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994 records · Page 56

Contact angles from Young’s equation in molecular dynamics simulations

In this work, we propose a method to calculate the equilibrium contact angle of heterogeneous 3-phase solid/fluid/fluid systems using molecular dynamics simulations. The proposed method, which combines the phantom-wall method [F. Leroy and F. Müller-Plathe, J. Chem. Phys. 133, 044110 (2010)] and Bennett’s acceptance ratio approach [C. H. Bennett, J. Comput. Phys. 22, 245 (1976)], is able to calculate the solid/fluid surface tension relative to the solid surface energy. The calculated relative surface tensions can then be used in Young’s equation to estimate the equilibrium contact angle. A fluid droplet is not needed for the proposed method, in contrast to the situation for direct simulations of contact angles. In addition, while prior free-energy based methods for contact angles mainly focused on the wetting of fluids in coexistence with their vapor on solid surfaces, the proposed approach was designed to study the contact angles of fluid mixtures on solid surfaces above the fluid saturation pressures. Using the proposed approach, the contact angles of binary Lennard-Jones fluid mixtures on a non-polar solid substrate were calculated at various interaction parameters and the contact angle of water in equilibrium with CO 2 on a hydrophilic polar silica surface was obtained. For both non-polar and polar systems, the calculated contact angles from the proposed method were in agreement with those obtained from the geometry of a cylindrical droplet. The computational cost of the proposed method was found to be comparable to that of simulations that use fluid droplets, but the new method provides a way to calculate the contact angle directly from Young’s equation without ambiguity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Carbon dioxide (CO 2 ) concentrations and emission in the newly constructed Belo Monte hydropower complex in the Xingu River, Amazonia

The Belo Monte hydropower complex located in the Xingu River is the largest run-of-the-river (ROR) hydroelectric system in the world and has one of the highest energy production capacities among dams. Its construction received significant media attention due to its potential social and environmental impacts. It is composed of two ROR reservoirs: the Xingu Reservoir (XR) in the Xingu's main branch and the Intermediate Reservoir (IR), an artificial reservoir fed by waters diverted from the Xingu River with longer water residence time compared to XR. We aimed to evaluate spatiotemporal variations in CO 2 partial pressure ( p CO 2 ) and CO 2 fluxes ( F CO 2 ) during the first 2 years after the Xingu River impoundment under the hypothesis that each reservoir has contrasting F CO 2 and p CO 2 as vegetation clearing reduces flooded area emissions. Time of the year had a significant influence on p CO 2 with the highest average values observed during the high-water season. Spatial heterogeneity throughout the entire study area was observed for pCO2 during both low- and high-water seasons. F CO 2 , on the other hand, only showed significant spatial heterogeneity during the high-water period. F CO 2 (0.90±0.47 and 1.08±0.62 µmol m 2 d –1 for XR and IR, respectively) and p CO 2 (1647±698 and 1676±323 µatm for XR and IR, respectively) measured during the high-water season were on the same order of magnitude as previous observations in other Amazonian clearwater rivers unaffected by impoundment during the same season. In contrast, during the low-water season F CO 2 (0.69±0.28 and 7.32±4.07 µmol m 2 d –1 for XR and IR, respectively) and p CO 2 (839±646 and 1797±354 µatm for XR and IR, respectively) in IR were an order of magnitude higher than literature F CO 2 observations in clearwater rivers with naturally flowing waters. When CO 2 emissions are compared between reservoirs, IR emissions were 90 % higher than values from the XR during low-water season, reinforcing the clear influence of reservoir characteristics on CO 2 emissions. Based on our observations in the Belo Monte hydropower complex, CO 2 emissions from ROR reservoirs to the atmosphere are in the range of natural Amazonian rivers. However, the associated reservoir (IR) may exceed natural river emission rates due to the preimpounding vegetation influence. Since many reservoirs are still planned to be constructed in the Amazon and throughout the world, it is critical to evaluate the implications of reservoir traits on F CO 2 over their entire life cycle in order to improve estimates of CO 2 emissions per kilowatt for hydropower projects planned for tropical rivers.

54 ENVIRONMENTAL SCIENCES↗

Integration of Online Cross-Section Generation Capability with Depletion and Transient Solvers in Griffin

Griffin is a Multiphysics Object-Oriented Simulation Environment (MOOSE)-based reactor multiphysics analysis application jointly developed by Argonne and Idaho National Laboratories under the DOENE Nuclear Energy Advanced Modeling and Simulation (NEAMS) program. In FY25, an online crosssection generation capability based on the Self-Shielding Application Programming Interface (SSAPI) was demonstrated for TRISO-fueled reactor problems under steady-state conditions. This fiscal year, that capability was extended to support depletion and transient multiphysics calculations, enabling high-fidelity analyses that generate self-shielded cross sections on the fly from the actual evolving composition and temperature states rather than from pre-tabulated libraries. For depletion, a two-way coupling was established in which SSAPI computes compact-averaged self-shielded cross sections that the depletion solver then uses to advance the Bateman equations, with the updated compositions returned to SSAPI at each step; the depletion module was refactored to support both library-based and SSAPI-based cross sections, and additional logic was added to track daughter isotopes and to exclude minor isotopes for efficiency. For transient analysis, the SSAPI multigroup library was extended with the kinetics data required for time-dependent calculations, the Improved Quasi-Static (IQS) scheme was coupled with SSAPI, and several supporting capabilities were implemented, including a self-shielding treatment that lets control rods and drums move within a self-shielded model, which had previously been impossible and had ruled out rod- and drum-movement transients with on-the-fly cross sections altogether, a new mixing scheme for delayed-neutron precursor decay constants, a checkpoint-based restart workflow, and performance improvements such as pointwise cross-section interpolation and the bypassing of unnecessary Dancoff factor calculations. The implemented capabilities were verified against Serpent Monte Carlo solutions. For depletion, a prismatic pin-cell problem based on a Next Generation Nuclear Plant (NGNP) Very High Temperature Reactor benchmark showed excellent agreement, with eigenvalue differences within 200 pcm over the entire burnup range (up to 140 MWD/kgU) and fission-product and actinide inventories agreeing to within 0.8% and 2.5%, respectively; a heat-pipe microreactor assembly problem with a much higher fuel loading confirmed the same behavior and quantified the bias introduced when the multigroup equivalence effect is neglected. For transient analysis, a pin-cell problem with a step reactivity insertion and temperature feedback reproduced the analytically expected asymptotic power and showed close agreement between the direct and IQS solutions, and a two-dimensional microreactor core problem with control-drum rotation exercised the new moving-drum self-shielding treatment and demonstrated successful coupling of the online crosssection generation with both the direct and IQS transient methods. The capability was further exercised on a full-core pebble-bed problem, in which Griffin was coupled with the System Analysis Module (SAM) to simulate load-following operation of the gPBR with the Doppler feedback resolved at the TRISO fuel kernel temperature. These developments in Griffin provide a convenient, high-fidelity approach to cross-section generation for advanced thermal reactors with geometrically complex and highly heterogeneous configurations, including TRISO-fueled prismatic and pebble-bed systems, and support steady-state, depletion, and transient multiphysics calculations. They also enable self-shielded cross sections to be evaluated directly at the actual coupled state of the system, thereby establishing a foundation for high-fidelity, fully coupled multiphysics analysis of advanced reactors

Park, H.↗

Effects of Mineral Surface Properties on Supercritical CO 2 Wettability in a Siliciclastic Reservoir

Wettability is a key reservoir characteristic influencing geological carbon sequestration (GCS) processes, such as CO 2 transport and storage capacity. Wettability is often determined on a limited number of reservoir samples by measuring the contact angle at the CO 2 /brine/mineral interface, but the ability to predict this value remains a challenge. In this work, minerals comprising a natural reservoir sample were identified, and the influence of their surface roughness and mineralogy on the contact angle was quantified to evaluate predictive models and controlling mechanisms. The natural sample was obtained from the Mount Simon formation, a representative siliciclastic reservoir that is the site of a United States Department of Energy CO 2 injection project. A thin section of the Mount Simon sandstone was examined with compound light microscopy and environmental scanning electron microscopy (ESEM) coupled with energy-dispersive X-ray spectroscopy (EDS). Quartz and feldspar were identified as dominant minerals and were coated with various reddish black precipitates consistent with illite clay and iron oxide hematite. Contact angle (θ) measurements were conducted for the four representative minerals and the Mount Simon sample over a range of pressures (2–25 MPa) at 40 °C. At supercritical conditions, all samples are strongly water-wet, with contact angles between 27° and 45°. Several predictive models for contact angle were evaluated for the mineral and Mount Simon samples, including the Wenzel and Cassie–Baxter models, plus newly proposed modifications of these that account for the fraction of different minerals comprising the reservoir sample surface, the surface roughness, and the extent that roughness pits are filled with brine. Modeling results suggest that the fraction of mineral surfaces containing roughness pits filled with brine is the most important reservoir characteristic that controls wettability in the Mount Simon sandstone, followed by surface mineralogy. Finally, to our knowledge, this is one of the few studies to investigate the effects of individual minerals on the wettability of a natural reservoir sample.

58 GEOSCIENCES↗