PNNL-13501 - Pacific Northwest National Laboratory

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Study Control Number: PN00088/1495 Tracer Development for Tank Leak Detection Richard J. Cameron Tanks containing chemical and radioactive waste are the focus of stabilization and remediation efforts at DOE sites. These efforts require a reliable method of tank leak detection and quantification. Partitioning interwell tracer test technology provides reliable leak detection and quantification capabilities, immune to electrical and electromagnetic interference that can affect the accuracy of leak detection. Project Description Partitioning interwell tracer tests (PITTs) have been developed and field-proven as a new technology for detecting and quantifying nonaqueous-phase liquids at hazardous waste sites. <strong>Laboratory</strong> studies and field tests have proven that soil moisture content also can be quantified using partitioning interwell tracer tests. Repeated partitioning tracer tests beneath Hanford Site waste tanks provide soil moisture measurements that indicate a tank leak, and can quantify the size of the leak. Additionally, the constituents of tank wastes include volatile vapors (Agnew 1997) such as ammonia or radioactive gases ( 135 Xe) that may be detected in the partitioning interwell tracer tests advection flowfield, thus providing an additional (and perhaps faster) method of leak detection. We formulated mathematical models of tracer behavior under the fast-flow conditions required for timely leak detection. We also conducted laboratory experiments to confirm the theoretical predictions of tracer partitioning behavior under nonequilibrium transport conditions. A full-scale field test of soil moisture measurement in Hanford soils may be performed during in the next year of study on this project. Introduction The partitioning interwell tracer tests technology is carried out by establishing a flowfield in the subsurface using a system of wells that inject and extract air (for vadose zone tests or water (for saturated zone tests). A suite of conservative (non-partitioning) and partitioning tracers are injected and their elution curves analyzed by temporal-moment methods to determine the quantity of the component of interest in the subsurface. Gaseous tracers that partition into water can be used with a conservative tracer to quantify soil moisture. In the past, these tests have been carried out under equilibrium conditions, with the flow between wells slow enough for 248 FY 2000 <strong>Laboratory</strong> Directed Research and Development Annual Report mass-transfer processes to achieve equilibrium. Timely detection of tank leaks requires fast-flow conditions between injection and extraction wells that produce nonequilibrium mass-transfer conditions. This project focuses on the investigation and development of gasphase tracer suites for soil moisture quantification under nonequilibrium transport conditions, and the investigation of nonequilibrium partitioning properties of gaseous and vapor-phase tank-waste components for their use in tank leak detection. Previous partitioning interwell tracer tests have demonstrated the capability to accurately quantify even small amounts of nonaqueous-phase liquids in the subsurface. With the use of a water-partitioning tracer whose behavior under nonequilibrium transport conditions has been accurately characterized, partitioning interwell tracer tests should be able to detect and quantify a tank leak of well under 1500 gallons. In the presence of a leak, small amounts of radioactive gases and volatile waste components such as ammonia and butanol may be advected along the partitioning interwell tracer tests flowpath. Characterization of the nonequilibrium partitioning properties of these waste components will provide an estimate of retardation times and elution concentrations. A complete partitioning interwell tracer tests underneath a tank requires 4 to 12 hours to provide leak information. Since waste-tank components may be detected at any time during the partitioning interwell tracer tests such measurements provide early indication of a tank leak. The partitioning interwell tracer tests technology is not affected by heavy machinery, piping systems, or other metal artifacts in the vicinity of the tank. This is in sharp contrast to most electric and electromagnetic methods of leak detection that are adversely affected by these artifacts and suffer a loss of sensitivity, resolution, and an increase in the possibility of false positive leak-detection results.
Approach The adaptation of partitioning interwell tracer tests technology to tank leak detection requires the characterization of tracer and tank-waste partitioning behavior under nonequilibrium mass-transfer conditions and an analysis of flow-field design requirements. The partitioning interwell tracer tests concept is illustrated in Figure 1. A sample data analysis is shown in Figure 2. The proposed flow velocity for the partitioning interwell tracer tests would sweep one pore volume (the area under the tanks) every 4 to 12 hours. While tracer behavior can give real-time indications of a leak after only a short time, Tracer Injection Well Inject Tracer Extract Tracer Tracer Single Shell Tank Leak Tank Waste Tank Waste Vapor Conservative Tracer Partitioning Tracer Tracer Extraction Well Figure 1. Partitioning interwell tracer test for tank leak detection Experimental Results of Partitioning Tracer Test in a Soil Column at 3.83 cc/min Methane Difluoromethane Mean Residence Volume (cc) 37.6 61.7 % Tracer Recovered 93% 95% Retardation Factor 1.00 1.64 Water Saturation - 0.274 Mean Residence Time (hrs) 0.16 0.27 Tracer Co ncentration (pp m w 1000 100 10 1 0.1 M ethane (954 ppm inj.) Difluoromethane (1 132 ppm in j.) 0 50 100 150 200 250 Volum e (ml) Figure 2. Data from a fast-flow soil-column experiment, using methane as the conservative tracer and difluoromethane as the partitioning tracer. Temporal moment analysis measures the difference between the centroids under the elution curves to provide water saturation and mean residence volume (or pore volume). Note the higher concentration peak of the conservative tracer, and the lower peak concentration and higher tail concentration of the partitioning tracer; this is characteristic of partitioning tracer behavior. accurate quantification of the leak might require two or three swept pore volumes. One method of implementing the leak-detection technology is to use tank-waste components as leak detectors, and use the partitioning interwell tracer tests as a quantification method after a leak has been detected through the presence of volatile waste components or radioactive gases in the advection exhaust stream. Since tracer behavior governs the shape of the elution curve required for soil moisture quantification, the partitioning behavior of the tracer and its elution under conditions of exposure to actual tank-waste saline solutions must be fully understood before tank leaks may be accurately quantified. As this project continues, tracer behavior will be investigated both by theoretical studies that predict tracer behavior using mathematical modeling and thermodynamic approximations of partitioning behavior. Soil-column experiments using representative soil samples with varying moisture contents will be flushed at high flow rates with tracers (see Figure 3) and the elution curves will be studied for their adherence to theoretical models. The alterations of water-partitioning behavior in the presence of the concentrated metallic salts, ammonia, and organics present in the tank wastes are being investigated by thermodynamic modeling methods, and may soon be the subject of soil-column experiments using simulated tank wastes to experimentally quantify the non-ideal partitioning behavior of potential tracers. Non-Equilibrium Partitioning Experiments Chromatographic Column Apparatus N 2 Tracer Gas Flow Controller Sample Loop Chromatographic Column Gas Chromatograph (packed with soil) •Measure partitioning and elution in fast-flow regime •Values measured in experiments: –Gas flow rate –Water saturation of soil in chromatographic column –Swept pore volume –Tracer elution –Tracer recovery percentage Figure 3. Apparatus for nonequilibrium tracer characterization experiments using soil-column chromatography The soil moisture in the area under the tanks swept by the partitioning interwell tracer tests will affect the elution behavior and peak concentration of gaseous tank-waste components used as adjunct leak detection gases. Potential leak-detection gases will be screened for Earth System Science 249
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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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Page 226 and 227: Enhancing Emissions Pre-Processing
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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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