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Benzhong Zhao

Publications and source records attributed to Benzhong Zhao.

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Modeling Ostwald Ripening Dynamics in Porous Microstructures

Partially miscible ganglia trapped in a porous medium evolve through Ostwald ripening, driven by differences in interfacial curvature. In practice, ganglia can span multiple pores and undergo discrete capillary events - invasion, snap-off, retraction, fragmentation, coalescence, and dislocation - that alter their topology and induce local flow. Existing pore-network models (PNMs) for ripening are limited to single-pore ganglia, assume idealized pore shapes, and operate under quasi-static conditions that preclude flow. We present an image-based pore-network model (iPNM) that removes these limitations. Unlike existing PNMs, iPNM requires no idealization of pore shapes, as the effect on capillarity is encoded locally in curvature-saturation curves computed via the pore-morphology method. iPNM couples two-phase flow, solute transport, and Ostwald ripening within a unified framework. We first verify iPNM against a prior quasi-static PNM, then validate it against recent high-resolution microfluidic experiments of hydrogen ripening in a sandstone-patterned micromodel over 15-24 days at 40C and 80C. Good agreement is obtained without adjustable parameters. Comparison with a continuum model shows that while macroscopic saturation is captured by both approaches, iPNM uniquely resolves population statistics, individual ganglion curvatures, and pre-equilibrium ripening dynamics within a representative elementary volume. Its computational efficiency over direct numerical simulation makes it suitable for guiding the development of improved theories of ripening in confined geometries.

physics.flu-dyn

Implicit Nucleation and Competitive Dynamics of Electrogenerated Hydrogen Nanobubbles

Electrogenerated gas nanobubbles strongly influence the performance of electrochemical energy-conversion systems, yet their nucleation and early evolution remain poorly understood due to limitations of existing experimental and computational approaches. Operando imaging lacks the temporal resolution required to capture nucleation events, while molecular dynamics simulations are restricted to nanometer-scale domains containing at most a few bubbles. Here, we develop a thermodynamically consistent phase-field framework that unifies dissolved gas transport, curvature dependent interfacial thermodynamics, and implicit bubble nucleation within a single continuum description. Using hydrogen nanobubble formation during electrocatalysis as a canonical test case, the model captures nucleation without prescribing nuclei, resolves diffusion-controlled growth under curvature effects, and remains computationally tractable despite hydrogen's extremely low solubility. Simulations reveal how nanobubble nucleation occurs once a local supersaturation threshold is exceeded, triggering a reorganization of the chemical-potential field that focuses dissolved gas toward the nascent bubble. In multi-catalyst systems, overlapping diffusion fields lead to strong bubble-bubble interactions, including competitive growth, Ostwald ripening, and source occlusion. Extending the framework to dispersed catalyst populations shows that nanobubble survival is governed not only by catalyst size but also by spatial arrangement and diffusive competition, such that only a subset of bubbles persist while others dissolve and act as feeders. These results reframe electrogenerated nanobubbles as emergent, spatially organized features rather than unavoidable parasitic byproducts, and point toward electrode designs that deliberately control where bubbles nucleate and grow to preserve active area and mitigate transport losses.

cond-mat.soft

Ostwald Ripening in Underground Gas Storage

Underground gas storage is central to both climate mitigation and energy transition strategies, supporting both long-term carbon sequestration and seasonal hydrogen storage. A key mechanism governing the fate of injected gases is Ostwald ripening, the curvature-driven mass transfer between trapped gas ganglia in porous media. While ripening is well understood in open systems, its behavior in geometrically confined porous structures remains poorly characterized, especially over long timescales relevant to subsurface operations. Here, we present ultra-high-resolution microfluidic experiments that capture the evolution of residually trapped hydrogen over weeks in realistic, heterogeneous pore geometries under well-defined boundary conditions. We observe a distinct two-stage dynamic: a rapid local equilibration among neighboring bubbles, followed by slow global depletion driven by long-range diffusion toward low-chemical potential boundaries. Building on these insights, we develop and validate a continuum model that couples microscale capillary pressure-saturation (Pc-s) relationships, extracted via the pore-morphology method, with macroscopic diffusive transport. The model accurately predicts gas saturation evolution without fitting parameters and collapses experimental results across a range of experimental conditions. Extending the model to reservoir scales, we estimate equilibration timescales for CO2 and H2 in homogeneous sandstone aquifers. We find that ripening occurs much faster than convective dissolution in CO2 sequestration, and on timescales comparable to seasonal H2 storage operations. These findings establish a quantitative framework linking pore-scale heterogeneity to field-scale gas redistribution, with implications for the design and longevity of subsurface storage strategies.

cond-mat.soft

A computationally efficient queue-based algorithm for simulating volume-controlled drainage under the influence of gravity on volumetric images of porous materials

Simulating non-wetting fluid invasion in volumetric images of porous materials is of broad interest in applications as diverse as electrochemical devices and CO2 sequestration. Among available methods, image-based algorithms offer much lower computational cost compared to direct numerical simulations. Recent work has extended image-based method to incorporate more physics such as gravity and volume-controlled invasion. The present work combines these two developments to develop an image-based invasion percolation algorithm that incorporates the effect of gravity. Additionally, the presented algorithm was developed using a priority queue algorithm to drastically reduce the computational cost of the simulation. The priority queue-based method was validated against previous image-based methods both with and without the effect of gravity, showing identical results. It was also shown that the new method provides a speedup of 20X over the previous image-based methods. Finally, comparison with experimental results at three Bond numbers showed that the model can predict the real invasion process with a high accuracy with and without gravitational effects.

physics.flu-dyn

Characteristics of fluid-fluid displacement in model mixed-wet porous media: patterns, pressures, and scalings

We study the characteristics of fluid-fluid displacement in simple mixed-wet porous micromodels numerically using a dynamic pore network model. The porous micromodel consists of distinct water-wet and oil-wet regions, whose fractions are systematically varied to yield a variety of displacement patterns over a wide range of capillary numbers. We find that the impact of mixed-wettability is most prominent at low capillary number, and it depends on the complex interplay between wettability fraction and the intrinsic contact angle of the water-wet regions. For example, the fractal dimension of the displacement pattern is a monotonically increasing function of wettability fraction in flow cells with strongly water-wet clusters, but it becomes non-monotonic with respect to wettability fraction in flow cells with weakly water-wet clusters. Additionally, mixed-wettability also manifests itself in the injection-pressure signature, which exhibits fluctuations especially at low wettability fraction. Specifically, preferential filling of water-wet regions leads to reduced effective permeability and higher injection pressure, even at vanishingly small capillary numbers. Finally, we demonstrate that scaling analyses based on a weighted average description of the overall wetting state of the mixed-wet system can effectively capture the variations in observed displacement pattern morphology.

cond-mat.soft

Wettability alteration in thiolene-based polymer microfluidics: surface characterization and advanced fabrication techniques

Wettability plays a significant role in controlling multiphase flow in porous media for many industrial applications, including geologic carbon dioxide sequestration, enhanced oil recovery, and fuel cells. Microfluidics is a powerful tool to study the complexities of interfacial phenomena involved in multiphase flow in well-controlled geometries. Recently, the thiolene-based polymer called NOA81 emerged as an ideal material in the fabrication of microfluidic devices, since it combines the versatility of conventional soft photolithography with a wide range of achievable wettability conditions. Specifically, the wettability of NOA81 can be continuously tuned through exposure to high-energy UV. Despite its growing popularity, the exact physical and chemical mechanisms behind the wettability alteration have not been fully characterized. Here, we apply different characterization techniques, including contact angle measurements, X-ray photoelectron spectroscopy (XPS), and atomic force microscopy (AFM) to investigate the impact of high-energy UV on the chemical and physical properties of NOA81 surfaces. We find that high-energy UV exposure increases the oxygen-containing polar functional groups, which enhances the surface energy and hydrophilicity of NOA81. Additionally, our AFM measurements show that spin-coated NOA81 surfaces have a roughness less than a nanometer, which is further reduced after high-energy UV irradiation. Lastly, we advance the state-of-the-art of NOA81-based microfluidic systems by creating i) a 2D surface with controlled wettability gradient and ii) a 3D column packed with monodisperse NOA81 beads of controlled size and wettability.

cond-mat.soft

Fluid-fluid displacement in mixed-wet porous media

It is well-known that wettability exerts fundamental control over multiphase flow in porous media, which has been extensively studied in uniform-wet porous media. In contrast, multiphase flow in porous media with heterogeneous wettability (i.e., mixed-wet) is less well-understood, despite its common occurrence. Here, we study the displacement of silicone oil by water in a mostly oil-wet porous media patterned with discrete water-wet clusters that have precisely controlled wettability. Surprisingly, the macroscopic displacement pattern varies dramatically depending on the details of wettability alteration -- the invading water preferentially fills strongly water-wet clusters but encircles weakly water-wet clusters instead, resulting in significant trapping of the defending oil. We explain this counter-intuitive observation with pore-scale simulations, which reveal that the fluid-fluid interfaces at mixed-wet pores resemble an S-shaped saddle with mean curvatures close to zero. We show that incorporation of the capillary entry pressures at mixed-wet pores into a dynamic pore-network model reproduces the experiments. Our work demonstrates the complex nature of wettability control in mixed-wet porous media, and it presents experimental and numerical platforms upon which further insights can be drawn.

cond-mat.soft

Signatures of fluid-fluid displacement in porous media: wettability, patterns, and pressures

We develop a novel `moving capacitor' dynamic network model to simulate immiscible fluid-fluid displacement in porous media. Traditional network models approximate the pore geometry as a network of fixed resistors, directly analogous to an electrical circuit. Our model additionally captures the motion of individual fluid-fluid interfaces through the pore geometry by completing this analogy, representing interfaces as a set of moving capacitors. By incorporating pore-scale invasion events, the model reproduces, for the first time, both the displacement pattern and the injection pressure signal under a wide range of capillary numbers and substrate wettabilities. We show that at high capillary numbers the invading patterns advance symmetrically through viscous fingers. In contrast, at low capillary numbers the flow is governed by the wettability-dependent fluid-fluid interactions with the pore structure. The signature of the transition between the two regimes manifests itself in the fluctuations of the injection pressure signal.

physics.flu-dyn