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At least 1,099 records · Page 61

Radiolytic evaluation of a new technetium redox control reagent for advanced used nuclear fuel separations

Technetium is a problematic radioisotope for used nuclear fuel (UNF) and subsequent waste management owing to its high environmental mobility and coextraction in reprocessing technologies as the pertechnetate anion (TcO 4 - ). Consequently, several strategies are under development to control the transport of this radioisotope. A proposed approach is to use diaminoguanidine (DAG) for TcO 4 - and transuranic ion redox control. Although the initial DAG molecule is ultimately consumed in the redox process, its susceptibility to radiolysis is currently unknown under envisioned UNF reprocessing conditions, which is a critical knowledge gap for evaluating its overall suitability for this role. To this end, we report the impacts of steady-state gamma irradiation on the rate of DAG radiolysis in water, aqueous 2.0 M nitric acid (HNO 3 ), and in a biphasic solvent system composed of aqueous 2.0 M HNO 3 in contact with 1.5 M N,N-di-(2-ethylhexyl)isobutyramide (DEHiBA) dissolved in n-dodecane. In addition, we report chemical kinetics for the reaction of DAG with key transients arising from electron pulse radiolysis, specifically the hydrated electron (e aq - ), hydrogen atom (H ˙ ), and hydroxyl ( ˙ OH) and nitrate (NO 3 ˙ ) radicals. The DAG molecule exhibited significant reactivity with the ˙ OH and NO 3 ˙ radicals, indicating that oxidation would be the predominant degradation pathway in radiation environments. This is consistent with its role as a reducing agent. Steady-state gamma irradiations demonstrated that DAG is readily degraded within a few hundred kilogray, the rate of which was found to increase upon going from water to HNO 3 containing solutions and solvents systems. This was attributed to a thermal reaction between DAG and the predominant HNO 3 radiolysis product, nitrous acid (HNO 2 ), k(DAG + HNO 2 ) = 5480 ± 85 M -1 s -1 . Although no evidence was found for the radiolysis of DAG altering the radiation chemistry of the contacted DEHiBA/n-dodecane phase in the investigated biphasic system, the utility of DAG as a redox control reagent will likely be limited by significant competition with its degradation by HNO 2 .

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Characterization of Heat Melt Compactor (HMC) Product Water

The Heat Melt Compactor (HMC) is designed to sterilize and process wastes produced during space missions. Benefits of the HMC include reduction of biohazards to the crew, reduction in volume of wastes that would otherwise require storage, production of radiation shielding tiles, and recovery of water and other resources. Water reuse is critical onboard spacecrafts; it reduces the need for resupply missions and saves valuable storage space. The main sources of water in HMC batches are food, beverages, shampoo, disinfecting wipes, toothpaste, and diapers. Water reclaimed by the HMC was analyzed for concentrations of Na+, NH4+, K+, Mg2+, Ca2+, Cl-­‐, NO2-­‐, Br-­‐, NO3-­‐, PO43-­‐, SO42-­‐, total organic carbon (TOC), total inorganic carbon (TIC), % total solids, and pH. The data are discussed in relation to the current water input characteristics established for the International Space Station Water Processor Assembly system. Batches with higher than average amounts of food produced HMC product water with higher sulfate content, and batches with higher proportions of disinfectant wipes and food yielded HMC product water with higher ammonium concentration. We also compared theoretical chemical composition of HMC product water based on food labels and literature values to experimental results.

Heat Melt Compactor↗

Cell G 7606A Mockup Measurement Analysis Methods and Results

The production of research isotopes at the Radiochemical Engineering Development Center (REDC) invariably leads to the accumulation of radioactive waste. Storage of this waste onsite at ORNL serves as an interim solution prior to shipment to long term storage facilities, however onsite capacity is limited. Proper characterization of the activity of waste products is essential for determining the appropriate waste stream and, ultimately, mitigating the cost of disposal. This is typically done via gamma spectrometry and use of the In-Situ Object Counting System (ISOCS), a software package from Mirion that serves as an accepted community standard. However, variability in the contents, density, and activity distribution in waste containers can introduce large errors in ISOCS quantification. A measurement campaign using a mockup of the proposed setup in Cell G seeks to quantify the magnitude and source of these systematic errors. Analysis of this data will guide the creation of ISOCS geometry templates and measurement methods designed to minimize overall uncertainty in reported activities.

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Phase field-volumetric lattice Boltzmann model of ion uptake in porous nuclear waste form materials under continuous flow

The flow field within the mesopores of sorbent particles plays a crucial role in radionuclide diffusion and ion uptake kinetics, thus, impacting the overall performance of porous nuclear waste form materials. To fundamentally understand the influence of microstructures and material properties on the radionuclide absorption and retention processes requires a coupled multi-physics model that considers the advection and diffusion within the flow field, the reaction at liquid-solid interfaces, and finally, the solid-state diffusion within a complex nanoporous medium. Here, this study employs the volumetric lattice Boltzmann method (VLBM) to accurately and efficiently calculate the steady state velocity field inside the mesopores of sorbent particles. The obtained velocity field is then utilized to calculate the advection of ions in the steady flow. A phase field (PF) model of ion uptake is used to describe the reaction occurring at the solid-liquid interface and diffusion inside the porous medium. The integrated PF-VLBM model is verified in terms of the mass conservation and numerical efficiency and validated qualitatively with experimental observation data. Then, it is applied to study the influence of thermodynamic and kinetic properties, as well as flow field conditions on the ion uptake kinetics. The numerical results demonstrate that the ion uptake kinetics in porous particles has three distinct stages, which is in agreement with the observations in continuous flow experiments. In the first stage, the kinetics is predominantly controlled by the flow field and ion diffusivity in the liquid phase. The kinetics in the second stage is primarily governed by ion diffusivity in the solid phase. In the third stage the system reaches a dynamic equilibrium with a net zero uptake flux at the interface. It is also found that porous structures significantly affect the efficiency and capacity of ion uptake. The simulation results can help to understand the physics behind the observed ion uptake kinetics in experiments and to facilitate the development of constitutive equations that can account for heterogeneous microstructures in engineering performance codes.

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Increasing the Fissile Mass Loading of High-Level Waste Glass Canisters to Greater Than 2,500 g/m 3 at the Savannah River Site

To eliminate future fissile mass loading constraints for the Savannah River Site H-Canyon Facility and Liquid Waste system, the Savannah River National Laboratory recommends a repository evaluation of a uranium fissile mass loading in glass at 7,144 g/m 3 in addition to the existing International Atomic Energy Agency safeguards and security limit of 2,500 g/m 3 total plutonium. This recommended increase above the authorized 2,500 g/m 3 fissile mass loading limit is based on concentrations of uranium and plutonium shown to produce an acceptable glass waste form rather than projections of the maximum fissile mass loading in future sludge batches. An authorized fissile mass loading limit greater than 2,500 g/m 3 will increase facility flexibility, reduce the number of high-level waste canisters produced, and potentially avoid an increase in the Department of Energy Environmental Management mission life without compromising safety or glass product quality.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Environmental, Health and Safety Assessment Application of a Heat Integrated, Post-combustion CO2 Capture System Using Monoethanolamine and Hitachi H3-1 Solvent at the E.W. Brown Coal-fired Power Plant

An Environmental Health and Safety (EH&S) Assessment was completed for operation of a pilot scale carbon dioxide (CO2) capture system (CCS) at the Louisville Gas & Electric (LG&E) and Kentucky Utilities (KU) Energy, LLC (LG&E-KU) E. W. Brown Generating Station in Harrodsburg, Mercer County, Kentucky. The pilot system was evaluated using two CO2 capture solvents, monoethanolamine (MEA) and Hitachi’s H3-1 solvent. The purpose of the EH&S Assessment was to determine if there were any unacceptable environmental, health or safety concerns that may prevent operation or environmental permitting of a larger scale pilot scale plant. The assessment included review of process flow diagrams, input and output flow rates for primary materials, literature describing similar processes and chemicals used or created during the process, actual air emission and wastewater test data and air emission calculations. The evaluation included identification of risks related to hazardous chemicals, air emissions, wastewater discharges, solid wastes generated and employee hazards. Most potential EH&S issues that were identified are commonly found and successfully managed at large industrial facilities. No risks were identified that could not be successfully managed or would likely prevent implementation or environmental permitting of the pilot or larger scale plant. Potential exposures and resulting health risks from exposure to low concentrations of nitrosamines generated from degradation of the Hitachi H3-1 and possibly MEA solvents may be a health concern for site workers, but additional investigation is needed to accurately assess this risk. Applying the information gained from operating the pilot plant, performing air emission testing and used solvent testing to a large-scale facility at a commercial coal-fired electric generating plant suggests additional air emission control measures may be necessary to reduce potential site worker health risks and possibly community risks. Depending upon the location and regional air quality, considerable effort may be required to obtain the necessary air permit for construction and operation of a similarly configured large-scale PCCCS facility.

gas separation↗

Utilization of Unmanned Aircraft Systems for Environmental Purposes at the Savannah River Site – 26578

Born in the 1950s, the Savannah River Plant was constructed as a plutonium and tritium production plant. As the Cold War era came and went, a change of direction was signaled when the name of the facility changed from Savannah River Plant to Savannah River Site (1989) – the main mission at Savannah River shifted from “production” to “cleanup.” The Department of Energy is responsible for managing the 310 square miles of land that is the Savannah River Site and the cleanup/remediation activities that occur. The Savannah River National Laboratory utilizes unmanned aircraft systems to assist with some of those environmental monitoring and remediation activities. One function of unmanned aircraft systems at the Savannah River National Laboratory is conducting aerial photography and videography. Various infrastructure evaluations have been performed with unmanned aircraft – facility rooftop inspections, water tower lock verifications, earthen dam surveys, etc. An unmanned aircraft system has been used for progress footage of remediation projects – Dunbarton Bay remediation, Saltstone Disposal Unit construction, etc. Thermal cameras on an unmanned aircraft system are used to help identify cracks/leaks in structures from vantage points not readily accessible by personnel. Virtual tours of different waste units are conducted with unmanned aircraft systems for Site groups and federal/state regulators to save costs and travel time. Additionally, advanced remote sensing technologies are used on unmanned aircraft systems at the Savannah River Site. Light Detection and Ranging uses laser pulses to measure distances to the Earth's surface or other targets to create highly detailed topographic maps that accurately portray terrain (e.g., elevation changes, slopes, and contours). Data collection with a Light Detection and Ranging unit mounted on an unmanned aircraft system is quick and efficient – large-area surveys are conducted in shorter time frames. Because Light Detection and Ranging can penetrate through foliage and vegetation to ground level, it is being used in conjunction with a watershed model to study the General Separations Area of the Site to determine stormwater flow volume and direction, monitor stream stability, and forecast river flow behavior. A hyperspectral camera captures a wide spectrum of electromagnetic wavelengths across numerous narrow bands, beyond what the human eye can see. It provides detailed spectral information about the objects or surfaces in an image, which can be used to identify and analyze materials based on their spectral signatures. A hyperspectral camera mounted on an unmanned aircraft system has been used at the Savannah River Site for non-destructive evaluation of concrete and concrete structures. Unmanned aircraft systems at the Savannah River Site are also used for the application of herbicide on identified rooftops. P-Reactor and R-Reactor are entombed nuclear reactors at the Savannah River Site. Unwanted vegetation is often present on these rooftops – over time roots can penetrate seams, cracks, and joints of the general roof and concrete caps, leading to water ingress and deterioration of the structural components. For time and cost efficiencies as well as in the interest of personnel safety, an unmanned aircraft is used to dispense herbicide on rooftop areas where vegetation is noticed to help alleviate the issues/hazards.

Lorier, Troy [Savannah River National Laboratory (↗

Panel Session 46: Final Closure of Unlined LLW Disposal Facilities Worldwide (R3.5)

This panel discussed the on-going and emerging issues with the design and construction of final cover system of unlined disposal facilities (e.g., material disposal areas (MDAs), subsurface disposal areas (SDAs), burial grounds, and similar historical waste trenches, pits and vaults). The discussion focused on key technical and regulatory issues as well as lessons learned from years of engineering and construction in US and non-US locations. Panelists with presentations: Closure of Unlined LLW Disposal Sites (Craig Benson); Closure of LLW Facilities (Paul Pointon); Final Closure of Unlined LLW Disposal Facilities - Lessons Learned (Kevin Foye)

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APS Science 2020 (Vol. 2)

The U.S. Department of Energy's Advanced Photn Source (APS) is one of the world’s most productive x-ray light source facilities. Each year, the APS provides high-brightness x-ray beams to a diverse community of more than 5,000 researchers in materials science, chemistry, condensed matter physics, the life and environmental sciences, and applied research. Researchers using the APS produce over 2,000 publications each year detailing impactful discoveries, and solve more vital biological protein structures than users of any other x-ray light source research facility. APS x-rays are ideally suited for explorations of materials and biological structures; elemental distribution; chemical, magnetic, electronic states; and a wide range of technologically important engineering systems from batteries to fuel injector sprays, all of which are the foundations of our nation’s economic, technological, and physical well-being. The APS occupies an 80-acre site on the Argonne campus, about 25 miles from downtown Chicago, Illinois. It shares a site with the Center for Nanoscale Materials and the Advanced Protein Characterization Facility.

01 COAL, LIGNITE, AND PEAT↗

Tris(isodecyl)guanidine Degradation in the MCU System

The current solvent blend consists of four components; an extractant, the modifier, a suppressor, and the diluent. Of the four components, only the suppressor – tris(isodecyl)guanidine (TiDG) has exhibited an appreciable depletion rate during facility operations. Using data derived from Modular Caustic-Side Solvent Extraction Unit (MCU) process samples, Savannah River National Lab (SRNL) derived a method to predict the TiDG depletion based upon time and volume of feed processed.

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Hot, Cold, or Just Right? Using a Wide-View Infrared Biometric Sensor to Improve Occupant Comfort and Reduce Overcooling in Buildings via Closed-loop Control (CRADA Final Report)

This research adds to the understanding of building energy management by fundamentally challenging the long-standing paradigm of controlling an environmental parameter—air temperature—and assuming occupant comfort will follow. The project developed and demonstrated a novel approach that directly senses physiological indicators of human comfort to enable closedloop, human-centric control of heating, ventilation, and air conditioning (HVAC) systems. This work shifts the focus from open-loop environmental control to a closed-loop system that prioritizes the occupants' actual thermal state. The primary benefit to the public is the potential for a simultaneous improvement in the quality of indoor environments, where people spend most of their time, and a significant reduction in national energy consumption. Overcooling, or the overuse of cooling energy in a way that discomforts occupants, wastes approximately 0.5 Quads of primary energy annually in U.S. commercial buildings and creates unproductive indoor environments.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Environmental, Health and Safety Assessment Application of a Heat Integrated, Post-combustion CO 2 Capture System Using Monoethanolamine and Hitachi H3-1 Solvent at the E.W. Brown Coal-Fired Power Plant

An Environmental Health and Safety (EH&S) Assessment was completed for operation of a pilot scale carbon dioxide (CO 2 ) capture system (CCS) at the Louisville Gas & Electric (LG&E) and Kentucky Utilities (KU) Energy, LLC (LG&E-KU) E. W. Brown Generating Station in Harrodsburg, Mercer County, Kentucky. The pilot system was evaluated using two CO 2 capture solvents, monoethanolamine (MEA) and Hitachi’s H3-1 solvent. The purpose of the EH&S Assessment was to determine if there were any unacceptable environmental, health or safety concerns that may prevent operation or environmental permitting of a larger scale pilot scale plant. The assessment included review of process flow diagrams, input and output flow rates for primary materials, literature describing similar processes and chemicals used or created during the process, actual air emission and wastewater test data and air emission calculations. The evaluation included identification of risks related to hazardous chemicals, air emissions, wastewater discharges, solid wastes generated and employee hazards. Most potential EH&S issues that were identified are commonly found and successfully managed at large industrial facilities. No risks were identified that could not be successfully managed or would likely prevent implementation or environmental permitting of the pilot or larger scale plant. Potential exposures and resulting health risks from exposure to low concentrations of nitrosamines generated from degradation of the Hitachi H3-1 and possibly MEA solvents may be a health concern for site workers, but additional investigation is needed to accurately assess this risk. Applying the information gained from operating the pilot plant, performing air emission testing and used solvent testing to a large-scale facility at a commercial coal-fired electric generating plant suggests additional air emission control measures may be necessary to reduce potential site worker health risks and possibly community risks. Depending upon the location and regional air quality, considerable effort may be required to obtain the necessary air permit for construction and operation of a similarly configured large-scale PCCCS facility.

gas separation↗

RANGERS: Modeling Report on Integrity and Performance Assessment of Engineered Barrier Systems in a Salt Repository for HLW/SNF

The Engineered Barrier System (EBS) plays an important role in ensuring the long-term safety and containment of high-level waste (HLW) and spent nuclear fuel (SNF) in deep geological repositories in salt formation. As part of a multi-barrier system, the EBS works alongside the natural barrier, which is the salt formation itself and the technical barrier comprising the disposal casks. The primary function of the EBS is to maintain containment during a defined period until the backfill used in the repository made of crushed salt, develops its sealing capacity through compaction. Over the time, the backfill eventually compacts to a state of low porosity and permeability, acting as a long-term seal. However, until this process is complete, the EBS must retain its structural and functional integrity. Regulatory guidelines in Germany currently require the EBS to remain effective for up to next ice age, that is expected in 50,000 years. The significant hydro-geological and topographic changes expected during an ice age could make it impossible to accurately predict the hydro-chemical conditions within the repository system at that time. In response to these challenges, BGE TECHNOLOGY GmbH (BGE TEC) and Sandia National Laboratories (SNL) have jointly developed a comprehensive methodology for the design and safety assessment of engineered barrier systems within the scope of the RANGERS project. This methodology is tailored for repositories in salt formations. The developed methodology provides a structured approach for designing and assessing the performance of the EBS in salt-based repositories. It begins with defining a sealing concept based on the geological characteristics of the selected site and the overall repository design. The entire repository system, comprising the geological site, repository infrastructure, and EBS, is then subjected to a Features, Events, and Processes (FEP) analysis, focusing solely on those FEPs that affect the EBS. The derived FEPs help identify the loads and stresses acting on the EBS, which serve as the foundation for conducting an integrity assessment. This analysis helps predict the EBS’s evolution and performance over the regulatory time frame, feeding into integrated performance assessment simulations.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Transient Coupled Chemical-Thermal-Fluid Field Simulation for Sealed Aluminum-clad Spent Nuclear Fuel Storage Canister

As the first step toward developing three-dimensional (3D) multi-physics computational fluid dynamics (CFD) model for unsealed and vented canister storage system, a 3D CFD model coupled with bulk gas radiolysis reactions was developed first for sealed DOE standard canisters filled with inert gas and trace amount of air and water. The workflow for constructing canister-scale 3D CFD models and coupling with gas phase radiolysis reactions were established, which can be readily extended to unsealed, vented canister storage system. This interim milestone report documents the theory of the model, workflow to establish radiolysis reaction network, and initial simulations of the evolutions of thermal fields and hydrogen gas concentrations within sealed DOE standard canisters over long period of time. In addition, a mesh refinement test was done to show that increasing the models mesh refinement had negligible impact upon the temperature profiles.

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Potential Advantages to Employing an Onsite Laboratory at FUSRAP Sites Contaminated with Radionuclides and Metals - 20353

Various factors that support an evaluation of the relative costs, advantages and disadvantages of utilizing an onsite laboratory or an offsite laboratory for remediation of Formerly Utilized Sites Remedial Action Program (FUSRAP) sites contaminated with radionuclides and metals are presented. In terms of how much more quickly an onsite laboratory provides results versus an offsite laboratory, the results of this study provide tools for calculating the amount of cost savings per day for excavation of contaminated soils for various scenarios including: - State, municipal or local property remediation where the remediation schedule becomes time-critical due to the extra cost and inconvenience to the town or municipality caused by the need for increased security and safety personnel, possible road closures and detours, and the inconvenience to the public due to modified or decreased services of State or municipal facilities; - Residential property where the remediation schedule becomes time-critical due to the inconvenience to the homeowner as well as the importance of maintaining good community relations; - Commercial property where the remediation schedule becomes time-critical due to the hardship and potential loss of revenue endured by the property owner; - Open area where treatment of excavation water is required, and - Open area where treatment of excavation water is not required. For every scenario, the number of matrices, radionuclide and metal contaminants of concern and the project duration are important factors. The costs for the onsite laboratory included the capital costs associated with setting up the lab such as trailer(s) or building(s), power and water hookup, analytical testing equipment, balances, computers, desks and bookcases; support equipment such as hot plates, filtration assemblies, safety equipment, ovens, etc.; and supplies such as glassware, pipettes, filters, etc. and ongoing costs such as labor, chemicals and reagents, standards, cost of the laboratory obtaining certification and maintenance. Offsite laboratory sample testing costs are generally very competitive and typically substantially lower than onsite laboratory costs if only the sample testing costs are considered. The great disadvantage of using an offsite laboratory is that they often cannot guarantee rapid turnaround times for results which creates project delays associated with the remediation process including delays determining the completeness of the characterization and remediation processes, delays in backfilling a property and additional costs for treating wastewater (excavation water, stormwater or both). These costs will vary greatly depending upon the area of the country in which the project is located due to the wide range of labor costs for the onsite laboratory and field workers, as well as the contaminants of interest, matrices and most importantly the size of the impacted area and the number of properties located in that area. This paper provides guidelines for calculating the cost savings that may be realized if an onsite laboratory can generate results more quickly than an offsite laboratory by estimating the costs associated with the remediation process for the various scenarios noted above such as work crew labor costs, excavator and dump truck equipment rentals, wastewater treatment costs (if applicable) and the additional costs incurred by homeowners, commercial property owners and towns/municipalities that are reimbursed by the potentially responsible parties. Key assumptions involve the typical quickest turnaround time provided by the onsite and offsite laboratories. Costs for the operation of a wastewater treatment system and the remediation of a site area or property were provided by personnel who have been involved in the operation of a large FUSRAP site in New Jersey for many years. This study provides valuable information for determining the most cost-effective approach for analysis of project samples and therefore may be used on upcoming FUSRAP projects. (authors)

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BCSR on GPU: A Way Forward Extreme-scale Graph Processing on Accelerator-enabled Frontier Supercomputer

Handling large graphs in a distributed environment requires effective partitioning across processors and efficient management of local partitions. In 2D partitioning, local graphs often become too sparse, making memory-efficient data structures crucial. Using the Compressed Sparse Row (CSR) format wastes space, especially for > 83% of vertices with empty edges for the sparse graphs. This study explores bit-CSR (BCSR), a modified CSR representation, on GPUs to reduce memory usage in graph computations. We achieved 16.67% memory savings on a sparse rmat dataset with 268 million vertices and 357 million edges, without performance degradation, supported by both theoretical and experimental storage savings of 33%. However, we observed a 1.7× slowdown in degree lookup times due to bitwise operations on AMD CPUs. This analysis highlights the potential of BCSR on GPUs for improving Graph500 benchmark performance on GPU-accelerated systems, such as the Frontier supercomputer.

Sattar, Naw Safrin↗

A Threshold Helium Leakage Detection Switch with Ultra Low Power Operation

Detecting helium leakage is important in many applications, such as in dry cask nuclear waste storage systems. This work develops a helium detection system based on the relative permittivity (dielectric constant) difference between air and helium. This difference changes the status of an electrostatic microelectromechanical system (MEMS) switch. The switch is a capacitive-based device and requires a very negligible amount of power. Exciting the switch’s electrical resonance enhances the MEMS switch sensitivity to detect low helium concentration. This work simulates two different MEMS switch configurations: a cantilever-based MEMS modeled as a single-degree-freedom model and a clamped-clamped beam MEMS molded using the COMSOL Multiphysics finite-element software. While both configurations demonstrate the switch’s simple operation concept, the clamped-clamped beam was selected for detailed parametric characterization due to its comprehensive modeling approach. The beam detects at least 5% helium concentration levels when excited at 3.8 MHz, near electrical resonance. The switch performance decreases at lower excitation frequencies or increases the circuit resistance. The MEMS sensor detection level was relatively immune to beam thickness and parasitic capacitance changes. However, higher parasitic capacitance increases the switch’s susceptibility to errors, fluctuations, and uncertainties.

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