Quantitative and Mechanistic Analyses of Bond Selective Chemistry via Non-Thermal Excitation of Metal Nanostructures
Abstract
In this project we will utilize a comprehensive and combined experimental-computational approach to develop mechanistic descriptions of catalysis by metal nanostructures when excited via a non-thermal energy sources (photons, electrons and ions). The overall objective is to mechanistically characterize the most efficient and bond-selective selective approaches for driving chemical conversion processes at metal nanoparticle surfaces through non-thermal excitation mechanisms. A few common metal nanostructures (Ag, Pt, Ru nanoparticles) and extensively studied chemical systems (NO, CO, N2, CH4, and CH3OH desorption and dissociation) will be studied under non-thermal excitation conditions - using photon or electron excitation - or their combination (using a non-thermal low-temperature plasma excitation). There is a mounting body of scientific evidence suggesting that such mechanisms can provide improvements with respect to both yield and reaction selectivity for catalytic reactions on nanostructured metal surfaces, but further developments will only be accessible once a fundamental understanding of chemical reaction induced by non-thermal excitation of metal nanostructures is reached. Carefully designed experiments will be conducted to investigate the reactivity of metal nanostructures under photon irradiation and e-beam exposure. A non-thermal plasma reactor will be used to investigate their reactivity under the more complex scenario in which multiple non-thermal excitation processes are simultaneously occurring. Finally, a combination of ab-initio, non-adiabatic molecular dynamics, and time-dependent density functional theory calculations to complement experiments will be used to gain a fundamental, theoretical understanding of the processes under investigation. By correlating these findings with theoretical analysis of the non-thermal chemical processes, we expected to develop henomenological insights into properties of molecules, metals, and excitation sources that are critical for enabling bond selective chemistry in non-thermal processes on metal nanostructure surfaces.
Document Details
- Document Type
- DoD Grant Award
- Publication Date
- Oct 06, 2018
- Source ID
- W911NF1710340
Entities
People
- Lorenzo Mangolini
Organizations
- Army Contracting Command
- United States Army
- University of California, Riverside