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  1. Free, publicly-accessible full text available July 1, 2023
  2. Nucleation of clathrate hydrates at low temperatures is constrained by very long induction (wait) times, which can range from hours to days. Electronucleation (application of an electrical potential difference across the hydrate forming solution) can significantly reduce the induction time. This work studies the use of porous open-cell foams of various materials as electronucleation electrodes. Experiments with tetrahydrofuran (THF) hydrates reveal that aluminum and carbon foam electrodes can enable voltage-dependent nucleation, with induction times dependent on the ionization tendency of the foam material. Furthermore, we observe a non-trivial dependence of the electronucleation parameters such as induction time and the recalescence temperature on the water:THF molar ratio. This study further corroborates previously developed hypotheses which associated rapid hydrate nucleation with the formation of metal-ion coordination compounds. Overall, this work studies various aspects of electronucleation with aluminum and carbon foams.
  3. This article reviews the fundamental interfacial mechanisms underlying electrofreezing (promotion of ice nucleation via the application of an electric field). Electrofreezing has been an active research topic for many decades, with applications in food preservation, cryopreservation, cryogenics and ice formation. There is substantial literature detailing experimental and simulations-based studies, which aim to understand the complex mechanisms underlying accelerated ice nucleation in the presence of electric fields and electrical charge. This work provides a critical review of all such studies. It is noted that application-focused studies of electrofreezing are excluded from this review; such studies have been previously reviewed in literature. This review focuses only on fundamental studies, which analyze the physical mechanisms underlying electrofreezing. Topics reviewed include experimental studies on electrofreezing (DC and AC electric fields), pyroelectricity-based control of freezing, molecular dynamics simulations of electrofreezing, and thermodynamics-based explanations of electrofreezing. Overall, it is seen that electrofreezing can enable disruptive advancements in the control of liquid-to-solid phase change, and that our current understanding of the underlying mechanisms can be significantly improved through further studies of various interfacial effects coming into play.
  4. Nucleation of hydrates is constrained by very long induction (wait) times, which can range from hours to days. Electronucleation (application of an electrical potential across the precursor solution) can significantly reduce the induction time for nucleation. This study shows that porous aluminum foams (open-cell) enable near-instantaneous electronucleation at very low voltages. Experiments with tetrahydrofuran hydrates reveal that aluminum foam electrodes enable voltage-dependent nucleation with induction times of only tens of seconds at voltages as low as 20 V. Foam-based electrodes can reduce the induction time by up to 150X when compared to non-foam electrodes. Furthermore, this study reveals that electronucleation can be attributed to two distinct phenomena, namely bubble generation (due to electrolysis), and the formation of metal-ion coordination compounds. These mechanisms affect the induction time to different extents and depend on electrode material and polarity. Overall, this work uncovers the benefits of using foams for formation of hydrates, with foams aiding nucleation as well as propagation of the hydrate formation front.
  5. Nucleation of hydrates requires very long induction (wait) times, often ranging from hours to days. Electronucleation, i.e. nucleation stimulated by the presence of an electric field in the precursor solution can reduce the induction time significantly. This work reveals that porous aluminum foams enable near-instantaneous electronucleation at very low voltages. Experiments with tetrahydrofuran hydrate nucleation reveal that open-cell aluminum foam electrodes can trigger nucleation in only tens of seconds. Foam-based electrodes reduce the induction time by as much as 150X, when compared to non-foam electrodes. This work also discusses two mechanisms underlying electronucleation. These include bubble generation (due to electrolysis), and the formation of metal-ion coordination compounds. These mechanisms depend on electrode material and polarity, and affect the induction time to different extents. This work also shows that foams result in more deterministic nucleation (compared to stochastic) when compared with non-foam electrodes. Overall, electronucleation can lead to a new class of technologies for active control of formation of hydrates.
  6. Nucleation of hydrates requires very long induction (wait) times, often ranging from hours to days. Electronucleation, i.e. nucleation stimulated by the presence of an electric field in the precursor solution can reduce the induction time significantly. This work reveals that porous aluminum foams enable near-instantaneous electronucleation at very low voltages. Experiments with tetrahydrofuran hydrate nucleation reveal that open-cell aluminum foam electrodes can trigger nucleation in only tens of seconds. Foam-based electrodes reduce the induction time by as much as 150X, when compared to non-foam electrodes. This work also discusses two mechanisms underlying electronucleation. These include bubble generation (due to electrolysis), and the formation of metal-ion coordination compounds. These mechanisms depend on electrode material and polarity, and affect the induction time to different extents. This work also shows that foams result in more deterministic nucleation (compared to stochastic) when compared with non-foam electrodes. Overall, electronucleation can lead to a new class of technologies for active control of formation of hydrates.