PNNL-13501 - Pacific Northwest National Laboratory

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The Nature, Occurrence, and Origin of Atmospheric Aerosols and Their Role in Gas-Particle Chemistry Leonard A. Barrie, Herman Cho, Greg Patton, Michael Alexander, Chris Aardahl, V. Shuttahanandan, Don Baer, Dan Gaspar, Robert Disselkamp, James Cowin, Alex Laskin Study Control Number: PN00086/1493 This research enhances the Department of Energy’s ability to understand and manage problems involving atmospheric aerosol pollution related to energy production through application of sophisticated measurement capabilities. It contributes to a national effort to reduce the impacts of aerosols on human health, urban smog, visibility, and climate. Project Description Pacific Northwest National Laboratory staff are involved in the application of aerosol and related gas measurement methodologies to research on aerosol-related environmental problems associated with energy production. Measurement capabilities and methods are developed based on particle-induced x-ray emission spectrometry, mass spectrometry, nuclear magnetic resonance, laser spectroscopy, and micro-particle devices. These will be applied to yield new insight into the nature, occurrence, and origin of atmospheric aerosols and their role in gas-particle chemistry through measurements at the Laboratory and as part of Department of Energy research programs. Measurements are adapted for use in field campaigns using the Department of Energy research aircraft facility. Introduction The objective of this research is to apply the analytical capability of the Pacific Northwest National Laboratory to better understand, through laboratory and field measurement research, the important role of atmospheric particulate matter (aerosols) in environmental issues such as human health, urban smog, visibility, and climate change. Approach Specific hypotheses driving this project are that 1. Significant insights into the elemental composition and organic fraction of ambient aerosols—are gained using a combination of nuclear magnetic resonance spectroscopy, particle-induced x-ray emission spectroscopy, membrane ion trap mass spectrometry, 242 FY 2000 Laboratory Directed Research and Development Annual Report micro-particle analysis, and conventional aerosol measurement techniques. 2. Proton transfer mass spectrometry and ion trap mass spectrometry—can be used to measure the transformation of gaseous precursors of aerosols and improve understanding of aerosol production mechanisms. Specific activities incorporated in the project to test these hypotheses include 1. Nuclear magnetic resonance spectroscopy of aerosol extracts to investigate speciation of water soluble organics yielding insight into the origin of aerosols. 2. Volatile organic gas measurements using proton transfer mass spectrometry and membrane separation-ion trap mass spectrometry to study the mechanism of gas to particle conversion. 3. Proton-induced x-ray emission and proton elastic scattering analysis of atmospheric aerosols using the Environmental Molecular Sciences Laboratory tandem ion accelerator to make high time resolution multi-elemental aerosol analyses. 4. High resolution individual particle analyses to determine the origin and nature of atmospheric particles that enter the lung and potentially cause respiratory problems. 5. Nucleation detection of atmospheric mercury vapor to study the exchange of atmospheric mercury between Earth and atmosphere.
Results and Accomplishments This project effectively began in May 2000. After 5 months the following progress has been made on the following five activities: 1. Nuclear Magnetic Resonance Spectroscopy. A research plan was prepared. Concentrated fogwater samples collected by the research group of Professor S. Fuzzi who had attempted similar measurements (Descari et al. in press) were analyzed for soluble carbonaceous aerosol constituents (Figure 1). An aerosol high volume sampler for sample collection and a continuous PM2.5 aerosol mass sampler for high time resolution event characterization were acquired. Figure 1. A proton decoupled 13 C nuclear magnetic resonance (NMR) spectroscopy spectrum of fogwater measured at 75 MHz. The sample was collected in the polluted Po River valley of Italy. The frequency scale is expressed as a parts per million (ppm) shift from the reference 13 C signal of tetramethylsilane (TMS). Inset spectrum: Expansion of the alcohol region showing the power of this technique for even higher resolution than displayed. Identification of compounds by the frequency and their carbon content by the peaks makes this nondestructive analysis technique a powerful analytical tool for characterizing complex organic aerosol mixtures. 2. Volatile Organic Gas Measurements Using Proton Transfer Mass Spectrometry and Membrane Separation-Ion Trap Mass Spectrometry. Collaboration with the world’s leading authority on proton transfer mass spectrometry was initiated through a visit by Professor Werner Lindinger (U. of Innsbruck) to the Laboratory in June 2000. A plan was developed whereby M. Alexander will make a technical visit to Prof. Lindinger’s laboratory, we will acquire a proton transfer mass spectrometer, and a graduate student of Prof. Lindinger will spend 1 to 2 months at Pacific Northwest National Laboratory in a collaborative effort to apply the instrument to aircraft measurements. In late September, an experienced atmospheric instrumental chemist was interviewed for a research position that will expedite the application of this instrumentation. 3. Proton-Induced X-Ray Emission and Proton Elastic Scattering Analysis of Atmospheric Aerosols. The tandem ion linear accelerator facility was developed for high time resolution chemical analysis of atmospheric aerosols. An exchange of visits with Professor T. Cahill of the University of California at Davis and the DELTA group was followed by joint participation in aerosol collection and comparative multi-elemental analyses during the Texas 2000 Air Quality study (August and September 2000). An x-yz manipulator was installed on the accelerator’s beam end and tests with artificial aerosol samples were performed in preparation for analysis of ambient aerosols. Duplicate analysis of the same samples from Houston by Pacific Northwest National Laboratory and the DELTA group will mark the beginning of our multi-elemental capabilities. 4. High Resolution Individual Particle Analysis System. This activity involves the analysis of individual aerosol particles after collection on carbon films using automated scanning electron microscopy and on cascade impactor stages by time-of-flight secondary ion mass spectrometry. Samples from the Texas 2000 Air Quality study (August and September 2000) were collected. This proposal supported the time-of-flight secondary ion mass spectrometry analysis and resulted in a presentation by D. Gaspar at the American Vacuum Society Annual Meeting. 5. Nucleation Detector for Atmospheric Mercury Vapor. Proof-of-concept experiments were conducted to demonstrate the feasibility of two-photon laser excitation and nucleation detection of elemental mercury (Figure 2). The methodology shows sensitivity at better than 0.1 ng Hg /m 3 . Atmospheric Hg 0 is 1 to 5 ng Hg /m 3 . Summary and Conclusions In 5 months, a program of aerosol measurement research has been initiated within the Fundamental Science Division of Pacific Northwest National Laboratory. In this short period, collaborations with two internationally recognized measurement research groups have been established and the powerful analytical tools of the Environmental Molecular Sciences Laboratory mobilized Earth System Science 243
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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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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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PNNL-13501 - Pacific Northwest National Laboratory

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