报告时间：2013年9月24日，星期二，上午10:00-11:00

 报告地点：催化基础国家重点实验室三楼会议室 

　　　　报告人：Dr. Zdenek Dohnálek 

　　Pacific Northwest National Laboratory, Richland, WA 99354, USA 

　　报告摘要： 

　　Simple alcohols and diols are employed as models for deoxygenation reactions of biomass. TiO₂(110) is selected as a prototypical reducible oxide catalyst to attain detailed mechanistic understanding of such reactions. Atomically resolved imaging before and after adsorption reveals information about the preferred adsorption sites, O-H and C-O bond cleavage, and formation dynamics of high temperature reaction intermediates.  Further details are uncovered about the translational and rotation motion of surface species. The coverage dependent desorption kinetics of alkenes and aldehydes as final gas phase products are determined via temperature programmed desorption. Comprehensive theoretical calculations via dispersion-corrected density functional theory yield a deep insight into the mechanism and energetics of the observed reaction steps. 

　　This work was supported by the US Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences & Biosciences and performed in EMSL, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory (PNNL).  PNNL is a multiprogram national laboratory operated for DOE by Battelle. 

　　报告人简介： 

　　Senior Chief Scientist 

　　Chemical and Materials Sciences Division                               

　　Pacific Northwest National Laboratory                                              

　　P.O. Box 999, MS K8-88  

　　Richland, WA 99352  

　　Phone:   (509)-371-6150        

　　FAX:         (509)-371-6139 

　　Email:       Zdenek.Dohnalek@pnnl.gov 

　　Professional Interests 

　　My research focused on experimental studies of fundamental model systems that are necessary to understand complex processes that take place in heterogeneous catalysis and environment. The work concentrates on adsorption, diffusion, and desorption dynamics and kinetics, binding, and reactivity of adsorbates on model well characterized surfaces and clusters. A combined experimental approach involving both atomically resolved imaging and ensemble averaged methods is employed to provide a detailed, molecular level understanding of catalyst structure and reactivity. Novel deposition methods, developed in our laboratory, are further used to prepare clusters and nanoporous films of model oxide catalysts with tailored chemical properties. All studies are complemented by theoretical investigations carried out by collaborators and are intended to provide general structure-reactivity relationships. Systems recently investigated include a partial oxidation of alcohols on supported WO₃ clusters and on rutile TiO₂(110) surface, water-oxygen reactions on TiO₂(110), numerous adsorbates on epitaxial MgO(100) and nanoporous MgO films, ethylene hydrogenation on thin epitaxial and nanoporous Pd films, and most recently CO₂ on TiO₂(110). 

　　Education and Employment 

　　2000-present Senior Research Scientist II, Chemical Structure and Dynamics Department,        

　　                                Pacific Northwest National Laboratory, Richland, Washington 

　　1998-2000            Postdoctoral Fellow, Pacific Northwest National Laboratory, W. R. Wiley Environmental Molecular Sciences Laboratory, Richland, Washington 

　　1992-1997            University of Pittsburgh, Ph.D. in Physical Chemistry, November 1997 

　　1989-1991            Institute of Chemical Engineering, Prague, Czech Rep., M.S. in Chemical Engineering, Prague, Czech Republic, July 1991 

　　Professional Affiliation 

• Executive Board member of  Nanometer Scale Science and Technology Division of AVS,  2009 - present
• Secretary (2001-2003), Vice President (2005), and President (2006-2008) of Pacific Northwest Chapter of American Vacuum Society

　　Honors and Distinctions 

• M. T. Thomas Award for Outstanding Postdoctoral Achievement in the William R. Wiley Environmental Molecular Sciences Laboratory, PNNL, 2001 
• Graduate Fellowship funded by Lubrizol Corporation, 1994

　　Relevant Publications (Total: 89) 

1. Cryogenic CO₂ Formation on Oxidized Gold Clusters Synthesized via Reactive Layer Assisted Deposition, J. Kim, Z. Dohnálek, and B. D. Kay, J. Am. Chem. Soc. 127 (2005) 14592.
2. Formation of Monodisperse (WO₃)₃ Clusters on TiO₂(110), O. Bondarchuk, X. Huang, J. Kim, Bruce D. Kay, L.-S. Wang, J. M. White, and Z. Dohnálek, Angew. Chem. Int. Ed. 45 (2006) 4786.
3. Imaging Adsorbate O-H Bond Cleavage: Methanol on TiO₂(110), Z. Zhang, O. Bondarchuk, J. M. White, B. D. Kay, Z. Dohnálek, J. Am. Chem. Soc. 128 (2006) 4198.
4. Imaging Water Dissociation on TiO₂(110): Evidence for Inequivalent Geminate OH Groups, Z. Zhang, O. Bondarchuk, J. M. White, B. D. Kay, Z. Dohnálek, J. Phys. Chem. B 110 (2006) 21840. Journal Cover.
5. Reactive Ballistic Deposition of Porous TiO₂ Films: Growth and Characterization, D. W. Flaherty, Z. Dohnálek, A. Dohnálková, B. W. Arey, D. E. McCready, N. Ponnusamy, C. B. Mullins, and B. D. Kay, J. Phys. Chem. C 111 (2007) 4765.
6. Catalytic Dehydration of 2-Propanol on (WO₃)₃ Clusters on TiO₂(110), Y. K. Kim, R. Rousseau, B. D. Kay, J. M. White, and Z. Dohnálek, J. Am. Chem. Soc. 130 (2008) 5059.
7. Vacancy Assisted Diffusion of Alkoxy Species on Rutile TiO₂(110), Z. Zhang, R. Rousseau, J. Gong, S.-C. Li, B. D. Kay, Q. Ge, and Z. Dohnálek, Phys. Rev. Lett. 101 (2008) 156103.
8. Water as a Catalyst: Imaging Reactions of O₂ with Partially and Fully Hydroxylated TiO₂(110) Surfaces, Z. Zhang, Y. Du, N. G. Petrik, G. A. Kimmel, I. Lyubinetsky, and Z. Dohnálek, J. Phys. Chem. C 113 (2009) 1908.
9. Imaging Hindered Rotations of Alkoxy Species on TiO₂(110), Z. Zhang, R. Rousseau, J. Gong, B. D. Kay, and Z. Dohnálek, J. Am. Chem. Soc. 131 (2009) 17926.
10. Thermally-Driven Processes on Rutile TiO₂(110)-(1×1): A Direct View at the Atomic Scale, Z. Dohnálek, I. Lyubinetsky, and R. Rousseau, Prog. Surf. Sci. 85 (2010) 161.

　　Collaborators from other Institutions 

　　C. Buddie Mullins (U. Texas, Austin), Falko Netzer (U. Graz, Austria), Vladimir Matolin (Charles University, Czech Rep.), Eric Altman (Yale), Fumio Ohuchi (U Washington), Zhenrong Zhang (Baylor), Yu Kwon Kim (Ajou University, S. Korea) 

　　Graduate and Postdoctoral Advisors 

　　Ph.D.:  Prof. John T. Yates, Jr. (U. Pittsburgh) 

　　Postdoctoral:  Dr. Bruce D. Kay (PNNL) 

　　 Thesis Advisor and Postgraduate Scholar Sponsor 

　　D. W. Flaherty (U. Texas, Austin), J. Kim (LAM Research), O. Bondarchuk (SPECS, Germany), J. Gong (U. Texas, Austin), S. C. Li (Tulane U.), Y. K. Kim (Ajou University, S. Korea), Z. Zheng (Baylor University), G. Parkinson (Technische Universit？t Wien, Austria.), Zhenzhun Li (PNNL), Danda Acharya (PNNL), Xiao Lin (PNNL) 

　　报告联系人：502组 石瑛（9128）