Innovative strategies for nitrogen-incorporating silicon oxycarbide-based preceramic polymer synthesis

Abstract

In this study, we introduce a pioneering methodology for crafting silicon oxycarbonitride materials (SiOCN) by harnessing the intricate synergy between allyl-substituted hydrido polycarbosilane (AHPCS) and a novel triazine-based dendron, serving as a nitrogen-containing polymeric precursor. The synthetic journey involves meticulous hydrosilylation reactions between AHPCS's Si–H moieties and the –CHCH₂ groups embedded within the triazine dendritic architecture, followed by controlled pyrolysis under an argon atmosphere at temperatures up to 900 °C. Through systematic variations in reaction durations and pyrolytic temperatures, we uncover the prevalence of SiC_4−xO_x motifs within the material matrix, with oxygen content modulation observed in samples under extended reaction times and heightened pyrolysis temperatures. Nitrogen-based bonding's paramount importance within the N-containing polymeric precursor is also established, revealing a preference for retaining N sp²–C over N sp³–C bonds due to intricate nitrogen–AHPCS interactions that yield robust Si–N linkages. This inquiry not only advances our fundamental understanding but also charts a course for tailoring silicon oxycarbonitride –SiOCN– material properties. Promisingly, these advancements position such materials as prospective candidates for high-energy silicon oxycarbonitride-based supercapacitors, bridging pioneering materials science with sustainable energy storage technology.