Ni/CeO2 Nanocatalysts with Optimized CeO2 Support Morphologies for CH4 Oxidation

Junjie Chen; Hien N. Pham; Tala Mon; Todd J. Toops; Abhaya K. Datye; Zhenglong Li; Eleni A. Kyriakidou

doi:10.1021/acsanm.2c05496

Ni/CeO₂ Nanocatalysts with Optimized CeO₂ Support Morphologies for CH₄ Oxidation

Junjie Chen, Hien N. Pham, Tala Mon, Todd J. Toops, Abhaya K. Datye, Zhenglong Li, Eleni A. Kyriakidou

Applied Catalysis&Emissions Res. Group

Research output: Contribution to journal › Article › peer-review

24 Scopus citations

Abstract

Catalytic oxidation of CH₄ over nonprecious Ni/CeO₂ catalysts has attracted wide attention. Controlling the morphology of a CeO₂ support can enhance the CH₄ oxidation activity without changing the catalyst composition. Herein, a series of 2 wt % Ni/CeO₂ nanocatalysts with different CeO₂ support morphologies (nanoparticles (P), rods (R), cubes (C)) and synthetic procedures (precipitation, sol-gel (SG)) were evaluated for their CH₄ oxidation performance. The redox properties of CeO₂ supports and corresponding Ni loaded catalysts were characterized by H₂-temperature-programmed reduction and oxygen storage capacity (OSC) measurements. The relationship among the CeO₂ morphologies, surface areas, redox properties, and CH₄ oxidation activity for both CeO₂ supports and Ni/CeO₂ catalysts was established. The findings suggest that CeO₂-R has a greater amount of surface oxygen vacancies as well as an improved OSC and CH₄ oxidation activity compared to CeO₂-P and CeO₂-C supports. The same CH₄ oxidation activity pattern was observed for the Ni containing catalysts (Ni/CeO₂-R > Ni/CeO₂-P > Ni/CeO₂-C). Increasing the CeO₂ surface area by using a sol-gel synthesis method (CeO₂-SG) improved the amount of surface oxygen vacancies and CH₄ oxidation performance of CeO₂-SG and Ni/CeO₂-SG compared to CeO₂-R and Ni/CeO₂-R, respectively.

Original language	English
Pages (from-to)	4544-4553
Number of pages	10
Journal	ACS Applied Nano Materials
Volume	6
Issue number	6
DOIs	https://doi.org/10.1021/acsanm.2c05496
State	Published - Mar 24 2023

Funding

This work was partially supported by start-up funding from the Department of Chemical and Biological Engineering, University at Buffalo (UB), The State University of New York (SUNY). A portion of this research was sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy. Dr. Eleni Kyriakidou and Junjie Chen would also like to acknowledge the Mark Diamond Research Fund of the Graduate Student Association at UB, SUNY. Financial support for the catalyst characterization via TEM was provided by the U.S. Department of Energy (DOE)/BES Catalysis Science program, grant DE-FG02-05ER15712. Additional support was provided by the DOE Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (DE-FOA-0002197). Acquisition of the TEM was supported by the NSF MRI grant DMR-1828731. This manuscript has been coauthored by UT-Battelle, LLC, under Contract No. DE-AC0500OR22725 with the U.S. Department of Energy. The United States Government and the publisher, by accepting the article for publication, acknowledge that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for the United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan). This work was partially supported by start-up funding from the Department of Chemical and Biological Engineering, University at Buffalo (UB), The State University of New York (SUNY). A portion of this research was sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U.S. Department of Energy. Dr. Eleni Kyriakidou and Junjie Chen would also like to acknowledge the Mark Diamond Research Fund of the Graduate Student Association at UB, SUNY. Financial support for the catalyst characterization via TEM was provided by the U.S. Department of Energy (DOE)/BES Catalysis Science program, grant DE-FG02-05ER15712. Additional support was provided by the DOE Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (DE-FOA-0002197). Acquisition of the TEM was supported by the NSF MRI grant DMR-1828731. This manuscript has been coauthored by UT-Battelle, LLC, under Contract No. DE-AC0500OR22725 with the U.S. Department of Energy. The United States Government and the publisher, by accepting the article for publication, acknowledge that the United States Government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for the United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ).

Keywords

Ni/CeO
methane oxidation
morphology control
redox properties
support effect

Access to Document

10.1021/acsanm.2c05496

Cite this

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title = "Ni/CeO2 Nanocatalysts with Optimized CeO2 Support Morphologies for CH4 Oxidation",

abstract = "Catalytic oxidation of CH4 over nonprecious Ni/CeO2 catalysts has attracted wide attention. Controlling the morphology of a CeO2 support can enhance the CH4 oxidation activity without changing the catalyst composition. Herein, a series of 2 wt % Ni/CeO2 nanocatalysts with different CeO2 support morphologies (nanoparticles (P), rods (R), cubes (C)) and synthetic procedures (precipitation, sol-gel (SG)) were evaluated for their CH4 oxidation performance. The redox properties of CeO2 supports and corresponding Ni loaded catalysts were characterized by H2-temperature-programmed reduction and oxygen storage capacity (OSC) measurements. The relationship among the CeO2 morphologies, surface areas, redox properties, and CH4 oxidation activity for both CeO2 supports and Ni/CeO2 catalysts was established. The findings suggest that CeO2-R has a greater amount of surface oxygen vacancies as well as an improved OSC and CH4 oxidation activity compared to CeO2-P and CeO2-C supports. The same CH4 oxidation activity pattern was observed for the Ni containing catalysts (Ni/CeO2-R > Ni/CeO2-P > Ni/CeO2-C). Increasing the CeO2 surface area by using a sol-gel synthesis method (CeO2-SG) improved the amount of surface oxygen vacancies and CH4 oxidation performance of CeO2-SG and Ni/CeO2-SG compared to CeO2-R and Ni/CeO2-R, respectively.",

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author = "Junjie Chen and Pham, {Hien N.} and Tala Mon and Toops, {Todd J.} and Datye, {Abhaya K.} and Zhenglong Li and Kyriakidou, {Eleni A.}",

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AU - Chen, Junjie

AU - Pham, Hien N.

AU - Mon, Tala

AU - Toops, Todd J.

AU - Datye, Abhaya K.

AU - Li, Zhenglong

AU - Kyriakidou, Eleni A.

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N2 - Catalytic oxidation of CH4 over nonprecious Ni/CeO2 catalysts has attracted wide attention. Controlling the morphology of a CeO2 support can enhance the CH4 oxidation activity without changing the catalyst composition. Herein, a series of 2 wt % Ni/CeO2 nanocatalysts with different CeO2 support morphologies (nanoparticles (P), rods (R), cubes (C)) and synthetic procedures (precipitation, sol-gel (SG)) were evaluated for their CH4 oxidation performance. The redox properties of CeO2 supports and corresponding Ni loaded catalysts were characterized by H2-temperature-programmed reduction and oxygen storage capacity (OSC) measurements. The relationship among the CeO2 morphologies, surface areas, redox properties, and CH4 oxidation activity for both CeO2 supports and Ni/CeO2 catalysts was established. The findings suggest that CeO2-R has a greater amount of surface oxygen vacancies as well as an improved OSC and CH4 oxidation activity compared to CeO2-P and CeO2-C supports. The same CH4 oxidation activity pattern was observed for the Ni containing catalysts (Ni/CeO2-R > Ni/CeO2-P > Ni/CeO2-C). Increasing the CeO2 surface area by using a sol-gel synthesis method (CeO2-SG) improved the amount of surface oxygen vacancies and CH4 oxidation performance of CeO2-SG and Ni/CeO2-SG compared to CeO2-R and Ni/CeO2-R, respectively.

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