PNNL-13501 - Pacific Northwest National Laboratory

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allowable parameters using thermodynamic modeling, and candidate gases will undergo soil-column experiments using simulated tank wastes to verify predicted behavior. Results and Accomplishments Our research team derived a mathematical model of tracer behavior under nonequilibrium transport conditions. Soilcolumn experiments using the proposed tracer suite (methane and difluoromethane) have verified the theoretical conclusions. The tracer residence time was found to be independent of the Damkholer number (masstransfer rate/advection flow rate), and the mass-transfer rate was found to be independent of the water saturation of the soil. Experimental results from soil-column tests show that residence time (flow rate through the pore volume) has little effect on the accuracy of water saturation measurements under transport conditions with Damkholer numbers greater than unity (see Figure 4). Summary of Experimental Results Water saturation measured by mass balance = 0.269 Tracer Concentration (ppm w Mean Residence Time Damkohler Water for Difluoromethane (hrs) Number Saturation PITT #1 1.33 2.19 0.260 PITT #2 0.86 1.86 0.235 PITT #3 0.50 1.50 0.259 PITT #4 0.27 1.21 0.274 1000 100 10 1 0.1 Solid points - Methane Open points - Difluoromethane 0 50 100 150 200 250 Volume (ml) PITT #1 (0.81 cc/min) PITT #2 (1.24 cc/min) PITT #3 (2.20 cc/min) PITT #4 (3.83 cc/min) Figure 4. Experimental results for the methanedifluoromethane tracer system show accurate water saturation measurements are possible at fast flow rates (low mean residence times) Thermodynamic approximations of ammonia partitioning show that it would be severely retarded in its transport in the subsurface, but it is thought that preferential flowpatterns will saturate with continued passage of ammonia and reduce the apparent retardation. Butanol and other organics with lower aqueous partitioning coefficients are under consideration as waste-component leak indicators. 250 FY 2000 Laboratory Directed Research and Development Annual Report 135 Xe is present in tank wastes (Agnew 1997) at very low molar concentrations, but its gamma signature is easily detectable at 1 Bq/m 3 . Its relatively high solubility in water gives it a correspondingly high retardation factor, but soil-column experiments may reveal preferential flowpattern saturation (as with ammonia). We are studying other noble-gas, waste-component radioisotopes of lower atomic number (less polarizable, and so less soluble) and tritium as leak detection agents. Summary and Conclusions A mathematical model of tracer behavior under nonequilibrium mass-transfer conditions was formulated. Soil-column experiments verified the theoretical predictions of the independence of the Damkholer number and tracer residence time and the independence of masstransfer rate and soil water saturation. Our research team concluded that • The accuracy of water saturation measurements are substantially unaffected by advection flow rates or tracer residence times for transport conditions with Damkholer numbers greater than unity. • The methane/difluoromethane tracer suite is well suited for soil moisture characterization. • Volatile organic, inorganic, or radioactive tank-waste components may function effectively as leak indicators if partitioning and preferential-flow behavior is adequately characterized. This project will continue as we perform preferential-flow experiments and characterize tracer behavior in simulated Hanford tank waste. We also will seek to conduct a field demonstration where a soil-moisture partitioning interwell tracer tests will be used to quantify a simulated tank leak in Hanford soils. Reference Agnew SF. 1997. Hanford Tank Chemical and Radionuclide Inventories: HDW Model Rev. 4 LA-UR- 96-3860, Los Alamos National Laboratory, Los Alamos, New Mexico.
Study Control Number: PN00090/1497 Use of Reduced Metal Ions in Reductive Reagents John S. Fruchter, Jim E. Szecsody In the past 15 years, groundwater cleanup of chlorinated solvents has involved installation of reactive subsurface iron barriers in over 25 sites in the U.S. One method used, which relies upon the reduction of iron in natural sediments, is applicable to deep aquifers (more than 100 feet). In this laboratory study, we modified geochemically the sediment reduction method to make the process more efficient and, ideally, less expensive. Project Description The purpose of this study was to determine a more efficient method for introducing chemical reducing capacity into the subsurface. After an initial reduction of aquifer sediments with sodium dithionite, reduced cations, such as ferrous iron (Fe(II)) or titanous ion (Ti(III)) would be injected into the aquifer. The expected results are an understanding of the proportions of Fe(II) and Ti(III) metal ions to use and the chemical conditions needed for achieving a successful reduced zone. In this way, a reactive barrier can be developed that is more effective for destroying dissolved contaminants such as chlorinated solvents and explosives. Over the past several years, a major effort at Pacific Northwest National Laboratory was the development of reductive barrier remediation techniques for use on shallow and deep (>50 feet below ground surface) contaminant plumes. The most promising method is in situ redox manipulation. The basis of the method is the use of a strong reducing agent (dithionite) to reduce normally trivalent structural iron in the soil matrix to the more reactive divalent form. The presence of the immobile divalent iron in the treated zone creates a chemically active barrier to the transport of reducible species, which can last for decades before renewal. Despite these successes, dithionite addition alone is an inefficient and expensive way to add reducing capacity to the aquifer. Because the reduction of some contaminants (trichloroethylene for example), the surface has a catalytic or surface coordination role in reduction, the presence of specific metals on the iron oxide surface can increase the electron transfer (reduction) rate. This concept has been applied to zero-valent iron walls, with the incorporation of trace amounts of Cr and Ni. A more efficient method would be to inject dithionite to produce reducing conditions in the aquifer, then add one or more reduced metal ions directly. We propose to amend the in situ redox manipulation technique through addition of additional reduced metal ions (e.g., Fe(ii), Ti(III)) to the redox injection. Cationic adsorption of reduced metal ions on the soil matrix should the produce a more reactive barrier. Introduction In this study, we investigated electron donors or reaction catalysts potential chemical additions. Fe(II) and Mn(II) additions (electron donors) resulted in a significant increase in trichloroethylene dechlorination. Trichloroethylene dechlorination with the Fe(II) addition was predictable and more efficient than the Mn(II). The additions of Ti(III), Ni(II), Pd catalyst, and EDTA did not enhance the trichloroethylene dechlorination rate in sediments, even though these compounds are used in engineered systems. Because the addition of an electron shuttle had only a slight positive effect, the rate of trichloroethylene degradation is not limited by electron transfer, so an additional electron donor rather than catalyst is likely more efficient. While an Fe(II) addition is expected to be more cost efficient than the use of reduced sediment alone, amending the redox treatment at the field scale involves additional hydraulic and geochemical considerations. Upscaling these results of using small to large experimental systems is needed to design viable field-scale injection schemes. Trichloroethylene dechlorination with reduced sediment relies on the oxidation of ferrous iron [adsorbed Fe(II), Fe(II)CO3, reduced smectite clays; Szecsody et al. 2000a, b]. In addition, adsorbed or structural Fe II on an Fe III - oxide or clay surface is necessary for dechlorination, either as a catalyst, a semiconductor, or to provide surface Eh conditions (Scherer et al. 1999; Wehrli 1992). The trichloroethylene degradation pathway using zero-valent iron (Roberts et al. 1996) and reduced sediments (Szecsody et al. 2000b) is reductive elimination producing chloroacetylene, then acetylene: Earth System Science 251
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Laboratory Directed Research and De
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Laboratory Directed Research and De
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Computational Science and Engineeri
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Policy and Management Sciences Asse
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Introduction Department of Energy O
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5. After reviews by the Technical a
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• The Technical Council peer revi
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methods applicable to combustion, s
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Summary Each national laboratory mu
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Study Control Number: PN0004/1411 A
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Table 1. Positive and negative ions
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m/z Arbitrary Units Figure 1. Mass
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introduce low-volatility compounds
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arrangement, but the charge is reta
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two liquid chromatographic gradient
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Integrated Microfabricated Devices
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Matrix Assisted Laser Desorption/Io
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Molecular Beam Synthesis and Charac
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temperature distribution of the des
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expected to result in significant a
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Study Control Number: PN99069/1397
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Seuss DT and KA Prather. 1999. “M
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Analysis of Receptor-Modulated Ion
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laboratory (Lu and Xie 1997; Lu et
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Automated DNA Fingerprinting Microa
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Comparison of 4 Xanthomonas Isolate
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Approach Hematopoietic (bone marrow
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Anti-Human lgG Human lgG Protein G
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Characterization of Global Gene Reg
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PCR products for immobilization on
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identify novel proteins of importan
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Immunoprecipitaton of tyrosinephosp
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Coupled NMR and Confocal Microscopy
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In the optical microscopy image, th
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Development and Applications of a M
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Figure 3. Hepa-1 cells undergoing a
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cellular processing (such as post-t
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8. Initial demonstration of an off-
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expression systems for several year
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accumulation of protein products, i
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Fungal Conversion of Agricultural W
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Fungal Conversion of Waste Glucose/
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Summary and Conclusions We demonstr
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are shown in Figure 1(a) and 1(b),
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Anchorage-Independent Growth (% con
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selection of seedlings demonstratin
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NMR-Based Structural Genomics Micha
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Solution-State Structure and Fold-C
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Plant Root Exudates and Microbial G
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Summary and Conclusions • The gre
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Jones-Oliveira JB, JS Oliveira, HE
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• securely moves files to a targe
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Plenary invited lecture, “The Ele
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Figure 1. X3DGEN tetrahedral mesh o
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Figure 5a. OSO volume rendering of
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Development of Models of Cell-Signa
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SOS p 23 EGFR Professor Rodland at
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Oliveira JS, JB Jones-Oliveira, and
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Figure 2. Associating a dataset mar
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to 1) incorporate three-dimensional
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shown in Figure 1. Simulated result
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HostBuilder: A Tool for the Combina
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Invariant Discretization Methods fo
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Graphics, Inc., workstation. The co
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Mixed Hamiltonian Methods for Geoch
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guyanaite, and grimaldiite (see Fig
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in the Environmental Molecular Scie
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Simulation and Modeling of Electroc
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Summary and Conclusions We implemen
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Since the implementation of the gen
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asis of previous performance, perce
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Bioinformatics for High-Throughput
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Summary and Conclusions In previous
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User Cat - Supervisor (client) Anal
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The second goal was to research way
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Figure 1. A visualization technique
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and interactions. The flexibility o
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Figure 4. A filtered version of Fig
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Development of Modeling Tools for J
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Figure 2. Schematic of experimental
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Integrated Modeling and Simulation
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(a) (b) (c) (d) Figure 1. Results o
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Thurman DA. August 2000. Collaborat
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MARC Input initial m esh and result
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(Johnson 1999; Colligan 1999; Gould
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Modeling of High-Velocity Forming f
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Global divergence error 1 10 -14 0
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that users were unlikely to appreci
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Earth System Science
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the lateral extent of the plume so
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Figure 1. (a) - (c) Successive magn
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Component Fabrication and Assembly
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Development of a Low-Cost Photoelec
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elaxations, indicating the adequacy
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Promising chemical durability, as m
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Study Control Number : PN98028/1274
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High Power Density Solid Oxide Fuel
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Hybrid Plasma Process for Vacuum De
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Matson DW, PM Martin, WD Bennett, J
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We showed the proof-of-principle ap
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Bandgap Energy (eV) 2.9 2.85 2.8 2.
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Ultrathin Electrolyte Test Results
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Detailed Investigations on Hydrogen
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identified low energy step structur
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Development of Novel Photo-Catalyst
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-2 -1 Energy (eV) 0 1 2 Cu2O SrTiO3
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Here, we perform adsorption and des
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exceed those in the all-metal devic
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Intensity (a.u.) 0 100 200 300 400
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integrated voltage (V) 0.10 0.08 0.
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The first step was to implement thi
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Spontaneous Formation of Cu2O Nano-
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Actinide Chemistry at the Aqueous-M
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Figure 5. Close-up atomic force mic
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to 300°C and 400°C. Unfortunately
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Summary and Conclusions Transmutati
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Advanced Calibration/Registration T
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Figure 1a. Violet filter Figure 1b.
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Autonomous Ultrasonic Probe for Pro
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containing nitrous oxide, an optica
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Chemical Detection Using Cavity Enh
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Figure 3 is a color rendered simula
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appropriate study has been performe
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Exploitation of Conventional Chemic
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Figures 3 and 4 illustrate the impa
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enefits of using a modified spread-
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Single Channel Signal 0.0025 0.0020
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Therefore, in order to extract the
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A next-generation technology is nee
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Wind Dir. Figure 2. Negative ion co
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Volumetric Imaging of Materials by
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amplitude and peak frequency change
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Figure 3. 13 C NMR spectrum of corn
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Approach Two flow loops, one that o
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Modification of Ion Exchange Resins
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Permanganate Treatment for the Deco
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minimized by medium exchange. After
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Figure 1. Thermogravimetric analysi
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Validation and Scale-Up of Monosacc
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Concentration (g/100g solution) Con
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Analysis of High-Volume, Hyper-Dime
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ecent figure of merit values. Shoul
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Probabilistic Methods Development f
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a) Traditional PCA-based process co
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Acronyms and Abbreviations 2-D two-
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PNNL-13501 - Pacific Northwest National Laboratory

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