Macromolecule Sorption and Diffusion in HEMA/MAA Hydrogels

Liu, D. E.; Kotsmar, C.; Nguyen, F.; Sells, T.; Taylor, N. O.; Prausnitz, J. M.; Radke, C. J.

doi:10.1021/ie402148u

Macromolecule Sorption and Diffusion in HEMA/MAA Hydrogels

Journal Article · Thu Nov 14 04:00:00 EST 2013 · Industrial and Engineering Chemistry Research

DOI:https://doi.org/10.1021/ie402148u· OSTI ID:1570981

Liu, D. E. ^[1]; Kotsmar, C. ^[1]; Nguyen, F. ^[1]; Sells, T. ^[1]; Taylor, N. O. ^[1]; Prausnitz, J. M. ^[1]; Radke, C. J. ^[2]

Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering and Vision Science Group

Transient solute absorption and desorption concentration profiles were measured in a 70 wt % hydroxyethyl methacrylate (HEMA)/30 wt % methacrylic acid (MAA) anionic hydrogel using two-photon confocal microscopy. Dilute aqueous solutes included fluorescently labeled dextrans with molecular masses of 4, 10, and 20 kDa, and fluorescently labeled cationic avidin protein. Cross-linking densities with ethylene glycol dimethacrylate (EGDMA) varied from 0 to 1 wt % with polymer volume fractions increasing from 0.15 to 0.25. Average gel mesh sizes, determined from zero-frequency oscillatory shear storage moduli, ranged from about 3.6 to 8.4 nm over the cross-link ratios studied. All solutes exhibit Stokes-Einstein hydrodynamic radii obtained from measured free diffusion coefficients, D_o, comparable to or larger than the average gel mesh size. In spite of considerable size exclusion, the studied solutes penetrate the gels indicating a range of mesh sizes available for transport. Transient uptake and release concentration profiles for FITC-dextrans follow simple diffusion theory with diffusion coefficients, D, essentially independent of loading or release characteristic of reversible absorption. Although strongly size-excluded, these solutes do not interact specifically with the polymer network. Diffusivities are accordingly predicted from a large-pore effective-medium (LPEM) model developed to account for solute size, hydrodynamic drag, and distribution of mesh sizes available for transport in the polymer network. For this class of solute, anrs of magnitude slower than that of dextran of similar hydrodynamic radius. Desorption of avidin is not cd using no adjustable parameters, diffusivities predicted from the new effective-medium model demonstrate good agreement with experiment. For the specific-interacting cationic protein, avidin, gel loading is 3 ordeomplete even after 2 weeks of extraction. On the basis of size alone, avidin is strongly size-excluded, yet it exhibits a partition coefficient of over 20. For the positively charged protein, we observed specific ion binding on the negatively charged carboxylate groups of MAA-decorated polymer strands in the larger mesh spaces. Finally, simple linear sorption kinetics gives an adsorption time constant of 5 min and a desorption time constant of about 20 days, suggesting nearly irreversible uptake of cationic avidin on the anionic gel matrix.

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

DOE Contract Number:: AC02-05CH11231

OSTI ID:: 1570981

Journal Information:: Industrial and Engineering Chemistry Research, Journal Name: Industrial and Engineering Chemistry Research Journal Issue: 50 Vol. 52; ISSN 0888-5885

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

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