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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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