Supported Single-Atom Catalysts for Low Temperature Air Pollution Control

Catalytic low temperature oxidation is important for many applications including pollution abatement, indoor air quality control, as well as for breaking down chemical warfare agents. Despite extensive efforts, it remains a grand challenge to design catalysts with higher activity, at low temperature, even for a simple reaction such as CO oxidation. Our goal is to develop a methodology for tuning the catalyst properties for low temperature oxidation, a priori. Our approach uses a combination of in-situ/operando experimental and computational studies on a unique class of supported Ir single-atoms and subnanometer clusters. The proposed work will allow us control the size of active sites from a single-atom to subnanometer clusters and vary the electronic properties of the support. This will allow us to decipher the effects of metal nuclearity and support electronic properties on the reaction mechanisms, and to develop molecular-scale design rules for predicting the catalyst activity. The resources at EMSL will allow us to combine state of the art in-situ spectroscopy and microscopy with synchrotron-based spectroscopy at other DOE user facilities to identify the catalyst structure and reaction mechanisms on the molecular scale.
Impact:
The proposed work will have a major impact on the catalysis field by providing an unprecedented view of the structural, electronic and catalytic properties of supported single-atoms and subnanometer clusters. The molecular level details of the reaction mechanisms and the ability to control the electronic properties of single-atoms will be used to develop a new methodology for catalyst design. The results are expected to transform catalysis in the subnanometer regime from phenomenological into predictive, which will benefit many important chemical transformations, including pollution abatement and renewable synthesis of chemicals/fuels from biomass and shale gas.