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Adatom and Nanoparticle Dynamics on Single-Atom Catalyst Substrates

Cite this: ACS Catal. 2022, 12, 9, 4859–4871
Publication Date (Web):April 8, 2022
https://doi.org/10.1021/acscatal.2c00291
Copyright © 2022 American Chemical Society

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    Abstract

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    Single-atom catalysts represent an essential and ever-growing family of heterogeneous catalysts. Recent studies indicate that besides the valuable catalytic properties provided by single-atom active sites, the presence of single-atom sites on the catalyst substrates may significantly influence the population of supported metal nanoparticles coexisting with metal single atoms. Treatment of ceria-based single-atom catalysts in oxidizing or reducing atmospheres was proven to provide a precise experimental control of the size of supported Pt nanoparticles and, correspondingly, a control of catalyst activity and stability. Based on dedicated surface science experiments, ab initio calculations, and kinetic Monte Carlo simulations, we demonstrate that the morphology of Pt nanoparticle population on ceria surface is a result of a competition for Pt atoms between Pt single-atom sites and Pt nanoparticles. In an oxidizing atmosphere, Pt single-atom sites provide strong bonding to single Pt atoms and Pt nanoparticles shrink. In reducing atmosphere, Pt single-atom sites are depopulated and Pt nanoparticles grow. We formulate a generic model of Pt redispersion and coarsening on ceria substrates. Our model provides a unified atomic-level explanation for a variety of metal nanoparticle dynamic processes observed in single-atom catalysts under stationary or alternating oxidizing/reducing atmospheres and allows us to classify the conditions under which nanoparticle ensembles on single-atom catalyst substrates can be stabilized against Ostwald ripening.

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    • Acquisition and processing of experimental data, step-edge geometries considered in DFT, and energy scale and geometry of the KMC model (PDF)

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    Cited By

    This article is cited by 8 publications.

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    2. Florian Kraushofer, Gareth S. Parkinson. Single-Atom Catalysis: Insights from Model Systems. Chemical Reviews 2022, 122 (18) , 14911-14939. https://doi.org/10.1021/acs.chemrev.2c00259
    3. Zi-Jie Xiao, Bai-Qin Zhou, Xiao-Chi Feng, Hong-Tao Shi, Yi-Ning Zhu, Cai-Peng Wang, Bart Van der Bruggen, Nan-Qi Ren. Anchored Co–oxo generated by cobalt single atoms outperformed aqueous species from the counterparts in peroxymonosulfate treatment. Applied Catalysis B: Environmental 2023, 328 , 122483. https://doi.org/10.1016/j.apcatb.2023.122483
    4. Jingyi Han, Jingqi Guan. Heteronuclear dual-metal atom catalysts for nanocatalytic tumor therapy. Chinese Journal of Catalysis 2023, 47 , 1-31. https://doi.org/10.1016/S1872-2067(22)64207-4
    5. Xiaoxiao Wei, Yingying Liu, Xiaorong Zhu, Shuowen Bo, Lei Xiao, Chen Chen, Ta Thi Thuy Nga, Yuanqing He, Mengyi Qiu, Chao Xie, Dongdong Wang, Qinghua Liu, Fan Dong, Chung‐Li Dong, Xian‐Zhu Fu, Shuangyin Wang. Dynamic Reconstitution Between Copper Single Atoms and Clusters for Electrocatalytic Urea Synthesis. Advanced Materials 2023, 50 , 2300020. https://doi.org/10.1002/adma.202300020
    6. Shiming Yu, Xing Cheng, Yueshuai Wang, Bo Xiao, Yiran Xing, Jun Ren, Yue Lu, Hongyi Li, Chunqiang Zhuang, Ge Chen. High activity and selectivity of single palladium atom for oxygen hydrogenation to H2O2. Nature Communications 2022, 13 (1) https://doi.org/10.1038/s41467-022-32450-6
    7. Alexander J. Hill, Galen B. Fisher, Andrej Lenert, Johannes W. Schwank. Intermediate temperature exposure regenerates performance and active site dispersion in sintered Pd–CeO2 catalysts. Journal of Catalysis 2022, 415 , 186-199. https://doi.org/10.1016/j.jcat.2022.10.010
    8. Yuchun Guo, Jiangtao Ren, Erkang Wang. DNA‐Encoded Nanomaterials with Controllable Properties. Analysis & Sensing 2022, 52 https://doi.org/10.1002/anse.202200067

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