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Mixed-Metal Cu–Zn Thiocyanate Coordination Polymers with Melting Behavior, Glass Transition, and Tunable Electronic Properties

  • Chayanit Wechwithayakhlung
    Chayanit Wechwithayakhlung
    Department of Materials Science and Engineering, School of Molecular Science and Engineering, Vidyasirimedhi Institute of Science and Technology (VISTEC), Rayong 21210, Thailand
    Institute for Integrated Cell-Material Sciences (iCeMS), Institute for Advanced Study, Kyoto University, Yoshida-Honmachi, Sakyo-ku, Kyoto 606-8501, Japan
  • Suttipong Wannapaiboon
    Suttipong Wannapaiboon
    Synchrotron Light Research Institute (Public Organization), 111 University Avenue, Muang District, Nakhon Ratchasima 30000, Thailand
  • Sutassana Na-Phattalung
    Sutassana Na-Phattalung
    Division of Physics, School of Science, Walailak University, Nakhon Si Thammarat 80160, Thailand
    Functional Materials and Nanotechnology Center of Excellence, Walailak University, Nakhon Si Thammarat 80160, Thailand
  • Phisut Narabadeesuphakorn
    Phisut Narabadeesuphakorn
    Department of Materials Science and Engineering, School of Molecular Science and Engineering, Vidyasirimedhi Institute of Science and Technology (VISTEC), Rayong 21210, Thailand
  • Similan Tanjindaprateep
    Similan Tanjindaprateep
    Department of Materials Science and Engineering, School of Molecular Science and Engineering, Vidyasirimedhi Institute of Science and Technology (VISTEC), Rayong 21210, Thailand
  • Saran Waiprasoet
    Saran Waiprasoet
    Department of Materials Science and Engineering, School of Molecular Science and Engineering, Vidyasirimedhi Institute of Science and Technology (VISTEC), Rayong 21210, Thailand
  • Thidarat Imyen
    Thidarat Imyen
    Institute for Integrated Cell-Material Sciences (iCeMS), Institute for Advanced Study, Kyoto University, Yoshida-Honmachi, Sakyo-ku, Kyoto 606-8501, Japan
  • Satoshi Horike*
    Satoshi Horike
    Department of Materials Science and Engineering, School of Molecular Science and Engineering, Vidyasirimedhi Institute of Science and Technology (VISTEC), Rayong 21210, Thailand
    Institute for Integrated Cell-Material Sciences (iCeMS), Institute for Advanced Study, Kyoto University, Yoshida-Honmachi, Sakyo-ku, Kyoto 606-8501, Japan
    *Email: [email protected]
  • , and 
  • Pichaya Pattanasattayavong*
    Pichaya Pattanasattayavong
    Department of Materials Science and Engineering, School of Molecular Science and Engineering, Vidyasirimedhi Institute of Science and Technology (VISTEC), Rayong 21210, Thailand
    Research Network of NANOTEC-VISTEC on Nanotechnology for Energy, Vidyasirimedhi Institute of Science and Technology (VISTEC), Rayong 21210, Thailand
    *Email: [email protected]
Cite this: Inorg. Chem. 2021, 60, 21, 16149–16159
Publication Date (Web):October 19, 2021
https://doi.org/10.1021/acs.inorgchem.1c01813
Copyright © 2021 American Chemical Society

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    Abstract

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    The solid-state mechanochemical reactions under ambient conditions of CuSCN and Zn(SCN)2 resulted in two novel materials: partially Zn-substituted α-CuSCN and a new phase CuxZny(SCN)x+2y. The reactions take place at the labile S-terminal, and both products show melting and glass transition behaviors. The optical band gap and solid-state ionization potential can be adjusted systematically by adjusting the Cu/Zn ratio. Density functional theory calculations also reveal that the Zn-substituted CuSCN structure features a complementary electronic structure of Cu 3d states at the valence band maximum and Zn 4s states at the conduction band minimum. This work shows a new route to develop semiconductors based on coordination polymers, which are becoming technologically relevant for electronic and optoelectronic applications.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.inorgchem.1c01813.

    • Full descriptions of experimental and computational methods; supporting figures for results from PXRD (phase identification), TEM (microstructure), TG-DTA (further evidence of melting), DSC (glass transitions), UV–vis-NIR (band gap determination), and XAS (k-space and R-space plots) experiments; defect formation energies for ZnCu0 and ZnCu+ from DFT calculations; and tabulated atomic ratios from SEM-EDX and ICP measurements (PDF)

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    Cited By

    This article is cited by 2 publications.

    1. Maria V. Kashina, Mikhail A. Kinzhalov, Elena Yu. Tupikina, Vadim Yu. Kukushkin. Linear and Bent Noncovalent M···S═C═N–M′ Interactions: The Case of Palladium(II) and Platinum(II) Thiocyanate Species. Crystal Growth & Design 2023, 23 (6) , 4322-4335. https://doi.org/10.1021/acs.cgd.3c00116
    2. Pimpisut Worakajit, Pinit Kidkhunthod, Thanasee Thanasarnsurapong, Saran Waiprasoet, Hideki Nakajima, Taweesak Sudyoadsuk, Vinich Promarak, Adisak Boonchun, Pichaya Pattanasattayavong. Origin of Hole‐Trapping States in Solution‐Processed Copper(I) Thiocyanate and Defect‐Healing by I 2 Doping. Advanced Functional Materials 2023, 232 , 2209504. https://doi.org/10.1002/adfm.202209504