The development of versatile strategies for preparing functional carbon materials is essential for advancing a wide range of applications in materials science. Precursor design plays a pivotal role in governing the chemistry and structure of carbon materials for target applications. In this work, we report the synthesis of Meldrum's acid derivatives through Knoevenagel condensation with aromatic heterocycles such as pyrrole, furan, and thiophene, which serve as precursors for carbonaceous materials with tailored chemical and electronic properties. The thermal condensation of these precursors proceeds via highly reactive, electron-rich ketene intermediates, playing a crucial role in the formation of the carbon materials. The resulting heteroatom-doped carbon materials exhibit tunable chemical, physico-chemical, and structural properties, which we have correlated with their energy storage performances. Eventually, we deem this strategy of high interest for designing high-performance carbonaceous materials with tunable properties for a broad range of applications, from electrochemical energy storage to conversion, water filtration, environmental remediation, and beyond.
Keywords: Meldrum's acid, ketene, Knoevenagel condensation, reductive carbon, sodium-ion batteries.
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