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Studies on zeolite supported Cu/Fe as selective catalytic reduction (SCR) catalysts, and supported Pd as passive NOx adsorbers (PNA)


EMSL Project ID
51265

Abstract

To help meet DOE goals of enabling more fuel-efficient vehicle engine technologies, for the past ~15 years we have been carrying out research programs funded by DOE/Office of Energy Efficiency and Renewable Energy (EERE)/Vehicle Technologies Office (VTO), involving programs that include direct collaboration with industry partners in the form of CRADA programs, and more fundamental programs directly funded by VTO. Currently, the industry-partner CRADA programs with Cummins, Inc. and FCA aim at (1) understanding mechanisms of low-temperature constrains of selective catalytic reduction (SCR) of NOx catalyzed by small-pore zeolite supported Cu/Fe catalysts, and improving long-term stability of industrial SCR catalysts (primarily Cu/SSZ-13); and (2) lowering NOx emissions during vehicle cold start by invoking novel passive NOx adsorber (PNA) materials. For these programs to be successful, we rely on the use of a wide array of state-of-the-art catalyst characterization facilities in EMSL. Defect deficient beta zeolite materials will be synthesized as supports for Fe SCR catalysts. Small-pore zeolites SSZ-13, SSZ-16, SSZ-17 and SSZ-39 supported Pd will be developed as PNA materials. This project will also leverage previous work at PNNL engaged in developing active and stable noble metal based materials/catalysts for use in biomass upgrading and engine exhaust cleanup. For example, novel small pore zeolite supported Cu catalysts will be developed as alternatives to the current industrial Cu/SSZ-13 SCR catalyst with potentially improved performance and stability. This proposal contains the following essential components: (1) Large-pore beta zeolites, small-pore SSZ-family zeolites and zeolite supported metal materials synthesis; (2) material/catalyst performance evaluation using our home-built plug-flow reaction systems with MKS gas-phase FTIR analyzers; (3) in situ/operando spectroscopic and microscopic characterizations, e.g., solid-state nuclear magnetic resonance (NMR), electron paramagnetic resonance (EPR), X-ray photoelectron (XPS), Mossbauer and FTIR spectroscopies, scanning transmission electron microscopy (STEM), with EMSL support; (4) density functional theory (DFT) calculations in support of the experimental work performed with a mixed Gaussian and plane wave basis sets implemented in the CP2K code. Expected outcomes include 3-5 high impact journal publications, 3-5 national and international conference presentations and annual reports to DOE/EERE/VTO acknowledging the essential support from EMSL.

Project Details

Start Date
2020-01-01
End Date
2020-09-30
Status
Closed

Team

Principal Investigator

Feng Gao
Institution
Pacific Northwest National Laboratory

Team Members

Jinshu Tian
Institution
Pacific Northwest National Laboratory

Yiqing Wu
Institution
Pacific Northwest National Laboratory

Konstantin Khivantsev
Institution
Pacific Northwest National Laboratory

Yilin Wang
Institution
Pacific Northwest National Laboratory

Xavier Isidro Pereira Hernandez
Institution
Pacific Northwest National Laboratory

Donghai Mei
Institution
Tiangong University

Janos Szanyi
Institution
Pacific Northwest National Laboratory

Yong Wang
Institution
Washington State University