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Engineering topics

Greenhalgh, Mitchell

Publications and source records attributed to Greenhalgh, Mitchell.

At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Krypton Concentration using HZ-PAN

Idaho National Laboratory (INL) has developed and tested engineered sorbents to separate and capture volatile fission products such iodine, xenon (Xe), and krypton (Kr) from off-gas streams. As noble gases, Xe and Kr can be difficult to capture and separate. Historically, cryogenic distillation has been used to execute the separation. However, performing this separation from bulk air streams is expensive and can pose significant hazards. INL has successfully developed two different sorbents for Xe and Kr capture, silver mordenite polyacrylonitrile and hydrogen mordenite polyacrylonitrile (HZ-PAN). Adsorption studies to date successfully separated and captured Kr from carrier gas streams, but those studies focused primarily on initial separation and capture. Successful utilization in a used nuclear fuel (UNF) reprocessing facility, however, requires further concentration of the Kr to minimize long term storage volumes. This study focuses on the concentration of Kr utilizing HZ PAN as the concentrating media. Concentrating Kr during desorption is ideal for two reasons: one, to produce Kr that can be used for commercial and research applications, or two, to minimize the volume of the radioactive gaseous waste stream for disposal. This report investigates the Kr concentrating potential of HZ-PAN by running multiple Kr adsorption-desorption cycles, collecting the desorbed effluent from a saturated HZ-PAN column, and loading it onto a fresh column. This study demonstrates that four adsorption-desorption cycles can transform a 150 ppmv Kr stream into a 37.5% Kr stream, an overall concentration factor of 2497. Each concentration step results in successively smaller volumes desorbed, reducing volume by a factor of approximately 40,000. Depending on the operational goals, during desorption one could collect smaller volume fractions of high concentration Kr (~ 67%). This demonstration should be considered proof-of-concept. Further refinement is necessary to develop optimum operating schemes to integrate into UNF off-gas treatment.

12 - MGMT OF RADIOACTIVE AND NON-RADIOACTIVE WASTE↗
DOE OSTI2022

Novel Diglycolamide Extractant?s Performance in Liquid-Liquid Separations for Pilot Scale Application

Modified diglycolamide (DGA) extractants show high affinity for light lanthanides and improved separation factors compared to phosphonic acids used commercially. Previous studies with DGAs included flowsheet design and implementation into solvent extraction equipment but with low extractant concentration. Modifications on the alkyl chains of previous DGA extractants led to a competitive product for light rare earth separation with a higher extractant concentration. The scope of this project is to test a recently developed DGA extractant for application in pilot scale solvent extraction equipment with single stage testing, by narrowing down scrubbing conditions, and collecting distribution values for flowsheet planning.

42 ENGINEERING↗
DOE OSTI2022

Idea to Deliverable: The Engineering Design Process

The engineering design process is utilized to evolve an idea into a deliverable. This progression can take years, so to experience as much of the full design process as possible, this internship period was dedicated to working on several projects in different phases of the process. The result is a completed engineering project which provides a foundation that can be used to conduct research on a system by performing experiments, collecting data, and making changes as necessary to improve the system and answer new questions.

42 ENGINEERING↗
DOE OSTI2022

Use of Machine Learning for Signature Development in a Multi-Sensor Environment for Safeguard Applications of Solvent Extraction Processes

Idaho National Laboratory is constructing the Special Nuclear Material test bed (Beartooth) for research and development pertaining to nuclear fuel processing operations using centrifugal contactors. Beartooth will enable give researchers the opportunity to study the dissolution, separation, and conversion of special nuclear materials (e.g., plutonium, enriched uranium, and thorium). As a lead-in to Beartooth, this project constructed a test bed to study the process and equipment behavior with real time series data collection using a variety of non-traditional sensors, in order to identify process failures and label them as either accidental or purposeful, thus enhancing nuclear nonproliferation stewardship. The measurement sources in this test bed include vibration, acoustic, current, flow, colorimetric, and thermal data. These measurements vary in terms of magnitude, frequency, and location. This information will be combined and used within data-driven machine-learning methods to detect operation condition changes that are either intentional (i.e., changes in operating set points) or malicious (i.e., flow diversion) in nature. This presentation covers the data processing and signature development activities necessary for utilizing this heterogeneous dataset to classify process anomalies.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2022

An Overview in the Development of a Multi-Sensor Data Science System for Monitoring a Solvent Extraction Process

To enhance nuclear nonproliferation stewardship, Idaho National Laboratory is building the Beartooth nuclear fuel cycle processing test bed. The Beartooth test bed will allow researchers the opportunity to study nuclear fuel processing operations including the use of centrifugal contactors in solvent extraction processes. The test bed is designed to support data collection and machine learning to monitor process operations. As part of this project, researchers will study data collected from a host of sensors that have not been typically used to monitor solvent extraction processes such as vibration, acoustic, colormetric, and thermal measurement data. The goal of this research is to employ machine learning and data analytics to study the confluence of signals collected from both traditionally and non-traditionally used sensors to provide operator process awareness and discover process anomalies. An overview of planned sensors and experiments that will focus on signal discovery will be presented.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

An Overview in the Development of a Multi-Sensor Data Science System for Monitoring a Solvent Extraction Process

To enhance nuclear nonproliferation stewardship, Idaho National Laboratory is building the Beartooth nuclear fuel cycle processing test bed. The Beartooth test bed will allow researchers the opportunity to study nuclear fuel processing operations including the use of centrifugal contactors in solvent extraction processes. The test bed is designed to support data collection and machine learning to monitor process operations. As part of this project, researchers will study data collected from a host of sensors that have not been typically used to monitor solvent extraction processes such as vibration, acoustic, colormetric, and thermal measurement data. The goal of this research is to employ machine learning and data analytics to study the confluence of signals collected from both traditionally and non-traditionally used sensors to provide operator process awareness and discover process anomalies. An overview of planned sensors and experiments that will focus on signal discovery will be presented.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

MRWFD Kr Capture Project

Progress report presentation to DOE program representatives.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2022

Use of Novel Diglycolamide Extractants in Liquid-liquid Separations of Light Rare Earths

Creation of a novel extractant that can improve rare earth separations both economically and environmentally will be pivotal for industry progression. Diglycolamide (DGA) extractants provide chemistries that support this goal by serving as an extractant with high affinity for lanthanides and improved separation factors for light rare earths as compared to current extractants like PC88A. Initial organic phase loading capacity and phase dispersion tests performed with various modified DGAs generated results that were unfavorable for industrial processing, but further modification of the DGA alkyl chain substituents have resulted in new structures with promising results. Dispersion time measurements taken in small scale batch contacts of the extractant with a simulated leach liquor containing La, Ce, Nd, and Pr support implementation in both mixer-settlers and centrifugal contactors for larger scale separations. Furthermore, this confirmation allowed for preliminary flowsheet design using extraction equilibria at various organic to aqueous flow ratios (O/A) for extraction, scrubbing, and stripping stages. These values along with expected product/effluent compositions for each section aid in the testing for specific distribution ratios and final flowsheet design. Implementation of the DGA extractant into solvent extraction equipment will provide essential information for the next steps of this project and how this extractant may be optimized for future applications.

42 ENGINEERING↗
DOE OSTI2020

Evaluation of Engineered Form MOFs CaSDB and HKUST-1

Idaho National Laboratory (INL) and Pacific Northwest National Laboratory (PNNL) have studied different sorbents for the purpose of separating krypton (Kr) and xenon (Xe). PNNL has researched various metal-organic frameworks (MOFs) that have characteristics theoretically suitable for the separation. Based on computational analysis, PNNL chose Calcium–4,4’–sulfonyl dibenzoate (CaSDB) and Hong Kong University of Science and Technology MOF1 (HKUST–1). The raw MOFs are supplied in a powder form and must be incorporated into a robust engineered form to be viable for gas separation. In 2016, PNNL produced an engineered form of CaSDB by compressing and grinding the raw MOF material. This form was sent to INL for adsorption testing. Gentle mechanical agitation of the compressed form produced a large amount of powder, resulting in the conclusion that the form was not viable for the application. In 2019, INL successfully produced two engineered forms, CaSDB–EF1 and HKUST–EF2, by incorporating the active MOF powders into a polyacrylonitrile (PAN) binder. PNNL also produced two engineered forms, CaSDB–10pmma and HKUST–10pmma, by using polymethyl methacrylate (PMMA) as a binder. Surface area analysis indicated that the forms could be viable for separations in which the CaSDB–EF1 retained 84% of the raw CaSDB surface area and CaSDB–10pmma retained 48%. HKUST–EF2 retained all the raw HKUST–1 surface area, whereas HKUST–10pmma retained only 28%. Mechanical stability testing demonstrated that the PMMA forms formed a fine powder whereas, the PAN forms did not. In general, adsorption testing showed that CaSDB–10pmma had a lower Xe breakthrough capacity than CaSDB–EF1, but a higher saturation capacity at both room temperature and at 253 K. The CaSDB MOF was intended to be used as a room temperature sorbent to capture Xe. However, both CaSDB engineered forms displayed relatively short initial break through times. Reduced temperature increased the Xe capacity of both engineered forms. HKUST–1 was expected to be effective only at sub-zero temperatures. At 195 K, HKUST–10pmma had an initial Xe breakthrough capacity of 119 mmol/ kg, compared to HKUST–EF2 at 339 mmol/ kg. The saturation capacities were 275 and 383 mmol/ kg, respectively. HKUST–10ppm also had a lower Kr capacity of 1.7 mmol/kg, whereas the HKUST–EF had a Kr capacity of 3 mmol/ kg. Test results indicate that the PAN engineered forms are a more suitable choice for the complete separation of Xe and Kr, due to the increase in initial breakthrough capacity. CaSDB allows rapid breakthrough of Kr and Xe regardless of the type of engineered form. At 253 K, it is more viable, but is still not the most effective sorbent. HKUST–EF2 demonstrated viability for Xe capture at 195 K, which may merit further study, however it may be cost prohibitive.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Summary of GAIN BWR Off-Gas Study: Effect of Charcoal on Kr and Xe Delay

This is a summary of a more extensive report, written in collaboration with the GE-Hitachi BWR Owner's Group, detailing a study of BWR off-gas treatment. The study determined that aged charcoal continues to be effective for the delay of Kr and Xe through BWR off-gas treatment systems. It demonstrates the over-sized nature of existing charcoal beds, and highlights potential areas of improvement.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗
DOE OSTI2019

Separation of Xenon from Krypton in UNF Reprocessing Off-Gas

Reprocessing of used nuclear fuel (UNF) results emits several volatile radionuclides that must be removed from the bulk off gas prior to release in order to meet U.S. regulatory emission requirements. After other volatile radionuclides have been removed, krypton (Kr) remains, along with associated with xenon (Xe) in the gas stream. The half-life of Xe is short enough that by the time UNF is sufficiently cooled to be reprocessed Xe is no longer a radiological concern and it may be release to atmosphere or collected for other purposes. Kr, however, must be placed in long term storage. In order to ensure the smallest practical volume for long term storage, the Xe, which is nearly ten times the volume of Kr, must be separated from the Kr. Although cryogenic distillation has been used successfully for this purpose, high capital and operational cost, along with safety considerations, made development of gas adsorption processes for separation of Xe and Kr attractive. INL developed an engineered form sorbent consisting of silver mordenite in a polyacrylonitrile matrix (AgZ-PAN) capable of complete separation of Xe from Kr in a single pass, allowing Kr to be captured downstream with no detectable Xe present.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2019

Developing an Engineered Form of MOFs CaSDB and HKUST –1

Selective Kr and Xe capture to various adsorbents have been studied extensively as part of the Off-gas Sigma Team. In hopes to develop a better adsorbent, Pacific Northwest Nation Laboratory (PNNL) has suggested the use of metal-organic frameworks (MOFs). In 2016, PNNL developed compressed and ground engineered forms of calcium–4,4’–sulfonyl dibenzoate (CaSDB) MOF which was tested at Idaho National Laboratory (INL). The tests found that the CaSDB had a sufficient saturation capacity, but a low breakthrough capacity. The larger issue was that the CaSDB form was not robust enough to withstand handling necessary for installation in a column and flow system. In 2018, PNNL sent two MOFs, CaSDB and Hong Kong University of Science and Technology – 1 (HKUST–1), to INL. INL’s goal was to develop an engineered form that maintained adsorption properties comparable to the original MOFs and was robust enough to use in a column. Initial testing consisted of batch-wise contacts of the MOFs with aprotic solvents and water, to ensure there was not a dramatic degradation of the material. BET analyses confirmed that the MOFs could be exposed to water and DMSO without significant loses in surface area. MOF engineered forms were successfully produced, CaSDB–EF1 and HKUST–EF2, using the INL-patented PAN technique (USA Patent No. 8,686,083, 2013). Brunauer, Emmet and Teller (BET) analyses performed on the engineered forms yielded surface areas of 148 m 2 /g and 1487 m 2 /g for CaSDB–EF1 and HKUST–EF2 respectively, 67.6% and 83.7% of the surface areas of the respective pristine materials. Both engineered form MOFs are deemed acceptable for further study to determine efficacy for selective Kr and Xe capture.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2018

HZ-PAN and AgZ-PAN Desorption Characterization

While previous research focused on adsorption of Kr and Xe on HZ-PAN and AgZ-PAN, recent focus has shifted to desorption. Preliminary testing was completed last year, providing valuable information to guild further research. Preliminary studies indicated that thermal swing operations, along with a sweep gas, are required for effective desorption from both AgZ-PAN and HZ-PAN. This series of tests focused on characterizing the bulk gases removed from each sorbent and relative separation of Kr and Xe from each other and from the bulk air. Single stage adsorption/ resulted in 99-100% separation of Xe from Kr, and 77-83% separation of Kr from air while concentrating Xe seven to tenfold and Kr three to fivefold when Xe is not present. Previous isothermal studies of both sorbents have shown that sorbent capacity is proportional to feed gas concentration. Therefore, it is anticipated that additional HZ-PAN stages will further concentrate and purify the final Kr stream with higher efficiency. It is expected that Xe will be released to atmosphere after desorption. However, it could also be purified further with more AgZ-PAN stages. Further testing should be done to determine maximum purity achievable for both Kr and Xe. Additionally, renewed focus on increasing Xe capacity on AgZ-PAN and Kr capacity on HZ-PAN is recommended.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2018

Cycle Testing of AgZ-PAN and HZ-PAN

Idaho National Laboratory (INL) has been conducting, as part of the off-Gas Sigma Team, producing and testing sorbents for the selective capture of xenon and krypton from surrogate nuclear fuel recycling off-gas streams. AgZ-PAN and HZ-PAN, both developed and produced at INL, have shown promising results for the selective capture and separation of xenon and krypton, respectively. Previous testing of both sorbents has focused on saturation and initial breakthrough capacities across a variety of operating conditions. However, the sorbents can only be truly viable for use in a process if they have sufficient longevity through multiple adsorption/desorption cycles. This research, therefore, focused on putting both sorbents through as many thermal swing adsorption/desorption cycles as possible over the course of one year. The primary focus of cycling tests was on AgZ-PAN, which previously demonstrated possible loss of capacity after multiple cycles. While capacity was shown to be recoverable over the short term, the goal is to ensure effective long-term viability so it was placed through 100 cycles, the estimated equivalent of one year of operation. HZ-PAN had not shown any deleterious effects from cycling during previous testing. Additionally, due to the colder temperatures required for Kr capture, each cycle required considerably more time to complete, so this sorbent was subjected to 50 cycles. Both sorbents maintained their capacities throughout the series, indicating promising potential for long-term reliability.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2018

Initial Evaluation of CaSDB MOF Xe and Kr Capacities

Idaho National Laboratory (INL) and Pacific Northwest National Laboratory (PNNL) have been conducting parallel research, as part of the off-Gas Sigma Team, producing and testing sorbents for the selective capture of xenon and krypton from surrogate nuclear fuel reprocessing off-gas streams. Sorbents promising on a laboratory scale are tested further at INL in a system designed to emulate anticipated plant process conditions. This report summarizes INL’s initial testing of CaSDB MOF developed and produced at PNNL. Previous testing of the same base CaSDB MOF material, conducted at INL in 2016, indicated good saturation capacity for xenon, but a low xenon capacity at initial breakthrough. Additionally, the material displayed a propensity to break down into fine powder during use and handling. The current test series looks at the same base material, but with refinements to production and activation techniques. A series of ambient temperature tests were conducted to determine capacities of CaSDB MOF for krypton and xenon at initial breakthrough as well as at saturation. Adsorption tests were run in triplicate at superficial velocities of 21 and 53 cm/min, along with a single test at 373 cm/min. Saturation capacity across all tests was 30 mmol/kg +/- 2, with capacity at initial breakthrough of 8 mmol/kg +/- 1. It should be noted that while the usable portion of the material has a much tighter size distribution than that previously tested, propensity to physically break down into very fine powder with use and handling continues to be problematic. An improved engineered form is recommended prior to further testing

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2017

Preliminary Desorption studies for HZ-PAN and AgZ-PAN

Adsorption of Kr and Xe on HZ-PAN and AgZ-PAN has been the studied extensively. Prior research focused on sorbent capacity and breakthrough of Kr and Xe, with desorption cycles completed in order to close material balances and prepare sorbents for further adsorption testing. This series of tests was designed to determine preliminary information about desorption to guide further research to optimize desorption cycles for each sorbent. A series of desorption tests were run using thermal and pressure swing operations. For AgZ-PAN, these tests indicated that both heat and carrier gas are likely necessary to removed adsorbed gases. However, vacuum pressure and heat may be sufficient to desorb gases from HZ-PAN, which should result in a cleaner Kr stream during desorption. Desorption optimization for both sorbents merits further study in order to make final waste form volume as small as possible.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗