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At least 1,045 records · Page 58

Enabling Stable High‐Voltage LiCoO 2 Operation by Using Synergetic Interfacial Modification Strategy

Abstract Structural and interfacial instability of the LiCoO 2 cathode under a voltage exceeding 4.5 V (vs Li/Li + ) severely hinders its practical applications for high‐energy‐density lithium batteries. Herein, a modified electrolyte with nitriles (suberonitrile or 1,3,6‐hexanetricarbonitrile) and fluoroethylene carbonate (FEC) coadditives is demonstrated to form an ultrathin and uniform interface layer on LiCoO 2 cathode under a synergetic effect. As such, LiCoO 2 /Li cells display excellent cyclability at a cutoff voltage of 4.6 V with a capacity retention over 72% after 300 cycles and 60% after 200 cycles at 30 and 55 °C, respectively, even achieving operation at a high current rate (10 C) upon 500 cycles as compared to the controls with fast‐falling capacity to zero. Furthermore, an adsorption‐coordination mechanism between nitriles and cobalt and synergetic effect of coadditives are explored by the alliance of spectroscopic analysis and theoretical calculations. The contributed lone‐pairs on the N 2p orbital of nitriles in coordination lowers the real oxidation state of Co 3+/4+ so that it decreases its catalysis on electrolytes, and the synergy from nitrile‐derived species regulates FEC to form an LiF‐containing electron‐insulated interface layer. This work shares a new insight to nitriles with the synergy of coadditives and paves a way to refine (ultra)high‐voltage LiCoO 2 cathode for high‐energy‐density energy storages.

Yang, Xuerui↗

Halting Oxygen Evolution to Achieve Long Cycle Life in Sodium Layered Cathodes

Oxygen redox chemistries at high voltage have materialized as a revolutionary paradigm for cathodes with high-energy density; however, they are plagued by the challenges of labile oxygen loss and rapid degradations upon cycling, even after concerted endeavors from the research community. Here we propose a multi-concentration stratagem propelled by entropy reinforcement to enhance the electronic structure disorder (ESD) at high desodiation states for impeding undesired oxygen mobility and ensuring controlled oxygen activity, elucidated by density functional theory calculations. The increased disorder strengthens the reversible electrochemistry of lattice oxygen redox, leading to effectively suppressed P−O structural evolution and highly stable localized TMO 6 octahedral environments, as demonstrated by soft/hard X-ray absorption spectroscopy. Furthermore, through a comparative analysis of sodium-layered cathodes with different configuration entropy, we reveal that a high-entropy state induced by cationic disordering has the capacity to perturb cationic redox boundaries, significantly restraining the formation of detrimental O′3 phases. As a consequence, the high-voltage cycling stability has been greatly upgraded, up to 4.4 V versus Na + /Na, with an impressive 90.1 % capacity retention at 1 C over 100 cycles and 76.1 % capacity retention at 2 C over 300 cycles. In conclusion, the resilient oxygen redox, enabled through the control of ESD, broadens the horizons for entropy engineering and lays the foundation for advancements in high-energy, long-cycling, and safe batteries.

25 ENERGY STORAGE↗

Concentration dependent properties and plastic deformation facilitate instability of the solid-electrolyte interphase in Li-ion batteries

Lithium-ion batteries (LIBs) often suffer from capacity fading and poor cyclic performance due to mechanical degradation of the solid-electrolyte interphase (SEI). Here we perform numerical simulations and theoretical analysis to elucidate the role of plasticity in wrinkling and ratcheting behaviors of an SEI/electrode system. A coupled diffusion and finite deformation framework is formulated and numerically implemented as a user-element subroutine (UEL) to describe transient lithium diffusion and accompanying elastic–viscoplastic deformation of the electrode. It is found that concentration dependent properties and plastic deformation facilitate wrinkling in such a system. A wrinkled morphology may further lead to ratcheting and related failure under cycling. A phase diagram of four types of cyclic behaviorsis identified in terms of the charging rate and time. Our analysis suggests several potential strategies to avoid wrinkling and ratcheting instabilities, such as charging/discharging the electrode at a sufficiently slow rate, and/or introducing a thick artificial SEI with a pre-tension.

25 ENERGY STORAGE↗

Perspectives on Cobalt Supply through 2030 in the Face of Changing Demand

Lithium-ion battery demand, particularly for electric vehicles, is projected to increase by over 300% throughout the next decade. With these expected increases in demand, cobalt (Co)-dependent technologies face the risk of significant impact from supply concentration and mining limitations in the short term. In this study, increased extraction and secondary recovery form the basis of modeling scenarios that examine implications on Co supply to 2030. Demand for Co is estimated to range from 235 to 430 ktonnes in 2030. This upper bound on Co demand in 2030 corresponds to 280% of world refinery capacity in 2016. Supply from scheduled and unscheduled production as well as secondary production is estimated to range from 320 to 460 ktonnes. Our analysis suggests the following: (1) Co price will remain relatively stable in the short term, given that this range suggests even a supply surplus, (2) future Co supply will become more diversified geographically and mined more as a byproduct of nickel (Ni) over this period, and (3) for this demand to be met, attention should be paid to sustained investments in refined supply of Co and secondary recovery.

36 MATERIALS SCIENCE↗

Facile synthesis and phase stability of Cu-based Na 2 Cu(SO 4 ) 2 · x H 2 O ( x = 0–2) sulfate minerals as conversion type battery electrodes

Mineral exploration forms a key approach for unveiling functional battery electrode materials. The synthetic preparation of naturally found minerals and their derivatives can aid in designing of new electrodes. Herein, saranchinaite Na 2 Cu(SO 4 ) 2 and its hydrated derivative kröhnkite Na 2 Cu(SO 4 ) 2 ·2H 2 O bisulfate minerals have been prepared using a facile spray drying route for the first time. The phase stability relation during the (de)hydration process was examined synergising in situ X-ray diffraction and thermochemical studies. Kröhnkite forms the thermodynamically stable phase as the hydration of saranchinaite to kröhnkite is highly exothermic (-51.51 ± 0.63 kJ mol -1 ). Structurally, kröhnkite offers a facile 2D pathway for Na+ ion migration resulting in 20 times higher total conductivity than saranchinaite at 60 °C. Both compounds exhibited a conversion redox mechanism for Li-ion storage with the first discharge capacity exceeding 650 mA h g -1 (at 2 mA g -1 vs. Li + /Li) upon discharge up to 0.05 V. Post-mortem analysis revealed that the presence of metallic Cu in the discharged state is responsible for high irreversibility during galvanostatic cycling. This study reaffirms the exploration of Cu-based polyanionic sulfates, which while having limited (de)insertion properties, can be harnessed for conversion-based electrode materials for batteries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Mutations in penicillin-binding protein 2 from cephalosporin-resistant Neisseria gonorrhoeae hinder ceftriaxone acylation by restricting protein dynamics

The global incidence of the sexually transmitted disease gonorrhea is expected to rise due to the spread of Neisseria gonorrhoeae strains with decreased susceptibility to extended-spectrum cephalosporins (ESCs). ESC resistance is conferred by mosaic variants of penicillin-binding protein 2 (PBP2) that have diminished capacity to form acylated adducts with cephalosporins. To elucidate the molecular mechanisms of ESC resistance, we conducted a biochemical and high-resolution structural analysis of PBP2 variants derived from the decreased-susceptibility N. gonorrhoeae strain 35/02 and ESC-resistant strain H041. Our data reveal that mutations both lower affinity of PBP2 for ceftriaxone and restrict conformational changes that normally accompany acylation. Specifically, we observe that a G545S substitution hinders rotation of the β3 strand necessary to form the oxyanion hole for acylation and also traps ceftriaxone in a noncanonical configuration. In addition, F504L and N512Y substitutions appear to prevent bending of the β3–β4 loop that is required to contact the R1 group of ceftriaxone in the active site. Other mutations also appear to act by reducing flexibility in the protein. Overall, our findings reveal that restriction of protein dynamics in PBP2 underpins the ESC resistance of N. gonorrhoeae.

60 APPLIED LIFE SCIENCES↗

Electrolytes Containing Triethyl Phosphate Solubilized Lithium Nitrate for Improved Silicon Anode Performance

An electrolyte consisting of lithium nitrate (LiNO3) and lithium difluoro(oxalato)borate (LiDFOB) in ethylene carbonate (EC), ethylmethyl carbonate (EMC), and triethyl phosphate (TEP) is used to improve the long-term cycling stability of silicon anodes. TEP was selected for its ability to dissolve LiNO 3 in carbonates to a concentration of ~0.2 M. The large amount of LiNO 3 combined with the LiDFOB salt leads to a capacity retention of 87.1% after one hundred cycles due to the formation of a relatively stable solid electrolyte interphase (SEI). Ex-situ surface analysis reveals that the SEI consists of oxalates, lithium alkyl carbonates, borates, and nitrate reduction products. By selecting two components which are preferentially reduced (LiNO 3 and LiDFOB), the SEI is able to inhibit continuous solvent decomposition and allows for improved electrochemical cycling for pure silicon anodes.

25 ENERGY STORAGE↗

LLM Benchmarking with LLaMA2: Evaluating Code Development Performance Across Multiple Programming Languages

The rapid evolution of large language models (LLMs) has opened new possibilities for automating various tasks in software development. This paper evaluates the capabilities of the LLaMA 2-70B model in automating these tasks for scientific applications written in commonly used programming languages. Using representative test problems, we assess the model's capacity to generate code, documentation, and unit tests, as well as its ability to translate existing code between commonly used programming languages. Our comprehensive analysis evaluates the compilation, runtime behavior, and correctness of the generated and translated code. Additionally, we assess the quality of automatically generated code, documentation, and unit tests. Here, our results indicate that while LLaMA 2-70B frequently generates syntactically correct and functional code for simpler numerical tasks, it encounters substantial difficulties with more complex, parallelized, or distributed computations, requiring considerable manual corrections. We identify key limitations and suggest areas for future improvements to better leverage AI-driven automation in scientific computing workflows.

97 MATHEMATICS AND COMPUTING↗

Anodic Activity of Hydrated and Anhydrous Iron (II) Oxalate in Li-Ion Batteries

We discuss the applicability of the naturally occurring compound Ferrous Oxalate Dihydrate (FOD) (FeC2O4·2H2O) as an anode material in Li-ion batteries. Using first-principles modeling, we evaluate the electrochemical activity of FOD and demonstrate how its structural water content affects the intercalation reaction and contributes to its performance. We show that both Li0 and Li+ intercalation in FOD yields similar results. Our analysis indicates that fully dehydrated ferrous oxalate is a more promising anodic material with higher electrochemical stability: it carries 20% higher theoretical Li storage capacity and a lower voltage (0.68 V at the PBE/cc-pVDZ level), compared to its hydrated (2.29 V) or partially hydrated (1.43 V) counterparts.

Keshavarz, Fatemeh↗

Attitude stability of a flexible solar electric spacecraft - A parametric study

The influence of large area solar array flexibility on the attitude control of a solar electric spacecraft is analyzed. The spacecraft consists of a rigid central body, two flexible roll-out solar arrays, and a cluster of three electric propulsion engines. Each engine has gimballing or translational capacity, or both, for attitude control purposes. A parametric stability study of various spacecraft configurations was made, using hybrid coordinate techniques in an eigenvalue analysis. Parameters varied were solar array aspect ratio, solar array first natural frequency, solar array rotation angle about the yaw axis, and sensor gain factors. Only the first six modes of solar array vibration were included in the study. The attitude response characteristics of the various spacecraft configurations were obtained by means of a digital computer simulation program of the system's equations of motion. The feasibility of using the thrusters for attitude control of electric propulsion spacecraft is demonstrated. It is also shown that although the dynamics effects of large-area flexible solar arrays can be harmful, changes in the control system parameters can insure stable attitude control.

Marsh, E. L.↗

System life and reliability modeling for helicopter transmissions

A computer program which simulates life and reliability of helicopter transmissions is presented. The helicopter transmissions may be composed of spiral bevel gear units and planetary gear units - alone, in series or in parallel. The spiral bevel gear units may have either single or dual input pinions, which are identical. The planetary gear units may be stepped or unstepped and the number of planet gears carried by the planet arm may be varied. The reliability analysis used in the program is based on the Weibull distribution lives of the transmission components. The computer calculates the system lives and dynamic capacities of the transmission components and the transmission. The system life is defined as the life of the component or transmission at an output torque at which the probability of survival is 90 percent. The dynamic capacity of a component or transmission is defined as the output torque which can be applied for one million output shaft cycles for a probability of survival of 90 percent. A complete summary of the life and dynamic capacity results is produced by the program.

Savage, M.↗

Fast simulation of packet loss rates in a shared buffer communications switch

This paper describes an efficient technique for estimating, via simulation, the probability of buffer overflows in a queueing model that arises in the analysis of ATM (Asynchronous Transfer Mode) communication switches. There are multiple streams of (autocorrelated) traffic feeding the switch that has a buffer of finite capacity. Each stream is designated as either being of high or low priority. When the queue length reaches a certain threshold, only high priority packets are admitted to the switch's buffer. The problem is to estimate the loss rate of high priority packets. An asymptotically optimal importance sampling approach is developed for this rare event simulation problem. In this approach, the importance sampling is done in two distinct phases. In the first phase, an importance sampling change of measure is used to bring the queue length up to the threshold at which low priority packets get rejected. In the second phase, a different importance sampling change of measure is used to move the queue length from the threshold to the buffer capacity.

Chang, Cheng-Shang↗

Development and Application of an Integrated Approach toward NASA Airspace Systems Research

The National Aeronautics and Space Administration's (NASA) Airspace Systems Program is contributing air traffic management research in support of the 2025 Next Generation Air Transportation System (NextGen). Contributions support research and development needs provided by the interagency Joint Planning and Development Office (JPDO). These needs generally call for integrated technical solutions that improve system-level performance and work effectively across multiple domains and planning time horizons. In response, the Airspace Systems Program is pursuing an integrated research approach and has adapted systems engineering best practices for application in a research environment. Systems engineering methods aim to enable researchers to methodically compare different technical approaches, consider system-level performance, and develop compatible solutions. Systems engineering activities are performed iteratively as the research matures. Products of this approach include a demand and needs analysis, system-level descriptions focusing on NASA research contributions, system assessment and design studies, and common systemlevel metrics, scenarios, and assumptions. Results from the first systems engineering iteration include a preliminary demand and needs analysis; a functional modeling tool; and initial system-level metrics, scenario characteristics, and assumptions. Demand and needs analysis results suggest that several advanced concepts can mitigate demand/capacity imbalances for NextGen, but fall short of enabling three-times current-day capacity at the nation s busiest airports and airspace. Current activities are focusing on standardizing metrics, scenarios, and assumptions, conducting system-level performance assessments of integrated research solutions, and exploring key system design interfaces.

Barhydt, Richard↗

Application of Satellite Observations to Manage Natural Disasters in the Lake Victoria Basin

Lake Victoria, the second largest fresh water lake in the Eastern part of Africa is a vital natural resource for the economic well being and prosperity of over 30 million people located in riparian regions of Uganda, Kenya and Tanzania. It covers a large area of about 68,870 km2 and produces a GDP of about US $30 billion per year. The region is also very much prone to natural disasters such as severe floods during heavy precipitation periods in the Eastern part of Africa. In addition to floods, the precipitation also produces large infestations of mosquito larvae due to the standing water in many areas. This further causes multiple vector borne diseases such as Malaria, Rift Valley Fever and more. These problems are of serious concern and require active and aggressive surveillance and management to minimize the loss of human and animal lives and property damage. Satellite imagery and observations along with the in situ measurements provide a great tool to analyze and study this area and inform the policy makers to make calculated policy decisions which are more beneficial to the environment. Recently, NASA and USAID have joined forces with the Regional Center for Mapping of Resources for Development (RCMRD) located in Nairobi, Kenya to utilize multiple NASA sensors such as TRMM, SRTM and MODIS to develop flood potential maps for the Lake Victoria Basin. The idea is to generate a flood forecasts and "nowcasts" that can be sent to the disaster management organizations of Uganda, Kenya, and Tanzania. Post flood event satellite imagery is becoming a common tool to assess the areas inundated by flooding. However, this work is unique undertaking by utilizing land imaging and atmospheric satellites to build credible flood potential maps. At same time, we are also studying the potential occurrence and spread of Rift Valley Fever disease based on the short term climate records and precipitation data. These activities require multi-nation coordination and agreements and multiple operational agencies within each respective country. It also requires credible in situ data such as precipitation, river flow rates and lake levels to further validate the global and regional Hood models and algorithms. This also requires a considerable amount of training and capacity building for the RCMRD experts who will help us validate the model results and eventually transition it for operational use. In a final analysis, Disaster management and humanitarian aid organizations need accurate and timely information for making decisions regarding deployment of relief teams and emergency supplies during major floods. Flood maps based on the use of satellite data have proven extremely valuable to such organizations for identifying the location, extent, and severity of these events. However, despite extraordinary efforts on the part of remote sensing data providers to rapidly deliver such maps, there is typically a delay of several days or even weeks from the on-set of flooding until such maps are available to the disaster management community. This paper summarizes efforts at NASA to address this problem through development of an integrated and automated process of a) flood forecasting b) flood detection, c) satellite data acquisition, d) rapid Hood mapping and distribution, and e) validation of Hood forecasting and detection products.

Habib, Shahid↗

Cofactors in the RNA World

RNA world theories figure prominently in many scenarios for the origin and early evolution of life. These theories posit that RNA molecules played a much larger role in ancient biology than they do now, acting both as the dominant biocatalysts and as the repository of genetic information. Many features of modern RNA biology are potential examples of molecular fossils from an RNA world, such as the pervasive involvement of nucleotides in coenzymes, the existence of natural aptamers that bind these coenzymes, the existence of natural ribozymes, a biosynthetic pathway in which deoxynucleotides are produced from ribonucleotides, and the central role of ribosomal RNA in protein synthesis in the peptidyl transferase center of the ribosome. Here, we uses both a top-down approach that evaluates RNA function in modern biology and a bottom-up approach that examines the capacities of RNA independent of modern biology. These complementary approaches exploit multiple in vitro evolution techniques coupled with high-throughput sequencing and bioinformatics analysis. Together these complementary approaches advance our understanding of the most primitive organisms, their early evolution, and their eventual transition to modern biochemistry.

RNA↗

Localized High-Concentration Electrolytes Get More Localized

Liquid electrolytes in batteries are typically treated as macroscopically homogeneous ionic transport media, despite having complex chemical composition and atomistic solvation structures, thus leaving a knowledge gap of microstructural characteristics. A promising electrolyte system design has recently been developed with the title of a localized high-concentration electrolyte (LHCE). These electrolytes are a summation of three components – a charge-carrying salt, a solvent that solvates the salt, and a diluent that is sparingly interactive with the salt in terms of ion solvation. This creates the perception of a high-concentration electrolyte (HCE) with high anion-cation interactions that supports a salt-derived, stable solid-electrolyte interphase, while an LHCE improves bulk electrolyte properties, such as ionic conductivity and viscosity, when compared to an HCE. Much trial by error design of this LHCE concept has been supported by simulations to confirm ionic interactions, cycling data to confirm cell stability, and post-mortem analysis to provide evidence of mechanisms. However, a systematic design to extend the capabilities of LHCEs is still to be desired. Here, we analyzed a specific LHCE mixture to dictate the best viable mixture that extends the localization of solvation structures while maintaining viable cell-level capabilities. We seek to observe and understand solvent-to-salt interactions that impact electrolyte performance. These interactions range from single-ion solvation, multidentate interactions (i.e., solvation-driven clustering), to more widespread network-level interactions. With the support of both experimental and computational analysis of different electrolyte features, we have begun a methodology of formulating the most ideal LHCE mixtures for improving the cyclability of high-capacity battery chemistries.

25 ENERGY STORAGE↗

Charging location selection of an incoming electric vehicle for large EV depot infrastructure

As the use of renewable energy resources increases within charging infrastructures, the risk that charging an additional load within the charging infrastructure will create a violation of the applicable grid code also increases. In an embodiment, a charging location is selected for an incoming load based on a load flow analysis, to thereby mitigate the risk of a violation. This selection process may also account for the charging schedule of the load and the capacity of available charging stations (e.g., fast charging vs. slow charging).

Hafiz, Faeza↗

Characterization of pitch carbon coating properties affecting the electrochemical behavior of silicon nanoparticle lithium-ion battery anodes

Silicon is an exciting material for next-generation lithium-ion battery anodes, due to its high theoretical capacity and availability, but its widespread implementation has been limited by extensive volume changes during cycling that causes mechanical damage and limits cycle life. One approach to mitigating these deleterious effects while still maintaining silicon's benefits is the addition of a pitch carbon coating to nanometer-sized silicon particles. Here, in this study, we present characterization of pitch-coated silicon electrodes without annealing and annealed at 700 °C and 1000 °C to determine the optimum temperature treatment, as well as pitch-only and silicon-only electrodes with and without annealing to elucidate the impacts of each component on early electrochemical behavior. Using Fourier transform infrared and Raman spectroscopies, atomic force and scanning spreading resistance microscopy, and electrochemical analysis, we find 700 °C to be the optimal annealing temperature, as amorphous carbon is created, which improves conductivity prior to cycling and facilitates ion storage during cycling that increases capacity. We also present in situ Raman spectroscopy data demonstrating the heterogeneous aging that occurs across the electrode surface during cycling.

25 ENERGY STORAGE↗