Gaussian curvature engineering of self-pressurizing mesoporous nanoreactors boosts dynamic equilibrium of molecule adsorption-desorption

Modulating the molecule adsorption-desorption behaviors of solid catalysts is important for fulfilling complicated catalytic purposes. Herein, we quantitatively reveal the dynamic balancing of molecule adsorption/desorption by curvature modulation on a series of self-pressurizing mesoporous nanoreactors with controlled concave-convex Gaussian curvatures via a programmable nanodroplet buckling strategy. The encapsulation of Fe3O4 nanoparticles in the cavity produces a large temperature difference between the nanoreactor surface (193.8 °C) and the reaction medium (73.7 °C) under photoexcitation, forming thermally confined self-pressurizing nanoreactors. Together with the external pressure exerted by the liquid-surface-tension on the concave-convex surfaces, the self-pressurizing drives the dynamic regulation of molecule adsorption-desorption on the Gaussian surface. Based on this, the nanoreactor with catalytic metallic Ru on the outer shells achieves the high-selective cascade oxidation of biomass-derived 5-hydroxymethylfurfural to high-value-added 5-formyl-2-furancarboxylic acid (97.9% selectivity), showing a reaction efficiency that is an order of magnitude higher than that of conventional heating. Tuning the adsorption–desorption behavior of molecules on solid catalysts is crucial for achieving complex catalytic functions. Here, the authors show that Gaussian curvature engineering of self-pressurizing mesoporous nanoreactors enhances the dynamic equilibrium between molecular adsorption and desorption.