Abstract

Amino-functionalized inorganic silica nanoshells with a diameter of 511 ± 57 nm are efficiently used as hydrogen ion binders with a base dissociation constant of (1.2 ± 0.1) × 10-4. The hydrogen removal has been shown to produce reaction-diffusion fronts of constant propagation velocity in the autocatalytic chlorite-tetrathionate reaction when it is run in thin planar slices of nanoshell-containing agarose gel to exclude all convection related effects. By controlling the exact amount of amino-functionalized hollow nanospheres in the gel matrix it is possible to finely tune the propagation velocity of the chemical front in the 0.1-10 cm h-1 range. Remarkably, this can be achieved with very low amino-functionalized hollow inorganic nanosphere loadings between 0.1-0.01 (m V-1)%. The front width has also been determined experimentally, which increases by a factor of two with one magnitude decrease in the front velocity.

Highlights

  • Spatiotemporal structures of self-organized reactions can interact with a self-assembly on a much smaller lengthscale.[1]

  • Nanoparticles have been shown to be regulated with a pH-oscillator[2,3,4] or an autocatalytic reaction resulting in acidic fronts utilizing buoyancy.[5]

  • To obtain the number of aminogroups for a given volume of acid we subtracted the number of hydrogen ions in the sodium nitrate solution from that in the presence of the nanospheres

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Summary

Introduction

Spatiotemporal structures of self-organized reactions can interact with a self-assembly on a much smaller lengthscale.[1]. One of the first steps was Alan Turing’s reaction–diffusion model[9] in which stationary structures can evolve From this time, a large number of reactions yielding spatiotemporal patterns have been thoroughly studied. Using a highly viscous or gelled, elastic reaction medium like gelatin, polyacrylamide or agarose, where convection is negligible, pure reaction–diffusion fronts develop, so the effect of diffusion as a sole transport process can be investigated.[26,27,28,29,30] Typically an initially planar front retains its shape during propagation unless the mobility of the autocatalyst is significantly lower than that of the reactants. The impact is quantified by determining the characteristics of the reaction–diffusion fronts such as front velocity or width

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