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Nano Research 2020, 13(9): 2384-2392 https://doi.org/10.1007/s12274-020-2861-2
Research Article | Issue | Published: 09 June 2020

Tunable catalytic activity of gadolinium-doped ceria nanoparticles for pro-oxidation of hydrogen peroxide

Show Author's Information Anuja Bhalkikar1,  Tai-Sing Wu2,  Tamra J. Fisher1,  Anandakumar Sarella3,  Dawei Zhang4,  Yi Gao4,  Yun-Liang Soo2,5,  Chin Li Cheung1( )
Department of Chemistry, University of Nebraska-Lincoln, Lincoln, NE 68588, USA
Department of Physics, "National Tsing Hua University", Hsinchu 30013, Taiwan, China
Nebraska Center for Materials and Nanoscience, University of Nebraska-Lincoln, Lincoln, NEB 68588, USA
Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201800, China
"National Synchrotron Radiation Research Centre", Hsinchu 30076, Taiwan, China
Keywords:
ceria, hydrogen peroxide, cerium oxide, gadolinium, pro-oxidation, hydroxyl radicals, ozone
Topics:
Activation energyCatalytic oxidation Cerium oxideFree radical reactionsGadolinium compoundsHydrogen peroxideNanoparticlesOxidationPeroxidesReaction ratesSemiconductor dopingSynthesis (chemical)
Cite this article:
Bhalkikar A, Wu T-S, Fisher TJ, et al. Tunable catalytic activity of gadolinium-doped ceria nanoparticles for pro-oxidation of hydrogen peroxide. Nano Research, 2020, 13(9): 2384-2392. https://doi.org/10.1007/s12274-020-2861-2
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Abstract Full text Electronic supplementary material About this article

We report a study of the roles of gadolinium(III) (Gd3+) dopants in influencing the catalytic activity of gadolinium-doped ceria nanoparticles towards the pro-oxidation of hydrogen peroxide to hydroxyl radicals. These doped ceria nanoparticles with dopant concentrations of 0.6 wt.%, 3 wt.%, and 6 wt.% Gd3+ were synthesized using an ozone-mediated method for tuning their catalytic activities. The Gd dopants were found to foster an increase in the percentage of Ce3+ ions in the doped ceria nanoparticles. Our reaction kinetic study revealed that the relationship between the overall reaction rates and the Gd dopant concentrations in our doped materials followed a volcano-like trend. In contrast, the apparent activation energy values of these Gd-doped ceria nanoparticles were found to be positively associated with the concentrations of Gd dopants. The overall catalytic activity trend was attributed to the interplay between the promotion and degradation effects of the Gd dopants on the properties of doped ceria nanoparticles.


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About this article

Tunable catalytic activity of gadolinium-doped ceria nanoparticles for pro-oxidation of hydrogen peroxide

Show Author's information Anuja Bhalkikar1, Tai-Sing Wu2, Tamra J. Fisher1, Anandakumar Sarella3, Dawei Zhang4, Yi Gao4, Yun-Liang Soo2,5, Chin Li Cheung1( )
Department of Chemistry, University of Nebraska-Lincoln, Lincoln, NE 68588, USA
Department of Physics, "National Tsing Hua University", Hsinchu 30013, Taiwan, China
Nebraska Center for Materials and Nanoscience, University of Nebraska-Lincoln, Lincoln, NEB 68588, USA
Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201800, China
"National Synchrotron Radiation Research Centre", Hsinchu 30076, Taiwan, China

Abstract

We report a study of the roles of gadolinium(III) (Gd3+) dopants in influencing the catalytic activity of gadolinium-doped ceria nanoparticles towards the pro-oxidation of hydrogen peroxide to hydroxyl radicals. These doped ceria nanoparticles with dopant concentrations of 0.6 wt.%, 3 wt.%, and 6 wt.% Gd3+ were synthesized using an ozone-mediated method for tuning their catalytic activities. The Gd dopants were found to foster an increase in the percentage of Ce3+ ions in the doped ceria nanoparticles. Our reaction kinetic study revealed that the relationship between the overall reaction rates and the Gd dopant concentrations in our doped materials followed a volcano-like trend. In contrast, the apparent activation energy values of these Gd-doped ceria nanoparticles were found to be positively associated with the concentrations of Gd dopants. The overall catalytic activity trend was attributed to the interplay between the promotion and degradation effects of the Gd dopants on the properties of doped ceria nanoparticles.

Keywords: ceria, hydrogen peroxide, cerium oxide, gadolinium, pro-oxidation, hydroxyl radicals, ozone

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Publication history
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Acknowledgements

Publication history

Received: 30 October 2019
Revised: 14 April 2020
Accepted: 08 May 2020
Published: 09 June 2020
Issue date: September 2020

Copyright

© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2020

Acknowledgements

C. L. C., A. B., and T. J. F. gratefully acknowledge the financial support from the National Science Foundation (No. CHE-1362916). Y. G. and D. W. Z. were supported by the CAS-Shanghai Science Research Center (No. CAS-SSRC-YJ-2015-01) and the National Natural Science Foundation of China (Nos. 11574340 and 21773287). We acknowledge the assistance from Johnny Goodwin of the University of Alabama for part of the microscopy work. We also thank Joseph Brewer and Josh Beaudoin of Rare Earth Salts, LLC for their help with the ICP-OES analysis. The characterizations of catalysts were performed in part in the Nebraska Nanoscale Facility: National Nanotechnology Coordinated Infrastructure and the Nebraska Center for Materials and Nanoscience, which were supported by the National Science Foundation under Award ECCS: 1542182 and the Nebraska Research Initiative. We are also grateful to the "National Radiation Research Center" in Taiwan, China for the use of their synchrotron light sources. The computational resources for this research were provided by the Shanghai Supercomputer Center and the National Supercomputer Center in Tianjin and Shenzhen.

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