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 SiC4−xOx 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.