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Fundamental Studies of Heterogeneous Photocatalysis on Model TiO2 Surfaces


EMSL Project ID
35219

Abstract

The objective of this project is to provide the field of heterogeneous photocatalysis with unique insights into the molecular-level properties of photocatalytic transformations through joint experimental and theoretical studies of organic photooxidation reactions on model TiO2 materials. Heterogeneous photocatalysis on TiO2 has received considerable attention of late due to increased interest in using light to promote chemical transformations in remediation and energy technologies. Fundamental questions remain unaddressed, e.g., reaction and charge transfer mechanisms, specific surface reaction sites, selectivity, and interplay between thermal and non-thermal processes. The vast majority of research effort in the literature has been phemonological, resulting in conflicting explanations for such crucial issues as the performance differences between the polymorphs of TiO2 (rutile, anatase or mixtures thereof). In this project, molecular-level expertise at PNNL in material synthesis, surface chemistry, theory, photodynamics and scanning probe microscopy will be used to study three areas of fundamental importance to heterogeneous photocatalysis on TiO2. These are: (1) detailed reaction mechanisms, (2) mechanisms of charge transfer, charge trapping and energy redistribution, and (3) surface structure and material dependences, each as they relate to organic photooxidation reactions. These issues will be explored using a variety of model TiO2 systems including single crystal surfaces and epitaxially grown films of rutile and anatase, mixed phase films of the two, and surfaces prepared with controlled structural and electronic defects and varying degrees of porosity.

Project Details

Project type
Large-Scale EMSL Research
Start Date
2009-10-01
End Date
2011-09-30
Status
Closed

Team

Principal Investigator

Michael Henderson
Institution
Pacific Northwest National Laboratory

Team Members

Benjamin Clark
Institution
Inpria

Zhitao Wang
Institution
Pacific Northwest National Laboratory

Meena Rajachidambaram
Institution
Oregon State University

Jaana Rajachidambaram
Institution
Oregon State University

Mingmin Shen
Institution
Pacific Northwest National Laboratory

Jason Stowers
Institution
Inpria

Igor Lyubinetsky
Institution
Pacific Northwest National Laboratory

Gregory Herman
Institution
Oregon State University

Gregory Kimmel
Institution
Pacific Northwest National Laboratory

Janos Szanyi
Institution
Pacific Northwest National Laboratory

Zdenek Dohnalek
Institution
Pacific Northwest National Laboratory

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