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High-Refractive-Index Polysiloxanes Containing Naphthyl and Phenanthrenyl Groups and Their Thermally Cross-Linked Resins

Cite this: Macromolecules 2022, 55, 11, 4675–4691
Publication Date (Web):May 19, 2022
https://doi.org/10.1021/acs.macromol.2c00265
Copyright © 2022 The Authors. Published by American Chemical Society

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    Abstract

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    High-refractive-index polysiloxanes containing naphthyl, phenanthrenyl, phenyl, and methyl groups have been synthesized using a polycondensation reaction starting from substituted di- and trialkoxysilanes. The obtained polymers comprised linear siloxane and partially cross-linked silsesquioxane units and showed optical transparencies of up to 99% at a thickness around 120 μm and high refractive indices of up to 1.622. The polymeric structures contained stabilized silanol groups that were further cross-linked at increased temperatures of 200 °C resulting in the formation of hybrid inorganic–organic resins. These typical thermal treatments at 200 °C for 72 h kept the transparencies as high as 98% and slightly lowered the RIs to values up to 1.610. A detailed structure evaluation of the resulting systems showed, depending on the size of the polycyclic aromatic substituent, excimer formation, which is based on weak interactions of the aromatic groups in the polymeric material. After thermal consolidation, glass-transition temperatures of the cross-linked systems were in the range of 18–74 °C depending on the composition. Thermal stabilities of the final resins reached higher values than commonly used siloxane resins up to 470 °C. The final materials are potential resins for high-temperature optical applications.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.macromol.2c00265.

    • Spectroscopic data, elemental analysis, and RI measurements of dialkoxysilanes; spectroscopic, SEC, and MALDI-TOF data; DOC calculations; PXRD; and RI measurements of polysiloxanes (PDF)

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    Cited By

    This article is cited by 2 publications.

    1. Yujin Jeon, Jisung Choi, Donghwa Seo, Soon Hwa Jung, Jeewoo Lim. Low birefringence and low dispersion aliphatic thermosets with a high and tunable refractive index. Polymer Chemistry 2023, 14 (10) , 1117-1123. https://doi.org/10.1039/D2PY01327D
    2. Cedric P. Ambulo, Kyle J. Carothers, Ashford T. Hollis, Hannah N. Limburg, Lirong Sun, Carl J. Thrasher, Michael E. McConney, Nicholas P. Godman. Photo‐Crosslinkable Inorganic/Organic Sulfur Polymers. Macromolecular Rapid Communications 2023, 44 (5) , 2200798. https://doi.org/10.1002/marc.202200798

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