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Abstract
The dissolution dynamics between miscible liquids play a key role in many industrial, biological and environmental processes, including solvent-induced phase transformations such as the formation of polymer membranes or antisolvent crystallisation. The “common” current intuition that guides the design of diffusion processes in miscible liquids is rooted in Fick’s law. This hypothesis generally holds when the system is close to equilibrium and behaves like an ideal mixture. However, Fickian diffusion has limited applicability far from equilibrium, and many systems display “anomalous” behaviours such as uphill diffusion [1] or the Ouzo effect [2]. Despite the importance of diffusion processes, the mechanisms underlying anomalous mass transfer are still poorly understood [3]. This work provides a direct microscopic view into highly localized anomalous pathways that can occur during the mixing of miscible fluids.
Results will be presented for a model system of glycine-water-ethanol that represents a typical antisolvent crystallisation process where anomalous mass transport can have significant impacts on the critical quality attributes of the resulting crystalline product. We have deployed a novel experimental setup that includes a microfluidic flow cell that is monitored using a confocal Raman microscope, enabling the measurement of spectral maps of the mixing of the solution and antisolvent streams. These maps allow for the evolution of the composition of the multicomponent fluid to be determined as mixing progresses.
From the measured spectral maps, the equilibration trajectories of the mixing solution and antisolvent streams can be determined, providing information on what regions of the phase diagrams are accessed during the mixing process, while also revealing the conditions that lead to surprising diffusive behaviours. This work provides new insight into the underlying mechanisms of anomalous mass transport and a better understanding of the equilibration pathways that can occur during antisolvent crystallization.
References
[1] R. Krishna; Uphill diffusion in multicomponent mixtures, Chem. Soc. Rev., 44, 2812-2836 (2015).
[2] S. A. Vitale, and J. L. Katz; Liquid droplet dispersions formed by homogeneous liquid-liquid nucleation: “the ouzo effect”, Langmuir, 19, 4105-4110 (2003)
[3] A. Vorobev: Dissolution dynamics of miscible liquid/liquid interfaces, Curr. Opin. Colloid Interface Sci., 19, 300-308 (2014).
Results will be presented for a model system of glycine-water-ethanol that represents a typical antisolvent crystallisation process where anomalous mass transport can have significant impacts on the critical quality attributes of the resulting crystalline product. We have deployed a novel experimental setup that includes a microfluidic flow cell that is monitored using a confocal Raman microscope, enabling the measurement of spectral maps of the mixing of the solution and antisolvent streams. These maps allow for the evolution of the composition of the multicomponent fluid to be determined as mixing progresses.
From the measured spectral maps, the equilibration trajectories of the mixing solution and antisolvent streams can be determined, providing information on what regions of the phase diagrams are accessed during the mixing process, while also revealing the conditions that lead to surprising diffusive behaviours. This work provides new insight into the underlying mechanisms of anomalous mass transport and a better understanding of the equilibration pathways that can occur during antisolvent crystallization.
References
[1] R. Krishna; Uphill diffusion in multicomponent mixtures, Chem. Soc. Rev., 44, 2812-2836 (2015).
[2] S. A. Vitale, and J. L. Katz; Liquid droplet dispersions formed by homogeneous liquid-liquid nucleation: “the ouzo effect”, Langmuir, 19, 4105-4110 (2003)
[3] A. Vorobev: Dissolution dynamics of miscible liquid/liquid interfaces, Curr. Opin. Colloid Interface Sci., 19, 300-308 (2014).
Original language | English |
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Pages | 75 [B.02] |
Number of pages | 1 |
Publication status | Published - 21 Sept 2022 |
Event | IXth Diffusion Fundamentals Conference - Jagiellonian University, Krakow, Poland Duration: 21 Sept 2022 → 24 Sept 2022 |
Conference
Conference | IXth Diffusion Fundamentals Conference |
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Country/Territory | Poland |
City | Krakow |
Period | 21/09/22 → 24/09/22 |
Keywords
- miscible liquids
- crystallisation
- Fick's law
Fingerprint
Dive into the research topics of 'Unravelling anomalous mass transport in miscible liquids'. Together they form a unique fingerprint.Projects
- 1 Finished
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Unravelling anomalous mass and heat transport in miscible liquids (New Horizons)
Cardona Amengual, J. (Principal Investigator), Lue, L. (Co-investigator), Nordon, A. (Co-investigator) & Tachtatzis, C. (Co-investigator)
EPSRC (Engineering and Physical Sciences Research Council)
20/07/21 → 15/10/22
Project: Research
Datasets
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Data for: "New Horizons: Unravelling Anomalous Mass and Heat Transport in Miscible Liquids"
McKechnie, D. (Creator), Tachtatzis, C. (Contributor), Nordon, A. (Contributor), Lue, L. (Contributor) & Cardona Amengual, J. (Supervisor), University of Strathclyde, 28 Mar 2023
DOI: 10.15129/e51fe9f3-69d0-4dc8-a710-7a4bb1c88e45
Dataset
Activities
- 1 Participation in conference
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IXth Diffusion Fundamentals Conference
Moreno Flores, I. (Participant)
21 Sept 2022 → 24 Sept 2022Activity: Participating in or organising an event types › Participation in conference