Abstract
Multivalency-mediated interactions play an important role in governing dynamicity and self-assembly in biological systems. Despite its significance in supramolecular material chemistry to biomedicine, the role of multivalency in modulating colloidal transport or phoresis remains largely unexplored. Here, combining theory and experiment, we report diffusiophoretic motion of a positively-charged catalytic microbead during its multivalent interactions with a gradient of adenosine mono-, di- and trinucleotides (AM/D/TP) both in micro- and macroscale regimes. We find that the extent of drift diminishes with increasing number of phosphates. Subsequently, we exhibit nucleotide-specificity of the colloid in catalyzing a proton-transfer reaction, which in turn alters its phoretic behaviour. Finally, we demonstrate spatiotemporal control over colloidal phoretic leap (a sudden increase in phoretic velocity) and population dynamics driven by enzymatic downregulation of multivalent interactivity, which has been achieved by controlling ATP hydrolysis in situ. These findings open up avenues for utilizing multivalent surface-mediated catalytic activity to achieve precise control of particle transport relevant to reaction-diffusion driven spatiotemporal processes.
Supplementary materials
Title
Supporting Information
Description
Materials and methods, Synthesis of nanorods and CMB, Details of theoretical calculations, videos.
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Title
Supporting Video
Description
Migration of CMB in Frame A with time in presence of ATP, and 150 nM PA. Experimental condition: 0.025 mg/mL bead, [GNR] = 37.5 pM, [ATP] = 10 µM, [PA] = 150 nM, [Ca2+] = 0.25 mM in water at 25 °C.
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