Structural and mechanistic identification of heterogeneous catalysts

Due to their importance and widespread use in the chemical and energy industries, understanding and improving heterogeneous catalysts is essential to advance their development and enable more sustainable processes. Atomically disperse or single atom catalysts have shown particular promise for their ability to exceed nanoparticle catalysts with regards to activity, stability and selectivity for a growing number of chemical reactions. Understanding key properties of these materials, such as structure-property relationships, structural dynamics and reaction-driven restructuring, is, however, often complicated by issues including low weight loadings, strong metal-support interactions and heterogeneity in active component speciations. The following work details how these challenges may be addressed through a review of how a multimodal approach including scanning transmission electron microscopy, diffuse reflectance infrared Fourier transform spectroscopy, X-ray photoelectron spectroscopy and X-ray absorption spectroscopy may be employed to identify the catalytically relevant properties (charge state, electronic structure, atomic configuration, bonding interaction). Furthermore, this approach is demonstrated through its application to Pt-Ni bimetallic nanoparticles on mesoporous silica, single atom Pt on CeO2, nanoparticle Pt on CeO2 and single atom Pt on Gd-doped CeO2.

Name thesis:degree_name

Ph.D.

Level thesis:degree_level

Dissertation

Discipline thesis:degree_discipline

Chemistry

Grantor

University of Illinois at Urbana-Champaign

Year dc:date

2022

Author dc:creator

• Kottwitz, Matthew

Contributors dc:contributor

• Nuzzo, Ralph G.
• Gewirth, Andrew A.
• Kenis, Paul J. A.
• Murphy, Catherine J.

• single atom
• catalysis
• heterogeneous

Statement dc:rights

• Copyright 2021 Matthew Kottwitz

Language dc:language

en

Handle dc:identifier

http://hdl.handle.net/2142/113326

OAI identifier oai:identifier

oai:www.ideals.illinois.edu:2142/113326