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Eco-Friendly Electrophoretic Deposition of Fluorescent Nanocomposite Films in an Aqueous Dispersion of Hydrophilized Core/Shell CuInS2/ZnS Quantum Dots for Optoelectronic Applications

  • Asshu Morimoto
    Asshu Morimoto
    Department of Applied Chemistry, Faculty of Science and Technology, Keio University, 3-14-1 Hiyoshi, Kohoku-ku, Yokohama 223-8522, Japan
  • Yoshiki Iso*
    Yoshiki Iso
    Department of Applied Chemistry, Faculty of Science and Technology, Keio University, 3-14-1 Hiyoshi, Kohoku-ku, Yokohama 223-8522, Japan
    *Email: [email protected]. Phone: +81 45 566 1558. Fax: +81 45 566 1551.
    More by Yoshiki Iso
  • , and 
  • Tetsuhiko Isobe*
    Tetsuhiko Isobe
    Department of Applied Chemistry, Faculty of Science and Technology, Keio University, 3-14-1 Hiyoshi, Kohoku-ku, Yokohama 223-8522, Japan
    *Email: [email protected]. Phone: +81 45 566 1554. Fax: +81 45 566 1551.
Cite this: ACS Appl. Mater. Interfaces 2024, 16, 6, 7780–7789
Publication Date (Web):February 5, 2024
https://doi.org/10.1021/acsami.3c17264
Copyright © 2024 The Authors. Published by American Chemical Society

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    Abstract

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    Low-toxic and efficient fluorescent core–shell CuInS2/ZnS (CIS/ZnS) quantum dots (QDs) are good candidates for optoelectronic device applications. They are synthesized in a hydrophobic environment, while large amounts of organic solvents used in the preparation of fluorescent films have significant problems on environmental load and human health. CIS/ZnS QDs hydrophilized by adsorbing 3-mercaptopropionic acid on their surfaces can be used in the aqueous film fabrication process. In this work, the aqueous electrophoretic deposition (EPD) of the hydrophilized QDs with silicone-modified acrylic resin nanoparticles was performed to fabricate fluorescent nanocomposite films. The hydrophilized QDs and resin nanoparticles were simultaneously dispersed in basic aqueous solutions due to electrostatic repulsion resulting from their negatively charged surfaces. Transparent films were obtained on a transparent conductive substrate at the anode side by the EPD. They showed yellow fluorescence of the QDs. The thickness increased with increasing the deposition time; however, hemispherical holes attributed to oxygen gas generated by water electrolysis were observed at the longer time. The electron microscopy revealed that the films were densely and homogeneously deposited. The QDs were dispersed around the resin nanoparticles without aggregation. The fluorescence (FL) quantum yield was 43%. The optical absorption peak and FL intensity of the QDs increased accompanied by the film growth. The nanocomposite film showed good heat resistance at 80–120 °C for 5 h; therefore, the prepared films have feasibility in white light-emitting diode (LED) applications. A lightening device structured with the obtained EPD film placed on a blue LED successfully emitted white light. In addition, the flexibility of the nanocomposite film was demonstrated. The aqueous EPD method would be one of the suitable methods for the industrial production of fluorescent QD films. This technique can be applied to other hydrophilic fluorescent QDs with charged surfaces. Realization of various fluorescent QD films would expand the application possibilities.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.3c17264.

    • FL measurement method for an EPD film sample using an integrating sphere (Figure S1); XRD profiles of hydrophobic CIS/ZnS QDs and hydrophilized QDs (Figure S2); TEM images and corresponding size distributions of hydrophobic and hydrophilized QDs (Figure S3); TEM image of silicon-modified acrylic resin nanoparticles and corresponding size distribution (Figure S4); photographs of hydrophilized CIS/ZnS QDs dispersed in aqueous TMAS, TMAOH, and NaOH solutions at different pH values (Figure S5); UV–vis absorption spectra and corresponding Tauc plots for the hydrophobic QDs in toluene and hydrophilized QDs in TMAOH solution (Figure S6); change in FL spectrum of the dispersion for EPD after preparation (Figure S7); bright field and fluorescent microscope images of nanocomposite films deposited for 1–5 min (Figure S8); change in film thickness with deposition time of the EPD process (Figure S9); XRF spectra of powdered samples (Figure S10); change in net optical density at 380 nm of nanocomposite film with thickness (Figure S11); changes in transmission spectra and FL spectra due to heating (Figure S12); TG-DTA profiles of dried hydrophilized QDs and resin nanoparticles under air flow (Figure S13) (PDF)

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