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At least 19 records

Rupturing of Biological Spores As a Source of Secondary Particles in Amazonia

Airborne biological particles, such as fungal spores and pollen, are ubiquitous in the Earth’s atmosphere and play an important role in the atmospheric environment and climate, impacting air quality, cloud formation, and the Earth’s radiation budget. The atmospheric transformations of airborne biological spores at elevated relative humidity remain poorly understood and their climatic role is uncertain. Using an environmental scanning electron microscope (ESEM), we observed rupturing of Amazonian fungal spores and subsequent release of nanometer to submicron size fragments after exposure to high humidity. We find that fungal fragments contain elements of inorganic salts (e.g., Na and Cl). They are hygroscopic in nature with a growth factor up to 2.3 at 96% relative humidity, thus they may potentially influence cloud formation. Due to their hygroscopic growth, light scattering cross sections of the fragments are enhanced by up to a factor of 10. Furthermore, rupturing of fungal spores at high humidity may explain the bursting events of nanoparticles and may provide insight into new particle formation in Amazonia.

Environmental Molecular Sciences Laboratory↗

New Method for the Generation of Secondary Particle Beams at Accelerators

The generation of beams of secondary particles (π and K mesons) at proton accelerators is a difficult scientific and engineering problem. To obtain narrow directional particle beams for experiments, intense extracted proton beams are used, secondary particles (π and K mesons) are generated at an external target, and they are focused and transferred through long magneto-optical channels. In this work, a surprisingly simple method based on a crystal focusing device has been proposed to obtain secondary beams. An experiment on the production of a secondary beam using a crystal has been performed at the U-70 accelerator. Schemes for the formation of beams with energies E ~ 1 TeV have been proposed for large colliders such as the Large Hadron Collider.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Origin of Rapid Delithiation In Secondary Particles Of LiNi 0.8 Co 0.15 Al 0.05 O 2 and LiNi y Mn z Co 1− y − z O 2 Cathodes

Abstract Most research on the electrochemical dynamics in materials for high‐energy Li‐ion batteries has focused on the global behavior of the electrode. This approach is susceptible to misleading analyses resulting from idiosyncratic kinetic conditions, such as surface impurities inducing an apparent two‐phase transformation within LiNi 0.8 Co 0.15 Al 0.05 O 2 . Here, nano‐focused X‐ray probes are used to measure delithiation operando at the scale of secondary particle agglomerates in layered cathode materials during charge. After an initial latent phase, individual secondary particles undergo rapid, stochastic, and largely uniform delithiation, which is in contrast with the gradual increase in cell potential. This behavior reproduces across several layered oxides. Operando X‐ray microdiffraction (‐XRD) leverages the relationship between Li content and lattice parameter to further reveal that rate acceleration occurs between Li‐site fraction ( x Li ) ≈0.9 and ≈0.5 for LiNi 0.8 Co 0.15 Al 0.05 O 2 . Physics‐based modeling shows that, to reproduce the experimental results, the exchange current density ( i 0 ) must depend on x Li , and that i 0 should increase rapidly over three orders of magnitude at the transition point. The specifics and implications of this jump in i 0 are crucial to understanding the charge‐storage reaction of Li‐ion battery cathodes.

25 ENERGY STORAGE↗

Mesoscopic Phase Transition Kinetics in Secondary Particles of Electrode-Active Materials in Lithium-Ion Batteries

Many compounds used as battery storage electrodes undergo large composition changes during use that are accompanied by a first-order phase transition. Most studies of these phase transitions have focused on the unit cell to single-crystallite scale, whereas real battery electrodes are typically composed of mesoscopic assemblies of nanocrystallites, for which phase transformation mechanisms are poorly understood. Here in this work, a systematic study is conducted of the potentiostatic (constant driving force) kinetics of phase transition in secondary particles of representative intercalation compounds: LiFePO 4 , LiMn 1–x Fe x PO 4 , and Li 4 Ti 5 O 7 . Storage kinetics are studied as a function of overpotential, material composition, primary particle size, and temperature. We find that in regimes where phase transformation occurs, the results can be self-consistently explained as nucleation and growth kinetics within the framework of the Johnson–Mehl–Avrami–Kolmogorov model. This implies that despite the common secondary particle topology, the electrochemically driven phase transformations occur by nucleation and growth with little apparent resistance to phase propagation across the grain boundaries. Growth appears to be one-dimensional in nature, consistent with a hybrid growth model in which rapid surface propagation is followed by slower growth into particles.

36 MATERIALS SCIENCE↗

The Role of Secondary Particle Structures in Surface Phase Transitions of Ni-Rich Cathodes

Nanometer-thick reconstruction layers on layered cathode surfaces have been widely observed on both pristine and cycled materials. However, the mechanisms of reconstruction and the role that these structures play in electrochemical performance are not fully understood. From a crystallographic perspective, such surface reconstruction layers result from cation site-mixing between Li and transition-metal ions, but it remains far from clear as to what the critical factors are that control such cation mixing for various cathode chemistries. In this paper, we report observations on surface transformations during cycling of a Ni-rich cathode-oxide that are governed by direct contact with the liquid electrolyte. Specifically, within a secondary particle, the three-dimensional hierarchical aggregate of primary particles leads to the formation of grain boundaries of different characteristics, including open grain boundaries that allow the permeation of liquid electrolyte, and closed grain boundaries that exclude liquid electrolyte penetration. Upon battery cycling, surfaces in direct contact with the liquid electrolyte showed a surface reconstruction layer while the surfaces that did not have contact with the electrolyte showed no such reconstructions. In addition, the critical role of oxygen in reconstruction of grain boundaries is demonstrated, and the unexpected oxygen depletion at twin boundaries result in severe phase transitions. The present work provides further insights into phase transitions at solid-solid and solid-liquid interfaces within secondary cathode particles and suggests strategies for mitigating surface/interfacial degradation.

36 MATERIALS SCIENCE↗

Mutual modulation between surface chemistry and bulk microstructure within secondary particles of nickel-rich layered oxides

Abstract Surface lattice reconstruction is commonly observed in nickel-rich layered oxide battery cathode materials, causing unsatisfactory high-voltage cycling performance. However, the interplay of the surface chemistry and the bulk microstructure remains largely unexplored due to the intrinsic structural complexity and the lack of integrated diagnostic tools for a thorough investigation at complementary length scales. Herein, by combining nano-resolution X-ray probes in both soft and hard X-ray regimes, we demonstrate correlative surface chemical mapping and bulk microstructure imaging over a single charged LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) secondary particle. We reveal that the sub-particle regions with more micro cracks are associated with more severe surface degradation. A mechanism of mutual modulation between the surface chemistry and the bulk microstructure is formulated based on our experimental observations and finite element modeling. Such a surface-to-bulk reaction coupling effect is fundamentally important for the design of the next generation battery cathode materials.

25 ENERGY STORAGE↗

Nuclear Data for High Energy Ion Interactions and Secondary Particle Production

Understanding the harmful effects of galactic cosmic rays (GCRs) on space exploration requires a substantial amount of nuclear data. Specifically, the interaction of energetic GCR charged particles with spacecraft materials generates secondary radiations that, through energy deposition, can harm astronauts and electronic systems. By identifying the gaps in our knowledge of the relevant nuclear data – interaction cross sections – and identifying ways to fill those gaps – with measurements, compilations, evaluations, disseminations, reaction modeling, sensitivity studies, and uncertainty quantification – the safety and viability of space exploration can be improved. This work surveys the state of the art in this interdisciplinary field and identifies promising collaborative research topics that have significant potential to advance our understanding of the effects of the space radiation environment on space exploration.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Extending the reach of FASER, MATHUSLA, and SHiP towards smaller lifetimes using secondary particle production

Many existing or proposed intensity-frontier search experiments look for decay signatures of light longlived particles (LLPs), highly displaced from the interaction point, in a distant detector that is well-shielded from the StandardModel background. This approach is, however, limited to new particles with decay lengths similar to or larger than the baseline of those experiments. In this study, we discuss how this basic constraint can be overcome in non-minimal beyond standard model scenarios. If more than one light new particle is present in the model, an additional secondary production of LLPs may take place right in front of the detector, opening this way a new lifetime regime to be probed.We illustrate the prospects of such searches in the future experiments FASER, MATHUSLA, and SHiP, for representative models, emphasizing possible connections to dark matter or an anomalous magnetic moment of muon. We also analyze additional advantages from employing dedicated neutrino detectors placed in front of the main decay volume.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

High-Voltage Charging-Induced Strain, Heterogeneity, and Micro-Cracks in Secondary Particles of a Nickel-Rich Layered Cathode Material

Nickel-rich layered materials LiNi 1-x-y Mn x Co y O 2 are promising candidates for high-energy-density lithium-ion battery cathodes. Unfortunately, they suffer from capacity fading upon cycling, especially with high-voltage charging. It is critical to have a mechanistic understanding of such fade. Synchrotron-based techniques (including scattering, spectroscopy, and microcopy) and finite element analysis are utilized to understand the LiNi 0.6 Mn 0.2 Co 0.2 O 2 material from structural, chemical, morphological, and mechanical points of view. The lattice structural changes are shown to be relatively reversible during cycling, even when 4.9 V charging is applied. However, local disorder and strain are induced by high-voltage charging. Nano-resolution 3D transmission X-ray microscopy data analyzed by machine learning methodology reveal that high-voltage charging induced significant oxidation state inhomogeneities in the cycled particles. Regions at the surface have a rock salt–type structure with lower oxidation state and build up the impedance, while regions with higher oxidization state are scattered in the bulk and are likely deactivated during cycling. In addition, the development of micro-cracks is highly dependent on the pristine state morphology and cycling conditions. Hollow particles seem to be more robust against stress-induced cracks than the solid ones, suggesting that morphology engineering can be effective in mitigating the crack problem in these materials.

25 ENERGY STORAGE↗

Impact of secondary particle size and two-layer architectures on the high-rate performance of thick electrodes in lithium-ion battery pouch cells

Increasing lithium-ion battery gravimetric energy density to > 300 Wh/kg, while simultaneously meeting a cost target of $80/kWh, is of paramount importance to increasing the driving range and affordability of electric vehicles. One way to address this goal is to reduce inactive components by increasing electrode areal capacities, but conventional thick electrode designs typically perform poorly at high discharge rates due to Li + mass transport limitations. Here we compare the rate capability and cycle life of NMC 532/graphite pouch cells made with five different thick cathode and anode designs paired together in 25 combinations. We find that using different particle sizes to structure both the cathode and anode architectures in two-layer configurations results in a 2X capacity improvement over the worst-performing combination at high discharge rates (97 vs. 46 mAh/g at 2C). These different cathode/anode designs also translate to different cycle life performance, with many cells cycled at C/2 achieving ~80% capacity retention after 1000 cycles, and cells cycled at 2C showing different degrees of capacity fade. Altogether, these results demonstrate that simple, scalable changes in electrode design can significantly improve the performance of thick electrodes for high energy density batteries.

25 ENERGY STORAGE↗

Conductive polymer and Si nanoparticles composite secondary particles and structured current collectors for high loading lithium ion negative electrode application

Embodiments of the present invention disclose a composition of matter comprising a silicon (Si) nanoparticle coated with a conductive polymer. Another embodiment discloses a method for preparing a composition of matter comprising a plurality of silicon (Si) nanoparticles coated with a conductive polymer comprising providing Si nanoparticles, providing a conductive polymer, preparing a Si nanoparticle, conductive polymer, and solvent slurry, spraying the slurry into a liquid medium that is a non-solvent of the conductive polymer, and precipitating the silicon (Si) nanoparticles coated with the conductive polymer. Another embodiment discloses an anode comprising a current collector, and a composition of matter comprising a silicon (Si) nanoparticle coated with a conductive polymer.

25 ENERGY STORAGE↗

Conductive polymer and Si nanoparticles composite secondary particles and structured current collectors for high loading lithium ion negative electrode application

Embodiments of the present invention disclose a composition of matter comprising a silicon (Si) nanoparticle coated with a conductive polymer. Another embodiment discloses a method for preparing a composition of matter comprising a plurality of silicon (Si) nanoparticles coated with a conductive polymer comprising providing Si nanoparticles, providing a conductive polymer, preparing a Si nanoparticle, conductive polymer, and solvent slurry, spraying the slurry into a liquid medium that is a non-solvent of the conductive polymer, and precipitating the silicon (Si) nanoparticles coated with the conductive polymer. Another embodiment discloses an anode comprising a current collector, and a composition of matter comprising a silicon (Si) nanoparticle coated with a conductive polymer.

36 MATERIALS SCIENCE↗

Neutron and Gamma Correlations using CGM in MCNP 6.2.0

The general-purpose Monte Carlo radiation-transport code MCNP6{sup TM} came from the integration of MCNP5{sup TM} and MCNPX{sup TM}. The most recent release of MCNP, version 6.2.0, is scheduled for release in early 2017, which includes a variety of bug fixes and new features to the code. MCNP traditionally models nuclear reactions using Monte Carlo sampling techniques on measured and modeled cross-sectional data contained within ACE (A Compact Evaluated Nuclear Data File) libraries. In addition to reaction cross-sections, ACE libraries contain information relating to the production of secondary particles, such as secondary neutrons and photons. For example, an incident neutron on a nucleus can produce a nuclear reaction in the form (n, M{sub n}n'), where n is the incident neutron and M{sub n} is the number of secondary neutrons n' produced. Using this notation, different reactions can be described based on their neutron multiplicity, such as neutron capture (M{sub n} = 0), elastic and inelastic scattering (M{sub n} = 1), and reactions with multiple secondary neutrons (M{sub n} > 1). Accounting for secondary γ-rays emitted from the residual nuclei, this reaction can further be generalized as n, Mnn'M to describe a reaction producing M{sub n} neutrons and M -rays. These values M{sub n} and M are referred to as the neutron and multiplicities, respectively. ACE libraries contain the cross-sectional data for each reaction, and their corresponding statistically averaged multiplicities for neutrons and photons, M-bar{sub n} and M-bar{sub γ}. However, there are several limitations to reaction sampling using ACE libraries. First, the data contained within ACE libraries is limited by the accuracy of the model and/or experiment, which out of necessity can greatly simplify the true physics behind a reaction. For example, the value M{sub γ} in a (n, M{sub n}n'M{sub γ}γ) reaction is determined by the statistically averaged multiplicity M-bar{sub γ} instead of a distribution. Consequently, MCNP, unable to produce a continuous distribution, will utilizes a binary sampling around M-bar{sub γ}. While this sampling method provides a statistically average M{sub γ} over a large simulation, it is an inaccurate representation of an individual reaction and its corresponding secondary particles. Secondary neutrons are affected in a similar manner, such that different kinds of secondary neutrons can be sampled from the same interaction (eg., an inelastic neutron with an [n, 2n] neutron). Lastly, the random sampling technique for secondary particles remains completely independent of the sampled reaction, eliminating the ability to correlate secondary particles for a given reaction. To supplement these data libraries, additional codes and models describing certain nuclear reactions are employed. These codes can fill in the information missing from ACE, provide a better model to the true physics distribution, and can provide true correlated secondary particles, which has many useful applications in research and industry.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗