Autonomic molecular transport by polymer films containing programmed chemical potential gradients

Journal of the American Chemical Society
Chunjie ZhangPaul V Braun

Abstract

Materials which induce molecular motion without external input offer unique opportunities for spatial manipulation of molecules. Here, we present the use of polyacrylamide hydrogel films containing built-in chemical gradients (enthalpic gradients) to direct molecular transport. Using a cationic tertiary amine gradient, anionic molecules were directionally transported up to several millimeters. A 40-fold concentration of anionic molecules dosed in aerosol form on a substrate to a small region at the center of a radially symmetric cationic gradient was observed. The separation of mixtures of charged dye molecules was demonstrated using a boronic acid-to-cationic gradient where one molecule was attracted to the boronic acid end of the gradient, and the other to the cationic end of the gradient. Theoretical and computational analysis provides a quantitative description of such anisotropic molecular transport, and reveals that the gradient-imposed drift velocity is in the range of hundreds of nanometers per second, comparable to the transport velocities of biomolecular motors. This general concept of enthalpy gradient-directed molecular transport should enable the autonomous processing of a diversity of chemical species.

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Citations

Feb 24, 2016·Proceedings of the National Academy of Sciences of the United States of America·Isamar Ortiz-RiveraAnna C Balazs
May 30, 2017·ACS Applied Materials & Interfaces·Lydia KisleyDeborah E Leckband
Feb 18, 2017·Nature Communications·Sambeeta DasAyusman Sen
Mar 24, 2016·Nature Chemistry·Ian WheeldonMatthew Sigman
Apr 4, 2017·Angewandte Chemie·Tsung-Han TsaiPaul V Braun
Oct 25, 2017·Journal of the American Chemical Society·Rajarshi GuhaDarrell Velegol
Sep 27, 2018·Biochemistry·Farzad MohajeraniAyusman Sen
Sep 27, 2018·Accounts of Chemical Research·Xi ZhaoAyusman Sen
Sep 12, 2019·Chemical Reviews·Gadiel Saper, Henry Hess

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