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Humble, Paul H.

Publications and source records attributed to Humble, Paul H..

At least 19 records

Microchannel reactive distillation for the conversion of aqueous ethanol to ethylene

Here we demonstrate the proof-of-concept for microchannel reactive distillation for alcohol-to-jet application: combining ethanol/water separation and ethanol dehydration in one unit operation. Ethanol is first distilled into the vapor phase, converted to ethylene and water, and then the water co-product is condensed to shift the reaction equilibrium. Process intensification is achieved through rapid mass transfer—ethanol stripping from thin wicks using novel microchannel architectures—leading to lower residence time and improved separation efficiency. Energy savings are realized with integration of unit operations. For example, heat of condensing water can offset vaporizing ethanol. Furthermore, the dehydration reaction equilibrium shifts towards completion by immediate removal of the water byproduct upon formation while maintaining aqueous feedstock in the condensed phase. For aqueous ethanol feedstock (40% w ), 71% ethanol conversion with 91% selectivity to ethylene was demonstrated at 220 °C, 600 psig, and 0.28 h -1 wt hour space velocity. 2.7 stages of separation were also demonstrated, under these conditions, using a device length of 8.3 cm. This provides a height equivalent of a theoretical plate (HETP), a measure of separation efficiency, of ~3.3 cm. By comparison, conventional distillation packing provides an HETP of ~30 cm. Thus, 9.1× reduction in HETP was demonstrated over conventional technology, providing a means for significant energy savings and an example of process intensification. Finally, preliminary process economic analysis indicates that by using microchannel reactive distillation technology, the operating and capital costs for the ethanol separation and dehydration portion of an envisioned alcohol-to-jet process could be reduced by at least 35% and 55%, respectively, relative to the incumbent technology, provided future improvements to microchannel reactive distillation design and operability are made.

10 SYNTHETIC FUELS↗

Solar thermochemical processing system and method

A solar thermochemical processing system is disclosed. The system includes a first unit operation for receiving concentrated solar energy. Heat from the solar energy is used to drive the first unit operation. The first unit operation also receives a first set of reactants and produces a first set of products. A second unit operation receives the first set of products from the first unit operation and produces a second set of products. A third unit operation receives heat from the second unit operation to produce a portion of the first set of reactants.

Wegeng, Robert↗

Reactor assemblies and methods of performing reactions

Reactors are provided that can include a first set of fluid channels and a second set of fluid channels oriented in thermal contact with the first set of fluid channels. The reactor assemblies can also provide where the channels of either one or both of the first of the set of fluid channels are non-linear. Other implementations provide for at least one of the first set of fluid channels being in thermal contact with a plurality of other channels of the second set of fluid channels. Reactor assemblies are also provided that can include a first set of fluid channels defining at least one non-linear channel having a positive function, and a second set of fluid channels defining at least another non-linear channel having a negative function in relation to the positive function of the one non-linear channel of the first set of fluid channels. Processes for distributing energy across a reactor are provided. The processes can include transporting reactants via a first set of fluid channels to a second set of fluid channels, and thermally engaging at least one of the first set of fluid channels with at least two of the second set of fluid channels.

Zheng, Richard F.↗

Solar thermochemical processing system and method

A solar thermochemical processing system is disclosed. The system includes a first unit operation for receiving concentrated solar energy. Heat from the solar energy is used to drive the first unit operation. The first unit operation also receives a first set of reactants and produces a first set of products. A second unit operation receives the first set of products from the first unit operation and produces a second set of products. A third unit operation receives heat from the second unit operation to produce a portion of the first set of reactants.

Wegeng, Robert S.↗

Additively manufactured cryogenic microchannel distillation device for air separation

Abstract The efficiency of air separation is tested using three different small‐scale cryogenic distillation columns. The performance of a random packed column is compared to the performance of two microchannel distillation (MCD) columns that use thin wicking structures and gas flow channels to achieve process intensification. The MCD columns tested include a plate‐type layered column and an additively manufactured porous honeycomb (AMPH) column. For columns with 25.4 cm of active height and run under similar conditions, the packed, plate‐type layering, and AMPH columns achieved approximate height equivalent of a theoretical plate (HETP) values of 5.5, 3.7, and 3.2 cm for nitrogen, and 5.9, 4.9, and 3.3 cm for argon. The AMPH column can produce up to 0.4 SLM of more than 90% purity oxygen with 12 W of cooling lift. These results demonstrate the feasibility of using additive manufacturing to construct MCD devices and pave a way for constructing novel MCD designs.

36 MATERIALS SCIENCE↗

Manufacturing Supply Chain Development for Modular Solar-Thermochemical Conversion Platform - CRADA 387 (Final Report)

Modular chemical process intensification (MCPI) is an emerging field where chemical processing is performed using small-scale modular equipment instead of conventional large centralized chemical plants. Conventional chemical plants benefit from economies of scale that encourage scale-up to ever larger plants. A goal of MCPI is to develop technology that intensifies processing so that equipment can be dramatically smaller and integrated into modular systems. Scale-up occurs by adding more modules in parallel rather than making the equipment larger. A key concept is that equipment and modules can ultimately be cheaper by leveraging economies of mass production, analogous to the automotive industry, in manufacturing the equipment. This project made significant progress toward this outcome by meeting the RAPID institute metric to reduce equipment cost by 20% for each doubling in manufacturing volume. The MCPI application was thermochemical technology that is being commercialized by STARS Technology Corporation, one of the CRADA partners. The technology converts solar and renewable power to chemical energy to produce renewable hydrogen, fuels, and chemicals. The benefit to the public is reduction in greenhouse gases that are contributing to climate change. The project transitioned the steam methane reforming (SMR) reactor from conventional fabrication methods to additive manufacturing (AM) direct metal laser sintering (DMLS) process. This is projected to reduce the cost of making a reactor by 58% when producing 100 reactors per year. Innovations in the DMLS process produced a patented design that reduces reactor weight by 60%. Reductions in material costs and processing time extend the DMLS advantage to higher production volumes. The new design promises to be 38% cheaper than the conventional processes at 1000 units per year. The resulting 87% reduction in the steam methane reforming (SMR) module cost in scaling from current costs meets the RAPID metric. The project was successful in producing and testing the first ever additively manufactured SMR reactors. A reactor achieved over 82% efficiency in converting electric power to chemical energy, which is a world record for an inductively heated SMR. The project has contributed to the design and assembly of a first demonstration plant that is headed to a hydrogen bus filling station in Thousand Palms, CA.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Reactor assemblies and methods of performing reactions

Reactors are provided that can include a first set of fluid channels and a second set of fluid channels oriented in thermal contact with the first set of fluid channels where the channels of either one or both of the first of the set of fluid channels are non-linear. Reactor assemblies are also provided that can include a first set of fluid channels defining at least one non-linear channel having a positive function, and a second set of fluid channels defining at least another non-linear channel having a negative function in relation to the positive function of the one non-linear channel of the first set of fluid channels.

Zheng, Richard F.↗

Solar thermochemical processing system and method

A solar thermochemical processing system is disclosed. The system includes a first unit operation for receiving concentrated solar energy. Heat from the solar energy is used to drive the first unit operation. The first unit operation also receives a first set of reactants and produces a first set of products. A second unit operation receives the first set of products from the first unit operation and produces a second set of products. A third unit operation receives heat from the second unit operation to produce a portion of the first set of reactants.

Wegeng, Robert S.↗

High Throughput Argon-37 Field System

We report Pacific Northwest National Laboratory (PNNL) has developed a unique fieldable 37 Ar measurement system designed to measure 37 Ar activity concentrations from soil gas samples to detect above ground and underground nuclear explosions. The Argon-37 Field System is modular in design to accommodate both chemical processing and nuclear detection. The system can be packed into shipping crates and shipped to a location near where the sampling is taking place. The system can process six 2-m 3 whole-air samples in 24 hours and can measure the 37 Ar activity in each of the samples using six proportional counters. The proportional counters, designed and built at PNNL, are surrounded with both active and passive shielding to reduce background and can achieve a minimum detection concentration of 10 mBq/m 3 of 37 Ar in whole-air equivalent. The Argon-37 Field System has undergone extensive testing against rigorous requirements to assure the system meets the needs of the noble gas nuclear explosion monitoring community.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

An Ultra-microporous Metal-Organic Framework with Exceptional Xe Capacity

Molecular confinement plays a significant effect on trapped gas and solvent molecules. A fundamental understanding of gas adsorption within the porous confinement provides information necessary to design a material with improved selectivity. In this regard, metal organic frameworks (MOFs) adsorbents are ideal candidate materials to study confinement effects for weakly interacting gas molecules such as noble gases. Among the noble gases, Xenon (Xe) has practical applications in the medical, automotive and aerospace industries. In this communication, we report an ultra-microporous nickel-isonicotinate MOF with exceptional Xe uptake and selectivity compared to all benchmark MOF and porous organic cage materials. The selectivity arises because of the near perfect fit of the atomic Xe inside the porous confinement. Notably, at low partial pressure, the Ni-MOF interacts very strongly with Xe compared to the closely related Krypton gas (Kr) and more polarizable CO2. Further 129Xe NMR suggests a broad isotropic chemical shift due to the reduced motion as a result of confinement.

Confinement effects, atomically precise materials,↗

Iodine Effects on Medical Isotope Producer Delay & Guard Bed Temperature and Performance in Support of NA-23 Program

In support of NA-23’s objective to accelerate the establishment of a reliable commercial United States (U.S.) domestic supply of 99Mo produced without the use of highly enriched uranium (HEU), the Pacific Northwest National Laboratory (PNNL) was tasked with modeling the performance of activated carbon delay and guard beds that may be typical for non-HEU 99Mo production processes. The specific tasks accomplished by PNNL included calculations of long-term effects of iodine on delay bed performance and development of a finite element simulation to better understand delay bed performance under various scenarios specifically with radioxenon and radioiodine decay heating of the delay beds. The main issue of interest in this study is understanding the effect of iodine on the abatement performance of the beds if iodine is not sufficiently removed from gases prior to reaching the delay beds. Finite element simulations of delay bed performance were developed using COMSOL Multiphysics® Software. These simulations are based on partial differential equations that describe xenon and iodine adsorption, heat transfer and decay of radioxenon and radioiodine isotopes. Heat transfer in the activated carbon beds is simulated with a heat source tied to the decay of radioactive xenon and iodine species. These simulations were used to investigate delay bed temperature and hold up time using radioxenon and radioiodine activities and flowrates expected from a non-HEU production process. A bounding case scenario was simulated, where all the iodine was released into the delay beds due to insufficient guarding of the delay beds. In addition, preliminary investigations of the guard beds were conducted.

07 ISOTOPE AND RADIATION SOURCES↗

Xenon Abatement Simulations to Support the KAERI Medical Isotope Facility

To maintain and improve the verification regime that is outlined by the Preparatory Commission of the Comprehensive Nuclear Test-Ban Treaty there is a need to understand and reduce the radioxenon releases from medical isotope production facilities. In support of this objective Pacific Northwest National Laboratory (PNNL) was tasked with, modeling and evaluate the abatement process and delay bed designs for the medical isotope production facility under construction by the Korea Atomic Energy Research Institute (KAERI). This report includes this analysis and provides PNNL proposed modifications to the KAERI adsorption bed design.

07 ISOTOPE AND RADIATION SOURCES↗

Overview of 2016 through 2018 Testing of Air-Purifying Respirator (APR) Cartridge Performance on Multiple Hanford Tank Headspaces and Exhausters

Between 2016 and 2018, 28 air purifying respirator (APR) cartridge tests were performed on headspace vapors from seven Hanford waste storage tanks (SY-102, A-101, BY-108, AX-101, BY-110, SX-101, and SX-104) and seven waste tank exhausters (AP in 2016, AP in 2018, 702-AZ, AN and AW in 2016, and AX and 702-AZ in 2017). All but two tests were conducted under static conditions absent waste-disturbing activities in the subject tanks or tank farms. The two exceptions were cartridges tested with vapors from 702-AZ in 2017 when samples were taken during waste-disturbing activities. Multipurpose APR cartridges, SCOTT 7422-SD1 and 7422-SC1, were tested on samples from each of the 14 tanks or exhausters. Out of 612 Chemicals of Potential Concern (COPCs), only ammonia, mercury, N-nitrosodimethylamine (NDMA), 2,5-dimethylfuran, 2,5-dihydrofuran, furan, and 1,3-butadiene exhibited breakthroughs with outlet concentrations that were >10% of their Occupational Exposure Limits (OEL).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Effective field theory interactions for liquid argon target in DarkSide-50 experiment

We reanalize data collected with the DarkSide-50 experiment and recently used to set limits on the spin-independent interaction rate of weakly interacting massive particles (WIMPs) on argon nuclei with an effective field theory framework. The dataset corresponds to a total (16660 ± 270) kg d exposure using a target of low-radioactivity argon extracted from underground sources. We obtain upper limits on the effective couplings of the 12 leading operators in the nonrelativistic systematic expansion. For each effective coupling we set constraints on WIMP-nucleon cross sections, setting upper limits between 2.4×10-45 cm2 and 2.3×10-42 cm2 (8.9 ×10-45 cm2 and 6.0 ×10-42 cm2) for WIMPs of mass of 100 GeV/c2 (1000 GeV/c2) at 90% confidence level.

Agnes, P↗

Measurement of the ion fraction and mobility of 218Po produced in 222Rn decays in liquid argon

We report measurements of the charged daughter fraction of 218Po as a result of the 222Rn alpha decay, and the mobility of 218Po+ ions, using radon-polonium coincidences from the 238U chain identified in 532 live-days of DarkSide-50 WIMP-search data. The fraction of 218Po that is charged is found to be 0.37 ± 0.03 and the mobility of 218Po+ is (8.6 ± 0.1) × 10-4 cm2/Vs.

Agnes, P↗

Migration of noble gas tracers at the site of an underground nuclear explosion at the Nevada National Security Site

As part of an underground gas migration study, two radioactive noble gases and two stable tracer gases were injected into a nuclear explosion test chimney and allowed to migrate naturally. Soil gas samples were collected from a series of boreholes and a range of depths from the shallow subsurface (3 meters) to deeper levels (~160 meters) over a period of eleven months. These samples have provided insights into the development and evolution of the subsurface plume and constrained the relative migration rates of the radioactive and stable gas species. Analysis of the samples concluded that the stable tracer SF6 was consistently enriched in the subsurface samples relative to the radiotracer 127Xe, but the ratios of SF6 and 37Ar remained similar throughout the samples.

Johnson, Christine M.↗