the American Chemical Society 130(15):5059-5061. doi:10.1021/ja800730g