Determination Methods for Crystal Nucleation Kinetics in Solutions

Xiao, Yan; Wang, Jingkang; Huang, Xin; Shi, Huanhuan; Zhou, Yanan; Zong, Shuyi; Hao, Hongxun; Bao, Ying; Yin, Qiuxiang

doi:10.1021/acs.cgd.7b01223

Cited by 28 publications

(26 citation statements)

References 94 publications

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“…Droplet microfluidics are additionally finding increasing application for studying nucleation kinetics, where in contrast to droplet levitation, many hundreds of experiments can be performed simultaneously. [ 153 ] The droplet volume can also be precisely controlled, which is essential to the analysis of nucleation kinetics. [ 154 ] Measurement of the evolution of the fraction of droplets that contain crystals over time under constant supersaturation therefore yields the nucleation kinetics, [ 68 ] as discussed in Section 5.2.1.…”

Section: Crystallization In Dropletsmentioning

confidence: 99%

Crystallization in Confinement

2020

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Many crystallization processes of great importance, including frost heave, biomineralization, the synthesis of nanomaterials, and scale formation, occur in small volumes rather than bulk solution. Here, the influence of confinement on crystallization processes is described, drawing together information from fields as diverse as bioinspired mineralization, templating, pharmaceuticals, colloidal crystallization, and geochemistry. Experiments are principally conducted within confining systems that offer well‐defined environments, varying from droplets in microfluidic devices, to cylindrical pores in filtration membranes, to nanoporous glasses and carbon nanotubes. Dramatic effects are observed, including a stabilization of metastable polymorphs, a depression of freezing points, and the formation of crystals with preferred orientations, modified morphologies, and even structures not seen in bulk. Confinement is also shown to influence crystallization processes over length scales ranging from the atomic to hundreds of micrometers, and to originate from a wide range of mechanisms. The development of an enhanced understanding of the influence of confinement on crystal nucleation and growth will not only provide superior insight into crystallization processes in many real‐world environments, but will also enable this phenomenon to be used to control crystallization in applications including nanomaterial synthesis, heavy metal remediation, and the prevention of weathering.

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Section: Crystallization In Dropletsmentioning

confidence: 99%

Crystallization in Confinement

2020

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Section: Introductionmentioning

confidence: 99%

“…The need for a review about nucleation rate kinetics in solution was recognized by Xiao et al, in 2018. They published a review about nucleation rate determination methods in solutions for investigating the nucleation process 12 . They present five methods: the deterministic method, the droplet-based method, the double-pulse method, the microfluidic method and the stirred small volume solution method 12 .…”

Section: Introductionmentioning

confidence: 99%

A Review of Experimental Methods for Nucleation Rate Determination in Large-Volume Batch and Microfluidic Crystallization

Devos

Gerven

Kuhn

2021

Crystal Growth & Design

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Experimental nucleation rate determination for crystallization in solution has been acknowledged as an important topic for a long time, as it improves the design and control of industrial crystallization processes, and offers insights into the mechanisms of nucleation. Characterization of nucleation rates in large volume batch crystallizers has been widely studied in the past, which has led to the development of a variety of models linking the nucleation rate to the metastable zone width and induction time. These methods remain important due to their role in industrial crystallization. More recently, the use of microfluidic platforms has resulted in the development of methods to obtain nucleation rates based on the stochastic nature of nucleation. This has opened new pathways for understanding nucleation on a molecular level. This review presents a critical overview of nucleation rate determination methods: large volume batch crystallizer models (Part I), and microfluidic and microvial models (Part II) are presented in terms of equations, advantages and limitations. Published experimental nucleation rate values are summarized (SI). A critical discussion of experimental nucleation rate determination is given (Part III). The objective of the review is to be a starting point for researchers attempting to experimentally characterize nucleation behavior.

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“…Many examples of this kinetic behavior for cluster formation are found in the experimental literature. [10][11][12][13][14] Nanev and Tonchev find this kinetic behavior specifically for nucleation within supersaturated insulin solutions for seven different initial supersaturations. 7 Morris et al used the Finke-Watzky two-step kinetic model to study over 10 cases of protein aggregation from the literature.…”

Section: Introductionmentioning

confidence: 67%

“…The solution for Equation is the sigmoid function for

n (t)

. Many examples of this kinetic behavior for cluster formation are found in the experimental literature . Nanev and Tonchev find this kinetic behavior specifically for nucleation within supersaturated insulin solutions for seven different initial supersaturations .…”

Section: Introductionmentioning

confidence: 90%

The kinetics of homogeneous and two‐step nucleation during protein crystal growth from solution

Barlow¹,

Gregus

2019

Int J of Chemical Kinetics

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Many experimental reports for the kinetics of crystal nucleation and growth, from an isothermal solution, point to a sigmoidal‐like behavior for the process. Here we consider three different nucleation models from the literature and show that all lead to sigmoidal or sigmoidal‐like behavior for the kinetics of nucleation. A two‐step nucleation process is known to occur within certain supersaturated protein solutions, and it is demonstrated in this report how the sigmoidal law yields kinetic information for the two‐step and homogeneous nucleation modes. We propose here that two‐step solute‐rich associates form in the solution around seed nuclei that are already present at or near the point in time when the solution is prepared. Using this hypothesis, we are able to model the time‐dependent volume of the two‐step phase per unit volume of solution and show that this compares well with reported experimental data. A kinetic model is given for the proposed process, which leads to a sigmoidal rate law. Additionally, a relation between the initial and final nuclei densities and the induction time is derived. As a result of this study, the conclusion is that two‐step activity increases with increasing initial supersaturation or increasing salt concentration.

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Determination Methods for Crystal Nucleation Kinetics in Solutions

Cited by 28 publications

References 94 publications

Crystallization in Confinement

Crystallization in Confinement

A Review of Experimental Methods for Nucleation Rate Determination in Large-Volume Batch and Microfluidic Crystallization

The kinetics of homogeneous and two‐step nucleation during protein crystal growth from solution

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