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Revealing Charge Transfer at the Interface of Spinel Oxide and Ceria during CO Oxidation

  • Sinmyung Yoon
    Sinmyung Yoon
    School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
  • Jinwoung Jo
    Jinwoung Jo
    Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea
    School of Chemical and Biological Engineering, and Institute of Chemical Processes, Seoul National University, Seoul 08826, Republic of Korea
    More by Jinwoung Jo
  • Beomjoon Jeon
    Beomjoon Jeon
    Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS), Daejeon 34141, Republic of Korea
    Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea
  • Jihyeon Lee
    Jihyeon Lee
    School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
    More by Jihyeon Lee
  • Min Gee Cho
    Min Gee Cho
    Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea
    School of Chemical and Biological Engineering, and Institute of Chemical Processes, Seoul National University, Seoul 08826, Republic of Korea
    More by Min Gee Cho
  • Myoung Hwan Oh
    Myoung Hwan Oh
    Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea
    School of Chemical and Biological Engineering, and Institute of Chemical Processes, Seoul National University, Seoul 08826, Republic of Korea
  • Beomgyun Jeong
    Beomgyun Jeong
    Research Center for Materials Analysis, Korea Basic Science Institute (KBSI), Daejeon 34133, Republic of Korea
  • Tae Joo Shin
    Tae Joo Shin
    UNIST Central Research Facilities, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
    More by Tae Joo Shin
  • Hu Young Jeong
    Hu Young Jeong
    UNIST Central Research Facilities, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
  • Jeong Young Park
    Jeong Young Park
    Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS), Daejeon 34141, Republic of Korea
    Department of Chemistry, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 34141, Republic of Korea
  • Taeghwan Hyeon*
    Taeghwan Hyeon
    Center for Nanoparticle Research, Institute for Basic Science (IBS), Seoul 08826, Republic of Korea
    School of Chemical and Biological Engineering, and Institute of Chemical Processes, Seoul National University, Seoul 08826, Republic of Korea
    *Email: [email protected]
  • , and 
  • Kwangjin An*
    Kwangjin An
    School of Energy and Chemical Engineering, Ulsan National Institute of Science and Technology (UNIST), Ulsan 44919, Republic of Korea
    *Email: [email protected]
    More by Kwangjin An
Cite this: ACS Catal. 2021, 11, 3, 1516–1527
Publication Date (Web):January 15, 2021
https://doi.org/10.1021/acscatal.0c04091
Copyright © 2021 American Chemical Society
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Abstract

The interface created between an active metal and an oxide support is known to affect the catalytic performance because of the charge transfer process. However, oxide–oxide interfaces produced by supported spinel oxide catalysts have been less studied owing to their complex interface structures and synthetic challenges. Herein, a synthetic strategy for Co3O4, Mn3O4, and Fe3O4 nanocubes (NCs) with a controlled CeO2 layer enables investigation of the role of the interface in catalytic oxidation. Notably, CeO2-deposited Co3O4 NCs exhibited a 12-times higher CO oxidation rate than the pristine Co3O4 NCs. In situ characterization demonstrates that the deposited CeO2 prevents the reduction of Co3O4 by supplying oxygen. The maximized interface resulting from Co3O4 NCs with three facets covered by CeO2 layers was found to exhibit the highest CO oxidation rate even under O2-deficient conditions, which resulted from the versatile variation in the oxidation state. This study provides a comprehensive understanding of the Mars–van Krevelen mechanism occurring on the nanoscale at the Co3O4–CeO2 interfaces. The same activity trend and hot electron flow are observed for H2 oxidation reactions using catalytic nanodiodes, thereby demonstrating that the origin of the activity enhancement is charge transfer at the interface.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acscatal.0c04091.

  • TEM, TGA, XRD, XANES, and EXAFS data of Co3O4, Mn3O4, and Fe3O4 NCs with CeO2 NCs; UV treatment and CO chemisorption results; CO oxidation activity of Mn3O4–CeO2 and Fe3O4–CeO2 NCs; in situ XRD and XANES; NAP-XPS spectra; Raman spectra of Co3O4–CeO2 NCs; SEM images of assembled Co3O4–CeO2 NCs; IV characteristics; and detailed TOFs for CO oxidation (PDF)

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Cited By


This article is cited by 5 publications.

  1. Jeongjin Kim, Hanseul Choi, Daeho Kim, Jeong Young Park. Operando Surface Studies on Metal-Oxide Interfaces of Bimetal and Mixed Catalysts. ACS Catalysis 2021, 11 (14) , 8645-8677. https://doi.org/10.1021/acscatal.1c02340
  2. Shuaiqi Zhao, Peng Wu, Jiajin Lin, Yifei Li, Anqi Li, Xiaojing Jin, Yu Chen, Bote Zhao, Yun Zhao, Guangxu Chen, Yongcai Qiu, Daiqi Ye, Shihe Yang. Unveiling the water-resistant mechanism of Cu(I)-O-Co interfaces for catalytic oxidation. Chemical Engineering Journal 2022, 429 , 132219. https://doi.org/10.1016/j.cej.2021.132219
  3. Chenxi Dong, Xupeng Zong, Ziwen Liu, Lijuan Niu, Zhao Zhao, Li An, Dan Qu, Xiayan Wang, Zaicheng Sun. Light-promoted activation of oxygen and carbon monoxide for low-temperature catalytic oxidation. Cell Reports Physical Science 2021, 50 , 100678. https://doi.org/10.1016/j.xcrp.2021.100678
  4. Sinmyung Yoon, Hyunwoo Ha, Jihun Kim, Eonu Nam, Mi Yoo, Beomgyun Jeong, Hyun You Kim, Kwangjin An. Influence of the Pt size and CeO 2 morphology at the Pt–CeO 2 interface in CO oxidation. Journal of Materials Chemistry A 2021, 9 (46) , 26381-26390. https://doi.org/10.1039/D1TA06850D
  5. Kasala Prabhakar Reddy, Hanseul Choi, Daeho Kim, Minkee Choi, Ryong Ryoo, Jeong Young Park. The facet effect of ceria nanoparticles on platinum dispersion and catalytic activity of methanol partial oxidation. Chemical Communications 2021, 57 (60) , 7382-7385. https://doi.org/10.1039/D1CC02728J