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Recent experimental results have demonstrated that zwitterionic ionogel comprised of polyzwitterion (polyZI)-supported lithium salt-doped ionic liquid exhibits improved conductivities and lithium transference numbers than the salt-doped base ionic liquid electrolyte (ILE). However, the underlying mechanisms of such observations remain unresolved. In this work, we pursued a systematic investigation to understand the impact of the polyZI content and salt concentration on the structural and dynamic properties of the poly(MPC) ionogel of our model polyZI ionogel, poly(2-methacryloyloxyethyl phosphorylcholine) [poly(MPC)] supported LiTFSI/N-butyl-N-methylpyrrolidinium TFSI base ionic liquid electrolyte. Our structural analyses show strong lithium–ZI interaction consistent with the physical network characteristic observed in the experiments. An increase in polyZI content leads to an increased fraction of Li+ ions coordinated with the polyZI. In contrast, an increase in salt concentration leads to a decreased fraction of Li+ ions coordinated with the polyZI. The diffusivities of the mobile ions in the poly(MPC) ionogel were found to be lower than the base ILE in agreement with experiments at T > 300 K. Analysis of ion transport mechanisms shows that lithium ions within the poly(MPC) ionogel travel via a combination of structural, vehicular diffusion, as well as hopping mechanism. Finally, the conductivity trend crossover between the poly(MPC) ionogel and the base ILE was rationalized via a temperature study that showed that the base ILE ions are influenced more by the variation of temperature when compared to the poly(MPC) ions. [ABSTRACT FROM AUTHOR]

Using large-scale molecular dynamics simulations, we investigate the surface properties of lithium, sodium, and potassium silicate glasses containing 25 mol % of alkali oxide. The comparison of two types of surfaces, a melt-formed surface (MS) and a fracture surface (FS), demonstrates that the influence of the alkali modifier on the surface properties depends strongly on the nature of the surface. The FS exhibits a monotonic increase of modifier concentration with increasing alkali size while the MS shows a saturation of alkali concentration when going from Na to K glasses, indicating the presence of competing mechanisms that influence the properties of a MS. For the FS, we find that larger alkali ions reduce the concentration of under-coordinated Si atoms and increase the fraction of two-membered rings, implying an enhanced chemical reactivity of the surface. For both types of surfaces, the roughness is found to increase with alkali size, with the effect being more pronounced for the FS than for the MS. The height–height correlation functions of the surfaces show a scaling behavior that is independent of the alkali species considered: The ones for the MS are compatible with the prediction of the frozen capillary wave theory while the ones for the FS show a logarithmic growth, i.e., on the nanoscale these surfaces are not self-affine fractals. The influence of the modifier on the surface properties are rationalized in terms of the interplay between multiple factors involving the size of the ions, bond strength, and charge balance on the surface. [ABSTRACT FROM AUTHOR]

Lithium-ion batteries (LIBs) has extensively utilized in electric vehicles and portable electronics due to their high energy density and prolonged lifespan. However, the current commercial LIBs are plagued by relatively low energy density. High-entropy materials with multiple components have emerged as an efficient strategic approach for developing novel materials that effectively improve the overall performance of LIBs. This article provides a comprehensive review the recent advancements in rational design of innovative high-entropy materials for LIBs, as well as the exceptional lithium ion storage mechanism for high-entropy electrodes and considerable ionic conductivity for high-entropy electrolytes. This review also analyses the prominent effects of individual components on the high-entropy materials' exceptional capacity, considerable structural stability, rapid lithium ion diffusion, and excellent ionic conductivity. Furthermore, this review presents the synthesis methods and their influence on the morphology and properties of high-entropy materials. Ultimately, the remaining challenges and future research directions are outlined, aimed at developing more effective high-entropy materials and improving the overall electrochemical performance of LIBs. [ABSTRACT FROM AUTHOR]

Perovskite SrVO 3 stands out as a promising anode material for lithium-ion batteries due to its inherent redox activity, excellent electrical conductivity, and structural adaptability. Despite these advantages, challenges persist, such as in achieving high tap density and volumetric specific capacity. In this study, we overcome these challenges by finely regulating particle size and constructing a tailored surface structure for SrVO 3. The implementation of ball milling during the synthesis process proves to be a simple yet highly efficient method for simultaneously tailoring particle size and in-situ creating an amorphous layer on SrVO 3 particles. The reduction in particle size not only facilitates enhanced electron and ion transport but also significantly improves the tap density of SrVO 3 , increasing it from 2.61 to 3.15 g cm−3. The in-situ construction of an amorphous layer introduces a multitude of defects and high valence V5+. These defects serve as active sites for lithium ions, while the V5+ species contribute to increased electron transfer, collectively resulting in a high gravimetric specific capacity. The engineered SrVO 3 anode delivers an impressive volumetric capacity of 1134 mAh cm−3 at 0.1 A g−1, surpassing both pristine SrVO 3 (733 mAh cm−3) and commercial graphite anode (∼460 mAh cm−3). [ABSTRACT FROM AUTHOR]

Carbon cloth (CC) possesses great potential as a sulfur host because of its excellent conductivity, flexibility, and easily modified free‐standing structure. However, the previous works do not take full advantage of CC except for the role of support and current collector. The smooth surface, small specific surface area, and poor binding force between coating materials and CC matrix are unfavorable for loading coating materials. The slow redox kinetics and low sulfur loading of sulfur cathodes still seriously restrict the development of Lithium–Sulfur (Li–S) batteries. Herein, the porous carbon cloth loading cobalt selenide (PCC@CoSe2) is constructed as an integrated sulfur host through a pore‐creating and selenylation strategy. The pore‐creating engineering greatly optimizes the 3D pore structure of CC to raise the sulfur and catalyst loading and provides enough space to accommodate the volume change of sulfur species. In addition, CoSe2 particles as nano‐catalyst units embedded in PCC can effectively adsorb‐catalyze polysulfides and improve the reaction kinetics. The resulting integrated sulfur cathode has realized the high‐efficiency polysulfide catalytic conversion and fast lithium ion migration, significantly enhancing redox kinetics and sulfur loading. [ABSTRACT FROM AUTHOR]

• Pyrolysis combined with ball milling is proposed to upcycle SG from retired LIBs. • Pyrolysis at 500 °C leads to about 82.2 % PVDF dissociation in TG. • Ball milling assisted by urea produces abundant graphite flakes at the edge of MG. • High purity and unique edge structural features of MG result in exceptional capacity. Vast quantities of anode graphite from waste lithium ion batteries (LIBs), as a type of underrated urban mine, has enormous potential to be exploited for resource recovery. Herein, we propose a benign process integrating low-temperature pyrolysis and mechanochemical techniques to upcycle spent graphite (SG) from end-of-life LIBs. Pyrolysis at 500 °C leads to about 82.2 % PVDF dissociation in thermal treated graphite (TG). Solid-phase exfoliation via ball milling assisted by urea successfully produces abundant graphite flakes and a small amount of monolayer graphene nanosheet at the edge of mechanochemically processed graphite (MG). Subsequent rinsing removes the residual LiF salts. High purity and unique edge structural features of the as-prepared MG offer more active sites and storage reservoir for intercalation and de-intercalation of lithium ions, resulting in enhanced lithium-ion diffusion kinetics, excellent reversible specific capacity and desirable rate capability. Inspiringly, MG exhibits a remarkably enhanced initial specific charge capacity of 521.3 mAh g−1 during the first charge–discharge, and only declines from 569.9 mAh g−1 to 538 mAh g−1 with slight attenuation after 50 consecutive cycles at 0.1 A/g, indicating satisfactory cycle stability. Additionally, the purification and reconstruction mechanism for MG have been illustrated in detail. This study offers a green strategy to reconstruct and upgrade anode graphite from LIBs, which can realize sustainable waste management. [ABSTRACT FROM AUTHOR]

Lithium‐ion batteries have found extensive applications due to their high energy density and low self‐discharge rates, spanning from compact consumer electronics to large‐scale energy storage facilities. Despite their widespread use, challenges such as inherent capacity degradation and the potential for thermal runaway hinder sustainable development. In this study, we introduce a unique approach to synthesize anode materials for lithium‐ion batteries, specifically imidazole‐intercalated cobalt hydroxide. This innovative material significantly enhances the Li+ desolvation/diffusion reaction and flame‐retardant dynamics through complexing and catalytic synergetic effects. The lithium‐ion batteries incorporating these materials demonstrate exceptional performance, boasting an impressive capacity retention of 997.91 mAh g−1 after 500 cycles. This achievement can be attributed to the optimization of the solid electrolyte interphase (SEI) interface engineering, effectively mitigating anode degradation and minimizing electrolyte consumption. Experimental and theoretical calculations validate these improvements. Importantly, imidazole intercalated Co(OH)2 (MI−Co(OH)2) exhibits a remarkable catalytic effect on electrolyte carbonization and the conversion of CO to CO2. This dual action suppresses smoke and reduces toxicity significantly. The presented work introduces a novel approach to realizing high‐performance and safe lithium‐ion batteries, addressing key challenges in the pursuit of sustainable energy solutions. [ABSTRACT FROM AUTHOR]

Photoinduced single‐electron reduction is an efficient method for the mono‐selective activation of the C−F bond on a trifluoromethyl group to construct a difluoroalkyl group. We have developed an electron‐donor‐acceptor (EDA) complex mediated single‐electron transfer (EDA‐SET) of α,α,α‐trifluoromethyl arenes in the presence of lithium salt to give α,α‐difluoroalkylarenes. The C−F bond reduction was realized by lithium iodide and triethylamine, two common feedstock reagents. Mechanistic studies revealed the generation of a α,α‐difluoromethyl radical by single‐electron reduction and defluorination, followed by the radical addition to alkenes. Lithium salt interacted with the fluorine atom to promote the photoinduced reduction mediated by the EDA complex. Computational studies indicated that the lithium‐assisted defluorination and the single‐electron reduction occurred concertedly. We call this phenomenon fluoride‐coupled electron transfer (FCET). FCET is a novel approach to C−F bond activation for the synthesis of organofluorine compounds. [ABSTRACT FROM AUTHOR]

Lithium‐ion batteries have found extensive applications due to their high energy density and low self‐discharge rates, spanning from compact consumer electronics to large‐scale energy storage facilities. Despite their widespread use, challenges such as inherent capacity degradation and the potential for thermal runaway hinder sustainable development. In this study, we introduce a unique approach to synthesize anode materials for lithium‐ion batteries, specifically imidazole‐intercalated cobalt hydroxide. This innovative material significantly enhances the Li+ desolvation/diffusion reaction and flame‐retardant dynamics through complexing and catalytic synergetic effects. The lithium‐ion batteries incorporating these materials demonstrate exceptional performance, boasting an impressive capacity retention of 997.91 mAh g−1 after 500 cycles. This achievement can be attributed to the optimization of the solid electrolyte interphase (SEI) interface engineering, effectively mitigating anode degradation and minimizing electrolyte consumption. Experimental and theoretical calculations validate these improvements. Importantly, imidazole intercalated Co(OH)2 (MI−Co(OH)2) exhibits a remarkable catalytic effect on electrolyte carbonization and the conversion of CO to CO2. This dual action suppresses smoke and reduces toxicity significantly. The presented work introduces a novel approach to realizing high‐performance and safe lithium‐ion batteries, addressing key challenges in the pursuit of sustainable energy solutions. [ABSTRACT FROM AUTHOR]

Lithium-ion batteries (LIBs) are greatly limited in their practical application because of their poor cycle performance, low conductivity and volume expansion. Herein, molten salts (MSs) FeCl3·6H2O-NMP with low temperature via simple preparation are used as the anode material of LIBs for the first time to break through the bottleneck of LIBs. The good fluidity and high self-healing of FeCl3·6H2O-NMP effectively avoid the collapse and breakage of the structure. Based on this feature, the initial discharge specific capacity reached 770.28 mA h g-1, which was more than twice that of the commercial graphite anode. After 200 cycles at a current density of 100 mA g-1, the specific capacity did not decrease rather it was found to be higher than the initial discharge specific capacity, reaching 867.24 mA h g-1. Besides, the good conductivity of MSs provides convenience for the removal and intercalation of Li+. The active H sites that can combine with lithium ions form LiH and provide capacity for LIBs. Density functional theory (DFT) calculation also provided theoretical proof for the mechanism of LIBs. [ABSTRACT FROM AUTHOR]

Here, lithium ions inserted crystalline carbon nitrides (LCCN) with different defect concentrations are prepared by elaborately regulating the mass transfer process in thermal polymerization. It is revealed that there is no conventional exciton–polarons‐induced exciton dissociation mechanism in LCCN due to the weak coupling between excitons and phonons. On the contrary, excitons continue to trap/detrap through defect‐induced traps, which weakens the Coulomb force between electron–hole pairs, thereby accelerating exciton dissociation. It is worth emphasizing that this is the first systematic research on the exciton dissociation characteristics and photocatalytic activity of LCCN of poly(heptazine imide) structure. A strategy of assisting exciton dissociation through defect‐induced traps to address the inherently high exciton binding energy and low exciton dissociation efficiency issues in polymer photocatalysts is proposed. [ABSTRACT FROM AUTHOR]

LiFePO 4 /Very-few-layer-graphene (LFP/VFLG) composites have been prepared using the sol-gel method for lithium-ion battery cathode. VFLG dominated by 1∼3 layers was obtained from an economical and environmentally benign process. Structural properties of LFP/VFLG composites were studied using Fourier-transform infrared spectra (FTIR) spectroscopy, X-ray diffractometry (XRD), high-resolution transmission electron microscopy (HRTEM) and Raman spectroscopy, while the electrochemical performance was measured using galvanostatic discharge, cyclic voltammetry (CV), and electrochemical impedance spectroscopy (EIS) tests. The FTIR analysis confirmed that incorporating VFLG neither affected the chemical structure of LiFePO 4 nor initiated any side reactions during the LiFePO 4 formation reaction. The XRD results showed that LFP/VFLG composites had better lattice parameters, crystallinity, and phase purity than LiFePO 4 without VFLG addition. The Raman spectroscopy analysis indicated that LFP/VFLG composites had a lower disorder in the carbon arrangement. HRTEM results indicated that a VFLG was successfully wrapped around the LFP particle offers a versatile way to enhanced electrochemical performance of LFP/VFLG composites. The galvanostatic discharge profiles showed an enhancing specific discharge capacity of up to 58.3% after incorporating VFLG. The cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS) tests revealed that LFP/VFLG delivered small polarization, low inner resistance, high electrochemical reaction reversibility, and high lithium-ion diffusion coefficient. VFLG is a promising additive to improve the structural and electrochemical properties of the LiFePO 4 cathode of lithium-ion batteries. [ABSTRACT FROM AUTHOR]

Silicon-based material is one of the most promising substitutes for commercial graphite anodes for the next generation lithium-ion batteries due to its extremely high theoretical capacity. However, the huge volume changes during the charging and discharging processes will cause rapid capacity decay and a short cycle life. Developing novel silicon-based materials requires a fundamental understanding of their properties. However, in many cases, the present experiments are incapable of completely mimicking real battery-operation conditions, and detailed information about the electrochemical mechanisms and ion and electron kinetic transport at the electrode/electrolyte interface is still ambiguous due to their complexity. First-principles calculations have become an effective method for predicting and interpreting the characteristics of electrode materials, understanding the electrochemical mechanisms at the atomic scale and delivering rational design strategies for electrode materials. In this review, the first-principles calculations of silicon-based anode materials in recent years, based on different modification strategies, are summarized. First, we introduce the diffusion kinetics of lithium ions in silicon and the mechanism of structure changes during the lithiation process. Then, typical examples of novel Si-based anodes, including 2D nanomaterials, silicide materials and coating materials based on theoretical predictions, are presented. Finally, we provide perspectives and future directions of first-principles calculations on Si-based anodes. [ABSTRACT FROM AUTHOR]

Graphite has been serving as the key anode material of rechargeable Li‐ion batteries, yet is difficultly charged within a quarter hour while maintaining stable electrochemistry. In addition to a defective edge structure that prevents fast Li‐ion entry, the high‐rate performance of graphite could be hampered by co‐intercalation and parasitic reduction of solvent molecules at anode/electrolyte interface. Conventional surface modification by pitch‐derived carbon barely isolates the solvent and electrons, and usually lead to inadequate rate capability to meet practical fast‐charge requirements. Here we show that, by applying a MoOx−MoNx layer onto graphite surface, the interface allows fast Li‐ion diffusion yet blocks solvent access and electron leakage. By regulating interfacial mass and charge transfer, the modified graphite anode delivers a reversible capacity of 340.3 mAh g−1 after 4000 cycles at 6 C, showing promises in building 10‐min‐rechargeable batteries with a long operation life. [ABSTRACT FROM AUTHOR]

Graphite has been serving as the key anode material of rechargeable Li‐ion batteries, yet is difficultly charged within a quarter hour while maintaining stable electrochemistry. In addition to a defective edge structure that prevents fast Li‐ion entry, the high‐rate performance of graphite could be hampered by co‐intercalation and parasitic reduction of solvent molecules at anode/electrolyte interface. Conventional surface modification by pitch‐derived carbon barely isolates the solvent and electrons, and usually lead to inadequate rate capability to meet practical fast‐charge requirements. Here we show that, by applying a MoOx−MoNx layer onto graphite surface, the interface allows fast Li‐ion diffusion yet blocks solvent access and electron leakage. By regulating interfacial mass and charge transfer, the modified graphite anode delivers a reversible capacity of 340.3 mAh g−1 after 4000 cycles at 6 C, showing promises in building 10‐min‐rechargeable batteries with a long operation life. [ABSTRACT FROM AUTHOR]

Solid-state electrolytes (SSEs) are the key materials in the new generation of all-solid-state lithium ion/metal batteries. Metal–organic frameworks (MOFs) are ideal materials for developing solid electrolytes because of their structural diversity and porous properties. However, there are several significant issues and obstacles involved, such as lower ion conductivity, a smaller ion transport number, a narrower electrochemical stability window and poor interface contact. In this review, a comprehensive analysis and summary of the unique ion-conducting behavior of MOF-based electrolytes in rechargeable batteries are presented, and the different design principles of MOF-based SSEs are classified and emphasized. Accordingly, four design principles for achieving these MOF-based SSEs are presented and the influence of SSEs combined with MOFs on the electrochemical performance of the batteries is described. Finally, the challenges in the application of MOF materials in lithium ion/metal batteries are explored, and directions for future research on MOF-based electrolytes are proposed. This review will deepen the understanding of MOF-based electrolytes and promote the development of high-performance solid-state lithium ion/metal batteries. This review not only provides theoretical guidance for research on new MOF-based SSE systems, but also contributes to further development of MOFs applied to rechargeable batteries. [ABSTRACT FROM AUTHOR]

Three‐dimensional (3D) self‐supported Ge anode is one of the promising candidates to replace the traditional graphite anode material for high‐performance binder‐free lithium‐ion batteries (LIBs). The enlarged surface area and the shortened ions/electrons transporting distance of the 3D electrode would greatly facilitate the rapid transfer of abundant lithium ions during cycling, thus achieve enhanced energy and power density during cycling. Cycle stability of the 3D self‐supported Ge electrode would be improved due to the obtained enough space could effectively accommodate the large volume expansion of the Ge anode. In this review, we first describe the electrochemical properties and Li ions storage mechanism of Ge anode. Moreover, the recent advances in the 3D self‐supported Ge anode architectures design are majorly illustrated and discussed. Challenges and prospects of the 3D self‐supported Ge electrode are finally provided, which shed light on ways to design more reliable 3D Ge‐based electrodes in energy storage systems. [ABSTRACT FROM AUTHOR]

Multiplex sampling, so far mainly used as a tool for S/N ratio improvement in spectroscopic applications and separation techniques, has been investigated here for its potential suitability for time-resolved monitoring where chromatograms of transient signals are recorded at intervals much shorter than the chromatographic runtime. Different designs of multiplex sample introduction were developed and utilized to analyze lithium-ion battery degradation products under normal or abuse conditions to achieve fast and efficient sample introduction. After comprehensive optimization, measurements were performed on two different GC systems, with either barrier discharge ionization detection (BID) or mass spectrometric detection (MS). Three different injector designs were examined, and modifications in the pertinent hardware components and operational conditions used. The shortest achievable sample introduction time was 50 ms with an interval of 6 s. Relative standard deviations were lower than 4% and 10% for the intra- and inter-day repeatability, respectively. The sample introduction system and column head pressure had to be carefully controlled, as this parameter most critically affects the amount of sample introduced and, thus, detector response. The newly developed sample introduction system was successfully used to monitor volatile degradation products of lithium-ion batteries and demonstrated concentration changes over the course of time of the degradation products (e.g., fluoroethane, acetaldehyde and ethane), as well as for solvents from the battery electrolyte like ethyl carbonate. [ABSTRACT FROM AUTHOR]

In this article, we employed concepts from Density Functional Theory to investigate the interaction energy behavior between the fragments of two‐dimensional systems composed of graphene‐based materials and lithium ions. Specifically, the proposed system consists of two graphene sheets separated by a controlled distance (face‐to‐face), with a lithium ion positioned at the center of this separation. Additionally, we examined potential electronic transitions within these systems and assessed the feasibility of quantum entanglement generation and manipulation. Our findings revealed that the interaction energies within the analyzed systems exhibited behavior akin to that described by the Lennard‐Jones potential, which characterizes systems with favorable energy for their formation. The results further yielded estimates for the constants ϵ and σ, with values of −66.59 kcal/mol and 1.63 Å, respectively. Specific electronic transitions were identified, suggesting the potential for quantum entanglement generation and manipulation among the two‐dimensional graphene system mediated by the lithium ion interactions. [ABSTRACT FROM AUTHOR]

Rationale: As 3‐OH‐containing steroids are prone to dehydration by conventional electrospray ionization, reducing detection sensitivity, Li ion adduction‐based ultrahigh‐performance liquid chromatography–tandem mass spectrometry (UHPLC/MS/MS), developed to prevent dehydration and effectively detect 3‐OH steroids, was applied for profiling total and free steroids in urine. Methods: Free urinary steroids were isolated directly from urine by solid‐phase extraction (SPE) with 80% acetonitrile. The total steroids were prepared by enzymatic treatment of urine with a cocktail of sulfatase and glucronidase, protein precipitation, and separation with the above SPE. In order to detect as many steroid types as possible, UHPLC/MS/MS (Li method) with Li+ solution added after the column was used for analysis in addition to the conventional method of detecting protonated ions (H method). The 13 3‐OH steroids and the remaining 16 steroids were quantified by standard curves prepared using product ion transitions derived from [M + Li]+ and MH+, respectively. Results: Two groups of human urine, male and female urine, were analyzed. 3‐OH steroids could be detected with greater sensitivity using the Li method than the conventional method. The absolute amounts of each steroid were normalized based on creatinine levels. The difference between the male and female groups are clearly attributable to sex steroids. Conclusions: Twenty‐nine total steroids and 19 free steroids were identified in a limited volume (240 mL) of urine. Of these, 13 3‐OH steroids were better detected by Li+ adduction‐based UHPLC/MS/MS. [ABSTRACT FROM AUTHOR]

7Li nuclear magnetic resonance (NMR) spectroscopy is an ideal tool to study hierarchically assembled helicates of the form Li[Li3L6Ti2]. Internally bound and external lithium ions can be well distinguished by solution‐ or solid‐state NMR spectroscopy and dimerization constants of the monomer/dimer equilibrium can be easily determined in solution. Averaged dimerization constants can be estimated in case of statistical mixtures of helicates formed from mixtures of ligands. [ABSTRACT FROM AUTHOR]

Compared to traditional lithium‐ion batteries with liquid electrolytes, all‐solid‐state lithium batteries have attracted extensive attention due to their heightened safety and energy density. Lithium argyrodite materials are promising solid electrolytes (SE) due to their high ionic conductivity, low grain boundary resistance, and favorable mechanical properties. However, the poor chemical/electrochemical stability of lithium argyrodite electrolytes toward the bare lithium metal anode inhibits their applications in all‐solid‐state lithium metal batteries (ASSLMBs). Here, Li‐SnF2 composite anodeswas used to induce the formation of solid electrolyte interphase (SEI) composed of LiCl, LiF, and Li22Sn5 at the Li/SE interface. The high interface energy barriers for LiF and LiCl induces the uniform deposition of lithium ions, thus hindering the growth of lithium dendrites. Meanwhile, the fast Li‐ion diffusion coefficient of the Li22Sn5 alloy accelerates Li‐ion migration across the interface section. The symmetrical cell exhibits stable cycling performance over long durations over 300 h at 0.5 mA cm−2. Moreover, the LiNbO3@NCM712/Li5.5PS4.5Cl1.5/Li‐10%SnF2 battery delivers a high initial discharge capacity of 170.9 mAh g−1 at 0.1C and retains 72.9% of its original capacity after 500 cycles at 0.5C. The facial approach for Li‐SnF2 composite anode enables the production of ASSLMBs with superior electrochemical performance. [ABSTRACT FROM AUTHOR]

Electrolyte is critical for transporting lithium‐ion (Li+) in lithium‐ion batteries (LIBs). However, there is no universally applicable principle for designing an optimal electrolyte. In most cases, the design process relies on empirical experiences and is often treated as highly confidential proprietary information. Herein, a solvation structure‐related model for the quantitative design of electrolytes is introduced, focusing on the principles of coordination chemistry. As a paradigmatic example, a high‐voltage electrolyte (i.e., 4.5 V vs anode) aimed at achieving a high energy density and fast charging LIB, which is specifically composed of an emerging, well‐constructed hybrid hard carbon‐silicon/carbon‐based anode, and lithium cobalt oxide cathode, is developed. Not only the functions of each electrolyte component at the molecular scale within the Li+ solvation structure are analyzed but also an interfacial model is introduced to elucidate their relationship with the battery performance. This study represents a pioneering effort in developing a methodology to guide electrolyte design, in which the mutual effects of the Li+ de‐solvation process and solid electrolyte interface (SEI) on the electrode surface are explored concurrently to understand the root cause of superior performance. This innovative approach establishes a new paradigm in electrolyte design, providing valuable insights at the molecular level. [ABSTRACT FROM AUTHOR]

Cyano‐containing electrodes usually promise high theoretical potentials while suffering from uncontrollable self‐dissolution and sluggish reaction kinetics. Herein, to remedy their limitations, an unprecedented core–shell heterostructured electrode of carbon nanotubes encapsulated in poly(1,4‐dicyanoperfluorobenzene sulfide) (CNT@PFDCB) is rationally crafted via molecule and microstructure modulations. Specifically, the linkage of sulfide bridges of PFDCB prevents the active cyano groups from dissolving, resulting in a robust structure. The fluorinations modulate the electronic configurations in frontier orbitals, allowing higher electrical conductivity and elevated output voltage. Combined with the core–shell architecture to unlock the sluggish diffusion kinetics for both electrons and guest ions, the CNT@PFDCB exhibits an impressive capacity (203.5 mAh g−1), remarkable rate ability (127.6 mAh g−1 at 3.0 A g−1), and exceptional cycling stability (retaining 81.1 % capacity after 3000 cycles at 1.0 A g−1). Additionally, the Li‐storage mechanisms regarding PFDCB are thoroughly revealed by in situ attenuated total reflection infrared spectroscopy, in situ Raman spectroscopy, and theoretical simulations, which involve the coordination interaction between Li ions and cyano groups and the electron delocalization along the conjugated skeleton. More importantly, a practical fully organic cell based on the CNT@PFDCB is well‐validated that demonstrates a tremendous potential of cyanopolymer as the cathode to replace its inorganic counterparts. [ABSTRACT FROM AUTHOR]

Cyano‐containing electrodes usually promise high theoretical potentials while suffering from uncontrollable self‐dissolution and sluggish reaction kinetics. Herein, to remedy their limitations, an unprecedented core–shell heterostructured electrode of carbon nanotubes encapsulated in poly(1,4‐dicyanoperfluorobenzene sulfide) (CNT@PFDCB) is rationally crafted via molecule and microstructure modulations. Specifically, the linkage of sulfide bridges of PFDCB prevents the active cyano groups from dissolving, resulting in a robust structure. The fluorinations modulate the electronic configurations in frontier orbitals, allowing higher electrical conductivity and elevated output voltage. Combined with the core–shell architecture to unlock the sluggish diffusion kinetics for both electrons and guest ions, the CNT@PFDCB exhibits an impressive capacity (203.5 mAh g−1), remarkable rate ability (127.6 mAh g−1 at 3.0 A g−1), and exceptional cycling stability (retaining 81.1 % capacity after 3000 cycles at 1.0 A g−1). Additionally, the Li‐storage mechanisms regarding PFDCB are thoroughly revealed by in situ attenuated total reflection infrared spectroscopy, in situ Raman spectroscopy, and theoretical simulations, which involve the coordination interaction between Li ions and cyano groups and the electron delocalization along the conjugated skeleton. More importantly, a practical fully organic cell based on the CNT@PFDCB is well‐validated that demonstrates a tremendous potential of cyanopolymer as the cathode to replace its inorganic counterparts. [ABSTRACT FROM AUTHOR]

In the field of lithium-ion batteries, the challenges posed by the low melting point and inadequate wettability of conventional polyolefin separators have increased the focus on ceramic-coated separators. This study introduces a highly efficient and stable boehmite/polydopamine/polyethylene (AlOOH-PDA-PE) separator. It is crafted by covalently attaching functionalized nanosized boehmite (γ-AlOOH) whiskers onto polyethylene (PE) surfaces. The presence of a covalent bond increases the stability at the interface, while amino groups on the surface of the separator enhance the infiltration of the electrolyte and facilitate the diffusion of lithium ions. The PE-PDA-AlOOH separator, when used in lithium-ion batteries, achieves a discharge capacity of 126 mAh g−1 at 5 C and retains 97.1% capacity after 400 cycles, indicating superior cycling stability due to its covalently bonded ceramic surface. Thus, covalent interface modification is a promising strategy to prevent delamination of ceramic coatings in separators. [ABSTRACT FROM AUTHOR]

Na+/H+ antiporters facilitate the exchange of Na+ for H+ across the cytoplasmic membrane in prokaryotic and eukaryotic cells. These transporters are crucial to maintain the homeostasis of sodium ions, consequently pH, and volume of the cells. Therefore, sodium/proton antiporters are considered promising therapeutic targets in humans. The Na+/H+ antiporter in Escherichia coli (Ec-NhaA), a prototype of cation–proton antiporter (CPA) family, transports two protons and one sodium (or Li+) in opposite direction. Previous mutagenesis experiments on Ec-NhaA have proposed Asp164, Asp163, and Asp133 amino acids with the significant implication in functional and structural integrity and create site for ion-binding. However, the mechanism and the sites for the binding of the two protons remain unknown and controversial which could be critical for pH regulation. In this study, we have explored the role of Glu78 in the regulation of pH by Ec-NhaA. Although we have created various mutants, E78C has shown a considerable effect on the stoichiometry of NhaA and presented comparable phenotypes. The ITC experiment has shown the binding of ~ 5 protons in response to the transport of one lithium ion. The phenotype analysis on selective medium showed a significant expression compared to WT Ec-NhaA. This represents the importance of Glu78 in transporting the H+ across the membrane where a single mutation with Cys amino acid alters the number of H+ significantly maintaining the activity of the protein. [ABSTRACT FROM AUTHOR]

Lithium and lithium-like elements look like hydrogen atoms if their two electrons and the nucleus are considered as having a core around which a single electron is orbiting. The energy and radii expressions for hydrogen atoms can be used for lithium and lithium-like elements; an important modification is introducing an effective principal quantum number. The effective principal quantum number differs from the principal quantum number of hydrogen by the quantum defect. The quantum defect has respective values for various levels of lithium and lithium-like ions. In this study, we used extended Ritz formulas to calculate quantum defects required to calculate the energies of the ns, np, nd, and nf series up to n < 31. Using these energies, we calculated transition probabilities and then the lifetimes of the lithium levels. The lifetimes were compared with the available published data; an excellent agreement was noticed. The work also extended the available list of lifetimes to higher quantum numbers. Forty lifetimes are newly calculated and presented for the first time. A polynomial formula for each of the ns, np, nd, and nf series lifetimes has been developed that fits well the lifetime values. [ABSTRACT FROM AUTHOR]

The all-solid-state batteries (ASSBs) are of particular interest because of their higher energy density and improved safety. However, the interfacial instability and resulting high interfacial resistance between the cathode and solid electrolyte (SE) have become the major challenges for the practical application of ASSBs. Herein, we report a stable LiFePO4 cathode/γ-Li3PO4 SE interface and systemically investigate the mechanism of Li-ion transport at the interface and the effects of surface nitrogen doping using first-principles calculations. It is found that delithiation at the LiFePO4/γ-Li3PO4 interface initially occurs at the topmost layer of the LiFePO4 cathode side, and hopping through the interface barrier is a rate-limiting step for Li mobility. Nitrogen doping leads to local structural distortion occurred at the interface, affecting the interfacial Li+ diffusion kinetics. Furthermore, the underlying mechanisms in which the different N doping sites alter the Li diffusion barrier are analyzed. We find that, by a rational design, N doping could significantly enhance Li+ diffusion kinetics. Further analysis of the electronic structure of the interface system reveals that the Li3PO4 electrolyte is electrochemically stable against the LiFePO4 cathode in the N-doped interface. Our findings provide a microscopic understanding of the Li+ transport at solid–solid LiFePO4/γ-Li3PO4 interface and suggest that controlling synthesis condition can be critical for enhancing Li+ transport at the N-doped LiFePO4/γ-Li3PO4 interface in an ASSB. [ABSTRACT FROM AUTHOR]

Cellulose nanocrystals (CNCs) are bioderived one-dimensional species with versatile surface chemistry and unique self-assembling behavior in aqueous solutions. This work presents a scientific approach to leverage these characteristics for creating CNC network templates and processing them to engineer a novel silicon (Si)-based material called silicon nano-quill (SiNQ) for energy storage applications. The SiNQ structure possesses a porous, tubular morphology with a substantial ability to store lithium ions while maintaining its structural integrity. The presence of Si suboxides in the SiNQ structure is demonstrated to be crucial for realizing a stable cycling performance. One of the defining attributes of SiNQ is its water dispersibility due to Si–H surface bonds, promoting water-based Si-graphite electrode manufacturing with environmental and economic benefits. The incorporation of only 17 wt% SiNQ enhances the capacity of graphitic anodes by ∼2.5 times. An initial coulombic efficiency of 97.5% is achieved by employing a versatile pre-lithiation. The SiNQ-graphite anodes with high active loading, when subjected to accelerated charging/discharging conditions at 5.4 mA cm−2, exhibit stable cycling stability up to 500 cycles and average coulombic efficiency of >99%. A generalized physics-based cyclic voltammetry model is presented to explain the remarkable behavior of SiNQs under fast-charging conditions. [ABSTRACT FROM AUTHOR]

High abundance 6Li and 7Li are essential materials for the nuclear industry. In this article, the lithium isotope separation effect and lithium-ion transport of a "lithium salt aqueous solution (anolyte)‖crown ethers–ionic liquid organic solution‖ammonium chloride aqueous solution (catholyte)" electromigration system with B12C4, B15C5 and B18C6 as phase transfer catalysts were investigated systematically. The results show that separation factors can reach 1.028 (B12C4), 1.024 (B15C5) and 1.011 (B18C6), respectively, when LiCl solution is used as the anolyte. The separation effect mainly originated from interfaces between anolytes and organic solutions, and was less affected by an electric field. The separation effect between organic solution and catholytes was greatly affected by the electric field for B12C4 and B15C5 systems, which converted from 7Li-enrichment to 6Li-enrichment with increased voltage. For the B18C6 system it was less affected. Furthermore, lithium ion transport in B12C4, B15C5 and B18C6 systems was greatly promoted by the electric field, with the Li+ concentration in catholytes of B12C4, B15C5 and B18C6 systems increased from 0.088 mg L−1, 0.286 mg L−1 and 0.778 mg L−1 to 8.321 mg L−1, 7.422 mg L−1 and 4.631 mg L−1 respectively as the voltage increased from 2 V to 16 V. The B12C4 system has been confirmed as the optimal solution considering both the Li+ transport and isotope separation effect. [ABSTRACT FROM AUTHOR]

Lithium isotopes with high abundances (6Li and 7Li) are crucial for the advancement of nuclear energy. In order to achieve the effective separation of 7Li, a Sudan I-[HMIm][BF4]-anisole extraction system was built employing Sudan I (1-benzeneazo-2-naphthol) as the extractant and hydrophobic ionic liquid [HMIm][BF4] as the co-extractant. By optimizing the organic and aqueous phase components, the extraction rate of the system could reach up to 26.30%, and the single-stage separation factor of the system could reach 1.015 ± 0.001. Meanwhile, the mechanism of the extraction process was investigated, and it was found that the ratio of Sudan I to lithium ions is 1 : 1, and the thermodynamic enthalpy change of the extraction process was less than zero (ΔH < 0), indicating that the extraction process of the system was an exothermic process. The construction of the Sudan-ionic liquid extraction separation system provides a new idea for the study of 7Li enrichment and separation and also provides a possibility for the industrialization of high-abundance 7Li enrichment. [ABSTRACT FROM AUTHOR]

The solid electrolyte Li10GeP2S12 (LGPS) plays a crucial role in the development of all-solid-state batteries and has been widely studied both experimentally and theoretically. The properties of solid electrolytes, such as thermodynamic stability, conductivity, band gap, and more, are closely related to their ground-state structures. However, the presence of site-disordered co-occupancy of Ge/P and defective fractional occupancy of lithium ions results in an exceptionally large number of possible atomic configurations (structures). Currently, the electrostatic energy criterion is widely used to screen favorable candidates and reduce computational costs in first-principles calculations. In this study, we employ the machine learning- and active-learning-based LAsou method, in combination with first-principles calculations, to efficiently predict the most stable configuration of LGPS as reported in the literature. Then, we investigate the diffusion properties of Li ions within the temperature range of 500–900 K using ab initio molecular dynamics. The results demonstrate that the atomic configurations with different skeletons and Li ion distributions significantly affect the Li ions' diffusion. Moreover, the results also suggest that the LAsou method is valuable for refining experimental crystal structures, accelerating theoretical calculations, and facilitating the design of new solid electrolyte materials in the future. [ABSTRACT FROM AUTHOR]

High ionic conductivity, outstanding mechanical stability, and a wide electrochemical window are the keys to the application of solid-state lithium metal batteries (LMBs). Due to their regular channels for ion transport and tailored functional groups, covalent organic frameworks (COFs) have been applied to solid electrolytes to improve their performance. Herein, we report a flexible polyethylene oxide-COF-LZU1 (abbreviated as PEO-COF) electrolyte membrane with a high lithium ion transference number and satisfactory mechanical strength, allowing for dendrite-free and long-time cycling for LMBs. Benefiting from the interaction between bis(triflfluoromethanesulonyl)imide anions (TFSI−) and aldehyde groups in COF-LZU1, the Li+ transference number of the PEO-5% COF-LZU1 electrolyte reached up to 0.43, much higher than that of neat PEO electrolyte (0.18). Orderly channels are conducive to the homogenous Li-+ deposition, thereby inhibiting the lithium dendrites. The assembled LiFePO4|PEO-5% COF-LZU1/Li cells delivered a discharge specific capacity of 146 mAh g−1 and displayed a capacity retention of 80% after 200 cycles at 0.1 C (60 °C). The Li/Li symmetrical cells of the PEO-5% COF-LZU1 electrolyte presented a longer working stability at different current densities compared to that of the PEO electrolyte. Therefore, the enhanced comprehensive performance of the solid electrolyte shows potential application prospects for use in LMBs. [ABSTRACT FROM AUTHOR]

The surging demand for Li rechargeable batteries with high energy densities and rapid rate capability has propelled research on materials that can replace the conventional anode materials like graphite. Vanadium pentoxides (V2O5) have emerged as promising anode candidates owing to their excellent rate capability. Specifically, V2O5 allows the electrochemical prelithiation process, in which three Li-ions can be inserted to form Li3V2O5, followed by reversible insertion and extraction of two Li-ions. Nevertheless, the unsatisfactory Li-ion diffusion coefficients and electrical conductivities of these materials remain major drawbacks. Here, we propose a Zn-doped V2O5 anode, fabricated using a two-step sol–gel method, for high-rate Li-ion batteries. Zn was incorporated into V2O5 to enhance the Li-ion transport kinetics through the electrode. The crystal structure (orthorhombic) of Zn-doped V2O5 was identified by X-ray diffraction analysis, and the Zn doping was confirmed by X-ray photoelectron microscopy. The effect of Zn doping was thoroughly examined using various analytical methods, such as cyclic voltammetry and galvanostatic intermittent titration technique. The Zn-doped V2O5 electrode exhibited remarkable cycling durability, enduring for 1000 cycles, while retaining an enhanced capacity, even under a high rate of 2C. [ABSTRACT FROM AUTHOR]

High-entropy oxides (HEOs), as a new type of single-phase solid solution with a multi-component design, have shown great potential when they are used as anodes in lithium-ion batteries due to four kinds of effects (thermodynamic high-entropy effect, the structural lattice distortion effect, the kinetic slow diffusion effect, and the electrochemical "cocktail effect"), leading to excellent cycling stability. Although the number of articles on the study of HEO materials has increased significantly, the latest research progress in porous HEO materials in the lithium-ion battery field has not been systematically summarized. This review outlines the progress made in recent years in the design, synthesis, and characterization of porous HEOs and focuses on phase transitions during the cycling process, the role of individual elements, and the lithium storage mechanisms disclosed through some advanced characterization techniques. Finally, the future outlook of HEOs in the energy storage field is presented, providing some guidance for researchers to further improve the design of porous HEOs. [ABSTRACT FROM AUTHOR]

The separation of Li+ and [Bmim]+(1-Butyl-3-methylimidazolium) using a cation exchange membrane in an electric field is studied in this work. The effects of the type of cation exchange membrane, current density, total cation concentration, temperature, and anion types on the separation efficiency are investigated. The results indicate that it is feasible to achieve the efficient separation of Li+ and [Bmim]+ using the selectivity of cation exchange membranes under an electric field. The CIMS membrane (a type of cation exchange membrane produced by ASTOM Corporation) shows obvious selectivity of Li+ from [Bmim]+. When the current density is 5 mA/cm2 and the feed concentrations of Li+ and [Bmim]+ are 0.3 mol/L and 0.2 mol/L, respectively, the selective transport coefficient of CIMS can reach 5.9 in the first 120 min of the process. The separation efficiency can be effectively improved by reducing the current density and increasing the total cation concentration. Decreasing the feed temperature can slightly improve the separation efficiency. Changing the type of anion in the feed from chloride to acetate has no detectable effect on the separation. [ABSTRACT FROM AUTHOR]

The creation of periodic domain structures in lithium niobate crystals makes it possible to realize highly efficient nonlinear optical interactions in optical waveguides. The influence of near-surface H+ ion concentration gradient on the domain kinetics in uniform electric field in lithium niobate crystals modified by soft proton exchange is studied. The spatial distribution of the Hþ ions concentration in the surface layer is obtained by confocal Raman microscopy. The observed anomalous evolution of the domain structure at the surface represents the formation of stripe domains and their anisotropic growth along three directions. The domain imaging in the bulk allows revealing a comb-like domain shape. The obtained strong influence of the proton exchange duration on the threshold field is attributed to the action of the concentration gradient in the nearsurface layer, which is considered as an analog of the internal bias electric field. It is shown that the internal bias field is proportional to the increase in the concentration gradient in the surface layer. The mechanism of the comb-like domain formation is proposed. The obtained results can be used for development of domain engineering methods in optical waveguides. [ABSTRACT FROM AUTHOR]

Ciguatera poisoning (CP) is the most common type of marine biotoxin food poisoning worldwide, and it is caused by ciguatoxins (CTXs), thermostable polyether toxins produced by dinoflagellate Gambierdiscus and Fukuyoa spp. It is typically caused by the consumption of large fish high on the food chain that have accumulated CTXs in their flesh. CTXs in trace amounts are found in natural samples, and they mainly induce neurotoxic effects in consumers at concentrations as low as 0.2 µg/kg. The U.S. Food and Drug Administration has established CTX maximum permitted levels of 0.01 µg/kg for CTX1B and 0.1 µg/kg for C-CTX1 based on toxicological data. More than 20 variants of the CTX1B and CTX3C series have been identified, and the simultaneous detection of trace amounts of CTX analogs has recently been required. Previously published works using LC-MS/MS achieved the safety levels by monitoring the sodium adduct ions of CTXs ([M+Na]+ > [M+Na]+). In this study, we optimized a highly sensitive method for the detection of CTXs using the sodium or lithium adducts, [M+Na]+ or [M+Li]+, by adding alkali metals such as Na+ or Li+ to the mobile phase. This work demonstrates that CTXs can be successfully detected at the low concentrations recommended by the FDA with good chromatographic separation using LC-MS/MS. It also reports on the method's new analytical conditions and accuracy using [M+Li]+. [ABSTRACT FROM AUTHOR]

[Display omitted] A recyclable hard-template method is proposed to exploit spindle-shaped hollow nitrogen-doped amorphous carbon (h-NAC) with a large number of short-range curved carbon fragments as anodes for lithium/sodium ion batteries (LIBs/SIBs). Besides providing adsorption sites due to the high existence of oxygen-containing functional groups (CO and COOH), the heavily exposed edge regions also provide a favorable storage environment with high adsorption energy for Li+/Na+ due to their short-range curved structure. Importantly, the etching solution of hard templates can be recycled to generate the FeOOH nanospindles as a precursor through a simple chemical titration, which supplies a new idea for the green preparation of hollow materials. The h-NAC electrode is proven to be bifunctional for storing lithium and sodium ions, displaying favorable rate capability (255 mAh g−1 and 106 mAh g−1 at 5 A g−1 for LIBs and SIBs, respectively). After 1000 cycles at 1 A g−1, the reproducible capacities of the LIBs and SIBs kept 496 mAh g−1 and 181 mAh g−1, respectively. [ABSTRACT FROM AUTHOR]

[Display omitted] Silicon (Si) is considered a promising anode material for lithium-ion batteries (LIBs) due to its high theoretical specific capacity of up to 4200 mAh/g. However, the poor cycling and rate performances of Si induced by the low intrinsic electronic conductivity and large volume expansion during the lithiation/delithiation process limit its practical application. Herein, a novel silicon/bismuth@nitrogen-doped carbon (Si/Bi@NC) composite with nanovoids was synthesized and investigated as an advanced anode material for LIBs. In such a structure, ultrafine bismuth nanoparticles coupled with an N -doped carbon layer were introduced to modify the surface of Si nanoparticles. Subsequently, the lithiated Li x Bi has excellent high ionic conductivity and acts as a fast transport bridge for lithium ions. The introduced carbon coating layer and nanovoids can buffer the volume expansion of Si during the lithiation/delithiation process, thus maintaining structural stability during the cycling process. As a result, the Si/Bi@NC composite exhibits excellent electrochemical performance, providing a relatively high capacity of 955.8 mAh/g at 0.5 A/g after 450 cycles and excellent rate performance with a high capacity of 477.8 mAh/g even at 10.0 A/g. Furthermore, the assembled full cell with LiFePO 4 as cathode and pre-lithium Si/Bi@NC as anode can provide a high capacity of 138.8 mAh/g at 1C after 90 cycles, exhibiting outstanding cycling performance. [ABSTRACT FROM AUTHOR]

Designing Solid-State Electrolytes (SSEs) exhibiting high ionic conductivity and high mechanical/thermal stability is the main concern for developing next-generation rechargeable batteries. Here we present the successful synthesis of colorless, transparent, and bubble-free phosphate glasses with high lithium-ion electrical conductivity within the system xLiCl–(1–x)(63Li2WO4–37P2O5) with 0 ≤ x ≤ 30 mol%. The structural study is performed using Raman spectroscopy. Electrical conductivity measurements of the glasses are investigated over a large frequency range at various temperatures using impedance spectroscopy. It is found that the electric conductivity increases with increasing lithium chloride content. The dc conductivity reaches 2.76 × 10−6 (Ω−1.cm−1) at room temperature (RT) for the glass (x = 30 mol%). The frequency dependence of the conductivity is investigated and the scaling of the conductivity spectra shows that the conduction mechanism in the glasses is both temperature and composition-independent. [ABSTRACT FROM AUTHOR]

Two‐dimensional (2D) layered materials demonstrate prominent advantage in regulating lithium plating/stripping behavior by confining lithium diffusion/plating within interlayer gaps. However, achieving effective interlayer confined lithium diffusion/plating without compromising the stability of bulk‐structural and the solid electrolyte interphase (SEI) remains a considerable challenge. This paper presents an electrochemical scissor and lithium zipper‐driven protocol for realizing interlayer confined lithium plating with pretty‐low strain and volume change. In this protocol, lithium serves as a "zipper" to reunite the adjacent MXene back to MAX‐like phase to markedly enhance the structural stability, and a lithium halide‐rich SEI is formed by electrochemically removing the terminals of halogenated MXenes to maintain the stability and rapid lithium ions diffusion of SEI. When the Ti3C2I2 serves as the host for lithium plating, the average coulomb efficiency exceeds 97.0 % after 320 lithium plating/stripping cycles in conventional ester electrolyte. Furthermore, a full cell comprising of LiNi0.8Mn0.1Co0.1O2 and Ti3C2I2@Li exhibits a capacity retention rate of 73.4 % after 200 cycles even under high cathode mass‐loading (20 mg cm−2) and a low negative/positive capacity ratio of 1.4. Our findings advance the understanding of interlayer confined lithium plating in 2D layered materials and provide a new direction in regulating lithium and other metal plating/stripping behaviors. [ABSTRACT FROM AUTHOR]

Two‐dimensional (2D) layered materials demonstrate prominent advantage in regulating lithium plating/stripping behavior by confining lithium diffusion/plating within interlayer gaps. However, achieving effective interlayer confined lithium diffusion/plating without compromising the stability of bulk‐structural and the solid electrolyte interphase (SEI) remains a considerable challenge. This paper presents an electrochemical scissor and lithium zipper‐driven protocol for realizing interlayer confined lithium plating with pretty‐low strain and volume change. In this protocol, lithium serves as a "zipper" to reunite the adjacent MXene back to MAX‐like phase to markedly enhance the structural stability, and a lithium halide‐rich SEI is formed by electrochemically removing the terminals of halogenated MXenes to maintain the stability and rapid lithium ions diffusion of SEI. When the Ti3C2I2 serves as the host for lithium plating, the average coulomb efficiency exceeds 97.0 % after 320 lithium plating/stripping cycles in conventional ester electrolyte. Furthermore, a full cell comprising of LiNi0.8Mn0.1Co0.1O2 and Ti3C2I2@Li exhibits a capacity retention rate of 73.4 % after 200 cycles even under high cathode mass‐loading (20 mg cm−2) and a low negative/positive capacity ratio of 1.4. Our findings advance the understanding of interlayer confined lithium plating in 2D layered materials and provide a new direction in regulating lithium and other metal plating/stripping behaviors. [ABSTRACT FROM AUTHOR]

The synthetic hydrous layered silicate ilerite was quantitatively converted into microporous nanoscrolls (NS). Delamination of ilerite that was ion‐exchanged for N‐Methyl‐D‐glucaminium (Meg+), through one‐dimensional (1D) dissolution initially yields lamellar liquid crystalline (nematic) suspensions. Subsequent protonation with acetic acid of tangling Si‐O− to silanol groups reduces the pH‐dependent charge of the basal surfaces. Complete NS formation is then triggered by diluting the nematic suspension below 0.05 wt%. As scrolling commonly has been attributed to hydrophobic interaction of organic counterions, Meg+ was replaced by lithium ions but this showed no detrimental effect on the scrolling efficiency. The resulting NS have a typical length of 2–4 μm that corresponds well with typical diameters of the parent nanosheets. Ar‐physisorption isotherms showed a bimodal micropore size with maxima around 0.8 and 1.9 nm. We attribute the first to the tubular hollow inner diameter of the NS and the latter to wedgelike interparticle porosity. The material showed a large specific surface area of 226 m2 g−1. [ABSTRACT FROM AUTHOR]

The interfacial effect is important for anodes of transition metal dichalcogenides (TMDs) to achieve superior lithium-ion storage performance. In this paper, a MoS2/FeS2 heterojunction is synthesized by a simple hydrothermal reaction to construct the interface effect, and the heterostructure introduces an inherent electric field that accelerates the de-embedding process of lithium ions, improves the electron transfer capability, and effectively mitigates volume expansion. XPS analysis confirms evident chemical interaction between MoS2 and FeS2 via an interfacial covalent bond (Mo–S–Fe). This MoS2/FeS2 anode shows a distinct interfacial effect for efficient interatomic electron migration. The electrochemical performance demonstrated that the discharge capacity can reach up to 1217.8 mA h g−1 at 0.1 A g−1 after 200 cycles, with a capacity retention rate of 72.9%. After 2000 cycles, the capacity retention is about 61.6% at 1.0 A g−1, and the discharge capacity can still reach 638.9 mA h g−1. Electrochemical kinetic analysis indicated an enhanced pseudocapacitance contribution and that the MoS2/FeS2 had sufficient adsorption of lithium ions. This paper therefore argues that this interfacial engineering is an effective solution for designing sulfide-based anodes with good electrochemical properties. [ABSTRACT FROM AUTHOR]

The commercialization of ternary layered cathode materials with a relative nickel content of more than 90 % faces serious challenges. Among them, it is urgent to address the issues of rapid capacity degradation and structural degradation. Herein, we provide a simple process for doping yttrium at the precursor preparation stage. The feasibility of yttrium doping in the precursor and the positive effects of yttrium ions on the crystal structure and properties of the cathode materials are scientifically explained by a variety of characterization and testing methods, such as Eh-pH, Particle Size Analyzer, ICP, SEM, EDS, XRD, XPS, HRTEM, dQ/dV, CV, EIS and DFT. Yttrium-doped NCMY cathode materials have more stable lattice oxygen and significantly less irreversible phase transition. Furthermore, the electrochemical performance of the NCMY cathode material is significantly improved, with a capacity retention rate of 82.71 % after 150 cycles at a current density of 1C, which is much higher than 65.39 % for NCM. The NCMY cathode material significantly improves the lithium ion diffusion ability, especially at the high rate of 10C, the discharge specific capacity is still as high as 177.05 mAh g−1. [ABSTRACT FROM AUTHOR]

Fast charging capability is a crucial aspect of next-generation ion battery development, but the ion diffusion rate in existing anode materials is limited. It is necessary to design an anode material with a suitable host structure to effectively promote the ion transport rate. In this study, a novel nickel niobate (Ni 4 Nb 2 O 9) is proposed as an anode material for lithium-ion battery, and a mixed-phase structure consisting of NiNb 2 O 6 and Ni 4 Nb 2 O 9 (M-NNO) is creatively constructed based on component engineering. The phase interfaces within the mix phases prove instrumental in facilitating the transmission of lithium ions and electrons. Notably, Ni-rich Ni 4 Nb 2 O 9 enhances the precipitation of metallic Ni nanoparticles during electrochemical reconstruction, thereby effectively improving the electrical conductivity of the electrode material and enhancing its rate performance. The composite delivers an impressive specific capacity of 216 mAh g−1 at 1C and maintains 98.9 % capacity retention after 1000 cycles at 10C. Moreover, the assembled full-cell with NCM811 as a cathode exhibits 173.1 mAh‍ g−‍1 at current densities of 1C. Therefore, the mixed-phase nickel niobates demonstrate good adaptability and stability in a wide voltage range (0.005–3 V), presenting a new approach for designing high-performance and fast charging lithium battery anodes. The rational construction of Ni-rich amorphous Li x Nb 2 O 5 , achieved through electrochemical reconstruction of mixed-phase NiNb 2 O 6 –Ni 4 Nb 2 O 9 during charge and discharge, effectively refines particle size and enhances material conductivity. Benefiting from these advancements, it presents significantly improved rate performance and cycling stability. [Display omitted] • A mixed-phase material, consisting of NiNb2O6 and Ni4Nb2O9, is prepared based on component engineering. • The electrochemical reconstruction of nickel niobate in a wide voltage range (0.005–3 V) is underscored. • Ni-rich Ni4Nb2O9 promotes the precipitation of metallic Ni nanoparticles during electrochemical reconstruction. • The composite demonstrates an impressive specific capacity and high-rate cycling stability. [ABSTRACT FROM AUTHOR]

The current study of the small lithium molecules Li2+,0,− and Li3+,0,− focuses on the nature of the bonding in these molecules as well as their structures and energetics (bond energies, ionization energies, and electron affinities). Valence CASSCF (2s,2p) calculations incorporate nondynamical electron correlation in the calculations, while the corresponding multireference configuration interaction and coupled cluster calculations incorporate dynamical electron correlation. Treatment of nondynamical correlation is critical for properly describing the Li2,3+,0,− molecules as well as the Li− anion with dynamical correlation, in general, only fine‐tuning the predictions. All lithium molecules and ions are bound, with the Li3+ and Li2+ ions being the most strongly bound, followed by Li3−, Li2, Li2− and Li3. The minimum energy structures of Li3+,0,− are, respectively, an equilateral triangle, an isosceles triangle, and a linear structure. The results of SCGVB calculations are analyzed to obtain insights into the nature of the bonding in these molecules. An important finding of this work is that interstitial orbitals, a concept first put forward by McAdon and Goddard in 1985, play an essential role in the bonding of all lithium molecules considered here except for Li2. The interstitial orbitals found in the Li3+,0 molecules likely give rise to the non‐nuclear attractors/maxima observed in these molecules. [ABSTRACT FROM AUTHOR]