scholarly journals Analysis of the effect of water activity on ice formation using a new thermodynamic framework

2014 ◽  
Vol 14 (2) ◽  
pp. 1525-1557
Author(s):  
D. Barahona

Abstract. In this work a new thermodynamic framework is developed and used to investigate the effect of water activity on the formation of ice within supercooled droplets. The new framework is based on a novel concept where the interface is assumed to be made of liquid molecules "trapped" by the solid matrix. Using this concept new expressions are developed for the critical ice germ size and the nucleation work, with explicit dependencies on temperature and water activity. However unlike previous approaches, the new model does not depend on the interfacial tension between liquid and ice. Comparison against experimental results shows that the new theory is able to reproduce the observed effect of water activity on nucleation rate and freezing temperature. It allows for the first time a phenomenological derivation of the constant shift in water activity between melting and nucleation. The new framework offers a consistent thermodynamic view of ice nucleation, simple enough to be applied in atmospheric models of cloud formation.

2014 ◽  
Vol 14 (14) ◽  
pp. 7665-7680 ◽  
Author(s):  
D. Barahona

Abstract. In this work a new thermodynamic framework is developed and used to investigate the effect of water activity on the formation of ice within supercooled droplets. The new framework is based on a novel concept where the interface is assumed to be made of liquid molecules "trapped" by the solid matrix. It also accounts for the change in the composition of the liquid phase upon nucleation. Using this framework, new expressions are developed for the critical ice germ size and the nucleation work with explicit dependencies on temperature and water activity. However unlike previous approaches, the new model does not depend on the interfacial tension between liquid and ice. The thermodynamic framework is introduced within classical nucleation theory to study the effect of water activity on the ice nucleation rate. Comparison against experimental results shows that the new approach is able to reproduce the observed effect of water activity on the nucleation rate and the freezing temperature. It allows for the first time a phenomenological derivation of the constant shift in water activity between melting and nucleation. The new framework offers a consistent thermodynamic view of ice nucleation, simple enough to be applied in atmospheric models of cloud formation.


2006 ◽  
Vol 108 (2) ◽  
pp. 188-195 ◽  
Author(s):  
A. Esteban ◽  
M.L. Abarca ◽  
M.R. Bragulat ◽  
F.J. Cabañes

2017 ◽  
Vol 200 ◽  
pp. 165-194 ◽  
Author(s):  
Joseph C. Charnawskas ◽  
Peter A. Alpert ◽  
Andrew T. Lambe ◽  
Thomas Berkemeier ◽  
Rachel E. O’Brien ◽  
...  

Anthropogenic and biogenic gas emissions contribute to the formation of secondary organic aerosol (SOA). When present, soot particles from fossil fuel combustion can acquire a coating of SOA. We investigate SOA–soot biogenic–anthropogenic interactions and their impact on ice nucleation in relation to the particles’ organic phase state. SOA particles were generated from the OH oxidation of naphthalene, α-pinene, longifolene, or isoprene, with or without the presence of sulfate or soot particles. Corresponding particle glass transition (Tg) and full deliquescence relative humidity (FDRH) were estimated using a numerical diffusion model. Longifolene SOA particles are solid-like and all biogenic SOA sulfate mixtures exhibit a core–shell configuration (i.e.a sulfate-rich core coated with SOA). Biogenic SOA with or without sulfate formed ice at conditions expected for homogeneous ice nucleation, in agreement with respectiveTgand FDRH. α-pinene SOA coated soot particles nucleated ice above the homogeneous freezing temperature with soot acting as ice nuclei (IN). At lower temperatures the α-pinene SOA coating can be semisolid, inducing ice nucleation. Naphthalene SOA coated soot particles acted as ice nuclei above and below the homogeneous freezing limit, which can be explained by the presence of a highly viscous SOA phase. Our results suggest that biogenic SOA does not play a significant role in mixed-phase cloud formation and the presence of sulfate renders this even less likely. However, anthropogenic SOA may have an enhancing effect on cloud glaciation under mixed-phase and cirrus cloud conditions compared to biogenic SOA that dominate during pre-industrial times or in pristine areas.


2006 ◽  
Vol 23 (7) ◽  
pp. 634-640 ◽  
Author(s):  
A. Esteban ◽  
M.L. Abarca ◽  
M.R. Bragulat ◽  
F.J. Cabañes

Batteries ◽  
2018 ◽  
Vol 4 (4) ◽  
pp. 60 ◽  
Author(s):  
Caihong Liu ◽  
Leon Shaw

In this study, we have proposed a novel concept of hybrid flow batteries consisting of a molten Na-Cs anode and an aqueous NaI catholyte separated by a NaSICON membrane. A number of carbonaceous electrodes are studied using cyclic voltammetry (CV) for their potentials as the positive electrode of the aqueous NaI catholyte. The charge transfer impedance, interfacial impedance and NaSICON membrane impedance of the Na-Cs ‖ NaI hybrid flow battery are analyzed using electrochemical impedance spectroscopy. The performance of the Na-Cs ‖ NaI hybrid flow battery is evaluated through galvanostatic charge/discharge cycles. This study demonstrates, for the first time, the feasibility of the Na-Cs ‖ NaI hybrid flow battery and shows that the Na-Cs ‖ NaI hybrid flow battery has the potential to achieve the following properties simultaneously: (i) An aqueous NaI catholyte with good cycle stability, (ii) a durable and low impedance NaSICON membrane for a large number of cycles, (iii) stable interfaces at both anode/membrane and cathode/membrane interfaces, (iv) a molten Na-Cs anode capable of repeated Na plating and stripping, and (v) a flow battery with high Coulombic efficiency, high voltaic efficiency, and high energy efficiency.


2009 ◽  
Vol 135 (1) ◽  
pp. 60-63 ◽  
Author(s):  
G. Pose ◽  
A. Patriarca ◽  
V. Kyanko ◽  
A. Pardo ◽  
V. Fernández Pinto

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