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Lithium fluoride (LiF) is a ubiquitous component in the solid electrolyte interphase (SEI) layer in Li-ion batteries. However, its nanoscale structure, morphology, and topology, important factors for understanding LiF and SEI film functionality, including electrode passivity, are often unknown due to limitations in spatial resolution of common characterization techniques. Ultrabroadband near-field synchrotron infrared nanospectroscopy (SINS) enables such detection and mapping of LiF in SEI layers in the far-infrared region down to ca. 322 cm-1 with a nanoscale spatial resolution of ca. 20 nm. The surface sensitivity of SINS and the large infrared absorption cross section of LiF, which can support local surface phonons under certain circumstances, enabled characterization of model LiF samples of varying structure, thickness, surface roughness, and degree of crystallinity, as confirmed by atomic force microscopy, attenuated total reflectance FTIR, SINS, X-ray photoelectron spectroscopy, high-angle annular dark-field, and scanning transmission electron microscopy. Enabled by this approach, LiF within SEI films formed on Cu, Si, and metallic glass Si40Al50Fe10 electrodes was detected and characterized. The nanoscale morphologies and topologies of LiF in these SEI layers were evaluated to gain insights into LiF nucleation, growth, and the resulting nuances in the electrode surface passivity.

Reversibility of metallic Zn anode serves as the corner stone for the development of aqueous Zn metal battery, which motivates scrutinizing the electrolyte‐Zn interface. As the representative organic zinc salt, zinc trifluorosulfonate (Zn(OTf)2) facilitates a broad class of aqueous electrolytes, however, the stability issue of Zn anode remains crucial. The great challenge lies in the lack of Zn anode protection by the pristinely formed surface structure in aqueous Zn(OTf)2 electrolytes. Accordingly, an electrochemical route was developed to grow a uniform zinc trifluorosulfonate hydroxide (ZTH) layer on Zn anode as an artificial SEI, via regulation on metal dissolution and strong coordination ability of zinc ions. Co‐precipitation was proposed to be the formation mechanism for the artificial SEI, where the reduction stability of OTf− anion and the low‐symmetry layer structure of ZTH was unmasked. This artificial SEI favors interfacial kinetics, depresses side reactions, and well maintains its integrity during cycling, leading to a prolonged lifespan of Zn stripping/plating with a high DOD of ~85 %, and an improved cycling stability of ~92 % retention rate for V2O5/Zn cell at 1 A g−1. The unveiled role of anion on Zn anode drives the contemplation on the surface chemistry for the blooming aqueous rechargeable battery. [ABSTRACT FROM AUTHOR]

The SEI is a crucial yet little understood component of lithium‐ion batteries. The specific formation processes creating the SEI are still a matter of current research. In our paper, we analyse the electrochemical processes by incremental capacity analysis (ICA) and correlate these results with the evolved gas species and subsequent performance of the cells. 101 cells in total divided in three groups with different electrolytes performed a formation cycle. Afterwards gas‐samples of half of the cells were extracted for analysis. We found a good correlation between variations of gas composition and noticeable ICA‐data. Furthermore we explore correlations between formation and initial cell performance after a total of 10 cycles. Our results open new possibilities for a better understanding of formation processes. [ABSTRACT FROM AUTHOR]

An artificial solid electrolyte interphase (SEI) with lithiophilic sites and chemical bonds anchoring lithium polysulfides (LiPSs) has been developed as a potential solution to protect the lithium (Li) metal anode of Lithium--sulfur (Li--S) batteries. This strategy aims to guide consistent Li deposition and relieve lithium corrosion. Herein, the evolution process of lithiophilic sites based on aluminum fluoride (AlF3) in an artificial SEI is disclosed in Li--S batteries with metal--based lithiophilic sites. The polyester polymer (PMMA and PPC)/AlF3 artificial SEI (MPAF--SEI) was homogeneously anchored on Li anode by in--situ polymerization. The conversion of AlF3 into Li--Al and LiF lithiophilic sites effectively reduce the Li nucleation overpotential and prevents the formation of Li dendrites. At the same time, the polymer can anchor LiPSs by chemical bonds and prevents Li corrosion. The optimized MPAF--SEI protected Li demonstrates excellent stability for over 3000 h at a capacity of 1 mAh cm-2 in Li jj Li symmetric cells. The Li--S battery with low N/P (4) exhibits a capacity of 532.6 mAh g-1 over 300 cycles lifespan at 0.5 C. [ABSTRACT FROM AUTHOR]

The poor lithium ion conductivity of solid electrolyte interface (SEI) layer limits the improvement of cycling performance of lithium metal batteries. Here, we pre-designed a Li2S/Li2S2 inorganic layer to participate into the formation of SEI through a simple one-step melting sulfur strategy. Its high ionic conductivity promotes the rapid and uniform transmission of lithium ion, and effectively inhibits the side reaction and the growth of lithium dendrites. Benefiting from these advantages, Li/Li symmetrical batteries using artificial SEI with Li2S/Li2S2 show small polarization voltages (25–40 mV), and can run for nearly 1500 h, which is 2 times than that of bare lithium. Moreover, the application of Li/LiFePO4 battery can be extended to 235 cycles with a high capacity retention of 90% under high load of 21.6 mg cm−2 and lean electrolyte of 2 µL mg−1. [ABSTRACT FROM AUTHOR]

An artificial solid electrolyte interphase (SEI) with lithiophilic sites and chemical bonds anchoring lithium polysulfides (LiPSs) has been developed as a potential solution to protect the lithium (Li) metal anode of Lithium−sulfur (Li–S) batteries. This strategy aims to guide consistent Li deposition and relieve lithium corrosion. Herein, the evolution process of lithiophilic sites based on aluminum fluoride (AlF3) in an artificial SEI is disclosed in Li–S batteries with metal−based lithiophilic sites. The polyester polymer (PMMA and PPC)/AlF3 artificial SEI (MPAF−SEI) was homogeneously anchored on Li anode by in−situ polymerization. The conversion of AlF3 into Li–Al and LiF lithiophilic sites effectively reduce the Li nucleation overpotential and prevents the formation of Li dendrites. At the same time, the polymer can anchor LiPSs by chemical bonds and prevents Li corrosion. The optimized MPAF−SEI protected Li demonstrates excellent stability for over 3000 h at a capacity of 1 mAh cm−2 in Li || Li symmetric cells. The Li–S battery with low N/P (4) exhibits a capacity of 532.6 mAh g −1 over 300 cycles lifespan at 0.5 C.

[Display omitted] • 1. An interfacial layer composed of nano-Si particles and cationic polymer (Si@PDDA) was constructed. • 2. PDDA provides an electrostatic shielding layer to achieve homogeneous electric field distribution and suppress the formation of Li dendrites. • 3. Uniformly dispersed nano-Si particles reduce the nucleation overpotential of Li+ and promote the stable deposition of Li metal. • 4. PDDA adsorbs electrolyte anions while transporting Li+, significantly accelerating the decomposition of inorganic salts to form SEI rich in Li 3 N. • 5. The electrode with Si@PDDA exhibits relatively high electrochemical performances. Lithium (Li) metal is a promising anode material for future high-energy rechargeable batteries due to its remarkable properties. Nevertheless, excess Li in traditional lithium metal anodes (LMAs) reduces the energy density of batteries and increases safety risks. Electrochemical pre-lithiation is an effective technique for regulating the lithium content of the anodes. However, Cu foil or other non-Li based substrates used for pre-lithiation often have inhomogeneous surfaces and high nucleation barrier, leading to uneven tip deposition of lithium metal and fragile SEI. Herein, we have designed an interfacial layer composed of nano-Si particles and cationic polymer (poly (diallyldimethylammonium chloride)) (denoted as Si@PDDA) to induce the formation of Li 3 N-rich inorganic SEI and regulate the homogeneous plating/stripping of lithium. The uniformly dispersed nano-Si particles can decrease the Li+ nucleation overpotential through alloying reaction with lithium. The surface of Si nano-particles modified by PDDA contains numerous cationic sites, providing an electrostatic shielding layer to seeding the growth of Li metal and inhibiting dendrites formation. More promisingly, PDDA adsorbs electrolyte anions while transporting Li+, significantly accelerating the decomposition kinetics of inorganic salts within the electrolyte. Therefore, a SEI film rich in Li 3 N was formed on the anodes, ensuring the excellent interfacial stability and electrochemical cycling performance of LMAs. The symmetrical cells exhibit a cycle life of 900 h at 1 mA cm−2. Moreover, the practical full cells operate at a low negative/positive (N/P) capacity ratio (∼3) for over 160 cycles. [ABSTRACT FROM AUTHOR]

In this paper, we propose a novel use of four distance‐based methods for constructing composite indicators: namely, the maximizing deviations method, the weighted least‐square (WLD) deviation from the mean method, the WLD deviation from the ideal method, and the WLD dissimilarity method. The main advantages of these methods are that they have analytical solutions. Thus, there is no need to solve the underlying programming problem for each application. They also result in common (but not necessarily equal) weights that allow complete comparison and ranking. We explore the potential of the suggested weighting method by using it to re‐estimate the Sustainable Energy Index and the Sustainable Development Goal 7 composite indicator. [ABSTRACT FROM AUTHOR]

In view of the problem of rapid estimation of capacity attenuation after multiple charge and discharge cycles of LIB(lithium-ion battery), a new method based on the capacity attenuation model of lithium-ion battery is proposed to rapidly estimate its internal capacity attenuation using the external expansion displacement of the battery. Based on the capacity attenuation model of LIB, the radial irreversible expansion model is derived, and the cylindrical LIB Sanyo UR18650E is modeled and solved by COMSOL Multiphysics, and the numerical results are compared with the experimental data, so as to verify the proposed model. Based on the above model, the causes of capacity attenuation and irreversible expansion of battery due to side reactions during the charge-discharge cycle are analyzed. The results show that the change of side reaction rate causes the gradient distribution of the concentration of side reaction products in the negative electrode, and the accumulation of side reaction products causes the expansion displacement of the battery to increase linearly with the cycle. The function formula of the cell capacity attenuation and its radial displacement is obtained by using the side reaction product as a bridge, which provides a new method for the rapid estimation of the capacity attenuation. [ABSTRACT FROM AUTHOR]

Compared to traditional lithium metal batteries, anode-free lithium metal batteries use bare current collectors as an anode instead of Li metal, making them highly promising for mass production and achieving high-energy density. The current collector, as the sole component of the anode, is crucial in lithium deposition-stripping behavior and greatly impacts the rate of Li depletion from the cathode. In this study, to investigate the lithiophilicity effect of the current collector on the solid electrolyte interface (SEI) film construction and cycling performance of anode-free lithium batteries, various lightweight paper-based current collectors were prepared by electroless plating Cu and lipophilic Ag on low-dust paper (LDP). The areal densities of the as-prepared LDP@Cu, LDP@Cu-Ag, and LDP@Ag were approximately 0.33 mg cm−2. The use of lipophilic Ag-coated collectors with varying loadings allowed for the regulation of lipophilicity. The impacts of these collectors on the distribution of SEI components and Li depletion rate in common electrolytes were investigated. The findings suggest that higher loadings of lipophilic materials, such as Ag, on the current collector increase its lipophilicity but also lead to significant Li depletion during the cycling process in full-cell anode-free Li metal batteries. Thus, moderately lithiophilic current collectors, such as LDP@Cu-Ag, show more potential for Li deposition and striping and stable SEI with a low speed of Li depletion. [ABSTRACT FROM AUTHOR]

Controlling the structure and chemistry of solid electrolyte interphase (SEI) underpins the stability of electrolyte‐electrode interface, and is crucial for advancing rechargeable lithium metal batteries (LMBs). Here, we utilized photo‐controlled copolymerization to achieve the on‐demand synthesis of fluorosulfonyl fluoropolymers as unprecedented artificial SEI layers on Li metal anodes. This work not only enables instant formation of a hybrid polymer‐inorganic interphase that consists of a polymer‐enriched top layer and a LiF‐fortified bottom layer, originating from a single polymeric component, but also imparts various desirable physical properties (e.g. good mechanical strength and flexibility, high ion conductivity, low overpotential) to SEI via a single‐to‐divergent strategy. Model reactions and structural characterizations supported the formation of a divergent fluorinated interphase, which furnished prolonged stabilization of Li deposition, high coulombic efficiency and improved cycling behavior in electrochemical experiments. This work highlights the great potential of exploring reactive polymers as versatile coatings to stabilize Li metal anodes, providing a promising avenue to solve electrode‐electrolyte interfacial problems for LMBs. [ABSTRACT FROM AUTHOR]

A novel approach for investigating the formation of solid electrolyte interphase (SEI) in Na‐ion batteries (NIB) through the coupling of in situ liquid electrochemical transmission electron microscopy (ec‐TEM) and gas‐chromatography mass‐spectrometry (GC/MS) is proposed. To optimize this coupling, experiments are conducted on the sodiation of hard carbon materials (HC) using two setups: in situ ec‐TEM holder and ex situ setup. Electrolyte (NP30) is intentionally degraded using cyclic voltammetry (CV), and the recovered liquid product is analyzed using GC/MS. Solid product (µ‐chip) is analyzed using TEM techniques in a post‐mortem analysis. The ex situ experiments served as a reference to for insertion of Na+ ions in the HC, SEI size (389 nm), SEI composition (P, Na, F, and O), and Na plating. The in situ TEM analysis reveals a cyclability limitation, this issue appears to be caused by the plating of Na in the form of a “foam” structure, resulting from the gas release during the reaction of Na with DMC/EC electrolyte. The foam structure, subsequently transformes into a second SEI, is electrochemically inactive and reduces the cyclability of the battery. Overall, the results demonstrate the powerful synergy achieved by coupling in situ ec‐TEM and GC/MS techniques. [ABSTRACT FROM AUTHOR]

Li metal batteries with polymer electrolyte are of great interest for next-generation batteries for high safety and high energy density. However, uneven deposition on the lithium metal surface can greatly affect battery life. Therefore, surface modification on the Li metal become necessary to achieve good performance. Herein, an artificial solid electrolyte interface (SEI) modified lithium metal anode is prepared using cation-polymerization process, as triggered by PF5 generated from CsPF6. As a result, the polarization voltage of Li||Li symmetric battery assembled with artificial SEI-modified Li metal anode was stable with a small over-potential of 25 mV after 3000 h at current density of 1.5 mA cm−2. Electrochemical performance of Li||NCM 622 (LiNi0.6Co0.2Mn0.2O2) full cell with soft-matter polymer electrolyte is significantly improved than bare Li-metal, the capacity retention is 75% after 120 cycles with N/P = 3:1 at a cut-off voltage of 4.3 V. Our work has shed lights on the commercialization of Li metal battery with polymer electrolyte. [ABSTRACT FROM AUTHOR]

The solid electrolyte interphase (SEI) is a thin heterogeneous layer formed at the anode/electrolyte interface in lithium‐ion batteries as a consequence of the reduction of the electrolyte. The initial formation of the SEI inhibits the direct contact between the electrode and the electrolyte and thus protects the battery. However, the composition, structure, and size of the SEI evolve over time and the growth of the SEI is considered the primary mechanism leading to the gradual deterioration of the battery performance. Despite the importance of the SEI and its growth, the atomistic understanding of the underlying elementary reaction steps remains partial. Molecular modeling of the electrolyte decomposition is key to gain detailed insights that are complementary to experiments for the reactions occurring in this heterogenous interphase. In this perspective, the electron transport mechanisms are first described from the anode to the electrolyte through the SEI and highlight the importance of the inorganic/organic interface within the heterogeneous SEI: it is where the electrolyte decomposition reactions are likely to occur. Finally, a view is provided on the current progress on molecular modeling techniques (e.g., Density Functional Theory, force fields, machine learning potentials) of the SEI and the challenges each method faces. [ABSTRACT FROM AUTHOR]

Sn4P3 has been recognized as a promising candidate for an anode material for lithium-ion batteries (LIBs) because of its appropriate operating potential and high theoretical capacity. Unfortunately, the rapid fading of capacity induced by volume change, low electrical conductivity, and limited lithium-ion charging speed hindered the actual application of Sn4P3. Building physical barriers of carbon-based material on the surface of Sn4P3 particles is a common way to handle the above issues. In our work, Sn4P3 particles were confined in an ordered mesoporous carbon framework (CMK-3) via a low-pressure vapor method. CMK-3 can not only improve the electric conductivity but also buffer the volume effect by using its mesopore channels to provide accommodation for the huge volume expansion of Sn4P3 particles. In addition, Sn4P3 nanoparticles were synthesized in CMK-3 frameworks via a low-pressure vapor method to obtain the Sn4P3/CMK-3 nanocomposite. The nanosize effect can shorten electron transfer distance, leading to faster reaction kinetics to improve electrochemical performance. The Sn4P3/CMK-3 was further grafted by a thin layer of poly-(3,4-ethylenedioxythiophene) (PEDOT) to prevent the continuing buildup of poorly conducting species and thus optimize the solid electrolyte interface, which has been evidenced by in-depth X-ray photoelectron spectroscopy via Ar cluster etching. As a result of the dual-confining strategy, Sn4P3/CMK-3@PEDOT showed relatively high rate performance (reversible capacity of 438 mAh g–1 at 2.0 A g–1) and stable cycling performance (923 mAh g–1 at 0.5 A g–1 over 740 cycles). [ABSTRACT FROM AUTHOR]

We examine the impact of water (160 ± 41 ppm of reference) on the anode, cathode, separator and electrolyte in two aging scenarios: calendric aging (60 °C, 80 days, charged state), resulting in a triggered current interrupt device (CID), and cycling 1680 times (charge/discharge with 1C, 2.75–4.2 V, 20 ± 2 °C), resulting in 24.5% residual capacity. We applied computer tomography (CT), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS) and secondary ion mass spectrometry (SIMS) to understand the capacity loss. The aged NMC/LCO–graphite cells were compared to a reference cell in pristine state. Both aging scenarios showed (a) thick depositions on the anode and cathode consisting mainly of oxygen, fluorine and phosphorous, (b) reduced separator pore sizes, (c) the deposition of Mn, Co and Ni on top of the anode and (d) the decomposition of the conductive salt LiPF6 accompanied by HF formation and a loss of active lithium. Calendric aging consumes the water content and additionally leads to (e) the decomposition of the organic solvent followed by CO2 gas formation. Cyclic aging increases the water content and additionally results in (f) the consumption of the additive fluoroethylene carbonate (FEC). These findings show how water affects aging phenomena and results in a capacity decrease in the cell.

Si anodes for Li-ion batteries are notorious for their large volume expansion during lithiation and the corresponding detrimental effects on cycle life. However, calendar life is the primary roadblock for widespread adoption. During calendar life aging, the main origin of impedance increase and capacity fade is attributed to the instability of the solid electrolyte interphase (SEI). In this work, we use ex situ nano-Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy to characterize the structure and composition of the SEI layer on amorphous Si thin films after an accelerated calendar aging protocol. The characterization of the SEI on non-washed and washed electrodes shows that brief washing in dimethyl carbonate results in large changes to the film chemistry and topography. Detailed examination of the non-washed electrodes during the first lithiation and after an accelerated calendar aging protocol reveals that PF6- and its decomposition products tend to accumulate in the SEI due to the preferential transport of PF6- ions through polyethylene oxide-like species in the organic part of the SEI layer. This work demonstrates the importance of evaluating the SEI layer in its intrinsic, undisturbed form and new strategies to improve the passivation of the SEI layer are proposed.

The emphasis in the automotive industry towards sustainable mobility has led to a significant interest in hybrid-electric drive-trains with high energy density batteries. Addressing the needs of this strategy, the battery market is exploring new technologies to improve the safety and lifespan of electric vehicles. To this end, there is a focus on the all-solid-state battery (ASSB) technology for its cycle capabilities. Filling the current void in the literature pertaining to accurate ageing models for ASSBs, in the present work, we propose an enhanced version of the numerical ageing model, originally developed for liquid electrolyte based batteries, to forecast the development of the solid electrolyte interface layer that is the major cause of battery capacity fading. The model has been tested on prototype batteries and reveals an accuracy of 99%. The capacity fade in ASSBs has been investigated under different conditions and the enhanced ageing model has been validated using experimental data from these batteries. The findings suggest that there is potential for solid-state batteries to be commercialized, although significant work is needed to match the manufacturing level of lithium-ion batteries embedded with liquid electrolytes. [ABSTRACT FROM AUTHOR]

Rechargeable aqueous zinc–metal batteries (AZBs) are a promising complimentary technology to the existing lithium‐ion batteries and the re‐emerging lithium–metal batteries to satisfy the increasing demands on energy storage. Despite considerable progress achieved in the past years, the fundamental understanding of the solid‐electrolyte interphase (SEI) formation and how its composition influences the SEI properties are limited. This review highlights the functionalities of anion‐tuned SEI on the reversibility of zinc–metal anode, with a specific emphasis on new structural insights obtained through advanced characterizations and computational techniques. Recent efforts in terms of key variables that govern the interfacial behaviors to improve the long‐term stability of zinc anode, i.e., Coulombic efficiency, plating morphology, dendrite formation, and side‐reactions, are comprehensively reviewed. Lastly, the remaining challenges and future perspectives are presented, providing insights into the rational design of practical high‐performance AZBs. [ABSTRACT FROM AUTHOR]

We examine the impact of water (160 ± 41 ppm of reference) on the anode, cathode, separator and electrolyte in two aging scenarios: calendric aging (60 °C, 80 days, charged state), resulting in a triggered current interrupt device (CID), and cycling 1680 times (charge/discharge with 1C, 2.75–4.2 V, 20 ± 2 °C), resulting in 24.5% residual capacity. We applied computer tomography (CT), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS) and secondary ion mass spectrometry (SIMS) to understand the capacity loss. The aged NMC/LCO–graphite cells were compared to a reference cell in pristine state. Both aging scenarios showed (a) thick depositions on the anode and cathode consisting mainly of oxygen, fluorine and phosphorous, (b) reduced separator pore sizes, (c) the deposition of Mn, Co and Ni on top of the anode and (d) the decomposition of the conductive salt LiPF6 accompanied by HF formation and a loss of active lithium. Calendric aging consumes the water content and additionally leads to (e) the decomposition of the organic solvent followed by CO2 gas formation. Cyclic aging increases the water content and additionally results in (f) the consumption of the additive fluoroethylene carbonate (FEC). These findings show how water affects aging phenomena and results in a capacity decrease in the cell. [ABSTRACT FROM AUTHOR]

The anode/electrolyte interface behavior, and by extension, the overall cell performance of sodium‐ion batteries is determined by a complex interaction of processes that occur at all components of the electrochemical cell across a wide range of size‐ and timescales. Single‐scale studies may provide incomplete insights, as they cannot capture the full picture of this complex and intertwined behavior. Broad, multiscale studies are essential to elucidate these processes. Within this perspectives article, several analytical and theoretical techniques are introduced, and described how they can be combined to provide a more complete and comprehensive understanding of sodium‐ion battery (SIB) performance throughout its lifetime, with a special focus on the interfaces of hard carbon anodes. These methods target various length‐ and time scales, ranging from micro to nano, from cell level to atomistic structures, and account for a broad spectrum of physical and (electro)chemical characteristics. Specifically, how mass spectrometric, microscopic, spectroscopic, electrochemical, thermodynamic, and physical methods can be employed to obtain the various types of information required to understand battery behavior will be explored. Ways are then discussed how these methods can be coupled together in order to elucidate the multiscale phenomena at the anode interface and develop a holistic understanding of their relationship to overall sodium‐ion battery function. [ABSTRACT FROM AUTHOR]

[Display omitted] Thermal runaway is a hazardous risk, occurring more readily in high-energy–density lithium-ion batteries (LIBs), which leads to a rapid temperature rise and even combustion or explosion when using flammable electrolyte systems. Flame retardants (FRs), such as trimethyl phosphate (TMPa) and triethyl phosphate (TEP), are commonly utilized due to their effective flame suppression, low toxicity, and excellent thermal stability. However, the lack of in-depth understanding of the flame retardancy mechanism and solid electrolyte interphase (SEI) formation process has made the development of functional electrolytes difficult at present. In this study, we clarified the flame retardancy and interfacial reaction mechanisms of low-flammable TMPa localized high-concentration electrolytes (LHCE) using hybrid ab initio and reactive force field (HAIR) schemes. Long-term HAIR simulation reveals that phosphorous radicals produced by the decomposition of TMPa capture carbon radicals, encouraging their polymerization into low-flammable oligomers, while fluorine-containing solvents in the electrolyte capture hydrogen radicals and produce nonflammable hydrofluoric acid (HF). This synergistic flame retardancy mechanism provides essential atomic-level insights for the rational design of high-safety electrolytes in the future. [ABSTRACT FROM AUTHOR]

Fast charging is a critical factor for the widespread adoption of electric vehicles (EVs), yet it poses challenges to the durability of lithium-ion batteries (LiBs). This study develops an aging model for a 10 Ah LiB cell using COMSOL Multiphysics, integrating a one-dimensional electrochemical model with a zero-dimensional thermal model. The model is constructed using cell design and electrochemical parameters derived from existing literature, tailored to the specific electrode and electrolyte materials utilized in this study. Key aging phenomena, such as the Solid Electrolyte Interface (SEI) growth and lithium plating, are embedded within the model to simulate the aging patterns and the interplay between these factors across various C-rates and temperatures. Simulation results suggest that while higher charging rates can reduce charging time, they also lead to increased degradation, with lithium plating becoming more severe at these elevated rates. The model also indicates that temperature management during cell operation can influence cycle life, with strategic temperature increases potentially mitigating some negative effects of fast charging. The study also explores the concept of total charging time as an alternative metric for battery wear, examining its relationship with the charging current profile and temperature. Results indicate that while fast charging offers convenience, it significantly impacts cycle life, underscoring the need for optimized charging strategies. The insights from this work enhance the understanding of Li-ion cell aging mechanisms, shedding light on the complex trade-offs between charging speed, temperature management, and lifespan. This contributes to the development of more sophisticated battery management systems and charging protocols that aim to extend the operational life of LiBs while accommodating the demands of fast charging.

Lithium dendrites pose a major hurdle for enhancing the energy density of lithium metal batteries, and the artificial solid electrolyte interface layer offers a potential solution. In this work, a cost‐effective and environmentally friendly guar gum film is applied to the artificial protective layer. The guar gum artificial solid electrolyte interface (SEI) layer formed naturally, enriched with OH and AOA groups, displayed exceptional electrochemical stability, and achieved an impressively high transference number of 0.88 for lithium‐ion movement. In symmetric cells, the Li@GG‐Cu anode displays remarkable cycling performance even during extended periods. This is evidenced by its ability to maintain a surface capacity of approximately 850 h (1 mA cm−2, 1 mAh cm−2). In addition, when utilizing a complete cell setup comprising a LiFPO4 cathode (weighing 1.5 mg cm−2) and anode coated with a guar gum film, the capacity retention of an impressive 96.2% showcases outstanding preservation of battery performance over time even after 700 cycles. This performance surpasses that of a lithium foil electrode (87.1%) and a copper anode with lithium deposition (0%). Our work exhibits a promising material for a novel configuration of artificial SEI, effectively stabilizing lithium metal anode. [ABSTRACT FROM AUTHOR]

Electrolytes play a crucial role in facilitating the ionic movement between cathode and anode, which is essential for the flow of electric current during the charging and discharging process of the rechargeable batteries. In particular, electrolyte additives are considered as effective and economical approaches into the advancements of the battery technologies in both the conventional non‐aqueous and burgeoning aqueous electrolyte systems. Herein, a systematic and comprehensive review of the electrolyte additives is reported for the interfacial engineering of Li and Zn metal anodes in the non‐aqueous and aqueous electrolytes, respectively. The types of electrolyte additives and their corresponding functionalities for the protection of these two metal anodes are discussed along with the electrochemical features of solid electrolyte interphase (SEI) derived from electrolyte additives. The recent progress on electrolyte additives for these two battery systems are also addressed from the perspectives of electrode, electrolyte, and the associated SEI. Finally, the outlook and perspective on the current issues and future directions in the field of electrolyte additive engineering are presented for next‐generation battery technologies beyond the conventional Li‐ion batteries. [ABSTRACT FROM AUTHOR]

The mechanically and electrochemically stable and ionically conducting solid electrolyte interphase (SEI) is important for the stabilization of metal anodes. Since SEIs are originally absent in aqueous zinc metal batteries (AZMBs), it is very challenging to suppress water‐induced side reactions and dendrite growth of Zn metal anodes (ZMAs). Herein, a gradient‐structured and robust solid gradient SEI, consisting of B,O‐inner and F,O‐exterior layer, in situ formed by hydrated eutectic electrolyte for the homogeneous and reversible Zn deposition, is demonstrated. Moreover, the molar ratio of acetamide to Zn salt is modulated to prohibit the water activity and the hydrolysis of BF4− as well as to achieve high ionic conductivity owing to the regulation of the solvation sheath of Zn2+. Consequently, the eutectic electrolyte allows Zn||Zn symmetric cells to achieve a cycling lifespan of over 4400 h at 0.5 mA cm−2 as well as Zn||PANI full cells to deliver a high capacity retention of 73.2% over 4000 cycles at 1 A g−1 and to demonstrate the stable operation at low temperatures. This work provides the rational design for the hydrated eutectic electrolyte and the corresponding gradient SEIs for dendrite‐free and stable Zn anodes even under harsh conditions. [ABSTRACT FROM AUTHOR]

Lithium salt LiHDI (lithium 4,5-dicyano-2-(n-heptafluoropropyl)imidazolide) is proposed as a solid electrolyte interphase-stabilising additive for lithium-ion batteries, which can be added in a smaller amount than fluoroethylene carbonate (FEC) and vinylene carbonate (VC) additives. Electrolytes containing either lithium 4,5-dicyano-2-(trifluoromethyl)imidazolide (LiTDI) or battery-standard LiPF6 were tested with various amounts of LiHDI additive. Chemical stability in the presence of water and the thermal stability of LiHDI are on par with LiTDI. LiHDI additive does not negatively affect the properties of electrolytes. Conductivity measurements of solutions, galvanostatic cycling of graphite-LiFePO4 cells at room temperature, cells' cycling at 60 °C, internal cell resistance monitoring during cycling, and XPS analysis of electrodes' surfaces after cycling have been performed. LiHDI, unlike the FEC-VC mixture, does not negatively affect the properties of the electrolyte. Cycling showed improved capacity retention with LiHDI additive with both graphite and LiFePO4 as capacity-limiting electrodes over samples without additives. At elevated temperatures, samples with LiHDI exhibited better capacity retention during cycling than those with FEC-VC. Internal cell resistance can be correlated with capacity retention. XPS results show changes in the composition of SEI depending on the composition of the electrolyte and the duration of cycling. [ABSTRACT FROM AUTHOR]

Maintaining the physical integrity of a silicon-based anode, which suffers from damage caused by severe volume changes during cycling, is a top priority in its practical applications. The performance of silicon-flake-based anodes has been significantly improved by mixing nanodiamond powders with silicon flakes for the fabrication of anodes for lithium-ion batteries (LIBs). Nanodiamonds adhere to the surfaces of silicon flakes and are distributed in the binder between flakes. A consistent and robust solid electrolyte interphase (SEI) is promoted by the aid of abundant reactive surface-linked functional groups and exposed dangling bonds of nanodiamonds, leading to enhanced physical integrity of the silicon flakes and the anode. The battery's high-rate discharge capabilities and cycle life are thus improved. SEM, Raman spectroscopy, and XRD were applied to examine the structure and morphology of the anode. Electrochemical performance was evaluated to demonstrate a capacity retention of nearly 75% after 200 cycles, with the final specific capacity exceeding 1000 mAh/g at a test current of 4 mA/cm2. This is attributed to the improved stability of the solid electrolyte interphase (SEI) structure that was achieved by integrating nanodiamonds with silicon flakes in the anode, leading to enhanced cycling stability and rapid charge-discharge performance. The results from this study present an effective strategy of achieving high-cycling-performance by adding nanodiamonds to silicon-flake-based anodes. [ABSTRACT FROM AUTHOR]

Compared to traditional lithium metal batteries, anode-free lithium metal batteries use bare current collectors as an anode instead of Li metal, making them highly promising for mass production and achieving high-energy density. The current collector, as the sole component of the anode, is crucial in lithium deposition-stripping behavior and greatly impacts the rate of Li depletion from the cathode. In this study, to investigate the lithiophilicity effect of the current collector on the solid electrolyte interface (SEI) film construction and cycling performance of anode-free lithium batteries, various lightweight paper-based current collectors were prepared by electroless plating Cu and lipophilic Ag on low-dust paper (LDP). The areal densities of the as-prepared LDP@Cu, LDP@Cu-Ag, and LDP@Ag were approximately 0.33 mg cm−2. The use of lipophilic Ag-coated collectors with varying loadings allowed for the regulation of lipophilicity. The impacts of these collectors on the distribution of SEI components and Li depletion rate in common electrolytes were investigated. The findings suggest that higher loadings of lipophilic materials, such as Ag, on the current collector increase its lipophilicity but also lead to significant Li depletion during the cycling process in full-cell anode-free Li metal batteries. Thus, moderately lithiophilic current collectors, such as LDP@Cu-Ag, show more potential for Li deposition and striping and stable SEI with a low speed of Li depletion.

It remains a challenge to design aqueous electrolytes to secure the complete reversibility of zinc metal anodes. The concentrated water‐in‐salt electrolytes, e.g., 30 m ZnCl2, are promising candidates to address the challenges of the Zn metal anode. However, the pure 30 m ZnCl2 electrolyte fails to deliver a smooth surface morphology and a practically relevant Coulombic efficiency. Herein, it is reported that a small concentration of vanillin, 5 mg mLwater−1, added to 30 m ZnCl2 transforms the reversibility of Zn metal anode by eliminating dendrites, lowering the Hammett acidity, and forming an effective solid electrolyte interphase. The presence of vanillin in the electrolyte enables the Zn metal anode to exhibit a high Coulombic efficiency of 99.34% at a low current density of 0.2 mA cm−2, at which the impacts of the hydrogen evolution reaction are allowed to play out. Using this new electrolyte, a full cell Zn metal battery with an anode/cathode capacity (N/P) ratio of 2:1 demonstrates no capacity fading over 800 cycles. [ABSTRACT FROM AUTHOR]

The lithium (Li) dendrite growth seriously hinders the applications of lithium metal batteries (LMBs). Numerous methods have been proposed to restrict the formation of Li dendrites by improving the Li‐ion transference number (tLi+) through separator modification according to Sand's time equation. However, ignoring the positive contribution of anion motion to solid electrolyte interphase (SEI) formation will result in insufficient inorganic components, which impedes practical implementation of LMBs. Herein, a "tandem" separator is constructed (ZSM‐5‐Poly dimethyl diallyl ammonium chloride (PDDA)/Polyethylene (PE)/SbF3), which anchored anions and built an inorganic‐rich SEI at the same time. The resulting SEI from SbF3 (SBF) coating on side facing Li is rich in Li‐Sb alloy (Li3Sb) and LiF. Li3Sb can significantly reduce the migration energy barrier of Li ion (Li+) and facilitate Li+ transport. Simultaneously, ZSM‐5‐PDDA (Z5P) coating at the other side can effectively immobilize anions and increase the tLi+. Moreover, the regular pore structure is conducive to homogenizing Li+ flux and also capable to uniform temperature distribution, significantly improving safety. Hence, the lifespan of Li|Li and Li|Cu cells assemble with Z5P/PE/SBF separator is significantly extended. In addition, full cells with LiNi0.8Co0.1Mn0.1O2 (NCM811) and LiFePO4 (LFP) cathodes show excellent cycle stability and superior rate performance. [ABSTRACT FROM AUTHOR]

The emphasis in the automotive industry towards sustainable mobility has led to a significant interest in hybrid-electric drive-trains with high energy density batteries. Addressing the needs of this strategy, the battery market is exploring new technologies to improve the safety and lifespan of electric vehicles. To this end, there is a focus on the all-solid-state battery (ASSB) technology for its cycle capabilities. Filling the current void in the literature pertaining to accurate ageing models for ASSBs, in the present work, we propose an enhanced version of the numerical ageing model, originally developed for liquid electrolyte based batteries, to forecast the development of the solid electrolyte interface layer that is the major cause of battery capacity fading. The model has been tested on prototype batteries and reveals an accuracy of 99%. The capacity fade in ASSBs has been investigated under different conditions and the enhanced ageing model has been validated using experimental data from these batteries. The findings suggest that there is potential for solid-state batteries to be commercialized, although significant work is needed to match the manufacturing level of lithium-ion batteries embedded with liquid electrolytes.

The combination of Li-metal anode and high-voltage cathode is regarded as a solution for the next-generation high-energy-density secondary batteries. However, a traditional electrolyte is either incompatible with the Li-metal anode or vulnerable to high voltage. This work reports a 1 M dual-salts Localized-High-Concentration-Electrolyte with Fluoroethylene carbonate (FEC) additive. It enables stable cycling of Li||LiNi0.8Co0.1Mn0.1O2 (NMC811) battery, which shows 81.5% capacity retention after 300 cycles with a charge/discharge current density of 1 C and a voltage range of 2.7–4.4 V. Scanning electron microscopy (SEM) images show that this electrolyte not only largely reduced Li dendrites and 'dead' Li on anode surface but also well protected the microstructure of NMC811 cathode. Possible components of both solid-electrolyte interlayer (SEI) and cathode-electrolyte interlayer (CEI) were characterized by energy-dispersive X-ray spectroscopy (EDX). The result illustrates that FEC protected Li salts from decomposition on the anode side and suppressed the decomposition of solvents on the cathode side. [ABSTRACT FROM AUTHOR]

Student engagement is a pivotal contributor to academic achievement, retention, and well-being, and yet the role of teacher influence on engagement is poorly understood. This is in part due to the contextual and 'hidden' nature of student engagement, and as such, levels of student engagement are assumed through observable factors such as attendance and conduct. It is also due to the difficulty in mapping student engagement simultaneously with understanding the teacher practices used to influence it. This article reports on a pre-post case study in which student survey and teacher focus group data were analysed together, revealing the nature and depth of association between the practices adopted by teachers and student engagement. By comparing the change of engagement at a class or homegroup level, it was possible to identify how approaches used by teachers impacted various elements of engagement. Furthermore, it found a high correlation between teacher practices and change in student engagement at a class or homegroup level, providing the opportunity for teachers to learn what practices were effective in their specific context. [ABSTRACT FROM AUTHOR]

The possibility of analyzing the electrochemical impedance spectra of lithium–lithium cells using the Distribution of Relaxation Times (DRT) function is studied. A comparative analysis of the electrochemical impedance spectra of lithium–lithium cells obtained during long-term storage at a constant temperature and at different temperatures was performed using the method of either equivalent electrical circuits or the DRT function. The analysis of the impedance of lithium–lithium cells by the DRT function is shown to allow estimating the number of layers in the surface film on the lithium electrodes and evaluating their physical parameters—the resistance and capacitance. It has been established that with a long exposure of lithium–lithium cells at the temperature of 30°C, the number of layers in the surface film and its resistance decreased. With the increase in the temperature, the physical properties of the layers of the surface film are differentiated and its total resistance decreased. The analysis of the electrochemical impedance spectra of lithium–lithium cells by the DRT functions is more informative than the method of equivalent electrical circuits. [ABSTRACT FROM AUTHOR]

The formation of a stable SEI with a hierarchical structure of functionalization is the key to improving the anode performance of secondary batteries. The effects of piperidine cation containing isobutyl as an additive in the SEI structure of hard carbon (HC) and corresponding Na+ transport functionality were comprehensively investigated. It is revealed that the large cationic groups of piperidine can promote the rapid migration of Na+ desolvation on the surface of HC anode, further promote the decomposition of anions, and induce the formation of a double‐layer SEI structure. As a result, the as‐fabricated batteries achieved high cyclic stability, good reversible specific capacity, and improved rate performance. The mixed electrolyte showed good reversible capacity and capacity retention rate (800 cycles @5 C, 67.31%), which was significantly better than the initial electrolyte with a capacity retention rate of 42.01% for 500 cycles @5 C. In particular, it is also observed some graphitized structural features on the surface of HC, which facilitate the migration of Na+. Meanwhile, the hierarchical structure of functionalization SEI in conjunction with "pseudo‐SEI" contributed to the improved performance of Na+ storage. This work provides the feasibility for the introduction of large cationic group additives in the electrolyte to enhance the cycle stability of the HC anode. [ABSTRACT FROM AUTHOR]

Specific emitter identification (SEI) is a powerful technique that identifies different emitters utilizing the features generated from hardware imperfections. The features, also known as radio frequency fingerprints (RFFs), can be extracted via model-based methods or data-based methods. In this paper, we analyze the identification accuracy of SEI system and provide criteria for evaluating different SEI schemes. We use in-phase/quadrature (I/Q) imbalance as an example to examine the identification performance by analyzing the Euclidean distance between radio frequency (RF) signals of different emitters. This derivation can also be generalized to different modulation schemes and distortion models.

The main objective of this present study is to prepare flood susceptibility mapping using bivariate approaches considering parameters such as rainfall, geomorphology, geology, soil, elevation, ground slope, curvature of the land, flow directions, stream density, distance from road, distance from river, land use land cover, topographic wetness index, normalized differentiate vegetation index and water index. Bivariate methods like Shannon's Entropy Index (SEI) and Weight of Evidence (WofE-IV) models have been used in conjunction with remote sensing and geographical information system and it was found that 17.77% (SEI) and 11.20% (WofE-IV) area of the district categorized as highly susceptible to flood especially found in the adjoining area of Tangon, Punarbhaba, and Atreyee rivers. Around 26–35% of the total area is safe from flood especially located in the Tapan and Banshihari block. The area under curve values (SEI = 0.954, WofE-IV = 0.913) shows that both models are performing well for flood susceptibility mapping.

The quest for high-performance lithium-ion batteries (LIBs) is at the forefront of energy storage research, necessitating a profound understanding of intricate processes like phase transformations and thermal runaway events. This review paper explores the pivotal role of X-ray spectroscopies in unraveling the mysteries embedded within LIBs, focusing on the utilization of advanced techniques for comprehensive insights. This explores recent advancements in in situ characterization tools, prominently featuring X-ray diffraction (XRD), X-ray tomography (XRT), and transmission X-ray microscopy (TXM). Each technique contributes to a comprehensive understanding of structure, morphology, chemistry, and kinetics in LIBs, offering a selective analysis that optimizes battery electrodes and enhances overall performance. The investigation commences by highlighting the indispensability of tracking phase transformations. Existing challenges in traditional methods, like X-ray absorption spectroscopy (XAS), become evident when faced with nanoscale inhomogeneities during the delithiation process. Recognizing this limitation, the review emphasizes the significance of advanced techniques featuring nanoscale resolution. These tools offer unprecedented insights into material structures and surface chemistry during LIB operation, empowering researchers to address the challenges posed by thermal runaway. Such insights prove critical in unraveling interfacial transport mechanisms and phase transformations, providing a roadmap for the development of safe and high-performance energy storage systems. The integration of X-ray spectroscopies not only enhances our understanding of fundamental processes within LIBs but also propels the development of safer, more efficient, and reliable energy storage solutions. In spite of those benefits, X-ray spectroscopies have some limitations in regard to studying LIBs, as referred to in this review.

Lithium salt LiHDI (lithium 4,5-dicyano-2-(n-heptafluoropropyl)imidazolide) is proposed as a solid electrolyte interphase-stabilising additive for lithium-ion batteries, which can be added in a smaller amount than fluoroethylene carbonate (FEC) and vinylene carbonate (VC) additives. Electrolytes containing either lithium 4,5-dicyano-2-(trifluoromethyl)imidazolide (LiTDI) or battery-standard LiPF6 were tested with various amounts of LiHDI additive. Chemical stability in the presence of water and the thermal stability of LiHDI are on par with LiTDI. LiHDI additive does not negatively affect the properties of electrolytes. Conductivity measurements of solutions, galvanostatic cycling of graphite-LiFePO4 cells at room temperature, cells’ cycling at 60 °C, internal cell resistance monitoring during cycling, and XPS analysis of electrodes’ surfaces after cycling have been performed. LiHDI, unlike the FEC-VC mixture, does not negatively affect the properties of the electrolyte. Cycling showed improved capacity retention with LiHDI additive with both graphite and LiFePO4 as capacity-limiting electrodes over samples without additives. At elevated temperatures, samples with LiHDI exhibited better capacity retention during cycling than those with FEC-VC. Internal cell resistance can be correlated with capacity retention. XPS results show changes in the composition of SEI depending on the composition of the electrolyte and the duration of cycling.

Lithium-ion battery heat generation characteristics during aging are crucial for the creation of thermal management solutions. The heat generation characteristics of 21700 (NCA) cylindrical lithium-ion batteries during aging were investigated using the mathematical model that was created in this study to couple electrochemical mechanisms, heat transfer, and aging loss. These findings indicate that, at the same operating current, the heat generation power of the cell increased significantly with battery aging. This increase was primarily due to the energy loss caused by the growth of the solid–electrolyte interface (SEI) and a reduction in the negative porosity and other physical characteristics of the SEI, such as its ionic conductivity and molar volume, which also had an impact on the heat generation power. By investigating the variations in battery heat generation in different aging modes, the electrochemical mechanisms underlying the effects of aging on battery heat generation can be comprehended in depth. [ABSTRACT FROM AUTHOR]

Electrolyte engineering is crucial for the commercialization of lithium metal batteries. Here, lithium metal is stabilized in the highly reactive sulfolane‐based electrolyte under low concentration (0.25 M) for the first time. Inorganic‐polymer hybrid solid electrolyte interphase (SEI) with high ionic conductivity, low bonding with lithium and high flexibility enables dense chunky lithium deposition and high plating/stripping efficiency. Low concentration electrolyte (LCE) also enables excellent cycling stability of LiNi0.5Co0.2Mn0.3O2 (NCM523)/Li cells at 1 C (90.7 % retention after 500 cycles) and 0.3 C (83.3 % retention after 1000 cycles). With a low N/P ratio (≈2), the capacity retention for NCM523/Li cells can achieve 94.3 % after 100 cycles at 0.3 C. Exploring the LCE is of paramount significance because it provides more possibilities of the lithium salt selections, especially reviving some lithium salts that are excluded before due to their low solubility. More importantly, LCE has the significant advantage of commercialization due to its cost‐effectiveness. [ABSTRACT FROM AUTHOR]

Severe lithium (Li) dendrite growth caused by the uneven overpotential deposition is a formidable challenge for high energy density Li metal batteries (LMBs). Herein, we investigate a synergetic interfacial kinetic to regulate Li deposition behavior and stabilize Li metal anode. Through constructing Li alloying matrix with a bi‐functional silver (Ag)‐Li3N blended interface, fast Li+ conductivity and high Li affinity can be achieved simultaneously, resulting in both decreased Li nucleation and mass transfer‐controlled overpotentials. Beyond these properties, a more important feature is demonstrated herein; that is, the inward diffusion depth of the Li adatoms inside of the Ag site can be restricted by the Li+ solvation structure in a highly coordinating environment. The latter feature can ensure the durability of the operational Ag sites, thereby elongating the Li protection ability of the Ag‐Li3N interface greatly. This work provides a deep insight into the synergetic effect of functional alloying structure and Li+ solvation mediated interfacial kinetic on Li metal protection. [ABSTRACT FROM AUTHOR]

A SnO 2 -QDs/PDA hollow nanosphere assembled by ultrafine SnO 2 quantum dots (SnO 2 -QDs) and nitrogen-doped carbon, containing residual polydopamine (PDA) core was prepared by PDA-assisted hydrothermal methods. PDA polymer acted as a steric hindrance and sacrificed template during the hydrothermal reaction of metal salts to achieve the formation of ultra-small metal oxide particles and hollow spheres. The strong interaction between the ultra-small SnO 2 -QDs and N -doping carbon layer in the hollow structure could effectively accommodate the volume expansion and maintain structural stability. Furthermore, the residual PDA core inside the hollow sphere further captures the oxygen free radicals in the rechargeable batteries and influences the composition of the SEI layer and interface dynamics which enhances the reversibility of the conversion reaction. This synergistic strategy makes SnO 2 -QDs/PDA hollow nanosphere obtain a high reversible capacity (∼1200 mAh g−1) and long cycle stability (>3000 cycles). Thus, the SnO 2 -QDs/PDA||LiFePO 4 full cell at 0.3 A g−1 exhibits excellent cycle stability with a good retention rate after 200 cycles. This study provides a new basis for the improvement of the lithium storage performance of metal oxide anode. [Display omitted] • Steric-hindrance effect and self-sacrificing template behavior induced PDA@SnO 2 -QDs/NC hollow nanospheres is designed. • The role of PDA core in the formation of the SEI layer on PDA@SnO 2 -QDs/NC hollow nanospheres is discussed. • Strong interaction between SnO 2 -QDs and the carbon outerwear derived from PDA accommodate the bulk expansion of electrode. • Li-ion half/full cells show superior rate performance and durable cyclic stability. Tin-based anode materials with high theoretical specific capacity are subject to huge volume expansion and poor reaction reversibility, leading to degradation of battery performance. Herein, the steric-hindrance effect and self-sacrificing template behavior of polydopamine were firstly developed to induce the formation of hollow nanospheres assembled by ultrafine SnO 2 quantum dots (SnO 2 -QDs) and nitrogen-doped carbon (NC), containing residual polydopamine (PDA) cores. The PDA@SnO 2 -QDs/NC hollow nanospheres could effectively accommodate the volume expansion and maintain structural stability. More importantly, the PDA core could capture oxygen free radicals produced by the charge/discharge process and be involved in the evolution of the SEI layer, achieving enhanced electrochemical reaction kinetics. The optimized PDA@SnO 2 -QDs/NC anode shows a specific capacity of 898 mAh g−1 after 300 cycles at 0.3 A g−1, and scarcely capacity attenuation after 1500 cycles at 1 A g−1. The long-cyclic life is up to 3000 cycles at 3 A g−1. Even after 200 cycles, the anode in the PDA@SnO 2 -QDs/NC||LFP full battery gives a reversible capacity of 489 mAh g−1 at 0.3 A g−1, with a capacity retention of 77 %. This work casts new light on tin-based anode materials and interface optimization. [ABSTRACT FROM AUTHOR]

[Display omitted] • The chemical presodiation approach is firstly extended to improve the ICE of red P-based (P/C@S) anode, and a desirable ICE of 98.7% is achieved. • A thin, uniform, and NaF-rich SEI film is formed on the surface of pNa-P/C@S anode. • All the pNa-P/C@S//Na 3 V 2 (PO4) 2 F 3 , pNa-P/C@S//Na 3 V 2 (PO 4) 3 , and pNa-P/C@S//NaCu 0.12 Ni 0.23 Fe 0.33 Mn 0.33 full cells deliver high ICEs (>98%), high energy densities, and outstanding cycling performance. • This presodiation method has been extended to SnO 2 anode, evidencing its universal applicability. Red phosphorus/carbon (P/C) materials have been extensively studied as promising anodes for sodium-ion batteries (SIBs) owing to their high capacities and moderate working potentials. However, the low initial Coulombic efficiency (ICE) and unstable solid-electrolyte interphase (SEI) of P/C composites limit their widespread applications. In this study, we develop an effective presodiation method to compensate for the irreversible sodium loss of the S-doped P/C (P/C@S) anode and yield a thin, uniform, and NaF-rich SEI layer on the presodiated P/C@S (pNa-P/C@S) anode during cycling. Consequently, the pNa-P/C@S anode exhibits a remarkable ICE of 98.7% as well as superior cycling performance and rate capability in the half cell. When pNa-P/C@S anode is coupled with conventional Na 3 V 2 (PO 4) 2 F 3 , Na 3 V 2 (PO 4) 3 , and NaCu 0.12 Ni 0.23 Fe 0.33 Mn 0.33 cathodes, all the full cells demonstrate desirable ICEs (>98%), high energy densities, and excellent cycling performance. The proposed method has been extended to another anode (SnO 2) to demonstrate its applicability in fabricating anodes with a high ICE and stable NaF-rich SEI layer. [ABSTRACT FROM AUTHOR]