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Atom by Atom Condensation of Sn Single Clusters within Gold–Phosphorus Metal–Inorganic Porous Networks

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Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Phys. Chem. Lett. 2021, 12, 2, 745-751
    Physical Insights into Chemistry, Catalysis, and Interfaces

    Atom by Atom Condensation of Sn Single Clusters within Gold–Phosphorus Metal–Inorganic Porous Networks
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    • Jia Lin Zhang
      Jia Lin Zhang
      Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543 Singapore
      Department of Physics, National University of Singapore, 2 Science Drive 3, 117542 Singapore
      More by Jia Lin Zhang
      Orcidhttp://orcid.org/0000-0002-6130-2294
    • Songtao Zhao
      Songtao Zhao
      Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science, MOE, Key Laboratory of Analytical Chemistry for Life Science in Universities of Shandong, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao, Shandong 266042, China
      More by Songtao Zhao
      Orcidhttp://orcid.org/0000-0003-0991-3677
    • Shuo Sun
      Shuo Sun
      Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543 Singapore
      Department of Physics, National University of Singapore, 2 Science Drive 3, 117542 Singapore
      More by Shuo Sun
      Orcidhttp://orcid.org/0000-0001-6092-7148
    • Wei Wang
      Wei Wang
      Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543 Singapore
      Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou 350207, China
      More by Wei Wang
    • Zhirui Ma
      Zhirui Ma
      Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543 Singapore
      More by Zhirui Ma
      Orcidhttp://orcid.org/0000-0002-1381-7752
    • Xu Lian
      Xu Lian
      Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543 Singapore
      More by Xu Lian
    • Zhenyu Li*
      Zhenyu Li
      Hefei National Laboratory for Physical Sciences at the Microscale, CAS Centre for Excellence and Synergetic Innovation Center of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei 230026, China
      *[email protected] (Z.L.).
      More by Zhenyu Li
      Orcidhttp://orcid.org/0000-0003-2112-9834
    • Wei Chen*
      Wei Chen
      Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543 Singapore
      Department of Physics, National University of Singapore, 2 Science Drive 3, 117542 Singapore
      Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou 350207, China
      National University of Singapore (Suzhou) Research Institute, 377 Lin Quan Street, Suzhou Industrial Park, Suzhou, Jiangsu 215123, China
      *[email protected] (W.C.).
      More by Wei Chen
      Orcidhttp://orcid.org/0000-0002-1131-3585
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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2021, 12, 2, 745–751
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.0c03302
    Published January 6, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    Surface supported single-atom catalysts (SACs) and single-cluster catalysts (SCCs) have been an area of rapidly growing interest due to their high efficiency of metal atom utilization and high selectivity and activity toward various catalytic reactions. However, achieving highly dispersed, structurally well-defined SACs and SCCs with high surface loadings while avoiding their sintering to larger nanoparticles (NPs) still remains a nontrivial challenge. Here, by utilizing a recently fabricated porous metal–inorganic gold–phosphorus (AuP) network, highly dispersed single Sn clusters with high surface density can be realized. This is attributed to a synergistic effect of the P6Au6 pores for providing the preferential binding sites to anchor Sn atoms and the role of P9 units as a blocking barrier to prevent the growth of Sn to larger NPs. The atom by atom condensation process of Sn single clusters with sizes ranging from monomers to heptamers as well as their binding configurations with the supporting surface are precisely identified at the atomic level, through the combination of a low-temperature scanning tunneling microscope and density functional theory calculations. Our approach opens new opportunities of utilizing metal–inorganic porous networks for the stabilization of highly dispersed and well-defined SACs and SCCs.

    Copyright © 2021 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.jpclett.0c03302.

    • Experimental methods, Supplementary Notes 1–13 for S1–S13 and Tables S1 and S2; figures of electrostatic potential slice cut through the P layer, adsorption configurations of Sn monomer on BlueP, bare Au(111) and Au(111) with a surface vacancy, structure models and simulated STM images of Sn monomers adsorbed on the P6Au6 pore, the P6Au2 pore, and the center of the P six-member ring, structure models and simulated STM images of Sn dimers with two Sn atoms adsorbed on the opposite hollow sites and the next-nearest-neighbor hollow sites of the P6Au6 pore, atomically resolved STM image showing the Sn monomers, dimers and trimers trapped into the P6Au6 pores of the AuP network, large scale and close-up STM images of Sn single-cluster superlattice on the AuP network, XPS core level spectra measured for Sn single atoms/clusters, 0.1 ML Au2Sn alloy on RT Au(111) surface, 0.2 ML Au2Sn alloy on Au(111) with the deposition performed at RT Au(111) and after annealing at 260 °C, sequential STM images showing the movable Sn atoms on Au(111) surface, structure model and simulated STM image of Au2Sn alloy layer on Au(111) surface, 1.3 ML Au2Sn alloy on Au(111) with the deposition performed at RT Au(111) and after annealing at 260 °C; tables of formation energies of Sn single clusters as a function of the cluster size N and of charge transfer data for Sn single atoms/clusters on AuP network(PDF)

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    The Journal of Physical Chemistry Letters

    Cite this: J. Phys. Chem. Lett. 2021, 12, 2, 745–751
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.jpclett.0c03302
    Published January 6, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

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