Passive Phase Separation Research Articles

Hyperuniformity in phase ordering: the roles of activity, noise, and non-constant mobility

Hyperuniformity emerges generically in the coarsening regime of phase-separating fluids. Numerical studies of active and passive systems have shown that the structure factor S(q) behaves as q ς for q → 0, with hyperuniformity exponent ς = 4. For passive systems, this result was explained in 1991 by a qualitative scaling analysis of Tomita, exploiting isotropy at scales much larger than the coarsening length. Here we reconsider and extend Tomita’s argument to address cases of active phase separation and of non-constant mobility, again finding ς = 4. We further show that dynamical noise of variance D creates a transient ς = 2 regime for q^≪q^∗∼Dt[1−(d+2)ν]/2 , crossing over to ς = 4 at larger q^ . Here, ν is the coarsening exponent for the domain size ℓ , such that ℓ(t)∼tν , and q^∝qℓ is the rescaled wavenumber. In diffusive coarsening ν=1/3 , so the rescaled crossover wavevector q^∗ vanishes at large times when d⩾2 . The slowness of this decay suggests a natural explanation for experiments that observe a long-lived ς = 2 scaling in phase-separating active fluids (where noise is typically large). Conversely, in d = 1, we demonstrate that with noise the ς = 2 regime survives as t→∞ , with q^∗∼D5/6 . (The structure factor is not then determined by the zero-temperature fixed point.) We confirm our analytical predictions by numerical simulations of continuum theories for active and passive phase separation in the deterministic case and of Model B for the stochastic case. We also compare them with related findings for a system near an absorbing-state transition rather than undergoing phase separation. A central role is played throughout by the presence or absence of a conservation law for the centre of mass position R of the order parameter field.

Deciphering the dynamical chromosome structural reorganizations in human neural development

Understanding the mechanisms of cell-fate determination in neural development is pivotal for advancing regenerative medicine and addressing neurodegenerative diseases. Cell-fate determination is controlled by the underlying gene expression networks, which are further regulated by the three-dimensional chromosome structures. During neural development, chromosomes progressively adapt their structures to accommodate the requisite gene expressions. However, elucidating the pathways of chromosome structural dynamics during these transitions remains a grand challenge. In this study, we employed the data-driven coarse-grained molecular dynamics simulations, coupled with the nonequilibrium landscape-switching model, to quantify the chromosome structural dynamics during human neural development. We focused on a simplified human neural developmental system, comprising of cell differentiation, reprogramming, and transdifferentiation among the neural progenitor cell (NPC), the glia cell, and the neuron cell. We identified significant large-scale chromosome structural reorganizations during cell-state transitions. From the chromosome structural perspective, the transdifferentiation processes between the glia and neuron cells exhibited nonmonotonic behaviors characterized by an initial increase followed by a subsequent decrease in cell stemness. The transdifferentiation appeared to share the same routes of differentiation after passing through the NPC. Additionally, our findings revealed that the chromosome structural dynamical pathways at the scale of topologically associating domains exhibited little overlap, in contrast to the ones at the long-range regions. This suggests that the active, ATP-driven molecular processes play dominant roles in modulating topologically associating domain (TAD) structures, while the compartmental segregation in chromosomes is primarily governed by the passive phase separation. Our study offers a theoretical exploration of neural cell-fate determination from the chromosome structural perspective, paving a way for potential applications in neuroregeneration. Published by the American Physical Society 2024

Colloid phase separation dynamics driven by chiral turbulent flows

Hydrodynamic interactions significantly influence phase-ordering kinetics in complex fluids. While passive fluid phase separation is well studied, the impact of active components remains relatively unexplored. We examine pure- and quasi-two-dimensional mixtures of attractive colloids and self-rotating particles in a solvent. Varying rotor rotational speed and area fraction yield diverse dynamic patterns such as percolated networks and round droplets composed of passive colloids alone. At intermediate rotation speeds, inertial chiral flows, accompanied by the inverse energy cascade, lead to self-similar power-law coarsening with a growth exponent of 1/2. The flows spontaneously organize within fluid domains, exhibiting turbulent and chiral characteristics. Surprisingly, these turbulent flows can sustain hexatic order hydrodynamically stabilized by the Magnus force under certain conditions. Conversely, at higher speeds, nonlinear hydrodynamic interactions impede phase separation. Our findings illuminate the intriguing dynamic interplay between phase separation and chiral turbulence, effectively bridging the realms of phase ordering and turbulent physics. Published by the American Physical Society 2024

Three-Dimensionally Complex Phase Behavior and Collective Phenomena in Mixtures of Acoustically Powered Chiral Microspinners.

The process of dynamic self-organization of small building blocks is fundamental to the emergent function of living systems and is characteristic of their out-of-equilibrium homeostasis. The ability to control the interactions of synthetic particles in large groups could lead to the realization of analogous macroscopic robotic systems with microscopic complexity. Rotationally induced self-organization has been observed in biological systems and modeled theoretically, but studies of fast, autonomously moving synthetic rotors remain rare. Here, we report switchable, out-of-equilibrium hydrodynamic assembly and phase separation in suspensions of acoustically powered chiral microspinners. Semiquantitative modeling suggests that three-dimensionally (3D) complex spinners interact through viscous and weakly inertial (streaming) flows. The interactions between spinners were studied over a range of densities to construct a phase diagram, which included gaseous dimer pairing at low density, collective rotation and multiphase separation at intermediate densities, and ultimately jamming at high density. The 3D chirality of the spinners leads to self-organization in parallel planes, forming a three-dimensionally hierarchical system that goes beyond the 2D systems that have so far been modeled computationally. Dense mixtures of spinners and passive tracer particles also show active-passive phase separation. These observations are consistent with recent theoretical predictions of the hydrodynamic coupling between rotlets generated by autonomous spinners and provide an exciting experimental window to the study of colloidal active matter and microrobotic systems.

Pressure-Driven Phase Separation Based on Modified Porous Mesh for Liquid Management in Microgravity.

Surface tension becomes the main force influencing the gas-liquid interface in microgravity environment. The instability of the gas-liquid distribution is a menace for spacecraft missions. Passive phase separation based on porous material is a promising technique for microgravity liquid management and advanced life support systems. Here, the mechanism of pressure-driven phase separation based on porous material is experimentally investigated, highlighting the synergistic influence of single-phase flow, breakthrough failure, and self-healing ability on liquid acquisition capability. The major parameters characterizing the separation efficiency are the breakthrough threshold pressure and the flow resistance. A fabrication strategy which elicits the surface wettability and maintains the original surface morphology is proposed and verified to increase the critical breakthrough threshold pressure without introducing extra flow resistance. Moreover, the modified mesh is integrated into a screen channel liquid acquisition device. The improvement of the overall separation performance is evaluated in an antigravity delivery experiment, where the acceleration of liquid is -g0. It has been demonstrated that the fabrication strategy increases the achievable flow rate over 80% and the reseal flow rate over 200% for gas-free water delivery. This work enriches the understanding of phase separation based on porous material and provides an alternative method for liquid management in microgravity.

The ejection of large non-oscillating droplets from a hydrophobic wedge in microgravity

When confined within containers or conduits, drops and bubbles migrate to regions of minimum energy by the combined effects of surface tension, surface wetting, system geometry, and initial conditions. Such capillary phenomena are exploited for passive phase separation operations in micro-fluidic devices on earth and macro-fluidic devices aboard spacecraft. Our study focuses on the migration and ejection of large inertial-capillary drops confined between tilted planar hydrophobic substrates (a.k.a., wedges). In our experiments, the brief nearly weightless environment of a 2.1 s drop tower allows for the study of such capillary dominated behavior for up to 10 mL water drops with migration velocities up to 12 cm/s. We control ejection velocities as a function of drop volume, substrate tilt angle, initial confinement, and fluid properties. We then demonstrate how such geometries may be employed as passive no-moving-parts droplet generators for very large drop dynamics investigations. The method is ideal for hand-held non-oscillatory ‘droplet’ generation in low-gravity environments.

Capillary Interfacial Tension in Active Phase Separation.

In passive fluid-fluid phase separation, a single interfacial tension sets both the capillary fluctuations of the interface and the rate of Ostwald ripening. We show that these phenomena are governed by two different tensions in active systems, and compute the capillary tension σ_{cw} which sets the relaxation rate of interfacial fluctuations in accordance with capillary wave theory. We discover that strong enough activity can cause negative σ_{cw}. In this regime, depending on the global composition, the system self-organizes, either into a microphase-separated state in which coalescence is highly inhibited, or into an "active foam" state. Our results are obtained for Active Model B+, a minimal continuum model which, although generic, admits significant analytical progress.

Cluster Phases and Bubbly Phase Separation in Active Fluids: Reversal of the Ostwald Process

It is known that purely repulsive self-propelled colloids can undergo bulk liquid-vapor phase separation. In experiments and large scale simulations, however, more complex steady states are also seen, comprising a dynamic population of dense clusters in a sea of vapor, or dilute bubbles in a liquid. Here we show that these microphase-separated states should emerge generically in active matter, without any need to invoke system-specific details. We give a coarse-grained description of them, and predict transitions between regimes of bulk phase separation and microphase separation. We achieve these results by extending the $\phi^4$ field theory of passive phase separation to allow for all local currents that break detailed balance at leading order in the gradient expansion. These local active currents, whose form we show to emerge from coarse-graining of microscopic models, include a mixture of irrotational and rotational contributions, and can be viewed as arising from an effective nonlocal chemical potential. Such contributions influence, and in some parameter ranges reverse, the classical Ostwald process that would normally drive bulk phase separation to completion.

Development of a passive phase separator for space and earth applications.

The limited amount of liquids and gases that can be carried to space makes it imperative to recycle and reuse these fluids for extended human operations. During recycling processes gas and liquid phases are often intermixed. In the absence of gravity, separating gases from liquids is challenging due to the absence of buoyancy. This paper describes development of a passive phase separator that is capable of efficiently and reliably separating gas-liquid mixtures of both high and low void fractions in a wide range of flow rates that is applicable to for both space and earth applications.

Gas/Water and Heat Management of PEM-Based Fuel Cell and Electrolyzer Systems for Space Applications

Hydrogen/oxygen fuel cells were successfully utilized in the field of space applications to provide electric energy and potable water in human-rated space mission since the 1960s. Proton exchange membrane (PEM) based fuel cells, which provide high power/energy densities, were reconsidered as a promising space power equipment for future space exploration. PEM-based water electrolyzers were employed to provide life support for crews or as major components of regenerative fuel cells for energy storage. Gas/water and heat are some of the key challenges in PEM-based fuel cells and electrolytic cells, especially when applied to space scenarios. In the past decades, efforts related to gas/water and thermal control have been reported to effectively improve cell performance, stability lifespan, and reduce mass, volume and costs of those space cell systems. This study aimed to present a primary review of research on gas/water and waste thermal management for PEM-based electrochemical cell systems applied to future space explorations. In the fuel cell system, technologies related to reactant supplement, gas humidification, water removal and active/passive water separation were summarized in detail. Experimental studies were discussed to provide a direct understanding of the effect of the gas-liquid two-phase flow on product removal and mass transfer for PEM-based fuel cell operating in a short-term microgravity environment. In the electrolyzer system, several active and static passive phaseseparation methods based on diverse water supplement approaches were discussed. A summary of two advanced passive thermal management approaches, which are available for various sizes of space cell stacks, was specifically provided

Design, Fabrication and Prototype testing of a Chip Integrated Micro PEM Fuel Cell Accumulator combined On-Board Range Extender

In this work we present the design, fabrication and prototype testing of Chip Integrated Micro PEM Fuel Cell Accumulator (CIμ-PFCA) combined On-Board Range Extender (O-BRE). CIμ-PFCA is silicon based micro-PEM fuel cell system with an integrated hydrogen storage feature (palladium metal hydride), the run time of CIμ-PFCA is dependent on the stored hydrogen, and in order to extend its run time an O-BRE is realized (catalytic hydrolysis of chemical hydride, NaBH4. Combining the CIμ-PFCA and O-BRE on a system level have few important design requirements to be considered; hydrogen regulation, gas -liquid separator between the CIμ-PFCA and the O-RE. The usage of traditional techniques to regulate hydrogen (tubes), gas-liquid phase membranes (porous membrane separators) are less desirable in the micro domain, due to its space constraint. Our approach is to use a passive hydrogen regulation and gas-liquid phase separation concept; to use palladium membrane. Palladium regulates hydrogen by concentration diffusion, and its property to selectively adsorb only hydrogen is used as a passive gas-liquid phase separator. Proof of concept is shown by realizing a prototype system. The system is an assembly of CIμ-PFCA, palladium membrane and the O-BRE. The CIμ-PFCA consist of 2 individually processed silicon chips, copper supported palladium membrane realized by electroplating followed by high temperature annealing process under inter atmosphere and the O-BRE is realized out of a polymer substrate by micromilling process with platinum coated structures, which functions as a catalyst for the hydrolysis of NaBH4. The functionality of the assembled prototype system is demonstrated by the measuring a unit cell (area 1 mm2) when driven by the catalytic hydrolysis of chemical hydride (NaBH4 and the prototype system shows run time more than 15 hours.

Gas pressure assisted microliquid-liquid extraction coupled online to direct infusion mass spectrometry: a new automated screening platform for bioanalysis.

In the field of bioanalysis, there is an increasing demand for miniaturized, automated, robust sample pretreatment procedures that can be easily connected to direct-infusion mass spectrometry (DI-MS) in order to allow the high-throughput screening of drugs and/or their metabolites in complex body fluids like plasma. Liquid-Liquid extraction (LLE) is a common sample pretreatment technique often used for complex aqueous samples in bioanalysis. Despite significant developments that have been made in automated and miniaturized LLE procedures, fully automated LLE techniques allowing high-throughput bioanalytical studies on small-volume samples using direct infusion mass spectrometry, have not been matured yet. Here, we introduce a new fully automated micro-LLE technique based on gas-pressure assisted mixing followed by passive phase separation, coupled online to nanoelectrospray-DI-MS. Our method was characterized by varying the gas flow and its duration through the solvent mixture. For evaluation of the analytical performance, four drugs were spiked to human plasma, resulting in highly acceptable precision (RSD down to 9%) and linearity (R(2) ranging from 0.990 to 0.998). We demonstrate that our new method does not only allow the reliable extraction of analytes from small sample volumes of a few microliters in an automated and high-throughput manner, but also performs comparable or better than conventional offline LLE, in which the handling of small volumes remains challenging. Finally, we demonstrate the applicability of our method for drug screening on dried blood spots showing excellent linearity (R(2) of 0.998) and precision (RSD of 9%). In conclusion, we present the proof of principe of a new high-throughput screening platform for bioanalysis based on a new automated microLLE method, coupled online to a commercially available nano-ESI-DI-MS.

The effect of crosslinking temperature on the permeability of PDMS membranes: Evidence of extraordinary CO2 and CH4 gas permeation

It is important for gas permeable membranes, employed in many industrial applications, to have a high permeability as the cost of many processes such as gas separation and sensing directly depend on it. Polydimethylsiloxane (PDMS) has been a widely utilized polymer within permeable membranes as it possesses high intrinsic flux. However, little attention has been placed on the effect of crosslinking temperatures during synthesis. In this work, PDMS membranes were prepared using a range of crosslinking temperatures and evaluated for their gas permeation towards CO2, N2 and CH4. The investigation of the effect of the crosslinking temperature on gas permeation of PDMS membranes revealed an optimum temperature of 75°C at which the permeability increased (for N2 from 360 to 590 Barrer, for CO2 from 3190 to 3970 Barrer, and for CH4 from 850 to 1000 Barrer). The vibrational and electron beam spectroscopy studies show that at this optimum temperature the structure of polymer chains is relaxed due to the reduction of the crosslinking density and an enhancement in the fractional free volume (FFV) within the polymer matrix, allowing more efficient diffusion of the gas molecules. Eventually, we demonstrate the extraordinary capability of the membranes crosslinked at 75°C by incorporating them in sensing systems. Remarkably the sensors’ response with and without the presence of the improved membrane are nearly the same for CO2 and only show a 30% decrease for CH4. This experiment depicts the strong potential of the developed membrane for efficient, passive and low cost gas phase separation of selected gas species.

Modulated flow patterns for vertical upflow by the phase separation concept

The passive phase separation concept was proposed to create thin liquid film on the wall surface. The inserted mesh cylinder made of a single layer of mesh pore surface divides the tube cross section into an annular region near the tube wall and a core region. Gas bubbles are prevented from entering the core region and liquids can be sucked towards the core region. Thus, the two-phases are majorly flowing in two different regions. The concept is expected to be used for multiphase (boiling/evaporation and condensation) heat transfer enhancement. Air–water two-phase flow experiments were performed with vertical upflows. Miniature bubbles are modulated to flow in the annular region. Cap/slug/plug bubbles are modulated to form the elongated-ring-slug bubble in the annular region to generate thin liquid films on the wall. For all the cases, the core region is full of liquid. Due to the large density difference between liquid in the core region and gas in the annular region, pulsating flow is self-sustained in the core region. The mesh pore surface promotes the mass and momentum exchange between the annular region and core region. For ring-slug bubbles such as longer than 10cm, miniature bubbles are emitted from the slug bubble front. The proposed concept is being verified by the phase change heat transfer experiment in our laboratory.

Numerical study of flow pattern modulation in a vertical phase separation condenser tube

The passive phase separation concept was proposed to modulate flow patterns for heat transfer enhancement. By the flow pattern modulation, the gas tends to be near the wall and the liquid tends to be in the tube core. Experiment has been performed to verify the fresh idea and the flow pattern modulation mechanism was analyzed qualitatively. This paper focuses on the numerical simulation of the bubble dynamics for a single bubble in the vertical phase separation condenser tube to quantitatively explore the flow pattern mechanism, based on a multiscale grid system and the volume-of-fluid (VOF) method. It is found that: (1) the modulated liquid film thickness can be decreased by 70% compared to that in the bare tube region; (2) the modulated bubble traveling velocity can be doubled, causing the increased liquid velocity and velocity gradient in the annular region to weaken the fluid boundary layer; (3) the significantly increased bubble traveling velocity in the annular region promotes the mass and momentum exchange between the annular region and the core region, and yields the self-sustained pulsating flow in the core region. The above three factors are benefit for the performance improvement of the heat transfer facilities.

Stratified two-phase flow pattern modulation in a horizontal tube by the mesh pore cylinder surface

Condensation heat transfer has been studied in the past century due to its wide applications in energy and power systems. The key scientific issue is the thick liquid thickness near the tube wall along the condenser tube length. The fabricated microstructures on the inner wall are the conventional technique to improve the performance. Here a passive phase separation concept was proposed to create distinct phase distribution. An empty cylinder made of a single layer of mesh pore surface was suspended in a tube, dividing the tube into an annular region and an inner region. The mesh pore surface prevents gas phase entering the inner region but sucks liquid towards the inner region. Thus largest possibility for gas directly contacted with the inner wall surface is ensured. An air/water two-phase flow experiment was performed and the stratified flow pattern modulation was investigated. When the liquid level in the horizontal tube is relatively higher, the liquid can be thoroughly within the mesh cylinder to form the “gas-floating-liquid” mode. The whole inner tube wall surface is covered by the gas phase. If the liquid content is relatively smaller, partial liquid can be sucked into the mesh cylinder. The contact area between the inner tube wall and gas is increased. The stratified flow pattern modulation is expected to significantly enhance the condensation heat transfer under low mass fluxes which is being verified by our continuous experiment.

Flow pattern modulation in a horizontal tube by the passive phase separation concept

A passive phase separation concept was proposed to modulate flow pattern in a condenser tube. An empty mesh cylinder is suspended in the condenser tube. The miniature mesh pores prevent gas bubble entering the mesh cylinder but capture liquid into the mesh cylinder, ensuring largest possibility for cold tube wall directly contacted with gas to form the perfect thin liquid film condensation heat transfer. We performed the air–water two-phase flow experiment. It was found that for a relatively higher liquid height in the horizontal tube, all liquid can be captured by the mesh cylinder to form the “gas-floating-liquid” mode. If the liquid height is small in the horizontal tube, partial liquid can be sucked by the mesh cylinder, the contact area between tube wall and gas is increased. When plug flow reaches the mesh cylinder surface, elongated saddle bubbles are formed in the annular region to envelop the mesh cylinder surface. When bubbly flow in the horizontal tube approaches the mesh cylinder area, miniature bubbles can merge to form large bubbles in the annular region. For the later two cases, all the gas flow rate is flowing in the annular region and the inside mesh cylinder is the liquid.

Performance Evaluation of a Pump-Assisted, Capillary Two-Phase Cooling Loop

A hybrid (pump-assisted and capillary) two-phase loop (HTPL) is experimentally investigated to characterize its thermal performance under stepwise heat input conditions. An integration of mechanical pumping with capillary pumping is achieved by using planar evaporator(s) and a two-loop design separating liquid and vapor flows. The evaporator(s) use a sintered copper grooved wick bonded with a liquid screen artery. No active flow control of the mechanical pumping is required because of the autonomous capillary pumping due to the self-adjusting liquid menisci to variable heat inputs of the evaporators. Unlike other active two-phase cooling systems using liquid spray and microchannels, the HTPL facilitates a passive phase separation of liquid from vapor in the evaporator using capillary action, which results in a lower flow resistance of the single-phase flows than two-phase mixed flows in fluid transport lines. In this work, a newly developed planar form-factor evaporator with a boiling heat transfer area of 135.3 cm2 is used aiming for the power electronics with large rectangular-shaped heat sources. This paper presents the experimental results of the HTPLs with a single evaporator handling a single heat source and dual evaporators handling two separate heat sources, while using distilled water as the working fluid for both cases. For the single evaporator system, the temperature results show that the HTPL does not create a big temperature upset under a stepwise heat load with sudden power increases and decreases. The evaporator thermal resistance is measured to be as low as 0.5 K cm2/W for the maximum heat load of 4.0 kW. A cold-start behavior characterized by a big temperature fluctuation was observed at the low heat inputs around 500 W. The HTPL with dual evaporators shows a strong interaction between the evaporators under an asymmetric heat load of the total maximum heat input of 6.5 kW, where each evaporator follows a different heat input schedule. The temperatures of the dual-evaporator system follow the profile of the total heat input, while the individual heat inputs determine the relative level of the temperatures of the evaporators.

A Novel Device Addressing Design Challenges for Passive Fluid Phase Separations Aboard Spacecraft

Capillary solutions have long existed for the control of liquid inventories in spacecraft fluid systems such as liquid propellants, cryogens and thermal fluids for temperature control. Such large length scale, ‘low-gravity,’ capillary systems exploit container geometry and fluid properties—primarily wetting—to passively locate or transport fluids to desired positions for a variety of purposes. Such methods have only been confidently established if the wetting conditions are known and favorable. In this paper, several of the significant challenges for ‘capillary solutions’ to low-gravity multiphase fluids management aboard spacecraft are briefly reviewed in light of applications common to life support systems that emphasize the impact of the widely varying wetting properties typical of aqueous systems. A restrictive though no less typifying example of passive phase separation in a urine collection system is highlighted that identifies key design considerations potentially met by predominately capillary solutions. Sample results from novel scale model prototype testing aboard a NASA low-g aircraft are presented that support the various design considerations.

Start-Up Characteristics and Gravity Effects on a Medium/High-Lift Heat Pump using Advanced Hybrid Loop Technology

Thermal characterization was performed on a vapor compression heat pump using a novel, hybrid two phase loop design. Previous work on this technology has demonstrated its ability to provide passive phase separation and flow control based on capillary action. This provides high quality vapor to the compressor without relying on gravity-based phase separation or other active devices. This paper describes the subsequent work done to characterize evaporator performance under various startup scenarios, tilt angles, and heat loads. The use of a thermal expansion valve as a method to regulate operation was investigated. The effect of past history of use on startup behavior was also studied.