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1. Aluminum foam-based ultrafast electronucleation of hydrates

   Acharya, P ; Shahriari, A ; Carpenter, K ; Bahadur, V ( July 2017 , Proceedings of the 2017 ASME Summer Heat Transfer Conference)

   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. 

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2. Mechanisms underlying rapid electronucleation and freezing of hydrates

   Acharya, P ; Shahriari, A ; Lin, D ; Bahadur, V. ( November 2017 , Proceedings of ASME 2017 International Mechanical Engineering Congress & Exposition)

   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. 

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3. Mechanisms underlying foam-based electronucleation of hydrates

   Acharya, P ; Lin, D ; Bahadur, V ( June 2018 , Proceedings of the 2018 International Conference on Nanochannels, Microchannels and Minichannels)

   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. 

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4. Spinodal stratification in ultrathin micellar foam films

   https://doi.org/10.1039/C8ME00102B  

   Yilixiati, Subinuer ; Wojcik, Ewelina ; Zhang, Yiran ; Sharma, Vivek ( June 2019 , Molecular Systems Design & Engineering)

   null (Ed.)

   We report the discovery of a hitherto unreported mechanism of drainage and rupture of micellar foam films that presents unexplored opportunities for understanding and controlling the stability, lifetime and properties of ubiquitous foams. It is well-known that ultrathin micellar foam films exhibit stratification, manifested as stepwise thinning and coexistence of thin–thick flat regions that differ in thickness by a nanoscopic step size equal to the intermicellar distance. Stratification typically involves the spontaneous formation and growth of thinner, darker, circular domains or thicker, brighter mesas. Mechanistically, domain expansion appears similar to hole growth in polymer films undergoing dewetting by nucleation and growth mechanism that can be described by considering metastable states resulting from a thickness-dependent oscillatory free energy. Dewetting polymer films occasionally phase separate into thick and thin regions forming an interconnected, network-like morphology by undergoing spinodal dewetting. However, the formation of thick–thin spinodal patterns has never been reported for freestanding films. In this contribution, we show that the thickness-dependent oscillatory contribution to free energy that arises due to confinement-induced layering of micelles can drive the formation of such thick-thin regions by undergoing a process we term as spinodal stratification. We visualize and characterize the nanoscopic thickness variations and transitions by using IDIOM (interferometry digital imaging optical microscopy) protocols to obtain exquisite thickness maps of freestanding films. We find that evaporation and enhanced drainage in vertical films play a critical role in driving the process, and spinodal stratification can occur in both single foam films and in bulk foam. 

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5. Polyelectrolyte Complex Stabilized CO2 Foam Systems for Hydraulic Fracturing Application

   https://doi.org/10.2118/187489-MS  

   Anandan, Rudhra ; Johnson, Stephen ; Barati, Reza ( September 2017 , SPE Liquids-Rich Basins Conference- North America)

   Hydraulic fracturing of oil and gas wells is a water intensive process. Limited availability, cost and increasing government regulations restraining the use and disposal of fresh water have led to the need for alternative fracturing fluids. Using CO2 foam as a fracturing fluid can drastically reduce the need for water in hydraulic fracturing. We address the addition of polyelectrolyte complex nanoparticles (PECNP) to surfactant solutions to improve foam stability, durability and rheological properties at high foam qualities. Polyelectrolyte pH and polyanion/polycation ratios were varied to minimize particle size and maximize absolute zeta potential of the resulting nanoparticles. Rheological tests were conducted on foam systems of varying surfactant/PECNP ratios and different foam quality to understand the effect of shear on viscosity under simulated reservoir conditions of 40°C and 1300 psi. The same foam systems were tested for stability and durability in a view cell at reservoir conditions. Supercritical CO2 foam generated by surfactant alone resulted in short lived, low viscosity foam because of surfactant drainage from foam lamellae. However, addition of PECNP strengthens the foam film by swelling the film due to increased osmotic pressure and electrostatic forces. Electrostatic interactions reduce dynamic movement of surfactant micelles, thereby stabilizing the foam lamellae, which imparts high durability and viscosity to supercritical CO2 foams. From the rheology test results, it was concluded that increasing foam quality and the presence of PECNP resulted in improved viscosity. Also, foam systems with PECNP showed promising results compared with foam generated using surfactant alone in the view cell durability test. The addition of optimized polyelectrolyte nanoparticles to the surfactant can improve viscosity and durability of supercritical CO2 foam during hydraulic fracturing, which can lead to large reductions in water requirements.

    

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