Influences of Biomass Compositions, Particle Sizes, and Operating conditions on Biomass Fast Pyrolysis
Presented by LRST at the AIChE 2020 Annual Meeting, Virtual, 11/15
Lu, Liqiang↗
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Heterogeneous Nucleation Drives Particle Size Segregation in Sequential Ozone and Nitrate Radical Oxidation of Catechol
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54 ENVIRONMENTAL SCIENCES↗
Measuring ejecta particle size distributions using dark field imaging versus light field imaging
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73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
Morphological Characterization of Uranyl Fluoride Particles via Atomic Force Microscopy
Uranium hexafluoride (UF 6 ) undergoes a rapid hydrolysis reaction when exposed to atmospheric water. In addition to producing hazardous HF gas, the hydrolysis reaction produces uranyl fluoride (UO 2 F 2 ), a radioactive solid phase particulate material. Because of the technological utility of UF 6 in the nuclear fuel cycle, understanding the transport properties of UO 2 F 2 aerosol produced via UF 6 hydrolysis is important for accident scenarios. Moreover, the fundamental chemical and physical properties of the UF 6 hydrolysis reaction are not completely understood. Recently, several experiments on the aerosol phase properties of UO 2 F 2 produced in this way have shown that under most relevant conditions, the particle size distribution (PSD) of UO 2 F 2 can be extremely small, approximately 3 to 5 nm, which is well below the threshold that can be routinely observed via scanning electron microscopy (SEM). Although readily observable in the aerosol phase, observation of nanometer-sized particles in the condensed phase (i.e. deposited on surfaces) remains a challenge. Here, in this study, we have used atomic force microscopy (AFM) to study the PSD and morphological characteristics of UO 2 F 2 deposited at low and high concentrations under different humidity conditions, a primary variable in the hydrolysis reaction. Here, we find strong agreement between PSD measured in the aerosol phase via scanning mobility particle sizing and PSD measured via AFM, with particle sizes peaked below 4 nm for low-humidity conditions. At higher humidity, the distribution is centered around 5 to 10 nm but extends up to 20 nm. These results are in stark contrast to previous measurements using SEM that show PSD on the order of 300- to 1000-nm particle sizes; moreover, these are the first direct measurements of individual particles of UO 2 F 2 having been produced via UF 6 hydrolysis deposited on surfaces. These measurements, therefore, open a new avenue for collecting and detecting UO 2 F 2 in the condensed phase and further refine the PSD, which is critical for environmental transport determinations.
Uranium hexafluoride↗
Colloidal Behavior of Plutonium Oxide in Concentrated Electrolyte Solutions
The Hanford Site in Washington State manages legacy high-level radioactive waste streams that display major chemistry and engineering challenges, including the high salt levels and pH values that correspond to conditions under which many classical concepts describing chemical reactivity cannot be applied. One particular challenge that needs to be tackled at Hanford is that Pu concentrations, [Pu], in the soluble phases of the tank wastes are higher than expected based on the solubility of crystalline PuO2, which is widely accepted to be caused by the formation of PuO2 colloid, consisting of nano- to submicron-sized particles (PuO2 NPs). Fundamental research underpinning the behavior of PuO2 NPs under conditions not only relevant to the Hanford tank waste but at high ionic strength in general is needed to reliably predict the chemical reactivity of PuO2 NPs and develop engineering solutions to safely and efficiently process high-level radioactive waste into forms suitable for long-term storage. In this work, we study the behavior of PuO2 NPs (particle size ~100 nm) under high ionic strength conditions by reacting it with highly concentrated (up to 5 M) salt solutions. We explore different electrolyte compositions to elucidate the impact of different anions (NO3-, Cl-, ClO4-, SO42-, C2O42-, CO32-) on the stability of PuO2 NP in the acidic and alkaline pH regime. PuO2 NP aggregation and precipitation as function electrolyte concentration is tracked by a combination of liquid scintillation counting, dynamic light scattering for determination of particle size distributions, and zeta potentials as a proxy for particle charge. At acidic pH, electrolytes containing non-coordinating anions, such as NaNO3, NaCl, and NaClO4 mostly stabilize PuO2 NPs over a large electrolyte concentration range, showing only subtle differences in their reactivity. Other electrolyte anions show a more pronounced effect on the PuO2 NP stability: SO42-, binds directly to the particles’ surface, reverses the particle charge, and precipitates the PuO2 NPs efficiently even at intermediate sulfate concentrations (>0.1 M). In contrast, C2O42- is found to lead to high [Pu] in solution, in the milli-molar range, even at mildly acidic pH (~4). Thermodynamic modeling of the dissolved Pu concentrations using PHREEQC is unable to predict the observed [Pu] in the acidic pH regime, supporting the influence of colloids in maintaining elevated [Pu]. It is noteworthy that the current thermodynamic databases do not include constants for colloidal Pu phases and cannot accurately predict many of the high ionic strength solutions relevant to this work. The mechanisms and models responsible for these observations will need further investigation in the future. At high pH values (~12), PuO2 NPs exhibits classical sol-gel chemistry, meaning that upon destabilization of the colloidal sol, for example by addition of concentrated NaOH, highly porous and viscid PuO2 coagulates are formed that consist of a three-dimensional network likely held together by physical interactions. The PuO2 NP coagulate shows no significant reversibility of the aggregation when contacted with concentrated brines; however, PuO2 NPs can be efficiently resuspended in solution by addition of diluted electrolytes, alkaline solutions containing high amounts of carbonate, or simple addition of water. Especially carbonate is shown to stabilize PuO2 NPs in solution at high pH, characterized by stable colloidal suspensions that are resistant against sedimentation during centrifugation. Thermodynamic modeling of the carbonate system was able to predict an increasing dissolved Pu concentration with increasing carbonate concentration. However, the model was profoundly sensitive to the fixed redox potential and does not include any thermodynamic constants for colloidal Pu species.
Neumann, Julia↗
Micron Size NaCrO 2 Particles Enable High‐loading Dry‐processed Electrode for Sodium Ion Batteries
Dry-process fabrication using fibrillatable binder is emerging as a promising method to produce high-loading electrodes for energy storage applications, favored by its cost-efficiency and eco-friendliness. While previous studies have demonstrated the advantages of dry process over the traditional slurry method, there remains a gap in understanding how the particle size of active materials influences the mechanical and electrochemical performance of dry electrodes. In this study, four different particle size NaCrO 2 materials (Average size, S-NCO: 0.6 µm, M1-NCO 1.5 µm, M2-NCO: 4.4 µm, and L-NCO: 9.9 µm) are synthesized to investigate the effect of particle size on dry-processed high-loading electrodes. The findings reveal that the larger micron-sized (>4.4 µm) NCO dry films exhibit significantly improved tensile strength and electrochemical performance, primarily ascribed to the low film porosity, abundant inter-particle connection by the binder, comprehensive carbon coverage, and efficient percolation of the conductive pathway. Notably, a full cell incorporated with a high loading (5.2 mAh cm −2 ) and high active material ratio (96.5 wt.%) L-NCO film electrode demonstrates promising cycling stability and rate capability. Furthermore, these results provide valuable insights regarding the design and fabrication of dry-processed electrodes for future energy storage applications.
25 ENERGY STORAGE↗
Long-Lived Triplet Excited State in a Heterogeneous Modified Carbon Nitride Photocatalyst
Heterogeneous carbon nitrides have numerous advantages as photocatalysts, including strong light absorption, tunable band edges, and scalability, but their performance and continued development are limited by fast charge recombination and an under-developed mechanistic understanding of photodriven interfacial electron transfer. These shortcomings are a result of complex photophysics, leading to rate asynchrony between oxidation and reduction, as well as redox processes driven out of electronic trap states rather than excited states. We show that a well-defined triplet excited state in cyanamide-modified carbon nitride is realized with appropriately sized particles. The utility of this long-lived excited state is demonstrated by its ability to drive a hydroamidation photoredox cycle. By the tuning of the particle size of CN x , the oxidation–reduction photochemistry of carbon nitride may be balanced to achieve a redox-neutral closed photocatalytic cycle. Here, these results uncover a triplet excited state chemistry for appropriately sized CNx particles that preludes a rich energy and electron transfer photochemistry for these materials.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Observations of particle number size distributions and new particle formation in six Indian locations
Atmospheric new particle formation (NPF) is a crucial process driving aerosol number concentrations in the atmosphere; it can significantly impact the evolution of atmospheric aerosol and cloud processes. This study analyses at least 1 year of asynchronous particle number size distributions from six different locations in India. We also analyze the frequency of NPF and its contribution to cloud condensation nuclei (CCN) concentrations. We found that the NPF frequency has a considerable seasonal variability. At the measurement sites analyzed in this study, NPF frequently occurs in March–May (pre-monsoon, about 21% of the days) and is the least common in October–November (post-monsoon, about 7% of the days). Considering the NPF events in all locations, the particle formation rate (J SDS ) varied by more than 2 orders of magnitude (0.001–0.6 cm –3 s –1 ) and the growth rate between the smallest detectable size and 25nm (GR SDS-25nm ) by about 3 orders of magnitude (0.2–17.2nm h –1 ). We found that J SDS was higher by nearly 1 order of magnitude during NPF events in urban areas than mountain sites. GR SDS did not show a systematic difference. Our results showed that NPF events could significantly modulate the shape of particle number size distributions and CCN concentrations in India. The contribution of a given NPF event to CCN concentrations was the highest in urban locations (4.3 × 10 3 cm –3 per event and 1.2 × 10 3 cm –3 per event for 50 and 100nm, respectively) as compared to mountain background sites (2.7 × 10 3 cm –3 per event and 1.0 × 10 3 cm –3 per event, respectively). We emphasize that the physical and chemical pathways responsible for NPF and factors that control its contribution to CCN production require in situ field observations using recent advances in aerosol and its precursor gaseous measurement techniques.
54 ENVIRONMENTAL SCIENCES↗
Effects of magnetic field annealing on the hard magnetic properties of milled Nd-Fe-B powders
In this study, we report the effect of magnetic field annealing (MA) in relieving the stress induced during the milling of Nd-Fe-B sintered magnets. The effect of MA processing parameters and particle size on the magnetic properties were investigated. Based on the results, magnetic field annealing is more effective in improving the magnetic properties of larger size particles, compared to finer particles. Our computational study on the role of particle surface defects in bi-modal particle distribution agrees with results obtained experimentally. In conclusion, magnetic field annealed powder has been successfully used to develop 4.6 g.cm -3 density bonded magnets with 75 vol% of magnetic powder and polyamide 12 (nylon 12) polymer binder resulting in 11.3 MGOe energy product.
36 MATERIALS SCIENCE↗
Active learning of polarizable nanoparticle phase diagrams for the guided design of triggerable self-assembling superlattices
Polarizable nanoparticles are of interest in materials science because of their rich and complex phase behavior that can be used to engineer nanostructured materials with long-range crystalline order. To understand and rationally navigate the design space of polarizable nanoparticles for self-assembling highly ordered superlattices, we developed a coarse-grained computational model to describe the nanoparticle-nanoparticle interactions in implicit solvent and employ the computationally efficient image method to model many-body polarization interactions. We conducted high-throughput virtual screening over a five-dimensional particle design space spanned by temperature, particle size, particle charge, particle dielectric, and solvent dielectric using enhanced sampling molecular dynamics calculations within an active learning framework to efficiently map out the regions of thermodynamic stability of the self-assembled aggregates. We validate our predictions in comparisons against small angle x-ray scattering measurements of gold nanoparticles surface functionalized with metal chalcogenide ligands. Lastly, we use our validated phase maps to computationally design switchable nanostructured materials capable of triggered assembly and disassembly as a function of temperature and solvent dielectric with potential applications as sensors, smart windows, optoelectronic devices, and in medical diagnostics.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Modeling Rate Dependent Volume Change in Porous Electrodes in Lithium-Ion Batteries
Automotive manufacturers are working to improve individual cell, module, and overall pack design by increasing the performance, range, and durability, while reducing cost. One key piece to consider during the design process is the active material volume change, its linkage to the particle, electrode, and cell level volume changes, and the interplay with structural components in the rechargeable energy storage system. As the time from initial design to manufacture of electric vehicles decreases, design work needs to move to the virtual domain; therefore, a need for coupled electrochemical-mechanical models that take into account the active material volume change and the rate dependence of this volume change need to be considered. In this study, we illustrated the applicability of a coupled electrochemical-mechanical battery model considering multiple representative particles to capture experimentally measured rate dependent reversible volume change at the cell level through the use of an electrochemical-mechanical battery model that couples the particle, electrode, and cell level volume changes. By employing this coupled approach, the importance of considering multiple active material particle sizes representative of the distribution is demonstrated. The non-uniformity in utilization between two different size particles as well as the significant spatial non-uniformity in the radial direction of the larger particles is the primary driver of the rate dependent characteristics of the volume change at the electrode and cell level.
Electrochemistry↗
Statistical Uncertainty of Inhalation Dose Coefficients: Impact of Particle Deposition in ICRP 66 Human Respiratory Tract Model
Inhaled radioactive materials can pose a long-term health concern, as the material can be incorporated into the body’s metabolic pathways and remain in organs and tissues for extended durations. During the retention period, the radioactive material may localize in a source organ and irradiate adjacent target organs and tissues. Distribution of these materials changes over time, requiring biokinetic modeling to evaluate their movement through various tissues and organs. The evolving distribution depends on multiple inputs characterizing the inhaled material, such as particle size and size distribution, particle density, aspect ratio, specific radionuclide, the chemical form, and solubility. In addition, biological parameters such as breathing rate, breathing type (nasal or nasal/oral), respiratory system morphometry, tidal volume, functional residual capacity, and anatomical dead space all influence material transport. These aerosol properties and physiological characteristics of the respiratory tract jointly define a range of initial conditions that influence the time-dependent distribution of radioactive material. To evaluate both uncertainty in the initial conditions of inhalation exposure and the final output (committed effective dose) from biokinetic models, a Python-based software tool, Radiological Exposure Dose Calculator (REDCAL), was developed to propagate uncertainty within the human respiratory tract model. Focusing on deposition fraction uncertainty, the primary objective was to characterize the initial activity distribution across respiratory regions as a function of anticipated particle sizes and distributions. The impact of the deposition fraction uncertainty was propagated to committed effective dose coefficients for selected radionuclides in a companion publication. For each particle size, a lognormal distribution, characterized by its geometric mean as defined within ICRP Publication 66, serves as the basis for introducing uncertainty into the physical processes governing deposition in various lung regions. Finally, this study addresses the deposition process and examines how uncertainty in deposition mechanisms affects activity distribution in the airways, ultimately presenting the expected range and standard deviation of deposited activity as a function of particle size.
International Commission on Radiological Protectio↗
Protecting building occupants against the inhalation of outdoor-origin aerosols
During normal operations, buildings can protect their occupants from outdoor airborne particle hazards of all types, including airborne pollutants. A long-term international research effort has advanced our knowledge of building protection physics. Recently we have developed an operationally efficient, regional-scale methodology - Regional Shelter Analysis - to account for both building protection effects and the typical distribution of people in and among buildings. To provide input to this capability, we estimate here the degree of protection afforded by the currently existing US building stock. Here, we first assemble and summarize the published literature relevant to indoor particle losses including (a) deposition to indoor surfaces, (b) losses that occur when particles penetrate through the building envelope, and (c) heating, ventilation and air conditioning (HVAC) system filtration efficiencies as well as general building operating conditions. Building protection against inhaling particulate hazards varies strongly, by orders of magnitude, according to particle size, airborne particle loss rate, and to a lesser extent building use (occupancy). Protection increases modestly as particle size increases from 0.1 to 1 μm and significantly as particle size increases from 1 to 10 μm. Model results are placed in context with previously reported measurements. Suggestions for future work, including enhanced validation datasets are provided.
63 RADIATION, THERMAL, AND OTHER ENVIRON. POLLUTAN↗
Optimizing Porous Transport Layer Porosity for Proton Exchange Membrane Water Electrolysis
An empirical model is presented that describes anode-side losses related to porous transport layer (PTL) morphology in proton exchange membrane water electrolysis (PEMWE). The model is based on an advanced voltage breakdown analysis that links various overpotentials to PTL morphology. Custom Ti PTLs, spanning uncommonly low porosities (22 - 31%), were fabricated and analyzed with X-ray CT to obtain pore and particle size distributions. Particle size distributions were consistent across samples with an average particle diameter of 12.0?..mu..m, whereas average pore diameters ranged from 6.0 to 7.0?..mu..m. The PTLs were tested in standard PEMWE cell assemblies with anode catalyst loadings of 0.1 mgIr cm-2 to obtain polarization curves, electrochemical impedance spectra, and augmented Tafel analysis. The PTL-dependent anode side losses were deconvoluted and assigned to excess utilization, concentration, ion transport resistance, and electrical contact resistance overpotentials. The data and model reveal an optimal 20 - 28% PTL porosity region where utilization and contact resistance overpotentials are minimized without triggering concentration and ion transport losses related to water deprivation. The optimal PTL porosity depends on the operating current density and is demonstrated at realistic PEMWE water flow rates to establish PTL design guidance for operation at scale.
08 HYDROGEN↗
Evaluation of the Radioactive Material Released in the Harborview Research and Training Building and Some Implications for Emergency Response
On 2 May 2019, during the 137 Cs source recovery operation, a source capsule in a research irradiator containing approximately 77.1 TBq was breached. Based on a geometric reconstruction analysis of the damage to the capsule, approximately 46.3 GBq (0.04%) was impacted by the chop saw (grinder) inside a mobile hot cell on the loading dock at the University of Washington Harborview Research and Training (HRT) Building. A very small fraction of the material impacted, less than 1%, was released from the mobile hot cell and then to the rest of the HRT Building. The objectives of this project were to assess the accidental release of 137 CsCl and its implications related to emergency response methods and the ramifications of 137 CsCl transport. The phenomenology of this event was also compared with past alkali halide dispersal events. The vast number of measurements and samples collected by the remediation contractors, the Department of Energy’s Nuclear Emergency Support Team, and the small number of retrospective samples collected by the authors informed the analysis. The techniques included (1) autoradiography and electron microscopy of samples collected from the HRT Building and the irradiator, (2) 3D visualization of deposition on surfaces and within the ventilation system, and (3) a study of the damage to the source capsule to evaluate the Cs particle size and particle composition due to the grinding accident. Subsequently, the cesium contaminant transport through the numerous pathways in the building was reconstructed to assess the deposition on surfaces as a function of particle size. Furthermore, the implications for emergency response are relevant to data quality and management. A Data Quality Objective guides data collection methods so that they have appropriate accuracy and precision for the intended application. Recommendations were made with respect to the sample collection protocols and archiving of samples.
46 - INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AN↗
Evaluation of the Radioactive Material Release in the Harborview Research and Training Building and Implications for Emergency Response
On May 2, 2019, during the 137 Cs source recovery operation, a source capsule in a research irradiator containing approximately 77.1 TBq was breached. Based on a geometric reconstruction analysis of the damage to the capsule, approximately 46.3 GBq (0.04%) was impacted by the chop saw (grinder) inside a Mobile Hot Cell (MHC) on the loading dock at the University of Washington Harborview Research and Training (HRT) Building. A very small fraction of the material impacted, less than 1%) was released from the Mobile Hot Cell and then to the rest of the HRT Building. The objectives of this project were to assess the accidental release of 137 CsCl and its implications related to emergency response methods and the ramifications of 137 CsCl transport. The phenomenology of this event was also compared with past alkali halide dispersal events. The vast number of measurements and samples collected by the remediation contractors, the Department of Energy's Nuclear Emergency Support Team, and the small number of retrospective samples collected by the authors informed the analysis. The techniques included (1) autoradiography and electron microscopy of samples collected from the HRT Building and the irradiator, (2) 3D visualization of deposition on surfaces and within the ventilation system, and (3) a study of the damage to the source capsule to evaluate the Cs particle size and particle composition due to the grinding accident. Subsequently, the cesium contaminant transport through the numerous pathways in the building was reconstructed to assess the deposition on surfaces as a function of particle size. The implications for emergency response are relevant to data quality and management. A Data Quality Objective (DQO) guides data collection methods so that they have appropriate accuracy and precision for the intended application. Recommendations were made with respect to the sample collection protocols and sample archival.
61 RADIATION PROTECTION AND DOSIMETRY↗
Copper carbon composite wire with a uniform carbon dispersion made by friction extrusion
Copper-carbon composites are a group of materials with excellent mechanical, electrical, thermal, and tribological properties. However, bulk size copper-carbon composites made by the traditional manufacturing processes, like rolling or extrusion, fall short of reaching some of these properties predicted by theory or demonstrated only by samples at centimeter scale or smaller. The two main challenges to the successful scaling-up are: 1) to uniformly disperse carbon in the metal matrix; 2) to avoid degradation due to oxidation or reaction from overheating. In this work, we first demonstrate friction extrusion as a new method to make bulk-size void-free copper-carbon composite wires with homogenized carbon dispersion. Three different carbon varieties, graphite powder, graphene nanopowder, and carbon nanotubes, were added to the copper matrix with the concentration ranging from 0.5 wt% to 15 wt%. Special tooling, processing parameters, and procedures were developed, especially for high carbon content samples. Ten-fold reductions of both copper grain size and carbon particle size were achieved and attributed to the high shear deformation. Energy dispersive X-ray spectrometry indicates the carbon powder was refined to a sub-micron level and uniformly dispersed in the copper matrix. Compared with that of pure copper, the thermal capacity of the composite wire increases by 30 % while density reduces by 29 %.
Friction extrusion, Metal matrix composite, Graphe↗
Filament Extension Atomization for High Solids Loading in Energy Efficient Spray Drying Systems
We demonstrate that we could scale FEA to reach outputs needed by industrial production, while increasing solids loading of the sprayed product by at least 30% and maintaining equal or better spray powder. After testing a wide range of products, in collaboration with industry partners we decided on our primary spray products of dry whey and WPC-80, two common materials processed and sold by US manufacturers with different parameters. We sprayed these with FEA at solids loadings of 70% for dry whey and 45% for WPC-80 with a spray output with particle sizes similar to industrial particles sizes and reduced variation in particle size. We simultaneously scaled up FEA first with a multi-nip with 6 nips surrounding a central roller with parallel axis of rotation and eventually with a tapered design that solved problems we encountered with our initial design. We were able to achieve output from a single array from our first design of up to 4.7 liters per minute (L/min) and from an array of our second multi-nip of 8 L/min exceeding expectations. This demonstrates that FEA technology can indeed be scaled up to meet the needs of industrial production. More arrays can be added as necessary to meet a wide range of spray dryer designs. We also tested FEA to create dried powders from a small scale (10 L/hour of water removal) spray dryer. Though we were not able to produce large quantities of powder from FEA due to challenges in integration, the powder we produced was higher quality and produced from higher solids loading materials. From our technoeconomic analysis we for a typically sized spray dryer, we estimate a 27% cost reduction and 41% energy and carbon reduction for WPC-80 and a 39-57% cost reduction and 52-76% energy reduction for sweet dry whey (depending on the exact product).
32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗