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On-Surface Synthesis of Nitrogen-Substituted Gold-Phosphorus Porous Network
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    On-Surface Synthesis of Nitrogen-Substituted Gold-Phosphorus Porous Network
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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
    • Songtao Zhao
      Songtao Zhao
      Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science, MOE, College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao, Shandong 266042, China
      More by Songtao Zhao
    • 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
    • Xu Lian
      Xu Lian
      Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore
      More by Xu Lian
    • Anton Tadich
      Anton Tadich
      Australian Synchrotron, 800 Blackburn Road, Clayton, Victoria 3168, Australia
      More by Anton Tadich
    • Dong-Chen Qi
      Dong-Chen Qi
      Centre for Materials Science, School of Chemistry and Physics, Queensland University of Technology, Brisbane, Queensland 4001, Australia
      More by Dong-Chen Qi
    • Chengding Gu
      Chengding Gu
      Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore
      More by Chengding Gu
    • Zhirui Ma
      Zhirui Ma
      Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore
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    • 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: [email protected]
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    • 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, Jiangsu 215123, China
      *Email: [email protected]
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    Other Access OptionsSupporting Information (1)

    Chemistry of Materials

    Cite this: Chem. Mater. 2020, 32, 19, 8561–8566
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    https://doi.org/10.1021/acs.chemmater.0c02889
    Published September 8, 2020
    Copyright © 2020 American Chemical Society

    Abstract

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    Porous metal–organic frameworks (MOFs) have become one of the fastest growing fields with broad applications due to the presence of various active sites (e.g., cavities, metal nodes, and organic linkers). Notably, an on-surface synthesis represents a facile method for the fabrication of two-dimensional (2D) MOFs, where the substrate not only supports and dictates the symmetry of the surface nanostructures but also provides the metal atoms to form the metal nodes. However, the realization of on-surface synthesized 2D metal–inorganic porous networks is rarely explored, except for a recently reported gold-phosphorus network. Here, we integrate one more dimension into the growth process (activated gas phase atoms) and demonstrate the on-surface synthesis of ternary metal–inorganic gold-phosphorus-nitrogen porous networks on Au(111). The atomic structure is precisely identified through a combination of low-temperature scanning tunneling microscopy, density functional theory calculations, and X-ray photoelectron spectroscopy. Using the thermal energy from the heated Au(111) substrate, the phosphorus precursor can simultaneously grab gold atoms from the surface and nitrogen atoms from activated nitrogen gas to build up a long-range ordered 2D surface porous structure. Our study opens a completely new platform for the on-surface synthesis of tailored metal–inorganic frameworks.

    Copyright © 2020 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.chemmater.0c02889.

    • Large-scale STM image of the nitrogen-substituted gold-phosphorus network on Au(111) grown in a nitrogen background pressure of 5 × 10–5 mbar, high-resolution STM image showing different nitrogen substitution configurations, STM image of the gold-phosphorus network grown in a nitrogen environment with a hot filament switched off, high-resolution STM images of the nitrogen-doped gold-phosphorus networks with the experiments performed independently three times, charge transfer calculation for N atoms substituted to different sites, and simulated STM image for the 6 N per unit cell substituted gold-phosphorus-nitrogen network (PDF)

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    This article is cited by 3 publications.

    1. Harjinder Singh, Imtiaz Ahmed, Rathindranath Biswas, Shouvik Mete, Krishna Kamal Halder, Biplab Banerjee, Krishna Kanta Haldar. Genomic DNA-mediated formation of a porous Cu 2 (OH)PO 4 /Co 3 (PO 4 ) 2 ·8H 2 O rolling pin shape bifunctional electrocatalyst for water splitting reactions. RSC Advances 2022, 12 (6) , 3738-3744. https://doi.org/10.1039/D1RA09098D
    2. Yihe Wang, Shuo Sun, Jialin Zhang, Yu Li Huang, Wei Chen. Recent progress in epitaxial growth of two‐dimensional phosphorus. SmartMat 2021, 2 (3) , 286-298. https://doi.org/10.1002/smm2.1055
    3. Shannon J. Lee, Juyeon Won, Lin‐Lin Wang, Dapeng Jing, Colin P. Harmer, Justin Mark, Georgiy Akopov, Kirill Kovnir. New Noncentrosymmetric Tetrel Pnictides Composed of Square‐Planar Gold(I) with Peculiar Bonding. Chemistry – A European Journal 2021, 27 (26) , 7383-7390. https://doi.org/10.1002/chem.202005312

    Chemistry of Materials

    Cite this: Chem. Mater. 2020, 32, 19, 8561–8566
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.chemmater.0c02889
    Published September 8, 2020
    Copyright © 2020 American Chemical Society

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