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All sourcesNASA NTRSDOE OSTI
DOE OSTI2013

Training and Mentoring the Next Generation of Scientists and Engineers to Secure Continuity and Successes of the US DOE's Environmental Remediation Efforts - 13387

The DOE Office of Environmental Management (DOE-EM) oversees one of the largest and most technically challenging cleanup programs in the world. The mission of DOE-EM is to complete the safe cleanup of the environmental legacy from five decades of nuclear weapons development and government-sponsored nuclear energy research. Since 1995, Florida International University's Applied Research Center (FIU-ARC) has supported the DOE-EM mission and provided unique research capabilities to address some of these highly technical and difficult challenges. This partnership has allowed FIU-ARC to create a unique infrastructure that is critical for the training and mentoring of science, technology, engineering, and math (STEM) students and has exposed many STEM students to 'hands-on' DOE-EM applied research, supervised by the scientists and engineers at ARC. As a result of this successful partnership between DOE and FIU, DOE requested FIU-ARC to create the DOE-FIU Science and Technology Workforce Development Initiative in 2007. This innovative program was established to create a 'pipeline' of minority STEM students trained and mentored to enter DOE's environmental cleanup workforce. The program was designed to help address DOE's future workforce needs by partnering with academic, government and private companies (DOE contractors) to mentor future minority scientists and engineers in the research, development, and deployment of new technologies and processes addressing DOE's environmental cleanup challenges. Since its inception in 2007, the program has trained and mentored 78 FIU STEM minority students. Although, the program has been in existence for only five years, a total of 75 internships have been conducted at DOE National Laboratories, DOE sites, DOE Headquarters and field offices, and DOE contractors. Over 85 DOE Fellows have participated in the Waste Management Symposia since 2008 with a total of 68 student posters and 7 oral presentations given at WM. The DOE Fellows participation at WM has resulted in three Best Student Poster Awards (WM09, WM10, and WM11) and one Best Professional Poster Award (WM09). DOE Fellows have also presented their research at ANS DD and R and ANS Robotics Topical meetings. Moreover, several of our DOE Fellows have already obtained employment with DOE-EM, other federal agencies, DOE contractors. This paper will discuss how DOE Fellows program is training and mentoring FIU STEM students in Department of Energy's Office of Environmental Management technical challenges and research. This training and mentoring has resulted in the development of well trained and polished young scientists and engineers that will become the future workforce in charge of carrying on DOE-EM's environmental cleanup mission. The paper will showcase FIU's DOE Fellows model and highlight some of the applied research the DOE Fellows have conducted at FIU's Applied Research Center and across the Complex by participating in summer internship assignments. This paper will also present and highlight other Fellowships and internships programs sponsored by National Nuclear Security Agency (NNSA), DOE-EM, NRC, Energy (NE), and other federal agencies targeting workforce development. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2021

Gas-phase stability of large lanthanide:diglycolamide clusters evaluated using collision-induced dissociation

Efficient utilization of long-term deep geologic storage repositories is critical for the large-scale deployment of nuclear energy. As the minor actinides (americium and curium) are the largest contributor to the decay heat of used nuclear fuel after a few hundred years, their removal from used fuel prior to disposal can significantly increase the amount of waste that can be stored in a given volume. The development of ligands that can effectively separate the minor actinides from other components of used nuclear fuel are crucial to efficient utilization of geological storage repositories. N,N,N’,N’-tetraoctyl diglycolamide (TODGA) is a promising extractant for the separation of lanthanides and the minor actinides from other components of used nuclear fuel. While the use of TODGA in f-element separations has been investigated in process-based formulations, gas-phase metal ion cluster experiments enable the study of covalent interactions in reprocessing systems absent from solvent effects. Exploring fundamental differences in lanthanide-ligand covalent interactions can impact the development and implementation of actinide-lanthanide separation systems in nuclear fuels reprocessing. In this study, lanthanide-TODGA clusters were synthesized in the gas-phase and identified using mass spectrometry fragmentation experiments. Large europium and samarium clusters were identified that contained up to 8 and 10 bound TODGA ligands, respectively; this was surprising due to the size and multidentate binding that is normal for TODGA. In addition, while smaller clusters showed evidence of sequential ligand fragmentation, larger clusters displayed the loss of neutral TODGA with applied collision voltage. Interestingly, the voltage required for this removal decreased as more TODGA ligands were bound to the metal, suggesting that the metal coordination sphere was becoming more saturated and TODGA ligands were more weakly bound as the clusters got larger.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Partnership for Radiation Studies (PaRS): A Consortium for Advancing Radiation Science among Underrepresented STEM Students

The Partnership for Radiation Studies (PaRS) consortium was recently awarded by U.S. Department of Energy’s National Nuclear Security Administration (NNSA). The five-year grant aims to increase the number of underrepresented students in STEM disciplines, with simultaneous advancement of nuclear radiation science. The goal is to hire more underrepresented minorities at national laboratories. The consortium’s progress will be tracked/reported annually. This paper and subsequent presentation cover details of the consortium, highlighting the key activities of participating national laboratories in assisting the minority-serving institutions.

Minority Serving Institutions Partnership Program,↗
DOE OSTI2020

Growth and Characterization of Arsenic-Doped CdTe 1-x Se x Single Crystals Grown by the Cd-Solvent Traveling Heater Method

The photovoltaic performance of CdTe solar cells is mainly limited by low doping and short minority carrier lifetime. Group-V element doping and Se-alloying have a significant impact on tuning these fundamental CdTe properties. In this paper, we report the growth of p-type As-doped, Cd-rich CdTe 1-x Se x single crystals using metallic Cd as the solvent in the traveling-heater method. The structural and electrical properties of CdTe1-xSex are examined for different Se concentrations. CdTe 1-x Se x single crystals (0 ≤ x ≤ 0.5) with zincblende structure indicate homogeneous composition. The 10 17 cm-3 As-doping activation efficiency can be maintained at close to 50% for x ≤ 0.2. Se alloying leads to bulk minority carrier lifetime exceeding 30 ns for samples doped near 1017 cm -3 . These results help us to overcome the current roadblocks in device performance.

14 SOLAR ENERGY↗
DOE OSTI2017

The laboratory environmental algae pond simulator (LEAPS) photobioreactor: Validation using outdoor pond cultures of Chlorella sorokiniana and Nannochloropsis salina

A bench-scale photobioreactor system, the Laboratory Environmental Algae Pond Simulator (LEAPS), was designed and constructed to simulate outdoor pond cultivation for a wide range of geographical locations and seasons. The LEAPS consists of six well-mixed glass column photobioreactors submerged in a temperature controlled waterbath (-2 °C to >60 °C) and illuminated from above by a programmable multicolor LED lighting system (0 to 2,500 µmol/m 2 -sec). Measured incident light intensities and water temperatures deviated from the respective light and temperature setpoints on average only 2.3% and 0.9%, demonstrating accurate simulation of light and temperature conditions measured in outdoor ponds. In order to determine whether microalgae strains cultured in the LEAPS exhibit the same linear phase biomass productivity as in outdoor ponds, Chlorella sorokiniana and Nannochloropsis salina were cultured in the LEAPS bioreactors using light and temperature scripts measured previously in the respective outdoor pond studies. For Chlorella sorokiniana, the summer season biomass productivity in the LEAPS was 6.6% and 11.3% lower than in the respective outdoor ponds in Rimrock, Arizona, and Delhi, California; however, these differences were not statistically significant. For Nannochloropsis salina, the winter season biomass productivity in the LEAPS was 9.2% higher than in the respective outdoor ponds in Tucson, Arizona, a difference shown to be not statistically significant. Potential reasons for the positive or negative divergence in LEAPS performance, relative to outdoor ponds, are discussed. To demonstrate the utility of the LEAPS in predicting productivity, two other strains – Scenedesmus obliquus and Stichococcus minor – were evaluated using the summer season script for Rimrock, Arizona. For both strains, the productivity was around 11.6 g/m 2 -day at 25 cm culture depth. In conclusion, the LEAPS is an accurate pond simulator and thus offers a reliable, fast, and cost-effective way to screen microalgae strains and operating conditions for high biomass productivity and co-product yields.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2018

Decreasing trend in passive tobacco smoke exposure and association with asthma in U.S. children

Highlights: • Passive smoke exposure among US children ages 3–11 is decreasing during 2003–2014. • Decreasing trend is more pronounced among children without household smokers. • Children in the higher exposure tertile are still associated with higher odds of asthma. • Minority groups are more likely to be in the higher exposure tertile. In this study, we assessed trends of serum cotinine levels over time among US children ages 3–11 years and compared the risk of asthma in groups exposed to passive tobacco smoke. We utilized National Health and Nutrition Examination Survey (NHANES) data collected from 2003 to 2014 (n = 8064). Serum cotinine level, household smoker status, asthma status, and sociodemographic information were extracted for multiple regression analyses. The adjusted biannual change in log (cotinine) in comparison to earlier NHANES survey cycles was − 0.196 (p < 0.001) overall, − 0.055 (p = 0.089) among children with household smoker(s), and − 0.129 (p < 0.001) among children without. The proportion of children living with household smokers decreased from 24.9% in the 2003–2004 cycle to 11.4% in the 2013–2014 cycle. The adjusted odds ratios (ORs) for asthma were 1.34 (95% confidence interval (CI): 1.00–1.80; 2nd tertile vs 1st tertile) and 1.69 (95%CI: 1.25–2.29; 3rd tertile vs1st tertile), respectively. Highly exposed asthmatic children, in the 3rd cotinine tertile (>0.13 ng/mL), were primarily Non-Hispanic Black (61.0%) and whose family incomes were below poverty guidelines. Overall results reveal passive smoke exposure level among children ages 3–11 in the US decreased over the study period. Nevertheless, higher exposure to passive smoke is still associated with higher odds of childhood asthma. Targeted smoking cessation interventions in clinical practices are needed to reduce tobacco smoke exposure and related asthma risk in children, particularly in low-income and minority groups.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Irradiation performance of nonfertile (Pu-MA-Zr) fast reactor metal fuels

This work was part of a program begun in 2001 to develop advanced nuclear fuels, originally as carriers for plutonium and minor actinides (neptunium, curium, and americium) taken from spent commercial light-water reactors (LWR) so that the plutonium and minor actinides could be ‘burned’ or transmuted in an accelerator or a fast nuclear reactor. A central part of these experiment programs has been the development of advanced fast reactor fuels, because a fast reactor was considered the most efficient vehicle to transmute the actinide waste products, and metallic fuels is a central focus of these tests. An experiment design was developed in which a thermal test reactor, the Advanced Test Reactor (ATR), was used to test small fuel pin prototypes, by creating areas in the core shielded by cadmium filters to produce a largely epithermal and fast neutron spectrum environment in which the pins could be irradiated. The results of non-fertile metallic fuel (no uranium) tests are presented here. Pu-Am-Np-Zr fuels were irradiated to fission densities up to 33 × 10 20 fission/cm 3 and Pu-239 depletions of up to 39%. The depletions were created by roughly 2/3 by fission and 1/3 by transmutation neutron capture. Up to five fuel ‘rodlets’ were irradiated in three sealed capsules stacked axially in the core, and the peak cladding temperatures ranged from 300°C to 500°C, depending on axial location as those near the core centerline are operating hotter and to higher fission densities. Several post-irradiation examinations (precision gamma scanning and fission gas release) were similar to other historical metal fuel experiments in fast reactors. However, optical metallography indicated that two of the rodlets had breached. The exact reasons are unclear. Due to the design of this irradiation experiment a rodlet breach could have increased the temperature in others in the same capsule by contaminating the thermal gap helium with heavier and less conductive fission product gases. Finally, some of those rodlets showed high amounts of fuel/cladding chemical interaction (FCCI).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2019

A review of separation processes proposed for advanced fuel cycles based on technology readiness level assessments

The results of an international review of separation processes for spent nuclear fuel (SNF) recycling in future closed fuel cycles are reported. This study was made by the Expert Group on Fuel Recycling Chemistry (EGFRC) organised by the Nuclear Energy Agency (NEA) of the Organisation for Economic Co-operation and Development (OECD). A unique feature of this study was that processes were classified according to a hierarchy of separations aimed at different elements within spent fuel (uranium; uranium-plutonium co-recovery; minor actinides; high heat generating radionuclides) and also the Head-end processes, used to prepare the SNF for chemical separation, were included. Separation processes covered both wet (hydrometallurgical) and dry (pyro-chemical) processes. A bespoke methodology suitable for assessing the technological maturities of separation processes for SNF recycling was then designed based on the well-established Technology Readiness Level (TRL) scale but adapted for spent nuclear fuel separations. The innovative feature of this was the use of a matrix approach that enabled information on both the scale of testing and materials used in testing to be combined in the evaluation of the TRL. TRLs for the Head-end, hydrometallurgical and pyrochemical processes that had been reviewed by the study have been evaluated. It is clear that, whilst more R&D is needed in most cases to raise TRLs, suitable options exist to enable the recovery of all actinide elements plus the HHRs by wet or dry processes, even up to the extraordinarily difficult isolation of americium alone. The technology readiness levels (TRL) for most processes fall in the ‘proof of principle’ range with TRLs between 4 and 6, although this is an evaluation at the system level and some gaps in the individual process steps may still exist that strictly would reduce the overall TRL. That is, flowsheets have been proposed for processes and tested with active materials under increasingly relevant conditions, through to initial hot tests with small quantities of SNF. The results of this work were shown to be comparable to a parallel European study that evaluated TRLs for minor actinide partitioning processes.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Tuning aminopolycarboxylate chelators for efficient complexation of trivalent actinides

The complexation of trivalent lanthanides and minor actinides (Am 3+ , Cm 3+ , and Cf 3+ ) by the acyclic aminopolycarboxylate chelators 6,6'-((ethane-1,2-diylbis–((carboxymethyl)azanediyl))bis–(methylene))dipicolinic acid (H 4 octapa) and 6,6'-((((4-(1-(2-(2-(2-hydroxyethoxy)ethoxy)ethyl)-1H-1,2,3-triazol-4-yl)pyridine-2,6-diyl)bis–(methylene))bis–((carboxymethyl)azanediyl))bis–(methylene)) dipicolinic acid (H 4 pypa-peg) were studied using potentiometry, spectroscopy, competitive complexation liquid–liquid extraction, and ab initio molecular dynamics simulations. Two studied reagents are strong multidentate chelators, well-suited for applications seeking radiometal coordination for in-vivo delivery and f-element isolation. The previously reported H 4 octapa forms a compact coordination packet, while H 4 pypa-peg is less sterically constrained due to the presence of central pyridine ring. The solubility of H 4 octapa is limited in a non-complexing high ionic strength perchlorate media. However, the introduction of a polyethylene glycol group in H 4 pypa-peg increased the solubility without influencing its ability to complex the lanthanides and minor actinides in solution.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Monitoring of asteroids in cometary orbits and activated asteroids through archival images and new observations

Transitional objects are minor bodies that share some characteristics with asteroids and others with comets. These objects include asteroids in cometary orbits (ACOs), which behave dynamically like comets, but lack observed activity, while activated asteroids (AAs) follow typical asteroidal orbits, but have shown dust ejections. The monitoring of a set of these objects carried out in 2015 and 2016 is continued using archival images from various observatories and new data from the IMPACTON telescope in Brazil. Two techniques were applied to detect activity: (i) surface brightness profiles were compared with those of field stars to identify widening, and (ii) the magnitudes reported in the Minor Planet Center, combined with our observations, were reduced and analyzed to identify abrupt brightness increases as a function of heliocentric distance. We analyzed the surface brightness profiles of 133 ACOs and 7 AAs. To study the reduced magnitude, we obtained data from the 705 ACOs that were known at the time of the analysis. Together with the data from our previous work, our analysis covered 23% of the total known ACOs; 8 deviated slightly in the surface brightness profile, 6 brightened in the reduced magnitude, and one object is in common in both samples. A very low percentage of objects might show activity (4% of the sample with brightness profiles and <1% in the reduced magnitudes). These results would rule out a slow transition from active to inert. Regarding AAs, 4 showed activity, and 3 of them matched previously reported periods, while the data we analyzed for P/2015 X 6 were obtained 19 days before the first existing activity report. The activity episodes of these objects are very restricted in time and do not always occur in the same region of the orbit.

asteroids: general↗
DOE OSTI2026

Calculations of enrichment cascade performance using enrichment probabilities – a new method

A new method for calculating the performance of uranium enrichment cascades is presented. The method assigns a unique “enrichment probability” for each isotope to move up or down from the basic enrichment unit, allowing independent material balance calculations for each isotope. The formulation is much simpler than previous methods, which rely on isotopic ratios, and this method can be used when previous methods fail. This method gives the same results as published cases for 235 U enrichment and also gives good agreement with published data on minor isotopes. Some comparisons with measured data and other calculations are given. One case shows that the maximum 235 U enrichment that can be obtained by enrichment of reprocessed uranium (0.02% 234 U initial) is 82%. Another example shows a large difference in the minor isotopic content of material enriched in batches compared to continuous enrichment.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
NASA NTRS1995

Torsional Eye Movements Evoked by Unilateral Labyrinthine Galvanic Polarizations in the Squirrel Monkey

Electrical stimulation of vestibular-nerve afferents innervating the semicircular canals has been used to identify the extraocular muscles receiving activation or inhibition by individual ampullary nerves. This technique was originally developed by Szentagothai (1950) and led to the description of three neuron reflex arcs that connect each semicircular canal through an interneuron traversing in the region of the medial longitudinal fasciculus to one ipsilateral and one contralateral eye muscle. Selective ampullary nerve stimulation was subsequently used by Cohen and colleagues (Cohen and Suzuki, 1963; Cohen et al., 1964; Suzuki et al., 1964; Cohen et al., 1966) to study movements of the eyes and activation of individual extraocular muscles in response to stimulation of combinations of ampullary nerves. This work led to a description of the now familiar relationships between activation of a semicircular canal ampullary nerves and the anticipated movement in each eye. Disconjugacy of eye movements induced by individual vertical canal stimulation and dependence of the pulling direction of vertical recti and oblique muscles on eye position were also defined in these experiments. Subsequent studies have defined the mechanisms by which externally applied galvanic currents result in a change in vestibular-nerve afferent discharge. The currents appear to act at the spike trigger site. Perilymphatic cathodal currents depolarize the trigger site and lead to excitation whereas anodal currents hyperpolarize and result in inhibition. Afferents innervating all five vestibular endorgans appear to be affected equally by the currents (Goldberg et al., 1984). Irregularly discharging afferents are about 5-10 times more sensitive than regularly discharging ones because of the steeper slope of the former's faster postspike recovery of excitability in encoder sensitivity (Smith and Goldberg, 1986). Response adaptation similar to that noted during acceleration steps is apparent for longer periods of current administration. This adaptation is manifested as a perstimulus return toward resting discharge and poststimulus after-response in the opposite direction (Goldberg et al., 1984; Minor and Goldberg, l991). Cathodal currents (with respect to the perilymphatic space of the vestibule) are excitatory whereas anodal currents are inhibitory. Horizontal eye movements evoked by unilateral galvanic polarizations administered through chronically implanted labyrinthine stimulating electrodes have been studied in alert squirrel monkeys (Minor and Goldberg, 1991). We sought to extend this analysis by recording three-dimensional eye movements during galvanic stimulation. As predicted based upon roughly equal stimulation of ampullary nerves innervating the vertical canals, a substantial torsional component to the nystagmus is noted. The trajectory of torsional slow phases and nystagmus profile after the polarization provide insight into the central mechanisms that influence these responses.

Minor, Lloyd B.↗
DOE OSTI2011

Comparison of Discrete and Continuous Thermal Neutron Scattering Treatments in MCNP5

The advanced nuclear system will significantly advance the science and technology of nuclear energy systems and to enhance the spent fuel proliferation resistance. Minor actinides (MA) are viewed more as a resource to be recycled, and transmuted to less hazardous and possibly more useful forms, rather than simply disposed of as a waste stream in an expensive repository facility. MAs can play a much larger part in the design of advanced systems and fuel cycles, not only as additional sources of useful energy, but also as direct contributors to the reactivity control of the systems into which they are incorporated. In this work, an Advanced CANDU Reactor (ACR) fuel unit lattice cell model with 43 UO 2 fuel rods will be used to investigate the effectiveness of a Minor Actinide Reduction Approach (MARA) for enhancing proliferation resistance and improving the fuel cycle performance. The main MARA objective is to increase the 238 Pu / Pu isotope ratio by using the transuranic nuclides ( 237 Np and 241 Am) in the high burnup fuel and thereby increase the proliferation resistance even for a very low fuel burnup. As a result, MARA is a very effective approach to enhance the proliferation resistance for the on power refueling ACR system nuclear fuel. The MA transmutation characteristics at different MA loadings were compared and their impact on neutronics criticality assessed. The concept of MARA significantly increases the 238 Pu/Pu ratio for proliferation resistance, as well as serves as a burnable absorber to hold-down the initial excess reactivity. It is believed that MARA can play an important role in atoms for peace and the intermediate term of nuclear energy reconnaissance.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2017

MHD Collimation Mechanism in Arched Flux Ropes Characterized Using Volumetric, Time-Dependent B -Vector Measurements

Laboratory measurements of B(x,t) in a volume enclosing portions of two arched flux ropes show flux rope collimation driven by gradients in axial current density. These measurements verify the three predictions of a proposed MHD collimation mechanism: (1) axial magnetic forces exist in current channels with spatially varying minor radius, (2) these forces can drive counterpropagating axial flows, and (3) this process collimates the flux rope. As a result, this mechanism may explain the axial uniformity of solar loops and is relevant to other systems with current channels of varying minor radius such as solar prominences and astrophysical jets.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Semiconductor-based photoelectrochemical water splitting at the limit of very wide depletion region

In semiconductor-based photoelectrochemical (PEC) water splitting, carrier separation and delivery largely relies on the depletion region formed at the semiconductor/water interface. As a Schottky junction device, the trade-off between photon collection and minority carrier delivery remains a persistent obstacle for maximizing the performance of a water splitting photoelectrode. Here, it is demonstrated that the PEC water splitting efficiency for an n-SrTiO 3 (n-STO) photoanode is improved very significantly despite its weak indirect band gap optical absorption (α < 10⁴ cm⁻¹), by widening the depletion region through engineering its doping density and profile. Graded doped n-SrTiO 3 photoanodes are fabricated with their bulk heavily doped with oxygen vacancies but their surface lightly doped over a tunable depth of a few hundred nanometers, through a simple low temperature re-oxidation technique. The graded doping profile widens the depletion region to over 500 nm, thus leading to very efficient charge carrier separation and high quantum efficiency (>70%) for the weak indirect transition. As a result, this simultaneous optimization of the light absorption, minority carrier (hole) delivery, and majority carrier (electron) transport by means of a graded doping architecture may be useful for other indirect band gap photocatalysts that suffer from a similar problem of weak optical absorption.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2025

Increased Voltage in CdSe Solar Cells by Mitigation of Charge Carrier Trapping Due to Se Vacancies

Cadmium selenide (CdSe), with a 1.7 eV bandgap, is a promising high-bandgap semiconductor for tandem solar cells, yet device efficiencies are hindered by rapid minority carrier recombination. Here, in this study, polycrystalline CdSe solar cells are investigated using radiative emission spectroscopy, time-resolved photoluminescence, and density functional theory, revealing fast (sub-nanosecond) minority carrier trapping by selenium vacancy-related defect states with densities of (5–50) × 10 17 cm −3 , limiting carrier mobility and increasing recombination. By reducing absorber thickness to ≈0.5 µm, trapping effects are mitigated, achieving a record open-circuit voltage of 917 mV, a 165 mV improvement over prior reports. These findings clarify the role of Se vacancies in limiting CdSe solar cell performance and provide insights applicable to CdSe and CdSeTe thin-film photovoltaics. This work advances understanding of defect-mediated losses in II–VI semiconductors and suggests pathways for improving solar cell performance through defect control.

14 SOLAR ENERGY↗
DOE OSTI2022

A separations and purification process for improving yields and meeting fuel contaminant specifications for high-octane gasoline produced from dimethyl-ether over a Cu/BEA catalyst

In this work, we have been developing a three-step conversion of biomass-derived syngas to methanol to dimethyl-ether (DME) to non-aromatic hydrocarbons for use as high-octane gasoline and sustainable aviation fuel. This process produces branched alkanes from DME using a Cu/BEA catalyst and is a promising alternative to other syngas conversion processes such as Fischer-Tropsch to linear alkanes and traditional ZSM-5 catalyzed methanol to aromatic gasoline. In this short article we describe some advances in our understanding related to separations and purification via the use of more detailed experimental speciation in an updated process model involving multiple phase equilibrium-based separation steps. Primary modeled reactor outlet constituents (and weight %) are: C3 and lighter hydrocarbon gases (11.1%), C4s (54.5%), H 2 (1.2%), CO 2 (2.9%), water (5.0%), unreacted DME (16.5%), methanol (2.3%), and C5+ hydrocarbons (6.4%). DME (the primary reactant) and H 2 recycle and reuse are important for the overall process efficiency, and the recycle of C4s is important to increase the C5+ yield via reactivation and homologation. Thus H 2 , C4s, and DME are targeted for recycle, while methanol and water need to be removed from the product to conform with fuel specifications. Model predictions from Aspen Plus using the NRTL-RK property method indicate a fuel composition with C5+ content of 97.1 wt%, with minor constituents: 2.4 wt% C4s, 0.3 wt% methanol, 0.1 wt% DME, 0.03 wt% water, and 0.01 wt% C3s. These ranges of minor components conform with fuel quality requirements, and the modeled product is amenable for unconstrained blending to boost gasoline octane ratings.

09 BIOMASS FUELS↗