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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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. doi:10.1039/c0cp01273d
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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PMID: 23045632
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61 References

Data provided by Europe PubMed Central.

Water activity and mobility in solutions of glycerol and small molecular weight sugars: Implication for cryo- and lyopreservation
He, Journal of Applied Physics 100(7), 2006
Estimation of Water Diffusion Coefficients in Freeze-Concentrated Matrices of Sugar Solutions Using Molecular Dynamics: Correlation Between Estimated Diffusion Coefficients and Measured Ice-Crystal Recrystallization Rates
Hagiwara, Food Biophysics 4(4), 2009
Heterogeneous nucleation of ice particles on glassy aerosols under cirrus conditions
Murray, Nature Geoscience 3(4), 2010
The role of organic aerosols in homogeneous ice formation
Kärcher, Atmospheric Chemistry and Physics 5(3), 2005
Characterization of the organic composition of aerosols from Rondônia, Brazil, during the LBA-SMOCC 2002 experiment and its representation through model compounds
Decesari, Atmospheric Chemistry and Physics 6(2), 2006
Do atmospheric aerosols form glasses?
Zobrist, Atmospheric Chemistry and Physics 8(17), 2008
Inhibition of ice crystallisation in highly viscous aqueous organic acid droplets
Murray, Atmospheric Chemistry and Physics 8(17), 2008
Amorphous and crystalline aerosol particles interacting with water vapor: conceptual framework and experimental evidence for restructuring, phase transitions and kinetic limitations
Mikhailov, Atmospheric Chemistry and Physics 9(24), 2009
Kinetic multi-layer model of aerosol surface and bulk chemistry (KM-SUB): the influence of interfacial transport and bulk diffusion on the oxidation of oleic acid by ozone
Shiraiwa, Atmospheric Chemistry and Physics 10(8), 2010
An amorphous solid state of biogenic secondary organic aerosol particles.
Virtanen A, Joutsensaari J, Koop T, Kannosto J, Yli-Pirila P, Leskinen J, Makela JM, Holopainen JK, Poschl U, Kulmala M, Worsnop DR, Laaksonen A., Nature 467(7317), 2010
PMID: 20944744

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