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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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238 records · Page 14

Poromechanical cohesive interface element with combined Mode I-II cohesive zone elastoplasticity for simulating fracture in fluid-saturated porous media

A combined Mode I-II cohesive zone (CZ) elasto-plastic constitutive model, and a two-dimensional (2D) cohesive interface element (CIE) are formulated and implemented at small strain within an ABAQUS User Element (UEL) for simulating 2D crack nucleation and propagation in fluid-saturated porous media. Here, the CZ model mitigates problems of convergence for the global Newton-Raphson solver within ABAQUS, which when combined with a viscous stabilization procedure allows for simulation of post-peak response under load control for coupled poromechanical finite element analysis, such as concrete gravity dam stability analysis. Verification examples are presented, along with a more complex ambient limestone-concrete wedge fracture experiment, water-pressurized concrete wedge experiment, and concrete gravity dam stability analyses. A calibration procedure for estimating the CZ parameters is demonstrated with the limestone-concrete wedge fracture process. For the water-pressurized concrete wedge fracture experiment it is shown that the inherent time-dependence of the poromechanical CIE analysis provides a good match with experimental force versus displacement results at various crack mouth opening rates, yet misses the pore water pressure evolution ahead of the crack tip propagation. This is likely a result of the concrete being partially-saturated in the experiment, whereas the finite element analysis assumes fully water saturated concrete. For the concrete gravity dam analysis, it is shown that base crack opening and associated water uplift pressure leads to a reduced Factor of Safety, which is confirmed by separate analytical calculations.

97 MATHEMATICS AND COMPUTING↗

Evaluating Polymer Properties with Different Additives for Carbon Capture and Other Applications

Anthropogenic climate change is one of this generation’s most pressing concerns, with the potential to completely alter the delicate balance we’ve struck with nature. Already, global temperatures have risen 1.29°C, leading to disrupted weather systems, extinctions, increased risks of wildfires, and sea level rise, to name a few effects. Carbon dioxide emission from the combustion of fossil fuels and other industrial activity is a large driver of this phenomenon, as it absorbs heat before it can be radiated away from Earth, trapping it. Carbon dioxide has reached unprecedented levels in our atmosphere, showing a 50% increase from preindustrial averages to a whopping 430 ppm. Thus, reducing the amount of carbon dioxide via carbon capture technology is an important endeavor that serves to benefit everyone. The Microencapsulated CO 2 Sorbent (MECS) team at Lawrence Livermore National Laboratory (LLNL) has turned to microencapsulation to approach this endeavor. Microcapsules provide an attractive approach to carbon capture, combining large surface areas for more efficient mass transfer, regenerative abilities, reduced solvent loss, and improved handling. Additionally, while existing carbon capture technology relies on industrial plants, capsules could present a modular approach to carbon capture, reducing the need for extensive physical infrastructure. The MECS team’s design consists of a polymer membrane that contains a liquid carbon sequestering sorbent, aqueous sodium carbonate. The carbon capturing reaction occurs in three distinct steps, the first of which is the dissolution of carbon dioxide into the sorbent solution and its conversion into carbonic acid (H 2 CO 3 ), shown in equations 1 and 2 respectively. Because this step hinges upon the ability of carbon dioxide to reach the solution inside the capsule, it is necessary that the microcapsule shell is permeable to carbon dioxide gas. The MECS team produces these microcapsules using the in-air droplet encapsulation apparatus (IDEA) shown in figure 1, which can produce uniform micron-scale droplets at speeds much faster than traditional single-dispersal microfluidic-based techniques. The IDEA Is 100 times faster than these current techniques and can reach up to 1000 times their speed when incorporating a multi-nozzle design. Additionally, because droplets are produced in-air via vibration, IDEA can decrease post-processing times and material waste by 99% and can fabricate microgels that are 10 to 100 times more viscous than can be produced via traditional microfluidics. While this design represents a breakthrough in the throughput, efficiency, and tunability of microcapsule production, it imposes a major constraint on the microcapsule curing process. Because microcapsule shells are crosslinked with UV light while falling 30 cm through the air, this gives them a reaction window of approximately 0.2 seconds. Thus, the system and shell formulations must be optimized such that the shells can be fully crosslinked within this very narrow window, prompting investigations into curing behavior.

36 MATERIALS SCIENCE↗

Co-synthesis of Hydrogen and High-Value Carbon Products from Methane Pyrolysis

The ARPA-E Methane Pyrolysis Project successfully developed a scalable technology for hydrogen production with low-CO x emission through methane pyrolysis, co-producing high-value carbon nanotubes (CNTs). The project focused on optimizing reactor design, enhancing catalyst performance, and assessing techno-economic feasibility to create a commercially viable and environmentally sustainable process. The fluidized bed reactor achieved over 90% methane (CH 4 ) conversion by using a 5% CO 2 co-feed, which stabilizes carbon yields and minimizes catalyst deactivation. This setup allowed for continuous operation across ten cycles, each consisting of a 14-minute pyrolysis phase followed by a 10-minute dislodging phase to remove a fraction of the accumulated carbon, resulting in stable performance and high-quality CNT production. In parallel, monolith reactors coated with Fe demonstrated a sustained methane conversion of 73% while producing CNTs with high crystallinity. Although promising for continuous operation, monolith reactors face challenges in coating durability and scalability, highlighting areas for further optimization in commercial applications. Catalyst formulation played a key role in enhancing process efficiency. The core catalyst used was 5%Fe/Al 2 O 3 (wt%), optimized through wet impregnation, which improved CNT morphology, yielding longer and more uniform CNTs. The catalyst's performance was further enhanced by adding promoters: 2.5 wt% Ni increased methane conversion close to the thermodynamic limit, while 2.5 wt% Mn improved CNT alignment and crystallinity, and 1.5 wt% NaCl boosted CNT morphology but slightly lowered methane conversion. These adjustments allowed the reactor to maintain high methane conversion while producing high-quality CNTs, enabling stable performance over multiple cycles. To address carbon buildup and ensure uninterrupted operation, a pneumatic conveying tube was implemented for effective carbon dislodging in the fluidized bed configuration. CO 2 and H 2 O co-feeds were also introduced to enhance carbon removal, with CO 2 boosting CNT yield by approximately 15%. This setup enabled stable reactor operation across multiple cycles, preventing clogging and minimizing catalyst wear, making the process suitable for industrial scaling. Techno-economic analysis (TEA) projected hydrogen production costs between $\$$1.00 and $\$$1.64 per kilogram, with CNT values assumed at $\$$375/ton and $\$$100/ton. The life cycle assessment showed that CO 2 emissions could be as low as 0.64 kg CO 2 e/kg H 2 at 95% methane conversion assuming an electricity input of 50 kg CO 2 e/MWh. Even at 50% methane conversion, emissions remained below 1 kg CO 2 e/kg H 2 , demonstrating the process's low-emission potential and making it a viable alternative to traditional steam methane reforming. Overall, the results from this project demonstrate the feasibility of a pyrolysis process where carbon is continuously removed from the catalyst surface and hydrogen is continuously produced until a catalyst regeneration step is required to fully clean the catalyst surface and renew catalyst performance. Major open challenges are related to avoiding the loss of catalyst material in the dislodged carbon during fluidized bed conditions, since our best result demonstrated a carbon purity of ~70 wt. % (rest being iron and alumina). A monolith reactor was used to favor dislodgement of carbon compared to fluidized bed conditions but our results do not demonstrate an advantage of the monolith configuration. Catalyst performance was similar to fluidized bed conditions with slower deactivation rates overall, but we could not observe carbon dislodging in any of the tens of experiments that were run at Stanford. Our results show that the most relevant areas of improvement are related to the fundamental understanding of the iron-carbon interface for dislodging, and the development of catalyst that can produce CNTs via a base-growth mechanism such that catalyst is not lost in the dislodgement steps. The final report documents all findings and methodologies in detail, providing a valuable resource for the scientific community. By building on these results, researchers can further advance methane pyrolysis technology, moving toward a more sustainable, scalable pathway for hydrogen production. This work lays the foundation for future research and commercial efforts to reduce emissions in hydrogen production while generating valuable carbon products.

08 HYDROGEN↗

Exploring the Neutron Substructure with Advanced Polarized Helium-3 Targets (Or: How I Learned to Stop Worrying and Love Spectroscopy)

As we seek to understand the smallest, physical aspects of our universe, we cannot simply rely on our senses to probe the world around us as we did in the past. The smallest physical elements of our universe behave in strange, probabilistic ways and are completely invisible to the naked eye/ear/etc. So, we design clever experiments (such as scattering experiments) to probe these minute realms. Then, just as with the larger, observable world, we devise models and equations to describe what we think is happening. Due to the nature of the physical universe at the quantum scale and with the aid of symmetries such as Lorentz invariance, we can write down equations that describe the scattering, but the expressions contain functions, which we call ?form factors? and ?structure functions?, that we cannot compute from first principles. We can, however, formulate models that make predictions for these functions. By comparing our predictions with the observed data, we can gain insight into the validity of our models and thus a better physical understanding of what is happening at these minuscule scales. Studying the constituents inside of the nucleus of an atom adds another layer of difficulty if we can?t remove those components from the nucleus. This is the case with the neutron. When not bound in the nucleus with protons and other neutrons, the neutron will decay into a proton after about 15 minutes. So, we?re forced to study the neutron while it is still bound in the nucleus of an atom such as helium-3 (3He). For the last 1,000 years (rounding up), our group has developed high quality, polarized 3He targets made of an aluminosilicate glass. These targets are made in order to perform experiments at Jefferson Lab (JLab), experiments which let us determine the form factors and structure functions of the neutron by scattering polarized electrons from polarized neutrons (or rather polarized 3He). The specific experiments reported on in this thesis push the bounds of our understanding of the internal structure of the neutron. Good science is often about pushing experimental techniques to a new level. Toward that goal we study our polarized 3He targets both to advance the technology and to choose the best ones for our experiments. We do this using a process called nuclear magnetic resonance (NMR) to gauge the maximum polarization of a target and how fast the polarization decays with time. While these tests primarily provide us information that make analysis of our experimental scattering data possible, they also let us determine whether or not a target-cell is useful or even, dare I say, of spectacular quality. Our latest targets utilize a novel convection design allowing 3He to be polarized and quickly moved in front of the electron-beam, making it possible to use larger targets with higher electron-beam currents than ever before. This means more electrons scatter and we get more data. And by studying our targets in detail prior to using them in our experiments, we have found techniques to take effects which could have been detrimental to target quality and turn them to our advantage! It?s a real case of making lemonade out of lemons. We also use laser spectroscopy to study the absorption lines of alkali-metals in the target (potassium and rubidium, specifically). We add these alkali-metals to our target to facilitate polarizing the 3He. We can use the measurement of these pressure broadened absorption lines to determine the 3He density inside of the target with great precision. Historically, we understood the width of these lines would be dependent on the temperature of the target. Specifically, if I raise the temperature, the width should get bigger. I found that was not the case, which was very confusing at first, though very exciting now that I realize the data are self-consistent and suggestive of unexpected behavior. This thesis details the development of high quality, glass, polarized 3He targets for the 2020 An 1 /dn 2 and 2023 Gn E experiments, which utilized the first 3He convection targets and broke records in target quality. This thesis also covers the initial development of metal windows for the next-generation of 3He target-cells. Finally, this thesis documents the temperature dependence of the width of potassium (K) and rubidium (Rb) absorption lines as measured with laser spectroscopy.

Jantzi, Christopher↗