Spectroscopic studies of ambiphilic molecular complexes. Activation of small molecules with non-transition metal catalysis
EMSL Project ID
39979
Abstract
This project will provide fundamental insight into the catalytic activation and transformation of small molecules, e.g., H2, CO2, N2, CH4, by non-metal Lewis pairs in condensed phase environments. The approach will use a combination of experimental approaches (NMR, calorimetry, x-ray and neutron scattering analyses) coupled with computational (Density Functional Theory and Molecular Orbital) electronic structure methods to characterize the properties of bifunctional/ambiphilic catalytic molecular complexes. The fundamental insight gained from these studies will be used to develop predictive molecular-level structure-function relationships models that will enable the optimized molecular design to enhance catalytic control and selectivity in small molecule molecular transformations.
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
Autrey T, ME Bowden, and AJ Karkamkar. 2011. "Control of hydrogen release and uptake in amine borane molecular complexes: Thermodynamics of ammonia borane, ammonium borohydride, and the diammoniate of diborane." Faraday Discussions 151(0):157-169. doi:10.1039/C0FD00015A
Camaioni DM, B Ginovska-Pangovska, GK Schenter, SM Kathmann, and T Autrey. 2012. "Analysis of the Activation and Heterolytic Dissociation of H2 by Frustrated Lewis Pairs: NH3/BX3 (X = H, F, and Cl) ." Journal of Physical Chemistry A 116(26):7228-7237. doi:10.1021/jp3039829.
Karkamkar AJ, K Parab, D Neiner, TK Nielsen, HM Cho, DM Camaioni, and T Autrey. 2012. "Thermodynamic Study of Heterolytic Hydrogen Activation by Frustrated Borane-Amine Lewis Pairs." Dalton Transactions. doi:10.1039/c2dt31628e [In Press]
Nielsen TK, AJ Karkamkar, ME Bowden, F Besenbacher, TR Jensen, and T Autrey. 2013. "Methods to Stabilize and Destabilize Ammonium Borohydride." Dalton Transactions 42(3):680-687. doi:10.1039/C2DT31591B
Potter RG, DM Camaioni, M Vasiliu, and DA Dixon. 2010. "Thermochemistry of Lewis Adducts of BH3 and Nucleophilic Substitution of Triethylamine on NH3BH3 in Tetrahydrofuran." Inorganic Chemistry 49(22):10512-10521. doi:10.1021/ic101481c