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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 1,009 records · Page 56
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Reviving the rock-salt phases in Ni-rich layered cathodes by mechano-electrochemistry in all-solid-state batteries

The rock-salt phase (RSP) formed on the surface of Ni-rich layered cathodes in liquid-electrolyte lithium-ion batteries is conceived to be electrochemically "dead". Here we show massive RSP forms in the interior of LiNi x Mn y Co (1–x-y) O 2 (NMC) crystals in sulfide based all solid state batteries (ASSBs), but the RSP remains electrochemically active even after long cycles. The RSP and the layered structure constitute a two-phase mixture, a material architecture that is distinctly different from the RSP in liquid electrolytes. The tensioned layered phase affords an effective percolation channel into which lithium is squeezed out of the RSPs by compressive stress, rendering the RSPs electrochemically active. Consequently, the ASSBs with predominant RSP in the NMC cathode deliver remarkable long cycle life of 4000 cycles at high areal capacity of 4.3 mAh/cm 2 . Our study unveils distinct mechano-electrochemistry of RSPs in ASSBs that can be harnessed to enable high energy density and durable ASSBs.

25 ENERGY STORAGE↗
DOE OSTI2023

Rational synthesis of high-performance Ni-rich layered oxide cathode enabled via probing solid-state lithiation evolution

Lithium (Li)-ion batteries using nickel (Ni)-rich layered oxide cathode have been pursued with interest due to high practical energy density. A fundamental understanding of the reaction pathways and structural evolution of the solid-phase synthesis of these materials is crucial for their rational design and process development for mass production. In this work, structural evolution during solid-state synthesis was traced via in situ technique, with a particular emphasis on the lithiation reaction and migration of transition metal (TM) ions. The sintering process is governed by the competitive relationship of decomposition and lithiation reactions, which can be regulated through temperature windows. Controlling the melting point of the Li sources, as well as their affinity to cathode precursors, is highly desired to maintain the layered ordering of TM ions throughout the whole synthesis process, which simplifies the manufacturing process and improves the quality of the manufactured cathode material.

25 ENERGY STORAGE↗
DOE OSTI2019

The large-area hybrid-optics CLAS12 RICH: Assembling, commissioning and first data-taking

Here, the first module of a Ring Imaging Cherenkov detector has been recently installed on the CLAS12 spectrometer at the Jefferson Lab (JLab) to provide the experiment with kaon identification in the momentum range between 3 and 8 GeV/c. The detector adopts a hybrid optics solution with aerogel radiator, light planar and spherical mirrors and highly-segmented photon detectors. We report here on the assembly and installation of the RICH and we show the first preliminary results obtained during the commissioning of the detector and the first physics data taking.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

A gaseous RICH detector for SiD or ILD

This paper describes a preliminary study of a gaseous Ring Imaging Cherenkov (RICH) system capable of discriminating between kaons and pions at high momenta — up to 50 GeV/c — and thus enhancing particle identification at future colliders. The system possesses a compact design, facilitating easy integration into existing detector concepts. Here, a study of the key contributions to the Cherenkov angle resolution is also presented.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2015

Reaction mechanism studies towards effective fabrication of lithium-rich anti-perovskites Li 3 OX (X=Cl, Br)

Lithium-rich Anti-perovskite (LiRAP), with general formula Li 3 OX (X = Cl, Br, I), and recently reported as superionic conductors with 3-dimensional Li + migrating channels, is emerging as a promising candidate for solid electrolyte of all-solid-state LIBs. But, it is still difficult to fabricate pure LiRAP due to the difficulty of the phase formation and moisture-sensitive nature of the products. In this work, we thoroughly studied the formation mechanism of Li 3 OCl and Li 3 OBr in various solid state reaction routes. We developed different experimental strategies in order to improve the syntheses, in purposes of improved phase stability and large-scale production of LiRAP. One feasible method is to use strongly reductive agents Li metal or LiH to eliminate OH species. The results show that LiH is more effective than Li metal because of negatively charged H - and uniform reaction. The other well-established method is using Li 2 O and LiX mixture as reagents to preventing OH phase at the beginning, and using protected ball milling to make fine powders and hence active the reaction. Finally, IR spectroscopy, thermal analyses and first-principle calculation were performed to give indications on the reaction pathway.

25 ENERGY STORAGE↗
DOE OSTI2017

Quantifying autonomous vehicles national fuel consumption impacts: A data-rich approach

Autonomous vehicles are drawing significant attention from governments, manufacturers and consumers. Experts predict them to be the primary means of transportation by the middle of this century. Recent literature shows that vehicle automation has the potential to alter traffic patterns, vehicle ownership, and land use, which may affect fuel consumption from the transportation sector. In this paper, we developed a data-rich analytical framework to quantify system-wide fuel impacts of automation in the United States by integrating (1) a dynamic vehicle sales, stock, and usage model, (2) an historical transportation network-level vehicle miles traveled (VMT)/vehicle activity database, and (3) estimates of automation's impacts on fuel efficiency and travel demand. The vehicle model considers dynamics in vehicle fleet turnover and fuel efficiency improvements of conventional and advanced vehicle fleet. The network activity database contains VMT, free-flow speeds, and historical speeds of road links that can help us accurately identify fuel-savings opportunities of automation. Based on the model setup and assumptions, we found that the impacts of automation on fuel consumption are quite wide-ranging - with the potential to reduce fuel consumption by 45% in our 'Optimistic' case or increase it by 30% in our 'Pessimistic' case. Second, implementing automation on urban roads could potentially result in larger fuel savings compared with highway automation because of the driving features of urban roads. Lastly, through scenario analysis, we showed that the proposed framework can be used for refined assessments as better data on vehicle-level fuel efficiency and travel demand impacts of automation become available.

33 ADVANCED PROPULSION SYSTEMS↗
DOE OSTI2023

Interphasial engineering for Ni-rich NMC cathode materials

Ni-rich LiNi 1-x-y Mn x CoyO 2 , (NMC: 1-x-y ≥ 0.6) are promising cathode materials for lithium-ion batteries (LIBs) due to high reversible capacity and low cost. However, the fast capacity decay and voltage fading caused by interphasial instability requires improvement. The unstable cathodeelectrolyte interphase (CEI) and transition metal (TM) dissolution at higher voltages can lead to the drastic deterioration of electrochemical performance. In this review, recent approaches to novel electrolyte and additive design, cathode engineering including artificial CEI, and doping/coating on the surface of particles or the whole electrode are comprehensively summarized. In conclusion, the importance of multi-model and multi-scale characterization methods in understanding the effects of interphasial chemistry on battery performance is highlighted.

25 ENERGY STORAGE↗
DOE OSTI2018

Fundamental Insight into Zr Modification of Li- and Mn-Rich Cathodes: Combined Transmission Eelctron Microscopy and Electrochemical Impedance Spectroscopy Study

Zr surface modification was performed on Li- and Mn-rich (LMR) cathode material (Li1.2Ni0.13Co0.13Mn0.54O2) to suppress the detrimental phase transformation upon cycling and enhance its electrochemical performance. Using a wet chemical method, a Zr-based rock-salt layer with a thickness of 1~2 nm was formed on the surface of the LMR. Controlled studies reveal that the Zr-based layers can effectively suppress the phase transformation, leading to an enhanced long-term cycling performance and rate capability. At C/3, the Zr-modified LMR material was found to deliver an initial discharge specific capacity of 211 mAh g-1, and maintain a capacity of 182 mAh g-1 after 100 cycles. Even at high rates of 1, 2 and 3C, it still displays high discharge capacities of 178, 156 and 143 mAh g-1, respectively. This work reports for the first time the detailed mechanisms at atomic scale of how Zr modification can be effectively used to tailor the surface microstructures of high energy cathode materials to improve their long-term stability and cycle life.

Li- and Mn-rich cathode, Li1.2Ni0.13Co0.13Mn0.54O2↗
DOE OSTI2021

Atomic Structure of Surface-Densified Phases in Ni-Rich Layered Compounds

In this work, we report the presence of surface-densified phases (β-Ni 5 O 8 , γ-Ni 3 O 4 , and δ-Ni 7 O 8 ) in LiNiO 2 (LNO)- and LiNi 0.8 Al 0.2 O 2 (LNA)-layered compounds by combined atomic level scanning transmission electron microscopy (STEM) and electron energy loss spectroscopy (EELS). These surface phases form upon electrochemical aging at high state of charge corresponding to a fully delithiated state. A unique feature of these phases is the periodic occupancy by Ni 2+ in the Li layer. This periodic Ni occupancy gives rise to extra diffraction reflections, which are qualitatively similar to those of the LiNi 2 O 4 spinel structure, but these surface phases have a lower Ni valence state and cation content than spinel. Furthermore, these experimental results confirm the presence of thermodynamically stable surface phases and provide new insights into the phenomena of surface phase formation in Ni-rich layered structures.

25 ENERGY STORAGE↗
DOE OSTI2019

Evaluation of Gas Formation and Consumption Driven by Crossover Effect in High-Voltage Lithium-Ion Batteries with Ni-Rich NMC Cathodes

Gas formation during lithium-ion battery (LIB) cycling impacts the stability and safety of these batteries, especially for those containing Ni-rich NMC cathodes. In this paper, the cycling performance and gassing behavior of NMC811/graphite full cells with 4.2 and 4.4 V upper cutoff voltages were first compared. We report cells with a 4.2 V upper cutoff voltage had good cycling stability, exhibiting a capacity retention of 96.8% after 100 cycles and generated little gas. On the other hand, cells with a 4.4 V upper cutoff voltage lost over 25% of initial capacity after 100 cycles and generated large amounts of gas in the first 10 cycles. Electrochemical cycling of anode and cathode symmetric cells was implemented to isolate gases formed at the electrode. Gas chromatography–mass spectrometry, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and scanning transmission electron microscopy were used to characterize the gas formation and associated material surfaces and structural properties. It was found that CO2 and fluorinated alkanes were the dominant gases evolved on the cathode side during cycling to 4.4 V. Gas crossover to the anode led to the depletion of gaseous products, which stabilized the cell performance to some extent. However, the growing surface reconstruction layer at the cathode, the thickening of the solid electrolyte interphase layer at the anode, and the gradual depletion of lithium inventory collectively contributed to the continuous capacity loss of full cells cycled to 4.4 V.

25 ENERGY STORAGE↗
DOE OSTI2014

Organic-Acid-Assisted Fabrication of Low-Cost Li-Rich Cathode Material (Li[Li1/6Fe1/6Ni1/6Mn1/2]O-2) for Lithium-Ion Battery

A novel Li-rich cathode Li[Li1/6Fe1/6Ni1/6Mn1/2]O-2 (0.4Li(2)MnO(3-)0.6LiFe(1/3)Ni(1/3)Mn(1/3)O(2)) was synthesized by a solgel method, which uses citric acid (SC), tartaric acid (ST), or adipic acid (SA) as a chelating agent. The structural, morphological, and electrochemical properties of the prepared samples were characterized by various methods. X-ray diffraction showed that single-phase materials are formed mainly with typical alpha-NaFeO2 layered structure (R3 m), and the SC sample has the lowest Li/Ni cation disorder. The morphological study indicated homogeneous primary particles in good distribution size (100 nm) with small aggregates. The Fe, Ni, and Mn valences were determined by X-ray absorption near-edge structure analysis. In coin cell tests, the initial reversible discharge capacity of an SA electrode was 289.7 mAh g(-1) at the 0.1C rate in the 1.54.8 V voltage range, while an SC electrode showed a better cycling stability with relatively high capacity retention. At the 2C rate, the SC electrode can deliver a discharge capacity of 150 mAh g(-1) after 50 cycles. Differential capacity vs voltage curves were employed to further investigate the electrochemical reactions and the structural change process during cycling. This low-cost, Fe-based compound prepared by the solgel method has the potential to be used as the high capacity cathode material for Liion batteries.

cathode↗
DOE OSTI2020

Structure and Interface Design Enable Stable Li-Rich Cathode

Li-rich layered-oxide cathodes have the highest theoretical energy density among all the intercalated cathodes, which have attracted intense interests for high energy Li-ion batteries. However, O3-structured layered-oxide cathodes suffer from a low initial Coulombic efficiency (CE), severe voltage fade, and poor cycling stability because of the continuous oxygen release, structural rearrangements due to irreversible transition-metal migration, and serious side reactions between the delithiated cathode and electrolyte. In this work, we report that these challenges are migrated by using a stable O2-structured Li 1.2 Ni 0.13 Co 0.13 Mn 0.54 O 2 (O2-LR-NCM) and all-fluorinated electrolyte. The O2-LR-NCM can restrict the transition metals migrating into the Li layer and the in situ formed fluorinated cathode electrolyte interphase (CEI) on the surface of the O2-LR-NCM from the decomposition of all-fluorinated electrolyte during initial cycles effectively restrains the structure transition, suppresses the O2 release, and thereby safeguards the transition metal redox couples, enabling a highly reversible and stable oxygen redox reaction. O2-LR-NCM in all fluorinated electrolytes achieves a high initial CE of 99.82 % and cycling CE of and cycling CE of >99.9%, high reversible capacity of 278 mAh/g, and high capacity retention of 83.3% after 100 cycles. The synergic design of electrolyte and cathode structure represents a promising direction to stabilize high-energy cathodes.

25 ENERGY STORAGE↗
DOE OSTI2018

Elucidating anionic oxygen activity in lithium-rich layered oxides

Recent research has explored combining conventional transition metal redox with anionic lattice oxygen redox as a new and exciting direction to search for high-capacity lithium-ion cathodes. For this study, we probe the poorly understood electrochemical activity of anionic oxygen from a material perspective by elucidating the effect of the transition metal on oxygen redox activity. We study two lithium-rich layered oxides, specifically lithium nickel metal oxides where metal is either manganese or ruthenium, which possess similar structure and discharge characteristics, but exhibit distinctly different charge profiles. By combining X-ray spectroscopy with operando differential electrochemical mass spectrometry, we reveal completely different oxygen redox activity in each material, likely resulting from the different interaction between the lattice oxygen and transition metals. This work provides additional insights into the complex mechanism of oxygen redox and development of advanced high-capacity lithium-ion cathodes.

25 ENERGY STORAGE↗
DOE OSTI2020

Depth-dependent valence stratification driven by oxygen redox in lithium-rich layered oxide

Abstract Lithium-rich nickel-manganese-cobalt (LirNMC) layered material is a promising cathode for lithium-ion batteries thanks to its large energy density enabled by coexisting cation and anion redox activities. It however suffers from a voltage decay upon cycling, urging for an in-depth understanding of the particle-level structure and chemical complexity. In this work, we investigate the Li 1.2 Ni 0.13 Mn 0.54 Co 0.13 O 2 particles morphologically, compositionally, and chemically in three-dimensions. While the composition is generally uniform throughout the particle, the charging induces a strong depth dependency in transition metal valence. Such a valence stratification phenomenon is attributed to the nature of oxygen redox which is very likely mostly associated with Mn. The depth-dependent chemistry could be modulated by the particles’ core-multi-shell morphology, suggesting a structural-chemical interplay. These findings highlight the possibility of introducing a chemical gradient to address the oxygen-loss-induced voltage fade in LirNMC layered materials.

25 ENERGY STORAGE↗
DOE OSTI2021

Understanding Co roles towards developing Co-free Ni-rich cathodes for rechargeable batteries

Reduction on cobalt reliance is an urgent requirement in the development of sustainable cathode materials for Li-ion batteries. Here the authors analyse the roles of cobalt and its interplay with other ions in high-nickel layered oxides, and deduce a material formula for promising cobalt-free cathodes. Current bottlenecks in cobalt (Co) supply have negatively impacted commercial battery production and inspired the development of cathode materials that are less reliant on Co. However, complete Co elimination is prevented by the lack of fundamental understanding of the impact of Co on cathode capacity and structural stability, as well as the lack of effective substitute components in practice. Here we investigate the roles of Co in purposely designed systems that include both Co-rich and Mn-substituted Co-free cathodes. Our results affirmed that Co plays an undeniable role in fast capacity and/or structural degradation, and found that Co is more destructive than Ni at high potentials, which offers unexpected but encouraging perspectives for Co reduction. Moreover, Mn substitution effectively alleviates the destructive effects of Co and enables a high potential functionality. Finally, with these fundamental discoveries, we demonstrated a series of LiNi α Mn β X γ O 2 (X = single or multiple dopants) as a promising candidate for Co-free cathodes.

25 ENERGY STORAGE↗
DOE OSTI2014

Framework Stabilization of Si-Rich LTA Zeolite Prepared in Organic-Free Media

Zeolite HOU-2 (LTA type) is prepared with the highest silica content (Si/Al = 2.1) reported for Na-LTA zeolites without the use of an organic structure-directing agent. The rational design of Si-rich zeolites has the potential to improve their thermal stability for applications in catalysis, gas storage, and selective separations.

catalysis↗
DOE OSTI2014

β-decay of neutron-rich Z∼60 nuclei and the origin of rare earth elements

A large fraction of the rare-earth elements observed in the solar system is produced in the astrophysical rapid neutron capture process (r-process). However, current stellar models cannot completely explain the relative abundance of these elements partially because of nuclear physics uncertainties. To address this problem, a β-decay spectroscopy experiment was performed at RI Beam Factory (RIBF) at RIKEN, aimed at studying a wide range of very neutron-rich nuclei with Z∼60 that are progenitors of the rare-earth elements with mass number A∼460. The experiment provides a test of nuclear models as well as experimental inputs for r-process calculations. This contribution presents the experimental setup and some preliminary results of the experiment.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2014

Symmetry energy and surface properties of neutron-rich exotic nuclei

The symmetry energy, the neutron pressure and the asymmetric compressibility of spherical Ni, Sn, and Pb and deformed Kr and Sm neutron-rich even-even nuclei are calculated within the coherent density fluctuation model using the symmetry energy as a function of density within the Brueckner energy-density functional. The correlation between the thickness of the neutron skin and the characteristics related with the density dependence of the nuclear symmetry energy is investigated for isotopic chains of these nuclei in the framework of the deformed self-consistent mean-field Skyrme HF+BCS method. The mass dependence of the nuclear symmetry energy and the neutron skin thickness are also studied together with the role of the neutron-proton asymmetry. The studied correlations reveal a smoother behavior in the case of spherical nuclei than for deformed ones. We also notice that the neutron skin thickness obtained for {sup 208}Pb with SLy4 force is found to be in a good agreement with the recent data. In addition to the interest that this study may have by itself, we give some numerical arguments in proof of the existence of peculiarities of the studied quantities in Ni and Sn isotopic chains that are not present in the Pb chain.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗