Department of Chemistry

Dr. Dario Stacchiola Research

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Current Research:

   Our research focus on understanding the elemental chemical processes on simple model surfaces under pristine conditions, to guide the preparation of real systems, which are complex materials operating under practical environmental conditions.
   Our work in nanocatalysis has been related to the synthesis of metal and oxide nanoparticles deposited on novel film oxides, and their multi-technique characterization by photoelectron and infrared spectroscopies and scanning probe microscopy, in combination with theoretical models [Proc. Natl. Acad. Sci. U.S.A. 106, 4975-4980 (2009)].


Au/CeOx/TiO2

   Some examples are the synthesis of 2D aluminosilicate films [Angew. Chem. Int. Ed. 45, 7636-7639 (VIP) (2006) ] and the growth of monomers, dimmers and nanoclusters of oxides (vanadia and ceria) supported on oxide substrates (ceria, titania and silica) [Angew. Chem. Int. Ed (2009)].


synthesis of 2D aluminosilicate films

   This body of research has established that sub-nanometer oxides with new structures can be prepared and stabilized. They exhibit chemical and catalytic properties not found in bulk oxides. Polarization modulated IR spectroscopy (PM-IRAS) can be employed to investigate species in-situ during catalytic reactions, and thus the molecular mechanisms of relevant chemical reactions can be probed under conditions ranging from ultrahigh vacuum to atmospheric pressure [J. Vac. Sci. & Techn. A 20, 2101-2105 (2002)]. In this manner we have deciphered the long-disputed mechanism of the industrial formation of vinyl acetate formation on palladium [Angew. Chem. Int. Ed. 44, 4572-4574 (2005)]. We have further tuned the surface chemistry of catalysts by using organic modifiers, including the chiral templating of palladium [J. Am. Chem. Soc. 124 8984-8989 (2002)].

   Our immediate plan is to undertake fundamental studies of surface organometallic chemistry. This topic is at the heart of the development of dye-sensitized solar cells and the preparation of single-site catalysts. Enzymes are the most elaborate catalysts in nature and their selectivity and efficiency cannot yet be matched by any manmade catalyst. However, major industrial processes rely on high volume chemical production and for that simpler inorganic catalysts are used. The crossroad of organometallic chemistry with material science allows the rational development of catalysts that incorporate elements found in enzymes. Single site catalysts offer the selectivity of organometallic complexes with the robustness of solid inorganic substrates. But their 3D complexity has hindered their characterization. By synthesizing and fully characterizing model structures we can determine how structural features of a surface organometallic complex affect desired properties, and interrogate if systematic variations of species at the designed system predictably affect these ensemble properties. Heterogeneous and homogeneous catalysis have been traditionally two separate fields of study; bridging the gap between these fields will allow the design of the next generation of green catalysts.

The nano-interface between material science and organometallic chemistry

   The overall goal of this proposed research is to elucidate the basic mechanisms involved in the organometallic functionalization of oxide surfaces. This area of research, coined as surface organometallic chemistry, is at the heart of the development of Lab on a Chip, sensors for biomedical applications, functionalization of semiconductors, layer-by-layer growth of films through atomic layer deposition (ALD), and the preparation of single-site catalysts. The study will be accomplished through the development of atomically resolved model systems with well-defined thin oxide films of Si, Al and mixed-oxide aluminosilicates grown in planar substrates.

Towards a rational design of heterogeneous catalysts: Model studies of ceria-manganese oxides

   This project proposes the synthesis of ceria-manganese mixed-oxide model films, for their atomic characterization and catalytic reaction mechanism study in connection with hydrogen production. Preparation of oxides with Mn in different valences will be systematically investigated, by controlling the environment and conditions during synthesis.

Use of INS for spectroscopic studies on the chemistry of hydride catalysts

   The work outlined in this proposal aims to extend the use of Inelastic Neutron Scattering (INS) to the fundamental research on hydride catalysts. It will be a continuation of a recent project from the author to investigate high surface area catalysts in the ISIS facility at the Rutherford Appleton Laboratory, in the U.K.. INS solves the problem of small frequency windows available to Raman and IR studies on high surface materials, and the extreme difficulty of hydrogen detection with most analytical tools.

Department of Chemistry

Chemical Sciences and Engineering Building
Houghton, MI 49931

Ph: 906-487-2048
Fax: 906-487-2061
Email: chemistry@mtu.edu

Michigan Technological University

1400 Townsend Drive
Houghton, Michigan 49931-1295
906-487-1885

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