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MXene has been found as a good host for lithium (Li) metal anodes because of its high specific surface area, lithiophilicity, good stability with lithium, and the in situ formed LiF protective layer. However, the formation of Li dendrites and dead Li is inevitable during long‐term cycle due to the lack of protection at the Li/electrolyte interface. Herein, a stable artificial solid electrolyte interface (SEI) is constructed on the MXene surface by using insulating g‐C3N4 layer to regulate homogeneous Li plating/stripping. The 2D/2D MXene/g‐C3N4 composite nanosheets can not only guarantee sufficient lithiophilic sites, but also protect the Li metal from continuous corrosion by electrolytes. Thus, the Ti3C2Tx/g‐C3N4 electrode enables conformal Li deposition, enhanced average Coulombic efficiency (CE) of 98.4%, and longer cycle lifespan over 400 cycles with an areal capacity of 1.0 mAh cm−2 at 0.5 mA cm−2. Full cells paired with LiFePO4 (LFP) cathode also achieve enhanced rate capacity and cycling stability with higher capacity retention of 85.5% after 320 cycles at 0.5C. The advantages of the 2D/2D lithiophilic layer/artificial SEI layer heterostructures provide important insights into the design strategies for high‐performance and stable Li metal batteries. A stable artificial solid electrolyte interface is constructed on the MXene surface by using insulating g‐C3N4 layer to regulate homogeneous Li plating/stripping. The amorphous g‐C3N4 enables highly uniform artificial SEI and MXene provides sufficient lithiophilic sites for Li nucleation. The obtained Ti3C2Tx/g‐C3N4 composite electrode enables conformal Li deposition, enhanced average Coulombic efficiency, and longer cycle lifespan.

HighlightsAn artificial solid–electrolyte interface composed of a perovskite type material, BaTiO3, is introduced to Zn anode surface in aqueous zinc ion batteries.The BaTiO3 layer endowing inherent character of the switched polarization can regulate the interfacial electric field at anode/electrolyte interface.Zn dendrite can be restrained, and Zn metal batteries based on BaTiO3 layer show stable cycling.Aqueous zinc ion batteries show prospects for next-generation renewable energy storage devices. However, the practical applications have been limited by the issues derived from Zn anode. As one of serious problems, Zn dendrite growth caused from the uncontrollable Zn deposition is unfavorable. Herein, with the aim to regulate Zn deposition, an artificial solid–electrolyte interface is subtly engineered with a perovskite type material, BaTiO3, which can be polarized, and its polarization could be switched under the external electric field. Resulting from the aligned dipole in BaTiO3 layer, zinc ions could move in order during cycling process. Regulated Zn migration at the anode/electrolyte interface contributes to the even Zn stripping/plating and confined Zn dendrite growth. As a result, the reversible Zn plating/stripping processes for over 2000 h have been achieved at 1 mA cm−2 with capacity of 1 mAh cm−2. Furthermore, this anode endowing the electric dipoles shows enhanced cycling stability for aqueous Zn-MnO2 batteries. The battery can deliver nearly 100% Coulombic efficiency at 2 A g−1 after 300 cycles.

The finite lithium-ion utilization, short cycling life, and lower capacity retention caused by irreversible dendrite growth become the maximum dilemma in lithium metal batteries’ (LMBs’) commercialization. Herein, a perfluoroalkyl-functionalized covalent organic framework (COF-F6) equipped with high stability and supernal proton conduction is introduced as an artificial solid electrolyte interface to stable the lithium metal anode. Benefiting from the strong electron-withdrawing effect of perfluoroalkyl, Li + will be freed more by the competition of electronegative fluorine (F) and bis(trifluoromethanesulphonyl)imide anion (TFSI − ). The dissociation of LiTFSI and process of Li + desolvation are easier to achieve. In addition, high electronegative fluorine can also regulate local electron-cloud density to induce the fast immigration of Li + . All the above roles contribute to improving the Li + transfer number (0.7) and achieving the goal of inhibiting Li dendrite. As a result, the perfluoroalkyl COF-F6 modified LMB presents outstanding cycling stability. The symmetric batteries accomplish an overlong life-span of more than 5000 h with a lower hysteresis voltage (11 mV) at 5 mA·cm −2 . Also, no dendrites are observed when using an in-situ optical microscope to learn the process of Li deposition. Therefore, this dendrite-free protection tactic holds broad prospects for the practical application of Li metal anodes.

3D bimetallic carbon nanofibers (CNFs) are promising interlayers for regulating Na deposition/dissolution on the Na metal or directly on current collectors like Cu. However, uncontrollable solid electrolyte interface (SEI) growth on the interlayer during the repeated Na plating/stripping process leads to low initial Coulombic efficiency (CE), impeding the practical applications of such a protective layer in Na metal batteries. Herein, an artificial SEI‐coated interlayer decorated with sodiophilic Ag and sodiophobic Cu on CNF is applied on Cu foil to regulate the Na deposition/dissolution behavior. The artificial SEI, consisting of organic components like RCO2Na/RCONa and inorganic reactants Na2CO3/NaxOy, minimizes irreversible electrolyte decomposition at the interlayer. The sodiophobic–sodiophilic bimetallic CNF interlayer is lightweight, porous, and mechanically robust. It can guide Na deposition toward the sodiophilic Ag‐rich region of the CNF matrix and cluster in the open pores facing the current collector, effectively preventing Na dendrite formation. The interlayer features with artificial SEI synergistically enhance the stability of Na deposition/dissolution on Cu foil, resulting in a high average CE of over 99.5% for 600 cycles spanning 6500 h. Furthermore, post‐analysis confirms the high electrochemical stability of the artificial SEI of the interlayer during cycling. The combination of three‐dimensional bimetallic carbon fibers with an artificial SEI created through chemical presodiation enables a stable and homogeneous sodium deposition/dissolution process.

Lithium–sulfur batteries (LSBs) that utilize sulfur and lithium (Li) metal as electrode materials are highly attractive for transportation applications due to their high theoretical gravimetric energy density. However, two major challenges currently impede the commercialization of LSB, which are the formation of Li dendrites and polysulfide shuttling. To mitigate these two effects, a protective film or artificial solid–electrolyte interface (SEI) can be applied directly to the Li‐metal surface. Herein, the preparation of freestanding polyethylene oxide (PEO)‐based films using tape casting as a scalable coating technique is presented. Moreover, the films are applied directly to the Li surface via a solvent‐free method. To demonstrate the suitability of the developed PEO‐based films, the long‐term cycling performance of the lithium–sulfur cells is discussed. It is shown that the cells with the Li‐metal surface protected by PEO‐based films achieve better stability and reproducibility, reaching ≈400 mA h g S−1 after 250 cycles compared to ≈200 mA h g S−1 after 250 cycles for the bare Li‐metal electrode. An extensive postmortem analysis of the Li‐metal electrode surface with scanning electron microscopy is additionally shown, revealing that the PEO‐based artificial SEIs form uniformly with a low level of defect layers at the interface with the Li‐metal electrode, which indicates the creation of a stable SEI. Within this research, a polymer‐based freestanding thin film is developed using a highly scalable technique. The as‐prepared films are coated onto lithium‐metal and serve as a protective artificial solid–electrolyte interface (SEI), diminishing the formation of lithium dendrites and the parasitic reaction of lithium with surrounding components. Battery cycling of lithium–sulfur coin cells using this artificial SEI shows increased performance and reproducibility.

Lithium (Li) is considered the most promising anode material for Li metal batteries (LMBs) because of its extraordinarily high theoretical capacity and the lowest electrochemical potential among all potential anode materials. Despite their advantages, Li metal anodes (LMAs) still have several critical shortcomings (such as high reactivity and considerable volume expansion), which result in dendritic Li growth and fatal damage to the natural solid electrolyte interphase (SEI) of LMAs. These issues raise safety concerns and cause poor cycling stability of LMAs owing to their continuous parasitic reactions, which hinder their practical use in LMBs. Herein, by employing dynamic chemical reactions for Li-antimony (Sb) self-alloying and tetrahydrofuran-induced ion-conducting SEI fabrication, an artificial composite SEI is proposed to build a stable and dendrite-free LMA. The smooth and dense surface architecture of the electron-insulating and ion-conductive SEI in the LMA (Li@SbCl 3 -20) not only promotes uniform Li-ion flux and current density but also prevents the direct Li-electrolyte contact, which results in a uniform and dense Li plating morphology underneath the SEI without side reactions. Moreover, symmetric Li@SbCl 3 -20||Li@SbCl 3 -20 cells demonstrate stable cyclability (over 400 h) and rate capability at metabolic current densities. When paired with LiNi 0.6 Co 0.2 Mn 0.2 or LiFePO 4 , the Li@SbCl 3 -20 full-cells achieved long-term cycling stability and rate performance.

HighlightsThe formation mechanism of solid electrolyte interface (SEI) is analyzed based on charge distributions at the electrode/electrolyte interface and molecular orbital theory.The factors affecting the formation of SEI are generalized from four aspects: Zn anode, electrolyte, current density and temperature.The design strategies for SEI layer are proposed from regulating temperature, electric and magnetic fields.Due to its high theoretical capacity (820 mAh g−1), low standard electrode potential (− 0.76 V vs. SHE), excellent stability in aqueous solutions, low cost, environmental friendliness and intrinsically high safety, zinc (Zn)-based batteries have attracted much attention in developing new energy storage devices. In Zn battery system, the battery performance is significantly affected by the solid electrolyte interface (SEI), which is controlled by electrode and electrolyte, and attracts dendrite growth, electrochemical stability window range, metallic Zn anode corrosion and passivation, and electrolyte mutations. Therefore, the design of SEI is decisive for the overall performance of Zn battery systems. This paper summarizes the formation mechanism, the types and characteristics, and the characterization techniques associated with SEI. Meanwhile, we analyze the influence of SEI on battery performance, and put forward the design strategies of SEI. Finally, the future research of SEI in Zn battery system is prospected to seize the nature of SEI, improve the battery performance and promote the large-scale application.

Traditionally, the discovery of new materials has often depended on scholars’ computational and experimental experience. The traditional trial-and-error methods require many resources and computing time. Due to new materials’ properties becoming more complex, it is difficult to predict and identify new materials only by general knowledge and experience. Material prediction tools based on machine learning (ML) have been successfully applied to various materials fields; they are beneficial for modeling and accelerating the prediction process for materials that cannot be accurately predicted. However, the obstacles of disciplinary span led to many scholars in materials not having complete knowledge of data-driven materials science methods. This paper provides an overview of the general process of ML applied to materials prediction and uses solid-state electrolytes (SSE) as an example. Recent approaches and specific applications to ML in the materials field and the requirements for building ML models for predicting lithium SSE are reviewed. Finally, some current obstacles to applying ML in materials prediction and prospects are described with the expectation that more materials scholars will be aware of the application of ML in materials prediction.

Aqueous zinc-ion batteries (AZIBs) have become a promising and cost-effective alternative to lithium-ion batteries due to their low cost, high energy, and high safety. However, dendrite growth, hydrogen evolution reactions (HERs), and corrosion significantly restrict the performance and scalability of AZIBs. We propose the introduction of a BaTiO3 (BTO) piezoelectric polarized coating as an interface modification strategy for ZIBs. The low surface energy of the BTO (110) crystal plane ensures its thermodynamic preference during crystal growth in experimental processes and exhibits very low reactivity toward oxidation and corrosion. Calculations of interlayer coupling mechanisms reveal a stable junction between BTO (110) and Zn (002), ensuring system stability. Furthermore, the BTO (110) coating also effectively inhibits HERs. Diffusion kinetics studies of Zn ions demonstrate that BTO effectively suppresses the dendrite growth of Zn due to its piezoelectric effect, ensuring uniform zinc deposition. Our work proposes the introduction of a piezoelectric material coating into AZIBs for interface modification, which provides an important theoretical perspective for the mechanism of inhibiting dendrite growth and side reactions in AZIBs.

Lithium (Li) metal has emerged as one of the most promising electrode materials with great potential to fulfill the demands of high-energy-density batteries. The solid electrolyte interphase (SEI) on the Li metal anode plays a critical role in electrochemical processes and undergoes large deformation. SEI failure could promote the growth of Li dendrites, leading to performance degradation and security hazards in Li metal batteries. The native SEI exhibits poor mechanical properties, which can be attributed to the presence of heterogeneous interfaces between various components. In this work, we construct the heterogeneous interface by two SEI inorganic components of LiF and Li2O. Using density functional theory calculations, we investigate the mechanical properties of the LiF/Li2O interface system and explore the diffusion mechanisms of Li ions through the strained LiF/Li2O interface. The results indicate that the heterogeneous interface system has relatively low Young's modulus and tensile strength. In addition, tensile strain increases the energy barriers of interface diffusion, thereby reducing the rate of electrochemical reactions. This study could contribute to the analysis of SEI failure, providing theoretical understanding for Li interface diffusion in the SEI.