Acid-Catalyzed Construction of High-Performance Polybenzoxazine-Based Carbon Aerogels with Tunable Multiscale Structures

Herein, we report a catalyst-directed polymerization pathway engineering strategy for the construction of polybenzoxazine-derived carbon aerogels via an acid-catalyzed sol–gel process combined with ambient-pressure drying.

By systematically tuning the hydrochloric acid dosage, the relative participation of carbocation- and iminium-derived crosslinking reactions was regulated, giving rise to precursor networks with distinct crosslinking densities and structural compactness. These chemically defined precursor architectures were largely inherited during carbonization, resulting in carbon frameworks with distinct microcrystalline continuity and hierarchical pore structures.