
Larry G. Sneddon
Blanchard Professor of Chemistry
Inorganic, Energy and Materials Chemistry
Office: 3001 IAST
Lab: 3110, 3150, 3160, 3170, 3180 IAST
Phone: (215) 898-8632
Email: lsneddon
sas
upenn
edu
Jump to: Research Statement | Education and Academic History | Selected Publications | Educational Interests
Research Statement
Our research in inorganic chemistry, energy-storage and materials science includes synthetic studies in main-group, transition metal and materials chemistry along with physical and structural investigations of molecular, polymeric, and solid-state materials. Brief overviews of ongoing projects are presented in the following sections.Alternative Energy Carriers: New Chemical Methods for Hydrogen Storage
The development of efficient methods for hydrogen storage is a major hurdle that must be overcome to enable the use of hydrogen as an alternative energy carrier. We are exploring the use of chemical hydrides such as ammonia borane and ammonia triborane to store and deliver large amounts of hydrogen through dehydrogenation and/or hydrolysis reactions. As depicted in the example in Figure 1, we have shown that the rate and the extent of hydrogen release from these amineboranes can be significantly increased through the use of metal catalysts, ionic liquids and/or chemical additives. We are continuing to investigate both new methods for the controlled hydrogen release from amineboranes and the development of energy-efficient methods for their regeneration from spent-fuel products.

Figure 1. Rhodium catalyzed hydrolysis of ammonia triborane
Chemical Precursors to Ultra High Temperature Aerospace Materials
The production of complex structural and electronic materials in useable forms is one of the most challenging problems of modern solid-state chemistry and materials science. Our research in this area is focused on the design, syntheses and applications of new processible molecular and/or polymeric precursors to advanced carbide, nitride and boride ceramics that allow the formation of these technologically important materials in forms that cannot be produced with conventional methods. We are especially interested in ultra high temperature materials, such as HfB2 and ZrB2 based composites, that are potentially important in hypersonic (i.e. flying faster than 5 times the speed of sound) aerospace vehicles (Figure 2). A second part of the project is focused on the formation and properties of micro- and nanostructured ceramics, including fibers, tubes and porous materials.

Figure 2. New chemical precursor systems for ultra high temperature hafnium-ceramics that were developed at Penn
Transition Metal-Promoted Reactions of Inorganic Compounds
We
are developing new general, metal-catalyzed methodologies that enable
the systematic, high-yield syntheses of important polyborane compounds
and materials. Our goals are both to discover new types of catalytic
reactions and to develop an understanding of their fundamental reaction
mechanisms and controlling factors.

Figure 3. (Left) Metal-catalyzed synthesis of the poly(norbornenyldecaborane) polymer; and (Right) The crystallographically determined structure of a new dendritic decaborane (you can manipulate this molecule online at
Ionic Liquid Promoted Reactions
Ionic liquids have properties
that make them attractive solvents for synthesis, including: negligible
vapor pressures, thermal stability to elevated temperatures; the
ability to dissolve a range of compounds, salts and gases,
immiscibility with many hydrocarbons and/or water thus enabling
two-phase reaction systems, weakly-coordinating anions and cations that
provide a polar, inert reaction medium, and the ability to stabilize
polar intermediates and/or transition states. While ionic liquids have
been widely employed for organic synthesis, our recent work showing
that decaborane olefin-hydroboration and alkyne-insertion reactions
proceed in biphasic ionic-liquid/hydrocarbon solvents without the need
of the catalysts required in conventional solvents, was the first
demonstration of the unique activating effects of ionic liquids for
polyborane syntheses. We are continuing to explore the scope of ionic
liquid mediated polyborane reactions along with experimental and
computational studies of the mechanisms by which these reactions occur.
Inorganometallic Chemistry
Because of the unusual ranges of their accessible charges and
coordination geometries, polyboranes can function as versatile ligands
that can stabilize transition metals in a much wider array of
environments than their organic counterparts, such as the
cyclopentadienide anion. We are using integrated synthetic, structural
(NMR and X-ray crystallography), electrochemical, and computational
(DFT/GIAO) investigations to elucidate the nature of polyborane-metal
bonding. The unique properties of metallapolyborane complexes are also
being exploited to design new metallocene-like complexes with chemical,
optical and/or bioactivity properties of importance to solid-state
and/or anticancer applications.

Figure 4. (Left) Comparisons of the bonding modes of the cyclopentadienyl and tricarbadecaboranyl ligands; (Right) The crystallographically determined structures of new maganatricarbadecaboranyl complexes illustrating a cage-slippage reaction analogous to a cyclopentadienyl ring-slippage process
Education and Academic History
- B.S. Centenary College of Louisiana (1967)
- Ph.D. Indiana University (1971)
- Postdoctoral Fellow, University of Virginia (1971-73)
- Postdoctoral Fellow, Massachusetts Institute of Technology (1973-74)
- Assistant Professor of Chemistry, University of Pennsylvania (1974-1980)
- Associate Professor of Chemistry, University of Pennsylvania (1980-1984)
- Professor of Chemistry, University of Pennsylvania (1984-2005)
- Chairman, Department of Chemistry (2002-2005)
- Edmund J. and Louise W. Kahn Endowed Term Professor of Chemistry (2005-2007)
- Blanchard Professor of Chemistry (2007- present)
- General Electric Assistant Professor of Materials Science (1979-80)
- Alfred P. Sloan Fellow (1980-82)
- Editorial Boards: Organometallics (1990-92), Inorganic Chemistry (1990-92)
- Examiner, OECD Review of Science and Technology Policy of the Republic of Korea
- Member, Laboratory for the Research on the Structure of Matter (1974-present)
- BUSA Award for Distinguished Achievements in Boron Science (1992)
- Lindback Award for Distinguished Teaching (1997)
- Alexander von Humboldt Foundation Research Award for Senior US Scientists (2002)
- 2007 DOE Hydrogen Program R & D Award in Recognition of Outstanding Achievement in Storage R & D
Selected Publications
R. Butterick, III, P. J. Carroll and L. G. Sneddon "A General Method for the Selective Functionalization of Cyclopentadienyliron Tricarbadecaboranyl Complexes via Halogenation and Sonogashira Coupling Reactions" Organometallics 2008, 27, 4419-4427.Y. Li and L. G. Sneddon "Synthesis and Characterization of 6-(RR'N)-nido-5,7-C2B8H11: A Carborane with a Cage-Boron Having an Exopolyhedral Dative Boron-Nitrogen Double Bond" J. Am. Chem. Soc. 2008, 130, 11494-11502.
M. J. Kim, S. Chatterjee, S. M. Kim, E. A. Stach, M. G. Bradley, M. J. Pender, L. G. Sneddon, B. Maruyama "Double-Walled Boron Nitride Nanotubes Grown by Floating Chemical Vapor Deposition" Nano. Lett. 2008, 8, 3298-3302.
Y. Li, P. J. Carroll and L. G. Sneddon " Ionic Liquid Promoted Decaborane Dehydrogenative Alkyne-Insertion Reactions: A New Route to o-Carboranes" Inorg. Chem. 2008, 47, 9193-9202.
U. Kusari, P. J. Carroll and L. G. Sneddon "Ionic Liquid Promoted Decaborane Olefin-Hydroboration: A New Efficient Route to 6-R-B10H13 Derivatives" Inorg. Chem. 2008, 47, 9203-9215.
C. W. Yoon, U. Kusari and L. G. Sneddon "Computational Studies of the Reactions of B10H13– with Alkynes and Olefins: Pathways for Dehydrogenative Alkyne-Insertion and Olefin-Hydroboration Reactions" Inorg. Chem. 2008, 47, 9216-9227.
W. E. Ewing, P. J. Carroll and L. G. Sneddon "High Yield Routes to 6-X-B10H13 Based on Acid-Induced Cage Opening Reactions of B10H102-" Inorg. Chem. 2008, 47, 8580-8582.
C. W. Yoon, P. J. Carroll and L. G. Sneddon " Ammonia Triborane: A New Synthesis, Structural Determinations and Hydrolytic Hydrogen-Release Properties" J. Am. Chem. Soc. 2009, 131, 855-864.
M. M. Guron, X. Wei, D. Welna, N. Krogman, M. J. Kim, H. Allcock and L. G. Sneddon “Preceramic Polymer Blends as Precursors for Boron-Carbide/Silicon-Carbide Composite Ceramics and Ceramic Fibers” Chem. Mater. 2009, 21, 1708-1715.
Educational Interests
Chem 102: General Chemistry IIChem 261: Advanced Inorganic Chemistry
Chem 565: Main Group Chemistry
