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Metal anode instability, including dendrite growth, metal corrosion, and hetero-ions interference, occurring at the electrolyte/electrode interface of aqueous batteries, are among the most critical issues hindering their widespread use in energy storage. Herein, a universal strategy is proposed to overcome the anode instability issues by rationally designing alloyed materials, using Zn-M alloys as model systems (M = Mn and other transition metals). An in-situ optical visualization coupled with finite element analysis is utilized to mimic actual electrochemical environments analogous to the actual aqueous batteries and analyze the complex electrochemical behaviors. The Zn-Mn alloy anodes achieved stability over thousands of cycles even under harsh electrochemical conditions, including testing in seawater-based aqueous electrolytes and using a high current density of 80 mA cm −2 . The proposed design strategy and the in-situ visualization protocol for the observation of dendrite growth set up a new milestone in developing durable electrodes for aqueous batteries and beyond. Metal anode instability due to several intrinsic factors limits their widespread use in energy storage. Here, the authors report a 3D alloy anode via a universal alloy electrodeposition approach to overcome the anode instability issues and demonstrate a seawater-based aqueous battery.

Designing a multifunctional separator with abundant ion migration paths is crucial for tuning the ion transport in rocking‐chair‐type batteries. Herein, a polydopamine‐functionalized PVDF (PVDF@PDA) nanofibrous membrane is designed to serve as a separator for aqueous zinc‐ion batteries (AZIBs). The functional groups (OH and NH) in PDA facilitate the formation of ZnO and ZnN coordination bonds with Zn ions, homogenizing the Zn‐ion flux and thus enabling dendrite‐free Zn deposition. Moreover, the PVDF@PDA separator effectively inhibits the shuttling of V‐species through the formation of VO coordination bonds. As a result, the Zn/NH4V4O10 battery with the PVDF@PDA separator exhibits enhanced cycling stability (92.3% after 1000 cycles at 5 A g−1) and rate capability compared to that using a glass fiber separator. This work provides a new avenue to design functionalized separators for high‐performance AZIBs. A polydopamine‐functionalized PVDF (PVDF@PDA) nanofibrous membrane is designed as a separator for aqueous zinc‐ion batteries. The PVDF@PDA separator homogenizes the Zn‐ion flux distribution to achieve the dendrite‐free Zn deposition via the metal‐PDA coordination chemistry. Moreover, the PVDF@PDA separator inhibits the shuttle of V‐species. Benefiting from the separator, the Zn/NH4V4O10 full cell retains 92.3% capacity after 1000 cycles at 5 A g−1.

Direct application of metallic lithium (Li) as the anode in rechargeable lithium metal batteries (LMBs) is still hindered by some annoying issues such as lithium dendrites formation, low Coulombic efficiency, and safety concerns arising therefrom. Herein, an advanced composite separator is prepared by facilely blade coating lightweight and thin functional layers on commercial 12 µm polyethylene separator to stabilize the Li anode. The composite separator simultaneously improves the Li ion transport and lithium deposition behaviors with uniform lithium ion distribution properties, enabling the dendrite‐free Li deposition. As a result, the lithium anode can stably cycle up to 3000 cycles with the high capacity of 3.5 mAh cm−2. Moreover, the composite separator exhibits wide compatibility in LMBs (Li–S and Li‐ion battery) and delivers stable cycling performance and high Coulombic efficiency both in coin and lab‐level soft‐pack cells. Thus, this cost‐effective modification strategy exhibits great application potential in high‐energy LMBs. The designed functionalized layer can regulate lithium (Li) ions distribution and ensure uniform Li ions flux and deposition even in the presence of rough defects or cracks disturbance. Therefore, ultralong cycling dendrite‐free Li anodes can be achieved with this special designed TV‐PE separator, endowing great potential in the practical application of future high energy lithium metal batteries.

Solid‐state lithium metal batteries (SLMBs) are attracting enormous attention due to their enhanced safety and high theoretical energy density. However, the alkali lithium with high reducibility can react with the solid‐state electrolytes resulting in the inferior cycle lifespan. Herein, inspired by the idea of interface design, the 1‐butyl‐1‐methylpyrrolidinium bis(trifluoromethanesulfonyl) imide as an initiator to generate an artificial protective layer in polymer electrolyte is selected. Time‐of‐flight secondary ion mass spectrometry and X‐ray photoelectron spectroscopy reveal the stable solid electrolyte interface (SEI) is in situ formed between the electrolyte/Li interface. Scanning electron microscopy (SEM) images demonstrate that the constructed SEI can promote homogeneous Li deposition. As a result, the Li/Li symmetrical cells enable stable cycle ultralong‐term for over 4500 h. Moreover, the as‐prepared LiFePO4/Li SLMBs exhibit an impressive ultra‐long cycle lifespan over 1300 cycles at 1 C, as well as 1600 cycles at 0.5 C with a capacity retention ratio over 80%. This work offers an effective strategy for the construction of the stable electrolyte/Li interface, paving the way for the rapid development of long lifespan SLMBs. A stable solid electrolyte interface layer with multiple phases of LiF, Li2Sx, and Li3N is successfully in situ formed on the electrolyte/Li surface with the ionic liquid of 1‐butyl‐1‐methylpyrrolidinium bis(trifluoromethanesulfonyl) imide as the initiator. Impressively, the LiFePO4/PIA‐SPE/Li solid‐state batteries exhibit admirable cyclic stabilities, and the current findings pave a new direction for fabricating long lifespan solid‐state lithium metal batteries.

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.

Rational architecture design of the artificial protective layer on the zinc (Zn) anode surface is a promising strategy to achieve uniform Zn deposition and inhibit the uncontrolled growth of Zn dendrites. Herein, a red phosphorous‐derived artificial protective layer combined with a conductive N‐doped carbon framework is designed to achieve dendrite‐free Zn deposition. The Zn–phosphorus (ZnP) solid solution alloy artificial protective layer is formed during Zn plating. Meanwhile, the dynamic evolution mechanism of the ZnP on the Zn anode is successfully revealed. The concentration gradient of the electrolyte on the electrode surface can be redistributed by this protective layer, thereby achieving a uniform Zn‐ion flux. The fabricated Zn symmetrical battery delivers a dendrite‐free plating/stripping for 1100 h at the current density of 2.0 mA cm–2. Furthermore, aqueous Zn//MnO2 full cell exhibits a reversible capacity of 200 mAh g–1 after 350 cycles at 1.0 A g–1. This study suggests an effective solution for the suppression of Zn dendrites in Zn metal batteries, which is expected to provide a deep insight into the design of high‐performance rechargeable aqueous Zn‐ion batteries. An artificial protective layer based on zinc‐phosphorus (ZnP) alloying reaction is designed to regulate the deposition behavior of Zn ions. The synergistic effect of the ZnP alloy artificial protective layer and carbon framework enables a uniform electric field strength distribution and a homogeneous Zn‐ion flux on the electrode surface, which results in the dendrite‐free Zn plating/stripping.

High energy density lithium metal batteries (LMBs) are promising next‐generation energy storage devices. However, the uncontrollable dendrite growth and huge volume change limit their practical applications. Here, a new Mg doped Li–LiB alloy with in situ formed lithiophilic 3D LiB skeleton (hereinafter called Li–B–Mg composite) is presented to suppress Li dendrite and mitigate volume change. The LiB skeleton exhibits superior lithiophilic and conductive characteristics, which contributes to the reduction of the local current density and homogenization of incoming Li+ flux. With the introduction of Mg, the composite achieves an ultralong lithium deposition/dissolution lifespan (500 h, at 0.5 mA cm−2) without short circuit in the symmetrical battery. In addition, the electrochemical performance is superior in full batteries assembled with LiCoO2 cathode and the manufactured composite. The currently proposed 3D Li–B–Mg composite anode may significantly propel the advancement of LMB technology from laboratory research to industrial commercialization. A Li–B–Mg composite with in situ formed 3D LiB fiber network shows a dendrite‐free morphology and less volume change during cycling. The symmetrical battery achieves a long and stable cycle lifespan of more than 500 h at 0.5 mA cm−2 due to the effect of skeleton and the addition of Mg. The full battery also displays improved electrochemical performance.

The interfacial instability of lithium (Li) metal is one of the critical challenges, which hinders the application of rechargeable Li metal batteries (LMBs). Designing facile and effective surface/interface is extremely important for practical LMBs manufacturing. Here, a highly stable Li anode with silver nanowires sowed in the patterned ditches via a simple calendaring process is developed. The remarkably increased electroactive surface area and the superior lithiophilic Ag seeds enable Li stripping/plating mainly inside the ditches. Benefitting from such unique structural design, the ditches‐patterned and Ag‐modified composite Li anode (D‐Ag@Li) achieves excellent cyclability under 2 mA cm−2 / 4 mAh cm−2 over 360 h cycling with low nucleation overpotential of 16 mV. Pairing with the D‐Ag@Li anode, the full cells with LiNi0.8Mn0.1Co0.1O2 and LiFePO4 (LFP) cathodes achieve long cycle life with 94.2% retention after 2000 cycles and 74.2% after 4000 cycles, respectively. Moreover, ultrasonic transmission mapping shows no gas generation for the LFP pouch full cell pouch cell based on D‐Ag@Li over prolonged cycling, demonstrating the feasibility and effectiveness of the authors' strategy for LMBs. A highly stable lithium (Li) anode with silver nanowires (AgNWs) sowed in the patterned ditches is developed. The interconnected ditches significantly enhance the surface area of Li metal, and at the same time, AgNWs can serve as preferred electrochemical active sites to induce homogeneous Li nucleation and growth from the bottom rather than the top surfaces.

Lithium metal anodes have long been considered as “holy grail” in the field of energy storage batteries, but dendrite growth and large volume changes hinder their practical applications. Herein, a facile and eco‐friendly CF4 plasma treatment is employed for the surface modification of Li anodes, and an artificial layer consisting of LiF and Li2C2 is fabricated for the first time. Experimental results and theoretical calculations reveal that the high adsorption energy of LiF and low Li+ diffusion barriers in Li2C2 induce uniform nucleation and planar growth of Li, guaranteeing a stable and dendrite‐free Li structure during the repeated plating/stripping process of cycling. Symmetric cells using CF4 plasma‐treated Li operate stably for more than 6500 h (at 2 mA cm−2 and 1 mAh cm−2) or 950 h (at 1 mA cm−2 and 10 mAh cm−2). When paired with a LiFePO4 cathode, full batteries deliver a high reversible capacity of 136 mAh g−1 (at 1 C) with considerable cycling stability (97.2% capacity retention over 200 cycles) and rate performance (116 mAh g−1 up to 5 C). This powerful application of plasma technology toward novel LiF‐Li2C2 artificial layers provide new routes for constructing environment‐friendly and high‐performance energy storage devices. An artificial layer consisting of LiF and Li2C2 is fabricated by a facile and eco‐friendly CF4 plasma treatment for the first time. The symmetric cells using the CF4 plasma‐treated Li can operate stably for more than 6500 h with an overpotential of 50 mV.

The increasing demands for efficient and clean energy-storage systems have spurred the development of Li metal batteries, which possess attractively high energy densities. For practical application of Li metal batteries, it is vital to resolve the intrinsic problems of Li metal anodes, i.e., the formation of Li dendrites, interfacial instability, and huge volume changes during cycling. Utilization of solid-state electrolytes for Li metal anodes is a promising approach to address those issues. In this study, we use a 3D garnet-type ion-conductive framework as a host for the Li metal anode and study the plating and stripping behaviors of the Li metal anode within the solid ion-conductive host. We show that with a solid-state ion-conductive framework and a planar current collector at the bottom, Li is plated from the bottom and rises during deposition, away from the separator layer and free from electrolyte penetration and short circuit. Owing to the solid-state deposition property, Li grows smoothly in the pores of the garnet host without forming Li dendrites. The dendrite-free deposition and continuous rise/fall of Li metal during plating/stripping in the 3D ion-conductive host promise a safe and durable Li metal anode. The solid-state Li anode shows stable cycling at 0.5 mA cm−2 for 300 h with a small overpotential, showing a significant improvement compared with reported Li anodes with ceramic electrolytes. By fundamentally eliminating the dendrite issue, the solid Li metal anode shows a great potential to build safe and reliable Li metal batteries.