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At least 73 records · Page 4

A Markov chain Monte Carlo (MCMC) Bayesian inference approach to analyze apparent activation barriers and reaction orders from microreactor data

Statistical analysis of steady-state catalytic kinetic data is often limited by data sparsity due to the slow pace at which the data is collected. Data sparsity and limitations in statistical analysis make it difficult to differentiate between mechanistic models and catalytic sites. A Bayesian inference tool is reported for catalysis researchers to estimate error in the determination of reaction orders from steady state microreactor data. The benefits of a Bayesian inference approach are discussed, as an alternative to the more common frequentist approach. The approach incorporates prior knowledge of the system and the data collected to form an error estimate on reaction orders. We investigated the effects of three distinct data treatments—individual fitting of trials, pooled analysis, and constrained regression methods—on the precision and uncertainty of reaction order determinations. To assess the robustness of our findings, we conducted sensitivity analyses to evaluate the influence of Bayesian parameters on uncertainty estimation. Additionally, we utilized synthetic data to illustrate how data quality impacts the precision of uncertainty assessments. We show Bayesian analysis can obtain a more precise estimation of error with a sparse data set than a frequentist analysis. Finally, this work provides strong evidence that the adoption of Bayesian analysis of kinetic data may help researchers make more precise arguments as to the strength of their evidence for a particular mechanistic hypothesis, or in comparing across different catalysts.

42 ENGINEERING

Effect of Preparation Conditions of Fe@SiO2 Catalyst on Its Structure Using High-Pressure Activity Studies in a 3D-Printed SS Microreactor

Fischer–Tropsch synthesis (FTS) in a 3D-printed stainless steel (SS) microchannel microreactor was investigated using Fe@SiO2 catalysts. The catalysts were prepared by two different techniques: one pot (OP) and autoclave (AC). The mesoporous structure of the two catalysts, Fe@SiO2 (OP) and Fe@SiO2 (AC), ensured a large contact area between the reactants and the catalyst. They were characterized by N2 physisorption, H2 temperature-programmed reduction (H2-TPR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), X-ray photoelectron microscopy (XPS), and thermogravimetric analysis–differential scanning calorimetry (TGA-DSC) techniques. The AC catalyst had a clear core–shell structure and showed a much greater surface area than that prepared by the OP method. The activities of the catalysts in terms of FTS were studied in the 200–350 °C temperature range at 20-bar pressure with a H2/CO molar ratio of 2:1. The Fe@SiO2 (AC) catalyst showed higher selectivity and higher CO conversion to olefins than Fe@SiO2 (OP). Stability studies of both catalysts were carried out for 30 h at 320 °C at 20 bar with a feed gas molar ratio of 2:1. The Fe@SiO2 (AC) catalyst showed higher stability and yielded consistent CO conversion compared to the Fe@SiO2 (OP) catalyst.

Biochemistry & Molecular Biology

Effect of Fe on Co-Based SiO2Al2O3 Mixed Support Catalyst for Fischer–Tropsch Synthesis in 3D-Printed SS Microchannel Microreactor

This research explores the effect of a composite support of SiO2 and Al2O3 with Fe and Co incorporated as catalysts for Fischer–Tropsch synthesis (FTS) using a 3D-printed stainless steel (SS) microchannel microreactor. Two mesoporous catalysts, FeCo/SiO2Al2O3 and Co/SiO2Al2O3, were synthesized via a one-pot (OP) method and extensively characterized using N2 physisorption, XRD, SEM, TEM, H2-TPR, TGA-DSC, FTIR, and XPS. H2-TPR results revealed that the synthesis method significantly affected the reducibility of metal oxides, thereby influencing the formation of active FTS sites. SEM-EDS and TEM further revealed a well-defined hexagonal matrix with a porous surface morphology and uniform metal ion distribution. FTS reactions, carried out in the 200–350 °C temperature range at 20 bar with a H2/CO molar ratio of 2:1, exhibited the highest activity for FeCo/SiO2Al2O3, with up to 80% CO conversion. Long-term stability was evaluated by monitoring the catalyst performance for 30 h on stream at 320 °C under identical reaction conditions. The catalyst was initially active for the methanation reaction for up to 15 h, after which the selectivity for CH4 declined. Correspondingly, the C4+ selectivity increased after 15 h of time-on-stream, indicating a shift in the product distribution toward longer-chain hydrocarbons. This trend suggests that the catalyst undergoes gradual activation or restructuring under reaction conditions, which enhances chain growth over time. The increase in C4+ products may be attributed to the stabilization of the active sites and suppression of methane or light hydrocarbon formation.

Biochemistry & Molecular Biology

Integrated Microreactor for Chemical and Biochemical Applications

A completely integrated microreactor was developed that allows for the processing of very small amounts of chemical solutions. The entire system comprises several pumps and valves arranged in different branches as well as a mixing unit and a reaction chamber. The streaming path of each branch contains two valves and one pump each. The pumps are driven by piezoelectric elements mounted on thin glass membranes. Each pump is about 3.5 mm x 3.5 mm x 0.7 mm. A pumping rate up to 25 microliters per hour can be achieved. The operational voltage ranges between 40 and 200 V. A volume stroke up to 1.5 millimeter is achievable from the membrane structures. The valves are designed as passive valves. Sealing is by thin metal films. The dimension of a valve unit is 0.8 x 0.8. 07 mm. The ends of the separate streaming branches are arranged to meet in one point. This point acts as the beginning of a mixer unit which contains several fork-shaped channels. The arrangement of these channels allows for the division of the whole liquid stream into partial streams and their reuniting. A homogeneous mixing of solutions and/or gases can be observed after having passed about 10 of the fork elements. A reaction chamber is arranged behind the mixing unit to support the chemical reaction of special fluids. This unit contains heating elements placed outside of the chamber. The complete system is arranged in a modular structure and is built up of silicon. It comprises three silicon wafers bonded together by applying the silicon direct bonding technology. The silicon structures are made only by wet chemical etching processes. The fluid connections to the outside are realized using standard injection needles glued into v-shaped structures on the silicon wafers. It is possible to integrate other components, like sensors or electronic circuits using silicon as the basic material.

Schwesinger, N.

Auto-Thermal Reforming of Jet-A Fuel over Commercial Monolith Catalysts: MicroReactor Evaluation and Screening Test Results

This paper describes the results of a series of catalyst screening tests conducted with Jet-A fuel under auto-thermal reforming (ATR) process conditions at the research laboratories of SOFCo-EFS Holdings LLC under Glenn Research Center Contract. The primary objective is to identify best available catalysts for future testing at the NASA GRC 10-kW(sub e) reformer test facility. The new GRC reformer-injector test rig construction is due to complete by March 2004. Six commercially available monolithic catalyst materials were initially selected by the NASA/SOFCo team for evaluation and bench scale screening in an existing 0.05 kW(sub e) microreactor test apparatus. The catalyst screening tests performed lasted 70 to 100 hours in duration in order to allow comparison between the different samples over a defined range of ATR process conditions. Aging tests were subsequently performed with the top two ranked catalysts as a more representative evaluation of performance in a commercial aerospace application. The two catalyst aging tests conducted lasting for approximately 600 hours and 1000 hours, respectively.

Yen, Judy C. H.

Ceramic Composite Inert Matrix Fuel Forms in High-Temperature Gas-Cooled Microreactors

Here, this work optimizes micro-prismatic high-temperature gas reactor (HTGR) designs to reduce the energy-normalized mass of spent nuclear fuel (SNF) and high-level waste (HLW) produced. The optimization was performed for the current graphite moderator and an inert matrix fuel (IMF) concept employing different composite moderators in a prismatic design architecture. The fuel matrix is magnesium oxide (MgO) with entrained tristructural-isotropic (TRISO) fuel. The moderator materials, including beryllium oxide (MgO-BeO) and beryllium (MgO-Be) at 40 vol % loading and yttrium hydride (MgO-YH x=1.9 ) and zirconium hydride (MgO-ZrH x=1.9 ) at 15 vol % loading, were entrained within the MgO host matrix. A generic graphite micro-prismatic HTGR is used as the baseline point design where the external dimensions are held constant. The composite moderator designs use 19.9% enriched uranium nitride TRISO fuel and hexagonal assemblies. For each IMF concept, an optimization study was performed to maximize the discharge burnup of the fuel by varying the TRISO packing fraction and the lattice pitch of the assemblies. The mass of SNF and HLW, other waste metrics, fuel cost, environmental impact metrics, and the activity of the SNF and HLW at 100 years and 100 000 years were calculated for the optimized IMF and graphite reference designs. The IMF results were subsequently compared to those of the graphite reference and the values for a light water reactor (LWR) and a small modular LWR. For the SNF and HLW, all the IMF concepts and the graphite reference produced less waste compared to the traditional LWR designs. However, the IMF concepts outperformed the graphite reference regarding the mass of SNF and HLW. For the other waste metrics, the IMF concepts showed reductions in fuel cost with improved environmental metrics relative to the graphite reference. Overall, the IMF concepts significantly reduced the SNF and HLW produced per unit of energy generated compared to traditional LWR designs.

TRISO

Phenomena Identification and Ranking Tables for High Temperature Gas-Cooled Microreactors

Micro-scaled high-temperature gas-cooled reactors (micro-HTGRs) offer a promising option for reliable power in remote or off-grid locations. While the safety characteristics of modular HTGRs have been widely studied, a micro-HTGR configuration alters several key thermal-fluid phenomena that govern both normal operation and passive decay-heat removal. In many proposed concepts, the reactor vessel is oriented horizontally and integrated into an ISO shipping container to enhance transportability and modular deployment. This report documents a Phenomena Identification and Ranking Table (PIRT) exercise focused on the thermal hydraulic safety phenomena relevant to all micro-HTGRs. The objective is to systematically identify, describe, and rank the importance, uncertainty, and modeling complexity of the key phenomena that control core and vessel temperatures during normal operation, pressurized conduction cooldown (PCC), and depressurized conduction cooldown (with air ingress) conditions.

22 - GENERAL STUDIES OF NUCLEAR REACTORS

Improving Thermal Management Strategies for Data Centers: A Physical Testbed Incorporating Small Modular Reactor and Microreactor Technology

This study aims to accelerate the demonstration of various thermal management systems for data centers using nuclear-generated heat to enhance energy and grid reliability. Utilizing mobile containerized and stationary test beds at INL's High Performance Computing (HPC) facility, this project integrates with various nuclear-related energy systems testing facilities. Key components include immersion cooling apparatus, absorption chillers, and adjustable thermal management simulators. Tasks involve acquiring necessary hardware, sensors, and cooling apparatus, engaging with data center industry stakeholders, and providing a testing platform for algorithms, models, tools, and software. The objective is to expedite the deployment of nuclear-powered data centers, thereby improving energy reliability and affordability.

21 - SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLAN

Development of an Advanced Multiphysics Simulation Capability for Radiant's Microreactor Design

Argonne National Laboratory and Idaho National Laboratory, through a Department of Energy Gateway for Accelerated Innovation in Nuclear Voucher, supported key analysis needs of Radiant related to (i) air jacket thermal fluid performance, (ii) evaluation of decay heat source terms defining air jacket technical requirements, and (iii) assessment of modeling methodologies employed for core analysis. All of these activities center on numerical simulation of various aspects of Kaleidos using the Multiphysics Object-Oriented Simulation Environment (MOOSE) framework, the Cardinal multiphysics application, the OpenMC Monte Carlo code, and the Nek5000 computational fluid dynamics (CFD) code. This project builds upon an earlier Nuclear Energy Advanced Modeling and Simulation (NEAMS) Thermal-Hydraulic (T/H) Center of Excellence (CoE) project focused on initial demonstration of Cardinal multiphysics simulation of High Temperature Gas Reactors (HTGRs) and now focuses on Radiant’s Kaleidos concept.

22 GENERAL STUDIES OF NUCLEAR REACTORS

Microreactor System Design for a NASA In Situ Propellant Production Plant on Mars

The NASA In Situ Resource Utilization (ISRU) program is planning near-term missions to Mars that will include chemical processes for converting the carbon dioxide (CO2) and possibly water from the Martian environment to propellants, oxygen, and other useful chemicals. The use of indigenous resources reduces the size and weight of the payloads from Earth significantly, representing enormous cost savings that make human exploration of Mars affordable. Extraterrestrial chemical processing plants will need to be compact, lightweight, highly efficient under reduced gravity, and extraordinarily reliable for long periods. Microchemical and thermal systems represent capability for dramatic reduction in size and weight, while offering high reliability through massive parallelization. In situ propellant production (ISPP), one aspect of the ISRU program, involves collecting and pressurizing atmospheric CO2, conversion reactions, chemical separations, heat exchangers, and cryogenic storage. A preliminary system design of an ISPP plant based on microtechnology has demonstrated significant size, weight, and energy efficiency gains over the current NASA baseline. Energy management is a strong driver for Mars-based processes, not only because energy is a scarce resource, but because heat rejection is problematic; the low pressure environment makes convective heat transfer ineffective. Energy efficiency gains are largely achieved in the microchemical plant through extensive heat recuperation and energy cascading, which has a small size and weight penalty because the added micro heat exchangers are small. This leads to additional size and weight gains by reducing the required area of waste heat radiators. The microtechnology-based ISPP plant is described in detail, including aspects of pinch analysis for optimizing the heat exchanger network. Three options for thermochemical compression Of CO2 from the Martian atmosphere, adsorption, absorption, and cryogenic freezing, are presented, as well as three options for water decomposition, low temperature electrolysis, high temperature electrolysis, and thermochemical decomposition. Other elements of the plant include Sabatier and reverse water gas shift reactors, water recovery, chemical separations, and cryogenic storage. Data are presented supporting preliminary sizing of components, and results of the system design are compared to the existing NASA baseline that is based on conventional technologies.

TeGrotenhuis, W. E.