Insights in catalytic transformations at the solid-liquid interface using MES-ATR-IR Spectroscopy
Abstract
The objective of this STIR effort is to investigate the utility of Operando Modulation Excitation Spectroscopy to decipher mechanistic pathways of interactions of small molecules at the gas-solid interface. This effort will investigate the utility of Operando Modulation Excitation Spectroscopy (OMES) to reveal detailed, mechanistic data at the molecular level. The production of butadiene from renewable ethanol using mesoporous silica supported-Ta will serve as the test reaction. Four different supported catalysts will be synthesized, varying the percent weight loading of silica support. The materials will be characterized using Raman, UV-Vis, and IR spectroscopy followed by reactivity assessments. The best materials will be downselected for micro-kinetic studies using OMES. The OMES set-up combines an IR spectrometer with a Diffuse Reflectance IR Transform Spectroscopy (DRIFfS) accessory and an online quadrupole mass spectrometer. Some experimental work will be required to establish and optimize the gas-phase set-up (flow rates, temperatures, calibration). Simple concentration-modulation studies will be carried out followed by measurements at different temperatures as well as in the presence of water. Temperature-dependent phase delays for product formation will be determined. and this data will be used to quantitate activation energies of the micro-kinetic rate-controlling step.
Document Details
- Document Type
- DoD Grant Award
- Publication Date
- Jan 12, 2017
- Source ID
- W911NF1510134
Entities
People
- Ive Hermans
Organizations
- Army Contracting Command
- United States Army
- University of Wisconsin–Madison