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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.

The formation of lithium dendrites induces the notorious safety issue and poor cycling life of energy storage devices, such as lithium–sulfur and lithium–air batteries. We propose a surface energy model to describe the complex interface between the lithium anode and electrolyte. A universal strategy of hindering formation of lithium dendrites via tuning surface energy of the relevant thin film growth is suggested. The merit of the novel motif lies not only fundamentally a perfect correlation between electrochemistry and thin film fields, but also significantly promotes larger‐scale application of lithium–sulfur and lithium–air batteries, as well as other metal batteries (e.g., Zn, Na, K, Cu, Ag, and Sn). A perfect marriage between electrochemistry and thin film fields! The formation of lithium dendrites induces the safety issue and poor cycling life of energy storage devices, such as lithium–sulfur batteries and lithium–air batteries. A surface energy model is proposed to describe the interface between the lithium anode and electrolyte. A universal strategy is suggested for hindering formation of lithium dendrites via tuning surface energy of the relevant thin film growth.

Aqueous zinc (Zn) ion batteries (AZIBs) are regarded as one of the promising candidates for next‐generation electrochemical energy storage systems due to their low cost, high safety, and environmental friendliness. However, the commercialization of AZIBs has been severely restricted by the growth of dendrite at the Zn metal anode. Tailoring the planar‐structured Zn anodes into three‐dimensional (3D) structures has proven to be an effective way to modulate the plating/stripping behavior of Zn anodes, resulting in the suppression of dendrite formation. This review provides an up‐to‐date review of 3D structured Zn metal anodes, including working principles, design, current status, and future prospects. We aim to give the readers a comprehensive understanding of 3D‐structured Zn anodes and their effective usage to enhance AZIB performance. This review systematically discusses the progress of advanced 3D structural Zn anodes, including preparation methods, surface composition modifications, gradient structure designs, and side reaction inhibitions. The article also concludes by outlining the existing challenges and prospects for further developing high‐performance 3D structural Zn anodes.

With its high theoretical capacity, lithium (Li) metal is recognized as the most potential anode for realizing a high‐performance energy storage system. A series of questions (severe safety hazard, low Coulombic efficiency, short lifetime, etc.) induced by uncontrollable dendrites growth, unstable solid electrolyte interface layer, and large volume change, make practical application of Li‐metal anodes still a threshold. Due to their highly appealing properties, carbon‐based materials as hosts to composite with Li metal have been passionately investigated for improving the performance of Li‐metal batteries. This review displays an overview of the critical role of carbon‐based hosts for improving the comprehensive performance of Li‐metal anodes. Based on correlated mainstream models, the main failure mechanism of Li‐metal anodes is introduced. The advantages and strategies of carbon‐based hosts to address the corresponding challenges are generalized. The unique function, existing limitation, and recent research progress of key carbon‐based host materials for Li‐metal anodes are reviewed. Finally, a conclusion and an outlook for future research of carbon‐based hosts are presented. This review is dedicated to summarizing the advances of carbon‐based materials hosts in recent years and providing a reference for the further development of carbon‐based hosts for advanced Li‐metal anodes. Graphical Carbon‐based hosts are of great significance for the future development of high‐performance Li‐metal anodes. This review summarizes the recent developments of carbon‐based hosts for Li‐metal accommodation. The carbon‐based hosts with high surface area and conductivity can suppress dendrites growth, relieve volume expansion, and stabilize interface, and further doping and compositing to the hosts can effectively regulate Li plating/stripping behaviors.

Li metal batteries offer the ultimate choice of high‐energy power source, but suffer the performance decay and safety risk originated from notorious dendrite problem and infinite volume change of Li metal anode. Herein, it is reported to strengthen the Li metal anode by ultralight but highly robust MXene aerogels (ULRMA) with build‐in strain‐resistant and molecular‐level lithiophilic properties. A hydrogen‐bonding crosslinking strategy is developed for rapidly assembling 2D MXene to ULRMA at ambient conditions with less sacrifice of intrinsic properties of MXene. The ULRMA with an ultralow density below 10 mg cm−3 are favorable to maximize the merit of Li metal in gravimetric energy density while offering exceptional stability of porous frameworks against mechanical strain of long‐term Li plating/stripping. The lithiophilic architecture with high conductivity and hierarchical porosity further largely reduces the potential polarization and guides the pattern of Li deposition. Uptaking Li metal into ULRMA leads to a stable Li metal anode with an ultralong lifetime of 1600 h with a high‐rate response up to 20 mA cm−2 and high coulombic efficiency. It yields a highly robust Li metal anode with high effectiveness in engineering stable Li‐ion and Li–S batteries even paring with commercial LiFePO4 or sulfur cathode without nanostructuring. A facile hydrogen‐bonding crosslinking strategy is developed for fast fabrication of ultralight but highly robust MXene aerogels (ULRMA). They allow for maximizing the gravimetric energy merit of Li metal while effectively strengthening Li metal anode. Uptaking Li metal into robust lithiophilic ULRMA yields stable Li metal anode for significantly enhancing the performance of Li‐ion and Li–S full cells.

Commercialization of Zn‐metal anodes with low cost and high theoretical capacity is hindered by the poor reversibility caused by dendrites growth, side reactions, and the slow Zn2+‐transport and reaction kinetics. Herein, a reversible heterogeneous electrode of Zn‐nanocrystallites/polyvinyl‐phosphonic acrylamide (Zn/PPAm) with fast electrochemical kinetics is designed for the first time: phosphonic acid groups with strong polarity and chelation effect ensure structural reversibility and stability of the three‐dimensional Zn‐storage‐host PPAm network and the Zn/PPAm hybrid; hydrophobic carbon chains suppress side reactions such as hydrogen evolution and corrosion; weak electron‐donating amide groups constitute Zn2+‐transport channels and promote “desolvation” and “solvation” effects of Zn2+ by dragging the PPAm network on the Zn‐metal surface to compress/stretch during Zn plating/stripping, respectively; and the heterostructure and Zn nanocrystallites suppress dendrite growth and enhance electrochemical reactivity, respectively. Thus, the Zn/PPAm electrode shows cycle reversibility of over 6000 h with a hysteresis voltage as low as 31 mV in symmetrical cells and excellent durability and flexibility in fiber‐shaped batteries. A reversible Zn nanocrystallites/polyvinyl‐phosphonic acrylamide (Zn/PPAm) heterozygote electrode with fast kinetics is designed. The heterostructure Zn/PPAm electrode comprising Zn nanocrystallites with the PPAm polymer suppresses dendrite growth and enhances the electrochemical activity of the Zn anode. Meanwhile, the carbon chains of the polymer can suppress side reactions and amide groups have Zn2+‐transport channels to promote the “desolvation” and “solvation” effects of Zn ions during the charging/discharging process.

Metal anodes promise improvements in energy density and cost; however, their performance is determined within the first several nanometers at the interface. This review reports on how polymer-based artificial solid electrolyte interphases (SEIs) are engineered to stabilize Li and aqueous-Zn anodes, and how these designs are now evaluated against operando readouts rather than post-mortem snapshots. We group the related molecular strategies into three classes: (i) side-chain/ionomer chemistry (salt-philic, fluorinated, zwitterionic) to increase cation selectivity and manage local solvation; (ii) dynamic or covalently cross-linked networks to absorb microcracks and maintain coverage during plating/stripping; and (iii) polymer–ceramic hybrids that balance modulus, wetting, and ionic transport characteristics. We then benchmark these choices against metal-specific constraints—high reductive potential and inactive Li accumulation for Li, and pH, water activity, corrosion, and hydrogen evolution reaction (HER) for Zn—showing why a universal preparation method is unlikely. A central element is a system of design parameters and operando metrics that links material parameters to readouts collected under bias, including the nucleation overpotential (ηnuc), interfacial impedance (charge transfer resistance (Rct)/SEI resistance (RSEI)), morphology/roughness statistics from liquid-cell or cryogenic electron microscopy (Cryo-EM), stack swelling, and (for Li) inactive-Li inventory. By contrast, planar plating/stripping and HER suppression are primary success metrics for Zn. Finally, we outline parameters affecting these systems, including the use of lean electrolytes, the N/P ratio, high areal capacity/current density, and pouch-cell pressure uniformity, and discuss closed-loop workflows that couple molecular design with multimodal operando diagnostics. In this view, polymer artificial SEIs evolve from curated “recipes” into predictive, transferable interfaces, paving a path from coin-cell to prototype-level Li- and Zn-metal batteries.

Lithium‐metal anodes offer exceptional theoretical capacity and the lowest electrochemical potential, but their practical use is limited by dendrite growth, unstable SEI formation, and large volume fluctuations. Carbon nanofibers (CNFs), with their low weight, high conductivity, and tunable structures, serve as effective hosts for regulating lithium deposition. Heteroatom doping further enhances lithiophilicity and interfacial stability: nitrogen creates abundant nucleation sites, oxygen and sulfur increase surface polarity and strengthen the SEI, and fluorine facilitates LiF‐rich interphases for dendrite‐free growth. Multi‐element doping can also provide synergistic improvements in Coulombic efficiency and cycling stability. Despite these advances, challenges remain, including electrolyte consumption in high‐surface‐area structures, nonuniform dopant distribution, and potential degradation of CNF properties at high doping levels. This article summarizes recent progress in heteroatom‐doped CNFs for lithium‐metal anodes and outlines key limitations and future directions toward scalable, high‐performance lithium‐metal batteries. This perspective analyzes heteroatom‐doped carbon nanofibers as hosts for lithium‐metal anodes, highlighting their roles in suppressing lithium dendrites, stabilizing interfaces, and accommodating volume changes, while outlining sustainable and scalable strategies toward high‐performance next‐generation energy storage.

Lithium‐metal anodes suffer from inadequate rate and cycling performances for practical application mainly due to the harmful dendrite growth, especially at high currents. Herein a facile construction of the porous and robust network with thermally conductive AlN nanowires onto the commercial polypropylene separator by convenient vacuum filtration is reported. The so‐constructed AlN‐network shield provides a uniform thermal distribution to realize homogeneous Li deposition, super electrolyte‐philic channels to enhance Li‐ion transport, and also a physical barrier to resist dendrite piercing as the last fence. Consequently, the symmetric Li|Li cell presents an ultralong lifetime over 8000 h (20 mA cm−2, 3 mAh cm−2) and over 1000 h even at an unprecedented high rate (80 mA cm−2, 80 mAh cm−2), which is far surpassing the corresponding performances reported to date. The corresponding Li|LiFePO4 cell delivers a high specific capacity of 84.3 mAh g−1 at 10 C. This study demonstrates an efficient approach with great application potential toward durable and high‐power Li–metal batteries and even beyond. A porous and robust network of thermally conductive aluminum nitride (AlN) nanowires is conveniently constructed onto the commercial polypropylene separator. Such an AlN‐network shield provides the uniform thermal distribution for homogeneous Li deposition and dendrite‐free plating thereof, super electrolyte‐philic channels for fast Li‐ion transport, and also a last physical barrier to resist dendrite piercing, leading to the unprecedented cycling performance at high rate.

With the development of energy storage technology, the new energy storage materials are more diverse. The sodium metal has the advantages of high energy density, rich resource reserves, and low costs for raw materials, becoming promising advanced energy storage materials for application. However, the low tensile strength of sodium metal makes it difficult to process deformation while its severe viscosity and low melting point affect the subsequent manufactory and application of batteries. These characteristics hinder the processing and preparation of thin‐sodium metal. The designs of composite‐supporting structure, alloying, and the interface strengthening for sodium metal can effectively overcome the difficulties in preparation of the thin sodium. In this review, the design principles of thin sodium in terms of processing and preparation, according to the physical and chemical properties of sodium metal, are discussed. Meanwhile, the key challenges and new development opportunities are addressed for the processing and preparation of the thin‐sodium metal, which is beneficial for deeply understanding the reliable fabrication and realizing the practical application of thin‐sodium metals. This review provides three design strategies systematically (Support structure composite, interface design and alloying) for the preparation of thin sodium metal based on the characteristics of sodium metal. The electrochemical application characteristics of each design are also explained. In addition, it provides an overview of the challenges on large‐scale processing thin sodium metal.