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Blending Ionic and Coordinate Bonds in Hybrid Semiconductor Materials: A General Approach toward Robust and Solution-Processable Covalent/Coordinate Network Structures

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Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Am. Chem. Soc. 2020, 142, 9, 4242-4253
    Article

    Blending Ionic and Coordinate Bonds in Hybrid Semiconductor Materials: A General Approach toward Robust and Solution-Processable Covalent/Coordinate Network Structures
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    • Xiuze Hei
      Xiuze Hei
      Department of Chemistry and Chemical Biology, Rutgers University, 610 Taylor Road, Piscataway, New Jersey 08854, United States
      More by Xiuze Hei
    • Wei Liu
      Wei Liu
      Hoffmann Institute of Advanced Materials, Shenzhen Polytechnic, 7098 Liuxian Blvd., Nanshan District, Shenzhen 518055, China
      Department of Chemistry and Chemical Biology, Rutgers University, 610 Taylor Road, Piscataway, New Jersey 08854, United States
      More by Wei Liu
    • Kun Zhu
      Kun Zhu
      Department of Chemistry and Chemical Biology, Rutgers University, 610 Taylor Road, Piscataway, New Jersey 08854, United States
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      Orcidhttp://orcid.org/0000-0001-9059-513X
    • Simon J. Teat
      Simon J. Teat
      Advanced Light Source, Lawrence Berkeley National Laboratory, 1 Cyclotron Road, Berkeley, California 94720, United States
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    • Stephanie Jensen
      Stephanie Jensen
      Department of Physics and Center for Functional Materials, Wake Forest University, Winston-Salem, North Carolina 27109, United States
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    • Mingxing Li
      Mingxing Li
      Center for Functional Nanomaterials, Brookhaven National Laboratory, 98 Rochester Street, Upton, New York 11973, United States
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    • Deirdre M. O’Carroll
      Deirdre M. O’Carroll
      Department of Chemistry and Chemical Biology, Rutgers University, 610 Taylor Road, Piscataway, New Jersey 08854, United States
      Department of Materials Science and Engineering, Rutgers University, 607 Taylor Road, Piscataway, New Jersey 08854, United States
      More by Deirdre M. O’Carroll
      Orcidhttp://orcid.org/0000-0001-7209-4278
    • Kevin Wei
      Kevin Wei
      Department of Materials Science & Engineering, University of Texas at Dallas, Richardson, Texas 75080, United States
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    • Kui Tan
      Kui Tan
      Department of Materials Science & Engineering, University of Texas at Dallas, Richardson, Texas 75080, United States
      More by Kui Tan
      Orcidhttp://orcid.org/0000-0002-5167-7295
    • Mircea Cotlet
      Mircea Cotlet
      Center for Functional Nanomaterials, Brookhaven National Laboratory, 98 Rochester Street, Upton, New York 11973, United States
      More by Mircea Cotlet
      Orcidhttp://orcid.org/0000-0002-5024-3540
    • Timo Thonhauser
      Timo Thonhauser
      Department of Physics and Center for Functional Materials, Wake Forest University, Winston-Salem, North Carolina 27109, United States
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    • Jing Li*
      Jing Li
      Department of Chemistry and Chemical Biology, Rutgers University, 610 Taylor Road, Piscataway, New Jersey 08854, United States
      Hoffmann Institute of Advanced Materials, Shenzhen Polytechnic, 7098 Liuxian Blvd., Nanshan District, Shenzhen 518055, China
      *[email protected]
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      Orcidhttp://orcid.org/0000-0001-7792-4322
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    Cite this: J. Am. Chem. Soc. 2020, 142, 9, 4242–4253
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    https://doi.org/10.1021/jacs.9b13772
    Published February 11, 2020
    Copyright © 2020 American Chemical Society
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    Abstract

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    Inorganic semiconductor materials are best known for their superior physical properties, as well as their structural rigidity and stability. However, the poor solubility and solution-processability of these covalently bonded network structures has long been a serious drawback that limits their use in many important applications. Here, we present a unique and general approach to synthesize robust, solution-processable, and highly luminescent hybrid materials built on periodic and infinite inorganic modules. Structure analysis confirms that all compounds are composed of one-dimensional anionic chains of copper iodide (CumIm+22–) coordinated to cationic organic ligands via Cu–N bonds. The choice of ligands plays an important role in the coordination mode (μ1-MC or μ2-DC) and Cu–N bond strength. Greatly suppressed nonradiative decay is achieved for the μ2-DC structures. Record high quantum yields of 85% (λex = 360 nm) and 76% (λex = 450 nm) are obtained for an orange-emitting 1D-Cu4I6(L6). Temperature dependent PL measurements suggest that both phosphorescence and thermally activated delayed fluorescence contribute to the emission of these 1D-AIO compounds, and that the extent of nonradiative decay of the μ2-DC structures is much less than that of the μ1-DC structures. More significantly, all compounds are remarkably soluble in polar aprotic solvents, distinctly different from previously reported CuI based hybrid materials made of charge-neutral CumXm (X = Cl, Br, I), which are totally insoluble in all common solvents. The greatly enhanced solubility is a result of incorporation of ionic bonds into extended covalent/coordinate network structures, making it possible to fabricate large scale thin films by solution processes.

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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/jacs.9b13772.

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    Cited By

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    This article is cited by 79 publications.

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    Cite this: J. Am. Chem. Soc. 2020, 142, 9, 4242–4253
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