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Featured Application: This work can be applied to sodium-ion batteries, especially for energy storage applications. The lack of a standard anode for sodium-ion batteries (SIBs) has greatly hindered their applications. Herein, we show that a novel phase of carbon, namely Q-carbon, is an effective anode material for sodium-ion batteries. The Q-carbon, which is a metastable phase of carbon consisting of about 80% sp3- and 20% sp2-bonded carbon, is synthesized by nonequilibrium pulsed laser annealing and arc-discharge methods. Two types of Q-carbons, Q1 and Q2, were evaluated as anode material for SIBs. Q1 had a slow quench and was used as the control, whereas Q2 was Q-carbon with a rapid quenching. Q1 exhibits a high initial columbic efficiency of 81% and a low-capacity retention of less than 60%, whereas Q2 has a low initial columbic efficiency of 58% and a high-capacity retention of 81%. Q2 exhibits a stable capacity of 168 mAh·g−1 at a cycling rate of C/3 (124 mA·g−1), which is comparable to other hard carbon anodes reported in the literature. This unique synthesis method opens a pathway for the further tuning of Q-carbon with higher trapping/charging of Na+ ions in improved SIBs. [ABSTRACT FROM AUTHOR]

High‐capacity cathodes (LiNi0.8Mn0.1Co0.1O2, NMC811) are promising for vehicle electrification because of their high gravimetric energy density. However, their electrochemical performance still relies upon the stability of the cathode electrolyte interphase (CEI). A highly reactive cathode interface leads to parasitic side reactions with electrolytes, resulting in accelerated capacity fading. Well‐developed LiF and LiF‐like inorganic compounds are believed to be good CEI components for stabilizing such reactive electrode interfaces. However, it is challenging to form an optimal surface sub‐nanolayer of LiF on the cathode surfaces because of the complexity of the electrochemical reaction during battery cycling. Herein, the formation of a conformal LiF layer on the NMC811 electrode surface via an in situ ion‐exchange metathesis process is reported, demonstrating a promising electrochemical performance because of a LiF‐stabilized CEI. In situ generated LiF‐coated NMC811 electrodes exhibit ≈97% capacity retention up to 100 cycles at a 0.3 C rate with average coulombic efficiency of ≈99.9% and ≈80% capacity retention up to 200 cycles at a 1 C rate with average coulombic efficiency of >99.6%. This finding may pave the way for reengineering the CEI to enhance the electrochemical performances and cycling stability of the high‐capacity cathodes. [ABSTRACT FROM AUTHOR]

Cost-effective production of low cobalt Li-ion battery (LIB) cathode materials is of great importance to the electric vehicle (EV) industry to achieve a zero-carbon economy. Among the various low cobalt cathodes, Ni-rich lithium nickel cobalt manganese oxide (NCM/NMC)-based layered materials are commonly used in EVs and are attracting more attention of the scientific community due to their high specific capacity and energy density. Various synthesis routes are already established to produce Ni-rich NCM cathodes with uniform particle size distribution and high tap density. Continuous production of highly pure Ni-rich cathode materials with uniformity in inter/intra-particle compositional distribution is critically required. On the other hand, cation mixing, particle cracking, and parasitic side reactions at higher voltage and temperature are some of the primary challenges of working with Ni-rich NCM cathodes. During the past five years, several advanced modification strategies such as coating, doping, core–shell, gradient structure and single crystal growth have been explored to improve the NCM cathode performance in terms of specific capacity, rate-capability and cycling stability. The scientific advancements in the field of Ni-rich NCM cathodes in terms of manufacturing processes, material challenges, modification techniques, and also the future research direction of LIB research are critically reviewed in this article. [ABSTRACT FROM AUTHOR]

In this research, anisotropic NdFeB + SmFeN hybrid and NdFeB bonded magnets are additively printed in a polyphenylene sulfide (PPS) polymer binder. Printed NdFeB + SmFeN PPS bonded magnets displayed excellent magnetic properties (Br [remanence] = 6.9 kG [0.69 T], Hcj [coercivity] = 8.3 kOe [660 kA/m], and BHmax [energy product] = 9.9 MGOe [79 kJ/m3]) with superior corrosion resistance and thermal stability. The anisotropic NdFeB bonded magnet shows a high coercivity of 14.6 kOe (1162 kA/m) with a BHmax of 8.7 MGOe (69 kJ/m3). The coercivity and remanence temperature coefficients for NdFeB + SmFeN hybrid bonded magnets are −0.10%/K and −0.46%/K, and for NdFeB bonded magnets are −0.14%/K and −0.53%/K in the range of 300–400 K, indicating that the hybrid bonded magnets are thermally stable. The average flux aging loss for hybrid magnets was also determined to be very stable over 2000 h at 448 K (175°C) in air with 2.04% compared to that of NdFeB magnets with 3.62%. [ABSTRACT FROM AUTHOR]

The formation of the solid electrolyte interphase (SEI) in an ionic liquid electrolyte of 0.5 m lithium bis(fluorosulfonyl)imide (LiFSI) in 1‐ethyl‐3‐methylimidazolium bis(fluorosulfonyl)imide at high cell voltages (1.7–1.9 V) is investigated in ordered mesoporous carbon (OMC) based Li metal cells using an operando small‐angle neutron scattering (SANS) technique coupled with electrochemical impedance spectroscopy and ex situ X‐ray photoelectron spectroscopy (XPS). It is demonstrated that discharging the OMC Li metal cells to ≈2 V and holding the cell voltage constant induces a rapid current increase with time, confirming extensive reduction and SEI formation. XPS analysis reveals that LiF is formed at open cell voltage (OCV), which is attributed to the carbenes generated at the lithium negative electrode because of its reaction with EMIm cation diffusing to and initiating the reaction with FSI− anions at the carbon positive electrode. It is confirmed that the chemical reaction at OCV and electrochemical reduction at high cell voltage of the FSI− anion plays a protective role against EMIm cation co‐intercalation into the carbon positive electrode during the initial discharge. Operando SANS studies also suggest that slight differences occur in the surface composition and reaction mechanism as a function of cell voltage. [ABSTRACT FROM AUTHOR]

We report a three-stage bench-scale column extraction process to selectively extract lithium chloride from geothermal brine. The goal of this research is to develop materials and processing technologies to improve the economics of lithium extraction and production from naturally occurring geothermal and other brines for energy storage applications. A novel sorbent, lithium aluminum layered double hydroxide chloride (LDH), is synthesized and characterized with X-ray powder diffraction, scanning electron microscopy, inductively coupled plasma optical emission spectrometry (ICP-OES), and thermogravimetric analysis. Each cycle of the column extraction process consists of three steps: (1) loading the surbent with lithium chloride from brine; (2) intermediate washing to remove unwanted ions; (3) final washing for unloading the lithium chloride ions. Our experimental analysis of eluate vs feed concentrations of Li and competing ions demonstrates that our optimized sorbents can achieve a recovery efficiency of ~91% and possess excellent Li apparent selectivity of 47.8 compared to Na ions and 212 compared to K ions, respectively in the brine. The present work demonstrates that LDH is an effective sorbent for selective extraction of lithium from brines, thus offering the possibility of effective application of lithium salts in lithium-ion batteries leading to a fundamental shift in the lithium supply chain. [ABSTRACT FROM AUTHOR]

Due to their high specific capacity and negligible volume expansion during cycling, anatase titanium dioxide (a-TiO2) nanotubes have been considered as a prime candidate for anodes in lithium-ion batteries. However, their rate capability for electrochemical cycling is limited by the low electronic conductivity of a-TiO2 nanotubes. Here, we show that a desirable amount of nitrogen doping can significantly enhance the electronic conductivity in a-TiO2 nanotubes, resulting in improvements in both the capacity stability and the rate capability at fast charge–discharge rates. Electron energy loss spectroscopy revealed a high doping concentration of nitrogen (∼5%) by substituting for oxygen ions in a-TiO2 nanotubes. The lithiation mechanism of N-doped a-TiO2 nanotubes was further investigated using in situ transmission electron microscopy, where a three-step lithiation mechanism was revealed. Lithium ions initially intercalate into the a-TiO2 lattice structure. Further insertion of lithium ions triggers a phase transformation from a-TiO2 to orthorhombic Li0.5TiO2 and finally to polycrystalline tetragonal LiTiO2. Our results reveal that nitrogen doping significantly facilitates lithiation in TiO2 through enhanced electronic conductivity, while the structural and chemical evolutions during the lithiation process remain similar to those of undoped TiO2. [ABSTRACT FROM AUTHOR]

Sulfonated tire-derived carbons have been demonstrated to be high value-added carbon products of tire recycling in several energy storage system applications including lithium, sodium, potassium ion batteries and supercapacitors. In this communication, we compared different temperature pyrolyzed sulfonated tire-derived carbons with commercial graphite and unmodified/non-functionalized tire-derived carbon by studying the surface chemistry and properties, vibrational spectroscopy of the molecular structure, chemical bonding such as C–H bonding, and intermolecular interactions of the carbon materials. The nitrogen adsorption–desorption studies revealed the tailored micro and meso pore size distribution of the carbon during the sulfonation process. XPS and neutron vibrational spectra showed that the sulfonation of the initial raw tire powders could remove the aliphatic hydrogen containing groups (⧸⧹CH2 and –CH3 groups) and reduce the number of heteroatoms that connect to carbon. The absence of these functional groups could effectively improve the first cycle efficiency of the material in rechargeable batteries. Meanwhile, the introduced –SO3H functional group helped in producing terminal H at the edge of the sp2 bonded graphite-like layers. This study reveals the influence of the sulfonation process on the recovered hard carbon from used tires and provides a pathway to develop and improve advanced energy storage materials. [ABSTRACT FROM AUTHOR]

The local structure around the mobile ions influences their dynamics. The knowledge about the relationship between these properties is of fundamental importance and may lead the way for development of improved solid state ionic conductors. In this study, we use inelastic neutron scattering and ab initio modeling to study a representative proton conductor, La0.8Ba1.2GaO3.9, where different local structures are possible for the same stoichiometry. The intrinsic correlations between the local bonding environment and the dynamical behavior of protons are presented. In particular, we identify how the local Ba/La concentration affects the proton vibrational frequencies, hydrogen bond strength, O–H rotations and in turn long-range proton mobility. Further, possible mechanism for proton transport, through the inter-tetrahedral bond switching, O–H rotations and tetrahedral reorientation is anticipated. [ABSTRACT FROM AUTHOR]

The recycling of waste-tire rubber is of critical importance since the discarded tires pose serious environmental and health hazards to our society. Here, we report a new application for hard-carbon materials derived from waste-tires as anodes in potassium-ion batteries. The sustainable tire-derived carbons show good reversible potassium insertion at relatively high rates. Long-term stability tests exhibit capacities of 155 and 141 mAh g-1 for carbon pyrolyzed at 1100°C and 1600°C, respectively, after 200 cycles at current rate of C/2. This study provides an alternative solution for inexpensive and environmental benign potassium-ion battery anode materials. [ABSTRACT FROM AUTHOR]

Lithium bis(2‐methyl‐2‐fluoromalonato)borate (LiBMFMB), as an additive for LiNi0.5Mn1.5O4, exhibits improved efficiencies and cycling stability. Cyclic voltammograms indicate the cells with additive form good solid‐electrolyte interphases (SEIs) during the first cycle, whereas no additive cell needs more cycles to form a functional SEI. X‐ray photoelectron spectroscopy reveals LiBMFMB could reduce the decomposition of LiPF6 salt and solvents, resulting in thinner SEI. [ABSTRACT FROM AUTHOR]

A new type of nitrogen‐enriched carbon materials is synthesized from nitrile‐rich alkali salts. High nitrogen content is obtained for these alkali salts precursors after annealing at 850 °C. These nitrogen‐enriched carbons exhibit high coulombic efficiency, high reversible capacity and good cycling stability as anode materials for both mature lithium ion batteries and newly rejuvenated sodium ion batteries. [ABSTRACT FROM AUTHOR]

Crystallization studies were performed of epitaxial La2Zr2O7 (LZO) films on biaxially textured Ni–3at.%W substrates having thin Y2O3 (10 nm) seed layers. LZO films were deposited under controlled humid atmosphere using reel-to-reel slot-die coating of chemical solution precursors. Controlled crystallization under various processing conditions has revealed a broad phase space for obtaining high-quality, epitaxial LZO films without microcracks, with no degradation of crystallographic texture and with high surface crystallinity. Crack-free and strong c-axis aligned LZO films with no random orientation were obtained even at relatively low annealing temperatures of 850°–950°C in flowing one atmosphere gas mixtures of Ar–4% H2 with an effective oxygen partial pressure of P(O2)∼10−22 atm. Texture and reflection high-energy electron diffraction analyses reveal that low-temperature-annealed samples have strong cube-on-cube epitaxy and high surface crystallinity, comparable to those of LZO film annealed at high temperature of 1100°C. In addition, these samples have a smoother surface morphology than films annealed at higher temperatures. Ni diffusion rate into the LZO buffer film is also expected to be significantly reduced at the lower annealing temperatures. [ABSTRACT FROM AUTHOR]

YBa2Cu3O7−δ (YBCO) films with thicknesses ranging from 1.0 to 6.4 μm were deposited by pulsed laser deposition on rolling-assisted biaxially textured substrates (RABiTS). The RABiTS were of the configuration CeO2/YSZ/Y2O3/Ni–3 at.% W. As the YBCO film thickness increased, Ic continued to increase and reached ∼300 A/cm width for a 4.3 μm-thick YBCO film. Commonly observed mechanisms for Jc decrease with increasing YBCO film thickness were not observed. Homogeneous microstructures obtained in even the thickest YBCO films, suggest that the Ic/width can still be enhanced considerably. [ABSTRACT FROM AUTHOR]

Solid Electrolyte Interphases: Insight into the Solid Electrolyte Interphase Formation in Bis(fluorosulfonyl)Imide Based Ionic Liquid Electrolytes (Adv. Funct. 1-ethyl-3-methylimidazolium bis(fluorosulfonyl)imide, ionic liquids, lithium bis(fluorosulfonyl)imide, neutron scattering, operando characterization, solid electrolyte interphase Keywords: 1-ethyl-3-methylimidazolium bis(fluorosulfonyl)imide; ionic liquids; lithium bis(fluorosulfonyl)imide; neutron scattering; operando characterization; solid electrolyte interphase EN 1-ethyl-3-methylimidazolium bis(fluorosulfonyl)imide ionic liquids lithium bis(fluorosulfonyl)imide neutron scattering operando characterization solid electrolyte interphase 1 1 1 06/07/21 20210615 NES 210615 In article number 2008708, Charl J. Jafta, Xiao-Guang Sun, Craig Bridges, and co-workers use high surface area mesoporous hard carbons to demonstrate that surface passivation for the bis(fluorosulfonyl)imide anion (FSI SP - sp ) occurs via chemical reactions at the open cell voltage, and through electrochemical reactions at cell voltages near 2 V. The research provides insight into the design of anions for stable inorganic salt passivation of electrode interfaces in next generation batteries. [Extracted from the article]

Lithium-ion batteries (LIBs) have revolutionized portable electronics and electric vehicles (EVs), but the growing accumulation of end-of-life (EOL) batteries poses environmental challenges. Recycling high-value cathodes from EOL LIBs can minimize waste and reduce the need for mining critical minerals. This study focuses on the direct recycling of Ni-rich cathodes, particularly lithium-manganese-cobalt-oxide (NMC) 622 in a "reciprocal ternary molten salts (RTMS)" system. The ionothermal relithiation in the RTMS system successfully restores the layered structure, lithium content, and electrochemical performance of the NMC 622 cathode, comparable to the pristine material. The cost analysis reveals that cathode regeneration through ionothermal relithiation is more economical than virgin production or conventional recycling methods. • A "reciprocal ternary molten salts" (RTMS) system for direct battery recycling. • Directly recycling of spent Ni-rich cathodes by topotactic reactions in RTMS. • A low cost and highly efficient direct recycling process for spent Li-ion batteries. [ABSTRACT FROM AUTHOR]

Abstract Three trimethylsilyl based malonate esters, bis(trimethylsilyl) 2-methyl-2-fluoromalonate (BTMSMFM), bis(trimethylsilyl) 2-ethyl-2-fluoromalonate (BTMSEFM) and bis(trimethylsilyl) 2-propyl-2-fluoromalonate (BTMSPFM), have been used as additives in 1.0 M LiPF 6 /ethylene carbonate (EC)-dimethyl carbonate (DMC)-diethyl carbonate (DEC) (1-1-1, by v) baseline electrolyte for LiNi 0.80 Co 0.15 Al 0.05 O 2 (NCA) based high voltage lithium ion batteries. The NCA half-cells with 5 wt% BTMSMFM exhibit higher capacity retention than that in the baseline electrolyte at different upper cut off voltages, that is, 4.2, 4.3, 4.4 and 4.5 V vs. Li/Li+. Scanning electron microscope (SEM) show that the additive successfully prevents the formation of thick solid electrolyte interphase (SEI) films on the surface of the NCA electrodes. X-ray diffraction (XRD) further reveals that the crystal structure of NCA is also maintained in the electrolyte with 5 wt% BTMSMFM at high cut off voltages. Besides beneficial to NCA cathode, the BTMSMFM additive also ensures better cycling performance of the graphite based half-cells and NCA/graphite full-cells, and thus is a promising additive for application in rechargeable lithium ion batteries. Highlights • BTMSMFM additive significantly improves long cycling stability of NCA half-cells up to 4.5 V. • BTMSMFM additive prevents the formation of thick SEI films in conventional carbonate electrolytes. • BTMSMFM additive preserves structural stability of NCA material at different upper cut off voltages. • Electrolyte decomposition and parasitic side reactions are suppressed effectively. [ABSTRACT FROM AUTHOR]

YBa2Cu3O7−δ (YBCO) films with thicknesses ranging from 1.0 to 6.4 μm were deposited by pulsed laser deposition on rolling-assisted biaxially textured substrates (RABiTS). The RABiTS were of the configuration CeO2/YSZ/Y2O3/Ni–3 at.% W. As the YBCO film thickness increased, Ic continued to increase and reached ∼300 A/cm width for a 4.3 μm-thick YBCO film. Commonly observed mechanisms for Jc decrease with increasing YBCO film thickness were not observed. Homogeneous microstructures obtained in even the thickest YBCO films, suggest that the Ic/width can still be enhanced considerably. [ABSTRACT FROM AUTHOR]

Recovery of lithium from brines by liquid-liquid solvent extraction (LLE) with diketones and synergistic co-ligands has been investigated for decades, but industrial application has been limited. In pursuit of a ligand with improved properties, a series of ketonamides with beta-carbonyl groups were designed, synthesized, and tested in extraction of lithium from sulfate and carbonate simulants of clay mineral tailing leachates. The best performing ligand, a novel tricarbonyl amide, was characterized for lithium extraction with and without four synergistic co-ligands. The tricarbonyl amide combined with the synergistic co-ligand Cyanex-923 was absorbed on a resin support. The ligand-modified resin was tested for performance in extraction of dilute brine simulants and up to 60 % recovery of lithium was achieved., (© 2024 Wiley-VCH GmbH.)