PNNL-13501 - Pacific Northwest National Laboratory

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Interrelationships Between Processes Controlling Loading Level, Release Rate, and Biological Activity of Contaminated Porous Media Study Control Number: PN00061/1468 Robert G. Riley, Christopher J. Thompson Hydrophobic organic contaminants are common sources of subsurface contamination at DOE and other federal sites. A better understanding of the magnitude and behavior of hydrophobic organic contaminants resistant fractions could 1) enhance the rationale for using more cost-effective, passive cleanup options (e.g., natural attenuation) at DOE sites, and 2) lead to improved approaches for evaluating soil/sediment organic contaminant analysis methods. In this project, circulating supercritical carbon dioxide is evaluated as a laboratory method for rapidly aging soils/sediments and investigating the behavior of hydrophobic organic contaminants resistant fractions. Project Description The objective of this project was to evaluate the potential for supercritical fluid technology to simulate on a laboratory time scale (hours to days) the natural aging process (the interaction of contaminants with soils and sediments over several years). Phenanthrene (a hydrophobic organic contaminant) was loaded onto Hanford formation soil using supercritical carbon dioxide. Aqueous desorption of phenanthrene from the loaded soil in laboratory columns showed release behavior consistent with what would be expected for hydrophobic organic contaminants releasing from a naturally aged soil or sediment. Of particular interest was the demonstration of the presence of a phenanthrene resistant fraction controlled by adsorption and diffusion processes in the organic carbon fraction of the soil. The results of this project suggest that application of the supercritical fluid technology to a broader range of soils and sediment types (such as those found across the DOE complex) would be possible with improved system robustness and parameter modification. Introduction A hydrophobic organic contaminant resistant fraction is defined as that fraction of hydrophobic organic contaminants that is slowly released to an aqueous phase (groundwater). Hydrophobic organic contaminant resistant fractions are generated over years (decades) of interaction of contaminants with soils and sediments under unsaturated and saturated conditions. Hydrophobic organic contaminants that have been in contact with soils, sediments, and aquifer solids for many years typically exhibit very slow releases to the environment (such as vadose zone unsaturated moisture or groundwater) as a result of the presence of resistant fractions within these 230 FY 2000 <strong>Laboratory</strong> Directed Research and Development Annual Report materials. Current scientific thinking suggests that organic matter diffusion is a major mechanism responsible for the presence of resistant fractions resulting in slow release of contaminants from geosorbents that contain organic carbon. This raises questions about the influence of resistant fractions on the availability of hydrophobic organic contaminants to the environment and how this relates to soil and sediment quality criteria for hydrophobic organic contaminants and remediation cleanup goals. As a consequence of sorption to soils or sediments and subsequent slow release, the resistant fractions of hydrophobic organic contaminants may be significantly less leachable by water and less toxic as measured by simple tests. Fate, transport, and risk assessment models all contain terms for desorption; therefore, an understanding of the dynamics of hydrophobic organic contaminant resistant fractions is crucial to their success. Ignoring the magnitude of a hydrophobic organic contaminant resistant fraction and its influence on slow kinetics can lead to an underestimation of the true extent of adsorption, false predictions about the mobility and bioavailability of contaminants, and perhaps the wrong choice of cleanup technology (Pignatello and Xing 1996; Luthy et al. 1997). Classes of hydrophobic organic contaminants most commonly found in DOE site soils and sediments subject to cleanup include fuel hydrocarbons, chlorinated hydrocarbons, and polychlorinated biphenyls (Riley and Zachara 1992). Understanding the magnitude and behavior of resistant fractions could lead to the development of more realistic release criteria that reduce the costs of remediation of sites contaminated with these chemicals. Higher concentrations of contamination may be allowed to remain in soils and sediments in meeting site closure requirements. Of particular interest is the application of natural attenuation as a remediation
strategy option at DOE sites (Brady et al. 1999). The first comprehensive assessment of natural attenuation for groundwater cleanup was recently reported (Macdonald 2000). A key assumption made in measuring the potential success of natural attenuation is the likelihood that release of hydrophobic organic contaminants from resistant fractions in the subsurface environment occur on time scales commensurate with natural attenuation process rates (such as microbial degradation). Growing acceptance of the natural attenuation option by regulators and the public as a viable cleanup option will depend on being able to demonstrate such assumptions are correct suggesting that there would be acceptable risk in its application. One method for providing support for acceptable risk would be to quantify the magnitude of the resistant fractions for different hydrophobic organic contaminant classes for a range of soil and sediment types found across the DOE complex. Unfortunately, laboratory study of hydrophobic organic contaminant resistant fractions has been confounded by the inability to accurately evaluate the performance of traditional analytical methodologies to quantify resistant fractions in naturally aged soils and sediments. Traditional methods for artificially aging soils and sediments have proven inadequate because contact times require years for adsorption and diffusion processes to achieve the extent of contaminant penetration found in naturally aged soils and sediments. These problems might be overcome by use of supercritical carbon dioxide for loading soils and sediments with hydrophobic organic contaminants. The solubility of hydrophobic organic contaminants in supercritical carbon dioxide is controllable through the adjustment of temperature and pressure. The favorable properties of supercritical carbon dioxide (i.e., high diffusivity and low viscosity) have the potential for allowing rapid incorporation of hydrophobic organic contaminants into the natural organic component of soils and sediments. Results and Accomplishments Phenanthrene was loaded onto nonporous glass beads and a Hanford formation soil using the closed loop supercritical carbon dioxide system. Both materials had similar surface areas (2 versus 9 m 2 /g), and the Hanford soil had an organic carbon content of 0.03%. Phenanthrene rapidly established equilibrium with the nonporous beads with no organic carbon content. In contrast, the Hanford formation soil showed a continuous slow uptake of phenanthrene likely attributable to adsorption/diffusion into the soil organic matter (Figure 1b versus 1a). Phenanthrene continued to adsorb (diffuse) into the Hanford soil after 24 hours of exposure (Figure 1b versus 1c). Adsorption and diffusion into the organic matter was expected to be more extensive in the 24-hour loaded Hanford soil than the 5-hour loaded Hanford soil. Differences in resistance of phenanthrene to aqueous soil column leaching was expected to be observed between 5-hour and 24-hour aqueous desorption experiments. After approximately 7 hours, desorption occurred slower for the 24-hour loaded soil than for the 5-hour loaded soil (Figure 2). Differences in the extent of adsorption/diffusion into Hanford soil organic matter (5-hour versus 24-hour loading) are likely responsible for differences in the observed leachate behavior. Evidence of a greater resistant fraction was demonstrated for the 24-hour loaded soil. Figure 1. Supercritical fluid loading profiles for nonporous glass beads and Hanford soil Figure 2. Aqueous desorption of phenanthrene from 5-hour and 24-hour loaded Hanford soil Summary and Conclusions Phenanthrene artificially loaded onto Hanford Site soil samples showed release behavior consistent with what would be expected for hydrophobic organic contaminants releasing from a naturally aged soil or sediment. The artificially aged soils demonstrated the presence of a Earth System Science 231
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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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98 99 100 6 7 10 3 1 12 11 15 16 17
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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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Development of a Preliminary Physio
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Development of a Virtual Respirator
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Figure 3. Use of the chest cavity a
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Examination of the Use of Diazolumi
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Indoor Air Pathways to Nuclear, Che
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Source Building Release Observed re
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To illustrate the potential impact
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Non-Invasive Biological Monitoring
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Materials Science and Technology
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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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