A series of multi-crosslinkable, self-healing, ladder-structured polysilsesquioxane inorganic-organic hybrid materials were developed to enhance the mechanical properties through tandem UV-curing and Diels-Alder chemistry. The introduction of UV-curable acryl- or epoxy groups allowed for a higher degree of crosslink density while bringing the inorganic backbones closer together for highly efficient self-healing properties, all with a singular material as the ternary organic functional groups consisting of UV-curable function, diene, and dienophile were tethered to the well-defined inorganic backbone. Exceptional thermal stability (>400 °C), optical transparency (>95%), solution processability, as well as robust surface mechanical properties in both bulk (pencil hardness 6H) and nanoscale (elastic modulus > 9 GPa), properties which can be adroitly recovered through mild and rapid thermal treatment hold great promise for next generation hybrid smart coating materials for application in optoelectronic devices.

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Volume 124, 25 August 2017, Pages 78-87