Atomically Resolved Studies of Catalytic Oxidation of Organics on TiO2(110)
EMSL Project ID
39940
Abstract
A fundamental understanding of the structure-related mechanisms and dynamics of catalytic reactions on oxide catalysts is essential for the development of better catalytic systems. Catalytic properties of TiO2 have attracted widespread interest due to a variety of applications, such as wastewater treatment, air purification, water splitting, self-cleaning, solar cells and full cells. Surface properties dominate the catalytic chemistry of the oxides. The decomposition of organic molecules on titania and other oxides has been used to ascertain the reactive sites and the elemental steps (adsorption, dissociation and diffusion) on oxides surfaces for heterogeneously catalyzed reactions. Scanning Tunneling Microscopy (STM) has significantly advanced our understanding of adsorbate dynamics on single crystalline surfaces of metals. Unfortunately, due to increased complexity of compound materials, our understanding of adsorbates and reaction intermediates on oxides is rather limited. Recently, we have successfully employed STM and DFT to study adsorption and dissociation of simple aliphatic alcohols as well as the diffusion and rotation dynamics of resulting fragments on TiO2(110). In this proposal, we will extend our study to aromatic alcohols (e.g. phenol and benzyl alcohol) and glycols (e.g. ethylene and propylene glycol). Our goal is to obtain the systematic detailed atomic/molecular level understanding of reaction mechanisms with the focus on the adsorbate/intermediate dynamics. The specific research tasks are 1) adsorption, dissociation organics on bridging oxygen vacancies of TiO2(110) and 2) diffusion and rotation of the dissociation intermediates on TiO2(110).
Project Details
Project type
Large-Scale EMSL Research
Start Date
2010-10-01
End Date
2013-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Team Members
Related Publications
Kim B, Z Li, BD Kay, Z Dohnalek, and YK Kim. 2012. "Unexpected Nondissociative Binding of N2O on Oxygen Vacancies on a Rutile TiO2(110)-1×1 ." Journal of Physical Chemistry C 116(1):1145-1150. doi:10.1021/jp210636j
Kim B, Z Li, BD Kay, Z Dohnalek, and YK Kim. 2014. "Low-Temperature Desorption of N2O from NO on Rutile TiO2(110)-1x1." Journal of Physical Chemistry C 118(18):9544-9550. doi:10.1021/jp501179y
Li Z, BD Kay, and Z Dohnalek. 2013. "Dehydration and Dehydrogenation of Ethylene Glycol on Rutile TiO2(110)." Physical Chemistry Chemical Physics. PCCP 15(29):12180-12186. doi:10.1039/c3cp50687h
Li Z, Z Zhang, BD Kay, and Z Dohnalek. 2011. "Polymerization of Formaldehyde and Acetaldehyde on Ordered (WO3)3 Films on Pt(111)." Journal of Physical Chemistry C 115(19):9692-9700. doi:10.1021/jp202169x
May RA, RS Smith, and BD Kay. 2013. "The Release of Trapped Gases from Amorphous Solid Water Films: II. “Bottom-Up” Induced Desorption Pathways." Journal of Chemical Physics 138(10):Article No. 104502. doi:10.1063/1.4793312
May RA, RS Smith, and BD Kay. 2013. "The Release of Trapped Gases from Amorphous Solid Water Films: I. “Top-Down” Crystallization-Induced Crack Propagation Probed using the Molecular Volcano." Journal of Chemical Physics 138(10):Article No. 104501. doi:10.1063/1.4793311
Tang M ,Zhang Z ,Ge Q 2016. "A DFT-based Study of Surface Chemistries of Rutile TiO2 and SnO2(110) Toward Formaldehyde and Formic Acid" Catalysis Today 274():103–108. 10.1016/j.cattod.2016.01.057
Xia Y, B Zhang, J Ye, Q Ge, and Z Zhang. 2012. "Acetone-Assisted Oxygen Vacancy Diffusion on TiO2(110)." Journal of Physical Chemistry Letters 3(20):2970–2974. doi:10.1021/jz301293y