Interfacial dynamics mediate surface binding events on supramolecular nanostructures

Ty Christoff-Tempesta, Yukio Cho, Samuel J. Kaser, Linnaea D. Uliassi, Xiaobing Zuo, Shayna L. Hilburg, Lilo D. Pozzo and Julia H. Ortony ()
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Ty Christoff-Tempesta: Massachusetts Institute of Technology
Yukio Cho: Massachusetts Institute of Technology
Samuel J. Kaser: Massachusetts Institute of Technology
Linnaea D. Uliassi: Massachusetts Institute of Technology
Xiaobing Zuo: Argonne National Laboratory
Shayna L. Hilburg: University of Washington
Lilo D. Pozzo: University of Washington
Julia H. Ortony: Massachusetts Institute of Technology

Nature Communications, 2024, vol. 15, issue 1, 1-8

Abstract: Abstract The dynamic behavior of biological materials is central to their functionality, suggesting that interfacial dynamics could also mediate the activity of chemical events at the surfaces of synthetic materials. Here, we investigate the influence of surface flexibility and hydration on heavy metal remediation by nanostructures self-assembled from small molecules that are decorated with surface-bound chelators in water. We find that incorporating short oligo(ethylene glycol) spacers between the surface and interior domain of self-assembled nanostructures can drastically increase the conformational mobility of surface-bound lead-chelating moieties and promote interaction with surrounding water. In turn, we find the binding affinities of chelators tethered to the most flexible surfaces are more than ten times greater than the least flexible surfaces. Accordingly, nanostructures composed of amphiphiles that give rise to the most dynamic surfaces are capable of remediating thousands of liters of 50 ppb Pb2+-contaminated water with single grams of material. These findings establish interfacial dynamics as a critical design parameter for functional self-assembled nanostructures.

Date: 2024
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DOI: 10.1038/s41467-024-51494-4

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