Nucleation and the Solid–Liquid Interfacial Free Energy

Wu, David T.; Gránásy, László; Spaepen, Frans

doi:10.1557/mrs2004.265

Cited by 53 publications

(67 citation statements)

References 72 publications

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“…The presence of impurities and crystal defects and the large temperature gradients near the ice-liquid interface also pose a challenge to the experimental determination of σ iw (Jones, 1974). Factors like crystal shape, type and size, and the characteristics of the ice-liquid interface may also affect the determination of σ iw (Wu et al, 2004;MacKenzie, 1997;Kashchiev, 2000).…”

Section: Barahona: Ice Formation and Water Activitymentioning

confidence: 99%

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

Barahona

2014

Atmos. Chem. Phys.

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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.

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Section: Barahona: Ice Formation and Water Activitymentioning

confidence: 99%

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

Barahona

2014

Atmos. Chem. Phys.

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“…The coefficient of ln(K ls ) in Equation (20) becomes equal to 1 at the homogeneous nucleation temperature T m /3 and the Equations (9) and (11) are respected. Homogeneously-condensed superclusters of n-atoms act as growth nuclei at a temperature generally higher than the homogeneous nucleation temperatures T m /3 of liquid elements because they reduce the critical energy barrier as shown in Equation (21) …”

Section: Crystal Homogeneous Nucleation Temperature and Effective Nucmentioning

confidence: 99%

“…where v is the sample volume, J the nucleation rate, t sn the steady-state nucleation time, lnK ls = 90 ± 2, ΔG* 2ls /k B T defined in Equation (20) and ΔG nm in Equation (15). The Equation (21) is applied, assuming that n-atom superclusters preexist in melts when they have not been melted by superheating above T m .…”

Section: Crystal Homogeneous Nucleation Temperature and Effective Nucmentioning

confidence: 99%

“…Column 9, the reduced crystallization temperature θ c calc calculated using Equation (21); Column 10, the thermally-activated effective energy barrier ΔG eff /k B T given in Equations (21) and (20) leading to the crystallization of the corresponding liquid element;…”

Section: Prediction Of Crystallization Temperatures T C Of 38 Undercomentioning

confidence: 99%

“…In this article, each cluster having a radius smaller than the critical radius has its own energy saving coefficient ε nm depending on θ 2 , n and its radius R nm . In this case too, the cluster surface energy is a linear function of ε nm instead of a function of θ or T [20][21][22][23][24][25]. The Gibbs free energy change derivative [d(ΔG 2ls )/dT] p = −ΔS m at T m continues to be equal to the entropy change whatever the particle radius is because (dε ls /dT) T=Tm is equal to zero.…”

Section: Introductionmentioning

confidence: 99%

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Crystallization of Supercooled Liquid Elements Induced by Superclusters Containing Magic Atom Numbers

Tournier

2014

Metals

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A few experiments have detected icosahedral superclusters in undercooled liquids. These superclusters survive above the crystal melting temperature T m because all their surface atoms have the same fusion heat as their core atoms, and are melted by liquid homogeneous and heterogeneous nucleation in their core, depending on superheating time and temperature. They act as heterogeneous growth nuclei of crystallized phase at a temperature T c of the undercooled melt. They contribute to the critical barrier reduction, which becomes smaller than that of crystals containing the same atom number n. After strong superheating, the undercooling rate is still limited because the nucleation of 13-atom superclusters always reduces this barrier, and increases T c above a homogeneous nucleation temperature equal to T m /3 in liquid elements. After weak superheating, the most stable superclusters containing n = 13, 55, 147, 309 and 561 atoms survive or melt and determine T c during undercooling, depending on n and sample volume. The experimental nucleation temperatures T c of 32 liquid elements and the supercluster melting temperatures are predicted with sample volumes varying by 18 orders of magnitude. The classical Gibbs free energy change is used, adding an enthalpy saving related to the Laplace pressure change associated with supercluster formation, which is quantified for n = 13 and 55.

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Ultrafast Formation of Amorphous Bimetallic Hydroxide Films on 3D Conductive Sulfide Nanoarrays for Large‐Current‐Density Oxygen Evolution Electrocatalysis

et al. 2017

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Developing nonprecious oxygen evolution electrocatalysts that can work well at large current densities is of primary importance in a viable water-splitting technology. Herein, a facile ultrafast (5 s) synthetic approach is reported that produces a novel, efficient, non-noble metal oxygen-evolution nano-electrocatalyst that is composed of amorphous Ni-Fe bimetallic hydroxide film-coated, nickel foam (NF)-supported, Ni S nanosheet arrays. The composite nanomaterial (denoted as Ni-Fe-OH@Ni S /NF) shows highly efficient electrocatalytic activity toward oxygen evolution reaction (OER) at large current densities, even in the order of 1000 mA cm . Ni-Fe-OH@Ni S /NF also gives an excellent catalytic stability toward OER both in 1 m KOH solution and in 30 wt% KOH solution. Further experimental results indicate that the effective integration of high catalytic reactivity, high structural stability, and high electronic conductivity into a single material system makes Ni-Fe-OH@Ni S /NF a remarkable catalytic ability for OER at large current densities.

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Nucleation and the Solid–Liquid Interfacial Free Energy

Abstract: This article reviews the current understanding of the fundamentals of nucleation theory and its use to extract values for the solid–liquid interfacial free energy from experimental and simulation data.

Cited by 53 publications

References 72 publications

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

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

Crystallization of Supercooled Liquid Elements Induced by Superclusters Containing Magic Atom Numbers

Ultrafast Formation of Amorphous Bimetallic Hydroxide Films on 3D Conductive Sulfide Nanoarrays for Large‐Current‐Density Oxygen Evolution Electrocatalysis

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