TY - JOUR
T1 - Autonomic molecular transport by polymer films containing programmed chemical potential gradients
AU - Zhang, Chunjie
AU - Sitt, Amit
AU - Koo, Hyung Jun
AU - Waynant, Kristopher V.
AU - Hess, Henry
AU - Pate, Brian D.
AU - Braun, Paul V.
N1 - Publisher Copyright:
© 2015 American Chemical Society.
PY - 2015/4/22
Y1 - 2015/4/22
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=84928485286&partnerID=8YFLogxK
U2 - 10.1021/jacs.5b00240
DO - 10.1021/jacs.5b00240
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AN - SCOPUS:84928485286
SN - 0002-7863
VL - 137
SP - 5066
EP - 5073
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 15
ER -