Ultra-slow water diffusion in aqueous sucrose glasses

Zobrist B, Soonsin V, Luo BP, Krieger UK, Marcolli C, Peter T, Koop T (2011)
PHYSICAL CHEMISTRY CHEMICAL PHYSICS 13(8): 3514-3526.

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Abstract
We present measurements of water uptake and release by single micrometre-sized aqueous sucrose particles. The experiments were performed in an electrodynamic balance where the particles can be stored contact-free in a temperature and humidity controlled chamber for several days. Aqueous sucrose particles react to a change in ambient humidity by absorbing/desorbing water from the gas phase. This water absorption (desorption) results in an increasing (decreasing) droplet size and a decreasing (increasing) solute concentration. Optical techniques were employed to follow minute changes of the droplet's size, with a sensitivity of 0.2 nm, as a result of changes in temperature or humidity. We exposed several particles either to humidity cycles (between similar to 2% and 90%) at 291 K or to constant relative humidity and temperature conditions over long periods of time (up to several days) at temperatures ranging from 203 to 291 K. In doing so, a retarded water uptake and release at low relative humidities and/or low temperatures was observed. Under the conditions studied here, the kinetics of this water absorption/desorption process is controlled entirely by liquid-phase diffusion of water molecules. Hence, it is possible to derive the translational diffusion coefficient of water molecules, D-H2O, from these data by simulating the growth or shrinkage of a particle with a liquid-phase diffusion model. Values for D-H2O-values as low as 10(-24) m(2)s(-1) are determined using data at temperatures down to 203 K deep in the glassy state. From the experiment and modelling we can infer strong concentration gradients within a single particle including a glassy skin in the outer shells of the particle. Such glassy skins practically isolate the liquid core of a particle from the surrounding gas phase, resulting in extremely long equilibration times for such particles, caused by the strongly non-linear relationship between concentration and DH2O. We present a new parameterization of DH2O that facilitates describing the stability of aqueous food and pharmaceutical formulations in the glassy state, the processing of amorphous aerosol particles in spray-drying technology, and the suppression of heterogeneous chemical reactions in glassy atmospheric aerosol particles.
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Zobrist B, Soonsin V, Luo BP, et al. Ultra-slow water diffusion in aqueous sucrose glasses. PHYSICAL CHEMISTRY CHEMICAL PHYSICS. 2011;13(8):3514-3526.
Zobrist, B., Soonsin, V., Luo, B. P., Krieger, U. K., Marcolli, C., Peter, T., & Koop, T. (2011). Ultra-slow water diffusion in aqueous sucrose glasses. PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 13(8), 3514-3526.
Zobrist, B., Soonsin, V., Luo, B. P., Krieger, U. K., Marcolli, C., Peter, T., and Koop, T. (2011). Ultra-slow water diffusion in aqueous sucrose glasses. PHYSICAL CHEMISTRY CHEMICAL PHYSICS 13, 3514-3526.
Zobrist, B., et al., 2011. Ultra-slow water diffusion in aqueous sucrose glasses. PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 13(8), p 3514-3526.
B. Zobrist, et al., “Ultra-slow water diffusion in aqueous sucrose glasses”, PHYSICAL CHEMISTRY CHEMICAL PHYSICS, vol. 13, 2011, pp. 3514-3526.
Zobrist, B., Soonsin, V., Luo, B.P., Krieger, U.K., Marcolli, C., Peter, T., Koop, T.: Ultra-slow water diffusion in aqueous sucrose glasses. PHYSICAL CHEMISTRY CHEMICAL PHYSICS. 13, 3514-3526 (2011).
Zobrist, Bernhard, Soonsin, Vacharaporn, Luo, Bei P., Krieger, Ulrich K., Marcolli, Claudia, Peter, Thomas, and Koop, Thomas. “Ultra-slow water diffusion in aqueous sucrose glasses”. PHYSICAL CHEMISTRY CHEMICAL PHYSICS 13.8 (2011): 3514-3526.
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