in Operando Characterization of Contact Catalysts at Mesoscale Distances
EMSL Project ID
47763
Abstract
We propose to measure and model the dipole-dipole interactions that shift and quench luminescence spectra of ligand-to-metal charge transfer bands of contact catalysts containing transition metal in order to quantify inter-site geometries and the polarizability of the reaction medium within 1-10 nm of the active sites. The former is needed to refine the syntheses that lead to well defined catalysts and to track their evolution. The latter is needed to understand molecular transport to and from the catalyst surface. We will develop the use of luminescence lifetime spectroscopy to probe the composition and geometry in that regime under conditions that could be employed to characterize catalysts under reaction conditions.The work relies on expertise resident at EMSL (spectroscopy) and PNNL (synthesis, modeling) with EMSL’s advanced facilities for spectroscopy (femtosecond LIF) and quantum chemical modeling (NWChem, CP2k running on large scale, parallel computers).
Project Details
Start Date
2013-01-25
End Date
2013-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members
Related Publications
Schwenzer B, L Cosimbescu, VA Glezakou, AJ Karkamkar, Z Wang, and RS Weber. 2015. "Use of Solvatochromism to Assay Preferential Solvation of a Prototypic Catalytic Site." Topics in Catalysis 58(4-6):258-270. doi:10.1007/s11244-015-0367-z