Abstract

Brønsted acidic ionic liquid (BAIL) functionalized hierarchically porous nitrogen-doped carbons (NHPCs) with interesting 3D interconnected macro-meso-microporous structure are successfully prepared by chemical bonding ‒[C3][SO3CF3−] (C3 = PrSO3H) groups throughout the NHPC supports that are obtained via a single step CaCO3 nanoparticle-directed nanocasting approach combined with K2C2O4 chemical activation and urea/melamine self-activation during the process of carbonization of glucose and urea/melamine. By changing initial urea-to-glucose weight ratio in the preparation systems, the macro/meso/micropore proportion of the resulting GU‒[C3N][SO3CF3] catalysts are well-adjusted. The morphological characteristics, porosity properties and chemical structure of the prepared catalysts are well-characterized so that the contribution of the synergistic effect of CaCO3 nanoparticle and K2C2O4 to the formation of hierarchically porous structure is revealed. Owing to super strong Brønsted acidity and unique hierarchically porous structure of the catalysts, they exhibit excellent heterogeneous acid catalytic activity in raw pyrolysis biofuel upgrading via esterification of acetic acid with high boiling point benzyl alcohol or 4-methoxybenzyl alcohol in toluene media, and therefore high acetic acid removal efficiency and efficient production of value-added benzyl acetate or 4-methoxybenzyl acetate are obtained simultaneously. The catalysts also show good reusability in target reactions, attributing to chemical interactions between BAILs and NHPC supports.

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