Efficient Flow Synthesis of Aspirin within 2D Sub-Nanoconfined Laminar Annealed Graphene Oxide Membranes

Adv Mater. 2024 Mar;36(11):e2310954. doi: 10.1002/adma.202310954. Epub 2023 Dec 14.

Abstract

The aim of this work is to develop an environmentally friendly, safe, and simple route for realizing efficient preparation of aspirin. Here, inspired by enzyme synthesis in vivo, the aspirin synthesis has been realized by sub-nanoconfined esterification with directional flow and ≈100% conversion in an unprecedented reaction time of <6.36 s at 23 °C. Such flow esterification reaction is catalyzed by thermally transformed graphene oxide (GO) membranes with tailored physicochemical properties, which can be obtained simply through a mild annealing method. A possible mechanism is revealed by density functional theory calculation, indicating that the synergistic effect of spatial confinement and surface electronic structure can significantly improve the catalytic performance. By restricting reactants within 2D sub-nano space created by GO-based laminar flow-reactors, the present strategy provides a new route to achieve rapid flow synthesis of aspirin with nearly complete conversion.

Keywords: aspirin synthesis; directional flow; graphene oxide membrane; interlayer sub-nanoconfinement; mild annealing.