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Thermally Induced Restructuring of [email protected]2 and [email protected]2 Nanoparticles as a Strategy for Enhancing Low-Temperature Catalytic Activity

  • Alexander J. Hill
    Alexander J. Hill
    Department of Chemical Engineering, University of Michigan, 2300 Hayward Street, Ann Arbor, Michigan 48109, United States
  • Chang Yup Seo
    Chang Yup Seo
    Department of Chemical Engineering, University of Michigan, 2300 Hayward Street, Ann Arbor, Michigan 48109, United States
  • Xiaoyin Chen
    Xiaoyin Chen
    Department of Chemical Engineering, University of Michigan, 2300 Hayward Street, Ann Arbor, Michigan 48109, United States
    More by Xiaoyin Chen
  • Adarsh Bhat
    Adarsh Bhat
    Department of Chemical Engineering, University of Michigan, 2300 Hayward Street, Ann Arbor, Michigan 48109, United States
    More by Adarsh Bhat
  • Galen B. Fisher
    Galen B. Fisher
    Department of Chemical Engineering, University of Michigan, 2300 Hayward Street, Ann Arbor, Michigan 48109, United States
  • Andrej Lenert*
    Andrej Lenert
    Department of Chemical Engineering, University of Michigan, 2300 Hayward Street, Ann Arbor, Michigan 48109, United States
    *E-mail: [email protected] (A.L.).
  • , and 
  • Johannes W. Schwank*
    Johannes W. Schwank
    Department of Chemical Engineering, University of Michigan, 2300 Hayward Street, Ann Arbor, Michigan 48109, United States
    *Email: [email protected] (J.S.).
Cite this: ACS Catal. 2020, 10, 3, 1731–1741
Publication Date (Web):December 30, 2019
https://doi.org/10.1021/acscatal.9b05224
Copyright © 2019 American Chemical Society
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Abstract

Retaining high catalytic activity after exposure to elevated temperatures remains a crucial challenge for applications such as automotive emissions control. While catalysts generally sinter and lose activity after aging at high temperature, here we illustrate that palladium in a [email protected] morphology responds very differently. After 800 °C aging in oxygen, palladium redisperses into the encapsulating shell. The redispersion is more pronounced, and nearly complete, when palladium is encapsulated by reducible ceria, as opposed to nonreducible silica. This difference is likely due to the availability of lattice oxygen. Through comparisons with polycrystalline ceria nanoparticles, surface decorated with Pd, we show that for favorable restructuring to occur under our simple aging conditions, the process must start from a particular initial configuration, the [email protected] Furthermore, the redispersion of palladium in ceria is accompanied by a change in oxidation state and coordination that inhibits the growth of ceria crystallites in the shell, thereby producing sites that better access the reducibility of the ceria shell support. Together, these effects result in a decrease in the temperature required for 90% conversion (T90) of carbon monoxide. Our findings demonstrate that thermally induced restructuring of [email protected] morphologies under controlled conditions provides a strategy for enhancing low-temperature catalytic activity.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.9b05224.

  • Additional electron microscopy and XEDS characterization of [email protected]2, [email protected]2, and Pd/CeO2, pore size distribution and adsorption/ desorption isotherms obtained from N2 physisorption, XRD patterns of bare CeO2 nanospheres, additional CO oxidation light-off experiments for [email protected]2, Mears’ and Weisz–Prater criterion analyses, Ce3d XPS spectra for fresh and O2-aged [email protected]2, Pd/CeO2, and bare CeO2, Arrhenius experiment data for fresh and O2-aged [email protected]2 (PDF)

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Cited By


This article is cited by 14 publications.

  1. Alexander J. Hill, Adarsh Bhat, Zachary J. Berquist, Galen B. Fisher, Andrej Lenert, Johannes W. Schwank. Stabilizing Highly Dispersed Halo Sites in Thermally Restructured Palladium [email protected] Nanoparticles for Improved Catalyst Activity and Durability. ACS Applied Nano Materials 2021, 4 (10) , 10985-10998. https://doi.org/10.1021/acsanm.1c02436
  2. Lidiya S. Kibis, Alexander A. Simanenko, Andrey I. Stadnichenko, Vladimir I. Zaikovskii, Andrei I. Boronin. Probing of Pd4+ Species in a PdOx–CeO2 System by X-Ray Photoelectron Spectroscopy. The Journal of Physical Chemistry C 2021, 125 (38) , 20845-20854. https://doi.org/10.1021/acs.jpcc.1c04646
  3. Shunsaku Yasumura, Hajime Ide, Taihei Ueda, Yuan Jing, Chong Liu, Kenichi Kon, Takashi Toyao, Zen Maeno, Ken-ichi Shimizu. Transformation of Bulk Pd to Pd Cations in Small-Pore CHA Zeolites Facilitated by NO. JACS Au 2021, 1 (2) , 201-211. https://doi.org/10.1021/jacsau.0c00112
  4. Chuanbo Gao, Fenglei Lyu, Yadong Yin. Encapsulated Metal Nanoparticles for Catalysis. Chemical Reviews 2021, 121 (2) , 834-881. https://doi.org/10.1021/acs.chemrev.0c00237
  5. Richuan Rao, Hanwen Liang, Chunming Hu, Huaze Dong, Xiongzi Dong, Yongqiang Tang, Song Fang, Qiang Ling. A melamine-assisted pyrolytic synthesis of Ag-CeO2 nanoassemblys for CO oxidation: Activation of Ag-CeO2 interfacial lattice oxygen. Applied Surface Science 2022, 571 , 151283. https://doi.org/10.1016/j.apsusc.2021.151283
  6. Adarsh Bhat, Alexander J. Hill, Galen B. Fisher, Johannes W. Schwank. Improving the thermal stability and n-butanol oxidation activity of Ag-TiO2 catalysts by controlling the catalyst architecture and reaction conditions. Applied Catalysis B: Environmental 2021, 297 , 120476. https://doi.org/10.1016/j.apcatb.2021.120476
  7. Huawang Zhao, Alexander J. Hill, Lei Ma, Adarsh Bhat, Guohua Jing, Johannes W. Schwank. Progress and future challenges in passive NO adsorption over Pd/zeolite catalysts. Catalysis Science & Technology 2021, 11 (18) , 5986-6000. https://doi.org/10.1039/D1CY01084K
  8. Mingyun Zhu, Kuibo Yin, Yifeng Wen, Shugui Song, Yuwei Xiong, Yunqian Dai, Litao Sun. Combining in-situ TEM observations and theoretical calculation for revealing the thermal stability of CeO2 nanoflowers. Nano Research 2021, 50 https://doi.org/10.1007/s12274-021-3659-6
  9. Abhaya K. Datye, Martin Votsmeier. Opportunities and challenges in the development of advanced materials for emission control catalysts. Nature Materials 2021, 20 (8) , 1049-1059. https://doi.org/10.1038/s41563-020-00805-3
  10. Jiaming Wang, Guilong Liu, Huixian Zhong, Pengfei Song, Kang An, Ziyang Zhang, Ang Cao, Yuan Liu. In situ topochemical carbonization derivative Co-Ni [email protected] for direct ethanol synthesis from syngas. Applied Surface Science 2021, 8 , 149826. https://doi.org/10.1016/j.apsusc.2021.149826
  11. Jochen Schütz, Heike Störmer, Patrick Lott, Olaf Deutschmann. Effects of Hydrothermal Aging on CO and NO Oxidation Activity over Monometallic and Bimetallic Pt-Pd Catalysts. Catalysts 2021, 11 (3) , 300. https://doi.org/10.3390/catal11030300
  12. Chenxi Dong, Xupeng Zong, Wenshuai Jiang, Lijuan Niu, Ziwen Liu, Dan Qu, Xiayan Wang, Zaicheng Sun. Recent Advances of Ceria‐Based Materials in the Oxidation of Carbon Monoxide. Small Structures 2021, 2 (2) , 2000081. https://doi.org/10.1002/sstr.202000081
  13. Nating Yang, Yonghui Zhao, Hao Zhang, Weikai Xiang, Yuhan Sun, Shuai Yang, Yu Sun, Gaofeng Zeng, Kenichi Kato, Xiaopeng Li, Miho Yamauchi, Zheng Jiang, Tong Li. Sintering Activated Atomic Palladium Catalysts with High-Temperature Tolerance of ∼1,000°C. Cell Reports Physical Science 2021, 2 (1) , 100287. https://doi.org/10.1016/j.xcrp.2020.100287
  14. Wei-Jing Li, Ming-Yen Wey. Design of a thermally resistant [email protected]/halloysite catalyst with optimized structure and surface properties for a Pd-only three-way catalyst. Applied Catalysis A: General 2020, 602 , 117732. https://doi.org/10.1016/j.apcata.2020.117732