PNNL-13501 - Pacific Northwest National Laboratory

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minimized by medium exchange. After the preconcentration step, the complex sample matrix was replaced by a clean electrolyte solution (carrier solution) and the stripping step was conducted in the same electrolyte solution as the standard. This makes the FI/SWASV system suitable for analysis of Tc in complex sample matrices (i.e., nuclear waste). In the future, the electrochemical detection approach will be compared and combined with the automated radiochemical monitoring technique that is currently being developed at Pacific Northwest National Laboratory. References Wang J. 1995. “Electrochemical sensors for environmental monitoring: A review of recent technology.” In Recommendations on the Development of Chemical Sensors and Field Deployable Instrumentation for DOE Needs. http://www.cmst.org Yuehe L, R Zhao, KD Thrall, CA Timchalk, WD Bennett, and DW Matson. 1999. “Integration of microfluidics/ electrochemical system for trace metal analysis by stripping voltammetrey.” In Proceedings of SPIE, Microfluidic Devices and Systems, Vol 3877, pp 248-256. Separations and Conversions 435
Thermochemical Methods for Measuring Ligand-Actinide Ion Binding Strength Study Control Number: PN00087/1494 Gregg J. Lumetta, Richard L. Sell, Bruce K. McNamara Safe management and disposal of highly radioactive spent fuel is a major problem threatening the future viability of nuclear energy. Chemical processing to separate and remove long-lived radionuclides before disposing of the spent nuclear fuel in geologic repositories would significantly improve the post-closure performance of these repositories. The results of this project expand the tools available for developing highly specific separating agents for actinide ions. Project Description Thermochemical methods are being employed to quantitatively determine the binding enthalpy for MLn complexes, where M is a lanthanide or actinide element and L is a ligand of the type that might form the basis of an extractant (an amide). The key tools employed in this study are differential thermal analysis and thermogravimetric analysis. Complementary spectroscopic measurements are conducted to fully characterize the chemical systems being examined. Introduction Actinide separations is an important scientific and technological research area because spent nuclear fuel contains dangerous levels of long-lived radionuclides. Coordination chemistry forms the basis for the development of efficient metal ion separations, and quantum leaps in efficient separation will hinge on understanding structure-function relationships central to coordination chemistry. This is especially true for the actinide ions. The results of this project expand the tools available for developing highly specific separating agents for actinide ions. The work has focused on applying direct thermochemical methods for measuring the thermodynamics of binding for ligands to actinide and other metal ions. Approach In this work, we applied thermochemical methods to quantitatively determine the binding enthalpy for MLn complexes, where M is a lanthanide or actinide element, and L is a ligand of the type that might form the basis of an extractant (an amide). The enthalpy of the following type of reaction is measured. MXzLn → MXz + nL 436 FY 2000 Laboratory Directed Research and Development Annual Report The key tools employed in this study have been differential thermal analysis and thermogravimetric analysis (TGA). Complementary spectroscopic measurements have been be conducted to fully characterize the chemical systems being examined. Results and Accomplishments The decomposition of NdCl3L (L = N,Ndimethylformamide [DMF] or N,N-dimethylacetamide [DMA]) compounds has been investigated by thermogravimetric analysis and differential thermal analysis, coupled with Fourier transform infrared (FTIR) spectroscopy. When heated in air, the NdCl3⋅L (L = DMF or DMA) compounds decompose by a mechanism involving the oxidation of the amide ligand. Figure 1 presents the TGA data for the thermal decomposition of NdCl3·DMF in air and the species identified by Fourier transform infrared in the off-gas. When NdCl3·DMF is heated from 80 to 150°C, TGA indicates a complex series of weight losses. Fourier transform infrared analysis of the off-gas indicates that these mass losses are from the release of water and methanol. Release of DMF becomes evident at ~155°C, although the DMF release is gradual from 155 to 270°C. From 270 to 340°C, a more rapid mass loss occurs. All of the DMF is released by the time the sample is heated to 340°C. Gas evolution becomes more complex during the accelerated mass loss between 270 and 340°C. In addition to DMF, HCl and CO2 are evident in the off-gas, indicating combustion of DMF. Similar to NdCl3·DMF, water and methanol are released in a complicated series of steps when NdCl3·DMA is heated to 165°C in air. DMA is first evident in the offgas at about 200°C. The DMA loss occurs primarily in two regimes. The first occurs from 270 to 310°C. In this regime, free DMA and a small amount of CO2 and H2O are evident in the off-gas. However, as the temperature is
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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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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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Biogeochemical Processes and Microb
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Analyses of populations of viable a
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The first task was to establish fiv
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purged for 2 minutes. The gas sampl
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developing code architecture to min
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Berkowitz, CM. June 2000. “Atmosp
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environmental monitoring, 2) portab
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corresponded to a current density o
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Enhancing Emissions Pre-Processing
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Environmental Fate and Effects of D
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nitrogen and unpredictable eutrophi
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Figure 1. Ordinary kriging of 2 m d
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precipitation of calcite occurred i
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Interrelationships Between Processe
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phenanthrene resistant fraction con
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injection of an immiscible gas phas
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still some key kinetic issues that
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Application of a Crop Model The res
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The Nature, Occurrence, and Origin
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Particle number concentration, 1/cm
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geometry optimized AlOOH and FeOOH
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allowable parameters using thermody
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TCE + 3H + + 3Fe 2+ Fe)=> acetylene
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Use of Shear-Thinning Fluids for In
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concentration of 0.5% AMX was the m
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Roberts AL, LA Totten, WA Arnold, D
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tetra-scale computing, envisioned a
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Energy Technology and Management
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Figure 2. Setup for the second expe
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phase. The algorithms will be teste
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[Pb-212]/[Pb-212] final 100 10 1 0.
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Plasma Particle Dielectric Fiber El
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(species, sub-species, and sex), sp
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Figure 3. Relative risk of bone and
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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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