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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 1,711 records · Page 95
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

A model study of assisted adiabatic transfer of population in the presence of collisional dephasing

Previous studies have demonstrated that when experimental conditions generate non-adiabatic dynamics that prevents highly efficient population transfer between states of an isolated system by stimulated Raman adiabatic passage (STIRAP), the addition of an auxiliary counter-diabatic field (CDF) can restore most or all of that efficiency. This paper examines whether that strategy is also successful in a non-isolated system in which the energies of the states fluctuate, e.g., when a solute is subject to collisions with solvent. We study population transfer in two model systems: (i) the three-state system used by Demirplak and Rice [J. Chem. Phys. 116, 8028 (2002)] and (ii) a four-state system, derived from the simulation studies of Demirplak and Rice [J. Chem. Phys. 125, 194517 (2006)], that mimics HCl in liquid Ar. Simulation studies of the vibrational manifold of HCl in dense fluid Ar show that the collision induced vibrational energy level fluctuations have asymmetric distributions. Representations of these asymmetric energy level fluctuation distributions are used in both models (i) and (ii). We identify three sources of degradation of the efficiency of STIRAP generated selective population transfer in model (ii): too small pulse areas of the laser fields, unwanted interference arising from use of strong fields, and the vibrational detuning. For both models (i) and (ii), our examination of the efficiency of STIRAP + CDF population transfer under the influence of the asymmetric distribution of the vibrational energy fluctuations shows that there is a range of field strengths and pulse durations under which STIRAP + CDF control of population transfer has greater efficiency than does STIRAP generated population transfer.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Measurement of the polarisation of single top quarks and antiquarks produced in the $t$-channel at $ \sqrt{s} $ = 13 TeV and bounds on the $tWb$ dipole operator from the ATLAS experiment

A simultaneous measurement of the three components of the top-quark and top-antiquark polarisation vectors in t-channel single-top-quark production is presented. This analysis is based on data from proton–proton collisions at a centre-of-mass energy of 13 TeV corresponding to an integrated luminosity of 139 fb –1 , collected with the ATLAS detector at the LHC. Selected events contain exactly one isolated electron or muon, large missing transverse momentum and exactly two jets, one being b-tagged. Stringent selection requirements are applied to discriminate t-channel single-top-quark events from the background contributions. The top-quark and top-antiquark polarisation vectors are measured from the distributions of the direction cosines of the charged-lepton momentum in the top-quark rest frame. The three components of the polarisation vector for the selected top-quark event sample are P x' = 0.01 ± 0.18, P y' = –0.029 ± 0.027, P z' = 0.91 ± 0.10 and for the top-antiquark event sample they are P x' = –0.02 ± 0.20, P y' = –0.007 ± 0.051, P z' = 0.79 ± 0.16. Normalised differential cross-sections corrected to a fiducial region at the stable-particle level are presented as a function of the charged-lepton angles for top-quark and top-antiquark events inclusively and separately. These measurements are in agreement with Standard Model predictions. The angular differential cross-sections are used to derive bounds on the complex Wilson coefficient of the dimension-six O tW operator in the framework of an effective field theory. The obtained bounds are C tW ϵ [–0.9, 1.4] and C itW ϵ [–0.8, 0.2], both at 95% confidence level.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Selective single-atom adsorption for precision separation of lead ions in tap water via capacitive deionization

Capacitive deionization (CDI) offers a cost-effective and low-energy method for selective removal of Pb 2+ from drinking water. Modifying CDI electrode surfaces with functional groups presents a versatile approach to enhancing selective ion adsorption capacity. However, a comprehensive understanding of the selectivity and removal efficiency of Pb 2+ among diverse functional groups remains unexplored. Here, we investigated the effects of different functional groups (-SH, -COOH, and -NH 2 ) attached to the graphene oxide (GO) electrode surfaces on Pb 2+ selectivity and removal efficiency. Surprisingly, GO-COOH demonstrated single-atom adsorption of Pb 2+ , displaying superior removal efficiency and selectivity compared with -SH and -NH 2 , although -SH possesses significant chelation capability for Pb 2+ . Both density functional theory (DFT) calculations and X-ray pair distribution function (PDF) analyses confirmed that Pb 2+ exhibits a theoretically higher affinity to -COOH. Further, this research deepens our understanding of the interactions between functional groups and heavy metal ions, enabling selective and rapid separation of target cations for water purification.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1986

Zonal and geographical distributions of cirrus clouds determined from SAGE data

Stratospheric Aerosol and Gas Experiment (SAGE) data obtained from February 1979-November 1981 are analyzed in order to evaluate the spatial extent and frequency occurrence of cirrus clouds. The capabilities of the SAGE measurement system which has a field of view of 100 sq km are discussed. The frequency of occurrence of the cirrus clouds and the frequency penetration of the clouds to fixed altitudes of 5, 7, and 9 km, and to altitudes of 1, 3 and 5 km below the troposphere are examined. It is observed that optically thick cirrus clouds form most frequently in the midlatitudes over the equator, with distinct minima near latitude bands of 20-30 deg north and south; height penetrations to 7 km occur 60 percent of the time in upper latitudes and drop to 30 percent over the tropics. The SAGE data are compared with selective chopper radiometer data and good correlation in shape and seasonal movement is displayed. The seasonal geographical distributions of cirrus clouds in regions of rising moist air associated with low-level convergence zones are described.

Woodbury, G. E.↗
NASA NTRS2017

Field Exploration and Life Detection Sampling Through Planetary Analogue Sampling (FELDSPAR).

Exploration missions to Mars rely on rovers to perform analyses over small sampling areas; however, landing sites for these missions are selected based on large-scale, low-resolution remote data. The use of Earth analogue environments to estimate the multi-scale spatial distributions of key signatures of habitability can help ensure mission science goals are met. A main goal of FELDSPAR is to conduct field operations analogous to Mars sample return in its science, operations, and technology from landing site selection, to in-field sampling location selection, remote or stand-off analysis, in situ analysis, and home laboratory analysis. Lava fields and volcanic regions are relevant analogues to Martian landscapes due to desiccation, low nutrient availability, and temperature extremes. Operationally, many Icelandic lava fields are remote enough to require that field expeditions address several sampling constraints that are experienced in robotic exploration, including in situ and sample return missions. The Fimmvruhls lava field was formed by a basaltic effusive eruption associated with the 2010 Eyjafjallajkull eruption. Mlifellssandur is a recently deglaciated plain to the north of the Myrdalsjkull glacier. Holuhraun was formed by a 2014 fissure eruptions just north of the large Vatnajkull glacier. Dyngjusandur is an alluvial plain apparently kept barren by repeated mechanical weathering. Informed by our 2013 expedition, we collected samples in nested triangular grids every decade from the 10 cm scale to the 1 km scale (as permitted by the size of the site). Satellite imagery is available for older sites, and for Mlifellssandur, Holuhraun, and Dyngjusandur we obtained overhead imagery at 1 m to 200 m elevation. PanCam-style photographs were taken in the field by sampling personnel. In-field reflectance spectroscopy was also obtained with an ASD spectrometer in Dyngjusandur. All sites chosen were 'homogeneous' in apparent color, morphology, moisture, grain size, and reflectance spectra at all scales greater than 10 cm. Field lab assays were conducted to monitor microbial habitation, including ATP quantification, qPCR for fungal, bacterial, and archaeal DNA, and direct cell imaging using fluorescence microscopy. Home laboratory analyses include Raman spectroscopy and community sequencing. ATP appeared to be significantly more sensitive to small changes in sampling location than qPCR or fluorescence microscopy. Bacterial and archaeal DNA content were more consistent at the smaller scales, but similarly variable across more distant sites. Conversely, cell counts and fungal DNA content have significant local variation but appear relatively homogeneous over scales of 1 km. ATP, bacterial DNA, and archaeal DNA content were relatively well correlated at many spatial scales. While we have observed spatial variation at various scales and are beginning to observe how that variation fluctuates over time as biodiversity recovers after an eruption, we do not yet fully understand what parameters lead to the observed spatial variation. Home laboratory analyses will help us further understand the elemental and structural composition of the basaltic matrices, but further field analyses are vital for the understanding how temperature, moisture, incident radiation, and so forth influence the habitability of a microclimate.

Field↗
DOE OSTI2016

SU-F-J-200: An Improved Method for Event Selection in Compton Camera Imaging for Particle Therapy

Purpose: The uncertainty in the beam range in particle therapy limits the conformality of the dose distributions. Compton scatter cameras (CC), which measure the prompt gamma rays produced by nuclear interactions in the patient tissue, can reduce this uncertainty by producing 3D images confirming the particle beam range and dose delivery. However, the high intensity and short time windows of the particle beams limit the number of gammas detected. We attempt to address this problem by developing a method for filtering gamma ray scattering events from the background by applying the known gamma ray spectrum. Methods: We used a 4 stage Compton camera to record in list mode the energy deposition and scatter positions of gammas from a Co-60 source. Each CC stage contained a 4×4 array of CdZnTe crystal. To produce images, we used a back-projection algorithm and four filtering Methods: basic, energy windowing, delta energy (ΔE), or delta scattering angle (Δθ). Basic filtering requires events to be physically consistent. Energy windowing requires event energy to fall within a defined range. ΔE filtering selects events with the minimum difference between the measured and a known gamma energy (1.17 and 1.33 MeV for Co-60). Δθ filtering selects events with the minimum difference between the measured scattering angle and the angle corresponding to a known gamma energy. Results: Energy window filtering reduced the FWHM from 197.8 mm for basic filtering to 78.3 mm. ΔE and Δθ filtering achieved the best results, FWHMs of 64.3 and 55.6 mm, respectively. In general, Δθ filtering selected events with scattering angles < 40°, while ΔE filtering selected events with angles > 60°. Conclusion: Filtering CC events improved the quality and resolution of the corresponding images. ΔE and Δθ filtering produced similar results but each favored different events.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2022

Probing Electrolyte Influence on CO 2 Reduction in Aprotic Solvents

Selective CO 2 capture and electrochemical conversion are important tools in the fight against climate change. Industrially, CO 2 is captured using a variety of aprotic solvents due to their high CO 2 solubility. However, most research efforts on electrochemical CO 2 conversion use aqueous media and are plagued by competing hydrogen evolution reaction (HER) from water breakdown. Fortunately, aprotic solvents can circumvent HER, making it important to develop strategies that enable integrated CO 2 capture and conversion. However, the influence of ion solvation and solvent selection within nonaqueous electrolytes for efficient and selective CO 2 reduction is unclear. In this work, we show that the bulk solvation behavior within the nonaqueous electrolyte can control the CO2 reduction reaction and product distribution occurring at the catalyst-electrolyte interface. We study different tetrabutylammonium (TBA) salts in two electrolyte systems with glyme ethers (e.g., 1,2 dimethoxyethane or DME) and dimethyl sulfoxide (DMSO) as a low and high dielectric constant medium, respectively. Using spectroscopic tools, we quantify the fraction of ion pairs that forms within the electrolyte. Also, we show how ion pair formation is prevalent in DME and is dependent on the anion type. More importantly, we show that as ion pair formation decreases within the electrolyte, CO 2 current densities increase, and a higher CO Faradaic efficiency is observed at low overpotentials. Meanwhile, in an electrolyte medium where the ion pair fraction does not change with the anion type (such as in DMSO), a smaller influence of solvation is observed on CO 2 current densities and product distribution. By directly coupling bulk solvation to interfacial reactions and product distribution, we showcase the importance and utility of controlling the reaction microenvironment in tuning the electrocatalytic reaction pathways. Insights gained from this work will enable novel electrolyte designs for efficient and selective CO 2 conversion to desired fuels and chemicals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2006

Nonlinear Acoustic Response of an Aircraft Fuselage Sidewall Structure by a Reduced-Order Analysis

A reduced-order nonlinear analysis of a structurally complex aircraft fuselage sidewall panel is undertaken to explore issues associated with application of such analyses to practical structures. Of primary interest is the trade-off between computational efficiency and accuracy. An approach to modal basis selection is offered based upon the modal participation in the linear regime. The nonlinear static response to a uniform pressure loading and nonlinear random response to a uniformly distributed acoustic loading are computed. Comparisons of the static response with a nonlinear static solution in physical degrees-of-freedom demonstrate the efficacy of the approach taken for modal basis selection. Changes in the modal participation as a function of static and random loading levels suggest a means for improvement in the basis selection.

Przekop, Adam↗
DOE OSTI2021

Galaxy assembly bias and large-scale distribution: a comparison between IllustrisTNG and a semi-analytic model

In this work, we compare large scale structure observables for stellar mass selected samples at z = 0, as predicted by two galaxy models, the hydrodynamical simulation IllustrisTNG and the Santa-Cruz semi-analytic model (SC-SAM). Although both models have been independently calibrated to match observations, rather than each other, we find good agreement between the two models for two-point clustering and galaxy assembly bias signatures. The models also show a qualitatively similar response of occupancy and clustering to secondary halo parameters other than mass, such as formation history and concentration, although with some quantitative differences. Thus, our results demonstrate that the galaxy–halo relationships in SC-SAM and TNG are quite similar to first order. However, we also find areas in which the models differ. For example, we note a strong correlation between halo gas content and environment in TNG, which is lacking in the SC-SAM, as well as differences in the occupancy predictions for low-mass haloes. Moreover, we show that higher order statistics, such as cumulants of the density field, help us to accurately describe the galaxy distribution and discriminate between models that show degenerate behaviour for two-point statistics. Our results suggest that SAMs are a promising cost-effective and intuitive method for generating mock catalogues for next generation cosmological surveys.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Quantitative Stable-Isotope Probing (qSIP) with Metagenomics Links Microbial Physiology and Activity to Soil Moisture in Mediterranean-Climate Grassland Ecosystems

The growth and physiology of soil microorganisms, which play vital roles in biogeochemical cycling, are shaped by both current and historical soil environmental conditions. Here, we developed and applied a genome-resolved metagenomic implementation of quantitative stable isotope probing (qSIP) with an H 2 18 O labeling experiment to identify actively growing soil microorganisms and their genomic capacities. qSIP enabled measurement of taxon-specific growth because isotopic incorporation into microbial DNA requires production of new genome copies. We studied three Mediterranean grassland soils across a rainfall gradient to evaluate the hypothesis that historic precipitation levels are an important factor controlling trait selection. We used qSIP-informed genome-resolved metagenomics to resolve the active subset of soil community members and identify their characteristic ecophysiological traits. Higher year-round precipitation levels correlated with higher activity and growth rates of flagellar motile microorganisms. In addition to heavily isotopically labeled bacteria, we identified abundant isotope-labeled phages, suggesting phage-induced cell lysis likely contributed to necromass production at all three sites. Further, there was a positive correlation between phage activity and the activity of putative phage hosts. Contrary to our expectations, the capacity to decompose the diverse complex carbohydrates common in soil organic matter or oxidize methanol and carbon monoxide were broadly distributed across active and inactive bacteria in all three soils, implying that these traits are not highly selected for by historical precipitation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2016

SU-F-T-397: Evaluating the Impact of Bladder Filling Status for the Organs at Risk Dose Distribution in Cervical Cancer Patients with Intensity Modulated Radiotherapy

Purpose: To investigate the impact of bladder filling status of the organs at risk (OARs) on dose distribution during intensity modulated radiotherapy (IMRT) for cervical cancer patients. Methods: Twelve cervical cancer patients treated with IMRT were selected for this study. The prescription dose was 45Gy/25 fractions with the 6 MV photon beam. All patients performed two CT scans, one with an empty bladder, the other one with bladder filled. For the registration of two CT scans, the fusion was automatically carried out upon the bony anatomy. The OARs (bladder, rectum, pelvic bone and small intestine) were delineated to planning CT to evaluate the dose distributions. These dose distributions were compared between empty bladder and bladder filling. Results: The bladder volume with empty bladder and bladder filling was 403.2±124.13cc and 101.4±87.5cc, respectively. There were no statistical differences between empty bladder and bladder filling in the mean value of pelvic bone V10Gy, V20Gy, V40Gy; rectum V40Gy and V45Gy. The bladder V40Gy and V45Gy were lower in the bladder filling group than in the empty bladder group (63.7%±5.8% vs 87.5%±7.8%, 45.1%±9.5% vs 62.4%±11.8%, respectively). The V45Gy for small intestine in the bladder filling group was significantly less than the empty bladder group (146.7cc±95.3cc vs 245.7cc±101.8cc). Conclusion: Our study finds that the bladder filling status did not have a significant impact on dose distribution in the rectum and pelvic bone. However, the changes of bladder filling have a large impact on bladder and small intestine doses. A full bladder is strongly recommended during treatment for cervical cancer patients.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2017

Morphology and the color-mass diagram as clues to galaxy evolution at z ∼ 1

We study the significance of mergers in the quenching of star formation in galaxies at z∼1 by examining their color–mass distributions for different morphology types. We perform two-dimensional light profile fits to GOODS iz images of ∼5000 galaxies and X-ray selected active galactic nucleus (AGN) hosts in the CANDELS/GOODS-north and south fields in the redshift range 0.7<z<1.3. Distinguishing between bulge-dominated and disk-dominated morphologies, we find that disks and spheroids have distinct color–mass distributions, in agreement with studies at z∼0. The smooth distribution across colors for the disk galaxies corresponds to a slow exhaustion of gas, with no fast quenching event. Meanwhile, blue spheroids most likely come from major mergers of star-forming disk galaxies, and the dearth of spheroids at intermediate green colors is suggestive of rapid quenching. The distribution of moderate luminosity X-ray AGN hosts is even across colors, in contrast, and we find similar numbers and distributions among the two morphology types with no apparent dependence on Eddington ratio. The high fraction of bulge-dominated galaxies that host an AGN in the blue cloud and green valley is consistent with the scenario in which the AGN is triggered after a major merger, and the host galaxy then quickly evolves into the green valley. This suggests AGN feedback may play a role in the quenching of star formation in the minority of galaxies that undergo major mergers.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2016

Fundamental Studies of the Reforming of Oxygenated Compounds over Supported Metal Catalysts

The main objective of our research has been to elucidate fundamental concepts associated with controlling the activity, selectivity, and stability of bifunctional, metal-based heterogeneous catalysts for tandem reactions, such as liquid-phase conversion of oxygenated hydrocarbons derived from biomass. We have shown that bimetallic catalysts that combine a highly-reducible metal (e.g., platinum) with an oxygen-containing metal promoter (e.g., molybdenum) are promising materials for conversion of oxygenated hydrocarbons because of their high activity for selective cleavage for carbon-oxygen bonds. We have developed methods to stabilize metal nanoparticles against leaching and sintering under liquid-phase reaction conditions by using atomic layer deposition (ALD) to apply oxide overcoat layers. We have used controlled surface reactions to produce bimetallic catalysts with controlled particle size and controlled composition, with an important application being the selective conversion of biomass-derived molecules. The synthesis of catalysts by traditional methods may produce a wide distribution of metal particle sizes and compositions; and thus, results from spectroscopic and reactions kinetics measurements have contributions from a distribution of active sites, making it difficult to assess how the size and composition of the metal particles affect the nature of the surface, the active sites, and the catalytic behavior. Thus, we have developed methods to synthesize bimetallic nanoparticles with controlled particle size and controlled composition to achieve an effective link between characterization and reactivity, and between theory and experiment. We have also used ALD to modify supported metal catalysts by addition of promoters with atomic-level precision, to produce new bifunctional sites for selective catalytic transformations. We have used a variety of techniques to characterize the metal nanoparticles in our catalysts, including scanning transmission electron microcopy (STEM) to measure size and structure, energy dispersive X-ray spectroscopy (EDS) to measure atomic composition, X-ray absorption spectroscopy (XAS) to measure oxidation state and metal coordination, Fourier transform infrared spectroscopy (FTIR) to study adsorbed species, laser Raman spectroscopy to probe metal oxide promoters, and temperature programmed reaction/desorption to study the energetics of adsorption and desorption processes. We have studied our bimetallic catalysts for the selective cleavage of carbon-oxygen bonds, and we have studied the effects of adding metal oxide promoters to supported platinum and gold catalysts for water-gas shift (i.e., the production of hydrogen by reaction of carbon monoxide with water). We anticipate that the knowledge obtained from our studies will allow us to identify promising directions for new catalysts that show high activity, selectivity, and stability for important reactions, such as the conversion of biomass-derived oxygenated hydrocarbons to fuels and chemicals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1994

Mg II absorption in a sample of 56 steep-spectrum quasars

We present an analysis of the statistical properties of Mg II absorbers found in the spectra of 56 intrinsically faint, steep-spectrum radio quasars. We observe for the first time a significant excess of associated Mg II absorbers over the number expected from cosmologically distributed absorbers. This result is in contrast to previous Mg II surveys in which the QSOs were optically selected. This distinction is similar to the result for associated C IV absorbers, in which intrinsically faint, steep-spectrum quasars show excess associated absorption and intrinsically bright QSOs (both radio-loud and radio-quiet) do not show an excess. From our spectra a statistically complete list of absorption lines is derived, and we find 29 Mg II absorbers, 18 of which have not been previously reported. We also determine several characteristics of the quasar emission lines in our spectra. The Mg II absorber distribution as a function of redshift and equivalent width is calculated both for our sample alone and from our sample combined with spectra from other surveys. For the redshift distribution n(z) = n(1 + z)(exp gamma), we obtain, using the combined sample, the values gamma = 1.11 +/- 0.46 for W(min) = 0.6 A and gamma = 2.47 +/- 0.68 for W(min) = 1.0 A. We find that the distribution fo strong absorbers is inconsistent with no evolution at a confindence level between 2.2 and 2.9 sigma, depending on the deceleration parameter q(sub 0). The deviation from no evolution is similar to what had been previously reported.

Aldcroft, Thomas L.↗
DOE OSTI2016

Directional Drilling Technology for HLW Disposal - Outline of System and its Application - 16078

During high-level waste (HLW) disposal site selection, borehole measurement and logging to investigate the hydro-geological and geo-mechanical conditions of the host rocks is a very important way to examine the potential of the disposal candidates. In Japan, attention is being given to Neogene soft sedimentary rock as the host rock for HLW disposal. In particular, the soft sedimentary rock in coastal areas is thought to be one of the best candidates, because there is little driving force from underground water. Directional drilling is supposed to be efficient under limited topographic and geological conditions, and the Central Research Institute of Electric Power Industry (CRIEPI) has been conducting a project on directional drilling and logging/measurement technologies since 2000. Basic directional drilling system was developed and the system was applied to the Neogene normal sedimentary rock at the Hokushin area of the Horonobe town in Hokkaido. The borehole was drilled to the 700 m long and the applicability of the system was confirmed until 2004. A basic directional drilling system was developed, and the system was applied to the Neogene normal sedimentary rock in the Hokushin area, in the town of Horonobe in Hokkaido. A 700-m borehole was drilled, and the applicability of the system was confirmed in 2004. After conducting a seismic reflection survey for the Omagari fault distribution at the Kami-Horonobe area in the town of Horonobe, a drilling site was selected, and a borehole trace was planned to perpendicularly intersect the fault zone in 2005. Considering the planned trace, a 1000-m-long borehole was drilled to a depth of 450 m. From 750 m to the bottom (1000 m), the borehole was horizontal. The total core recovery was 99.8%, even though it was drilled in the fault zone. The geological, hydrological, geo-mechanical, geophysical, and geochemical data were collected using borehole logging/measurement/survey and core logging/measurement/analysis, and the Omagari fault was characterized. After conducting all the work in the borehole, a steel pipe was inserted into the borehole to case the wall. Open hole sections for monitoring were constructed considering the hydro-geological conditions throughout the hole. Then, the monitoring system was inserted and set up to obtain the initial conditions of the groundwater pressure and chemistry. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2019

Integrated Two-Stage Alkaline-Oxidative Pretreatment of Hybrid Poplar. Part 1: Impact of Alkaline Pre-Extraction Conditions on Process Performance and Lignin Properties

We previously demonstrated that a two-stage pretreatment comprising of an alkaline pre-extraction followed by a Cu-catalyzed alkaline–oxidative treatment is effective at pretreating hardwoods under relatively mild reaction conditions. In this work, we focus on characterizing how biomass source and reaction conditions used during the alkaline pre-extraction impact the subsequent processing stages as well as lignin yields and properties. Specifically, three hybrid poplars were subjected to the first stage alkaline pre-extraction under various conditions including differences in time (15–300 min), temperature (95–155 °C), and alkali loadings (50–200 mg NaOH/g biomass), and the impact on total mass solubilization, lignin recovery, and lignin purity was determined. Empirical correlations were developed between reaction conditions and mass solubilization and lignin recovery during the pre-extraction stage. For select conditions, lignin properties were assessed and include β-O-4 content determined by 13C NMR, molecular mass distributions as determined by gel permeation chromatography, and susceptibility to depolymerization to aromatic monomers using thioacidolysis and formic acid catalyzed depolymerization. We found alkaline pre-extraction performed at higher temperatures generated lignins exhibiting lower contamination by polysaccharides, lower aromatic monomer yields from depolymerization, lower molar masses, and lower β-O-4 contents relative to the lower temperature pre-extractions. Lastly, the pre-extracted biomass from select conditions was assessed for its response to the subsequent Cu-catalyzed alkaline–oxidative treatment and enzymatic hydrolysis. It was demonstrated that minor differences in delignification during pre-extraction have quantifiable impacts on the subsequent efficacy of the second stage of pretreatment and enzymatic hydrolysis with improved lignin removal during the first pre-extraction stage resulting in improved hydrolysis yields.

09 BIOMASS FUELS↗