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Fine-tuned local coordination environment of Pt single atoms on ceria controls catalytic reactivity

Author

Listed:
  • Wei Tan

    (University of Central Florida
    Nanjing University)

  • Shaohua Xie

    (University of Central Florida)

  • Duy Le

    (University of Central Florida)

  • Weijian Diao

    (Villanova University)

  • Meiyu Wang

    (Nanjing University)

  • Ke-Bin Low

    (BASF Corporation)

  • Dave Austin

    (University of Central Florida)

  • Sampyo Hong

    (Brewton-Parker College)

  • Fei Gao

    (Nanjing University)

  • Lin Dong

    (Nanjing University)

  • Lu Ma

    (Brookhaven National Laboratory)

  • Steven N. Ehrlich

    (Brookhaven National Laboratory)

  • Talat S. Rahman

    (University of Central Florida)

  • Fudong Liu

    (University of Central Florida)

Abstract

Constructing single atom catalysts with fine-tuned coordination environments can be a promising strategy to achieve satisfactory catalytic performance. Herein, via a simple calcination temperature-control strategy, CeO2 supported Pt single atom catalysts with precisely controlled coordination environments are successfully fabricated. The joint experimental and theoretical analysis reveals that the Pt single atoms on Pt1/CeO2 prepared at 550 °C (Pt/CeO2-550) are mainly located at the edge sites of CeO2 with a Pt–O coordination number of ca. 5, while those prepared at 800 °C (Pt/CeO2-800) are predominantly located at distorted Ce substitution sites on CeO2 terrace with a Pt–O coordination number of ca. 4. Pt/CeO2-550 and Pt/CeO2-800 with different Pt1-CeO2 coordination environments exhibit a reversal of activity trend in CO oxidation and NH3 oxidation due to their different privileges in reactants activation and H2O desorption, suggesting that the catalytic performance of Pt single atom catalysts in different target reactions can be maximized by optimizing their local coordination structures.

Suggested Citation

  • Wei Tan & Shaohua Xie & Duy Le & Weijian Diao & Meiyu Wang & Ke-Bin Low & Dave Austin & Sampyo Hong & Fei Gao & Lin Dong & Lu Ma & Steven N. Ehrlich & Talat S. Rahman & Fudong Liu, 2022. "Fine-tuned local coordination environment of Pt single atoms on ceria controls catalytic reactivity," Nature Communications, Nature, vol. 13(1), pages 1-16, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-34797-2
    DOI: 10.1038/s41467-022-34797-2
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    References listed on IDEAS

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    1. Fei Wang & Jinzhu Ma & Shaohui Xin & Qiang Wang & Jun Xu & Changbin Zhang & Hong He & Xiao Cheng Zeng, 2020. "Resolving the puzzle of single-atom silver dispersion on nanosized γ-Al2O3 surface for high catalytic performance," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    2. Yuan Pan & Yinjuan Chen & Konglin Wu & Zheng Chen & Shoujie Liu & Xing Cao & Weng-Chon Cheong & Tao Meng & Jun Luo & Lirong Zheng & Chenguang Liu & Dingsheng Wang & Qing Peng & Jun Li & Chen Chen, 2019. "Regulating the coordination structure of single-atom Fe-NxCy catalytic sites for benzene oxidation," Nature Communications, Nature, vol. 10(1), pages 1-11, December.
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    Cited by:

    1. Tengfei Zhang & Peng Zheng & Jiajian Gao & Xiaolong Liu & Yongjun Ji & Junbo Tian & Yang Zou & Zhiyi Sun & Qiao Hu & Guokang Chen & Wenxing Chen & Xi Liu & Ziyi Zhong & Guangwen Xu & Tingyu Zhu & Fabi, 2024. "Simultaneously activating molecular oxygen and surface lattice oxygen on Pt/TiO2 for low-temperature CO oxidation," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    2. Hongqiang Jin & Kaixin Zhou & Ruoxi Zhang & Hongjie Cui & Yu Yu & Peixin Cui & Weiguo Song & Changyan Cao, 2023. "Regulating the electronic structure through charge redistribution in dense single-atom catalysts for enhanced alkene epoxidation," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    3. Yiming Zhu & Malte Klingenhof & Chenlong Gao & Toshinari Koketsu & Gregor Weiser & Yecan Pi & Shangheng Liu & Lijun Sui & Jingrong Hou & Jiayi Li & Haomin Jiang & Limin Xu & Wei-Hsiang Huang & Chih-We, 2024. "Facilitating alkaline hydrogen evolution reaction on the hetero-interfaced Ru/RuO2 through Pt single atoms doping," Nature Communications, Nature, vol. 15(1), pages 1-13, December.

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