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Aqueous zinc‐ion batteries (AZIBs) have attracted widespread attention due to their intrinsic merits of low cost and high safety. However, the poor thermodynamic stability of Zn metal in aqueous electrolytes inevitably cause Zn dendrites growth and interface parasitic side reactions, resulting in unsatisfactory cycling stability and low Zn utilization. Replacing Zn anode with intercalation‐type anodes have emerged as a promising alternative strategy to overcome the above issues but the lack of appropriate anode materials is becoming the bottleneck. Herein, the interlayer structure of MoSe2 anode is preintercalated with long‐chain polyvinyl pyrrolidone (PVP), constructing a periodically stacked p‐MoSe2 superlattice to activate the reversible Zn2+ storage performance (203 mAh g−1 at 0.2 A g−1). To further improve the stability of the superlattice structure during cycling, the electrolyte is also rationally designed by adding 1,4‐Butyrolactone (γ‐GBL) additive into 3 M Zn(CF3SO3)2, in which γ‐GBL replaces the H2O in Zn2+ solvation sheath. The preferential solvation of γ‐GBL with Zn2+ effectively reduces the water activity and helps to achieve an ultra‐long lifespan of 12,000 cycles for p‐MoSe2. More importantly, the reconstructed solvation structure enables the operation of p‐MoSe2||ZnxNVPF (Na3V2(PO4)2O2F) AZIBs at an ultra‐low temperature of −40°C, which is expected to promote the practical applications of AZIBs. The ultra‐large interlayer space of p‐MoSe2 superlattice can accommodate a large amount of Zn2+ ions at high rate and the cycling stability of p‐MoSe2 is further improved by the preferential solvation of γ‐GBL with Zn2+, therefore, the MoSe2||ZnxNVPF rocking chair full battery can even operate at an ultra‐low temperature of −40°C.

Rechargeable sodium metal batteries (SMBs) have emerged as promising alternatives to commercial Li‐ion batteries because of the natural abundance and low cost of sodium resources. However, the overuse of metallic sodium in conventional SMBs limits their energy densities and leads to severe safety concerns. Herein, we propose a sodium‐free‐anode SMB (SFA‐SMB) configuration consisting of a sodium‐rich Na superionic conductor‐structured cathode and a bare Al/C current collector to address the above challenges. Sodiated Na3V2(PO4)3 in the form of Na5V2(PO4)3 was investigated as a cathode to provide a stable and controllable sodium source in the SFA‐SMB. It provides not only remarkable Coulombic efficiencies of Na plating/stripping cycles but also a highly reversible three‐electron redox reaction within 1.0–3.8 V versus Na/Na+ confirmed by structural/electrochemical measurements. Consequently, an ultrahigh energy density of 400 Wh kg−1 was achieved for the SFA‐SMB with fast Na storage kinetics and impressive capacity retention of 93% after 130 cycles. A narrowed voltage window (3.0–3.8 V vs. Na/Na+) further increased the lifespan to over 300 cycles with a high retained specific energy of 320 Wh kg−1. Therefore, the proposed SFA‐SMB configuration opens a new avenue for fabricating next‐generation batteries with high energy densities and long lifetimes. Sodium‐rich Na superionic conductor‐structured cathodes are proposed to increase the energy density and lifespan of sodium‐free‐anode sodium metal batteries (SFA‐SMBs). The prestored Na in Na5V2(PO4)3 provides not only remarkable Na plating/stripping efficiencies but also a highly reversible three‐electron redox reaction, resulting in an ultrahigh energy density of 400 Wh kg−1 and superior cyclic stability.

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.

Aqueous zinc‐manganese (Zn–Mn) batteries have promising potential in large‐scale energy storage applications since they are highly safe, environment‐friendly, and low‐cost. However, the practicality of Mn‐based materials is plagued by their structural collapse and uncertain energy storage mechanism upon cycling. Herein, this work designs an amorphous manganese borate (a‐MnBOx) material via disordered coordination to alleviate the above issues and improve the electrochemical performance of Zn–Mn batteries. The unique physicochemical characteristic of a‐MnBOx enables the inner a‐MnBOx to serve as a robust framework in the initial energy storage process. Additionally, the amorphous manganese dioxide, amorphous ZnxMnO(OH)2, and Zn4SO4(OH)6·4H2O active components form on the surface of a‐MnBOx during the charge/discharge process. The detailed in situ/ex situ characterization demonstrates that the heterostructure of the inner a‐MnBOx and surface multicomponent phases endows two energy storage modes (Zn2+/H+ intercalation/deintercalation process and reversible conversion mechanism between the ZnxMnO(OH)2 and Zn4SO4(OH)6·4H2O) phases). Therefore, the obtained Zn//a‐MnBOx battery exhibits a high specific capacity of 360.4 mAh g−1, a high energy density of 484.2 Wh kg−1, and impressive cycling stability (97.0% capacity retention after 10 000 cycles). This finding on a‐MnBOx with a dual‐energy storage mechanism provides new opportunities for developing high‐performance aqueous Zn–Mn batteries. A conceptual amorphous manganese borate material for AZIBs is designed via a disordered coordination strategy. The unique physicochemical characteristic of a‐MnBOx can form the a‐MnO2, ZnxMnO(OH)2, and Zn4SO4(OH)6·4H2O phases, realizing multiple energy storage modes for enhancing the charge storage ability.

Rechargeable zinc-based batteries with near-neutral media are standing in the middle of the energy storage field by virtue of their high safety and low cost. However, it is still imperative for Mn-based cathode to improve rate capacity by facilitating ions/electron transfer and long-cycle stability by suppressing Mn dissolution. Herein, promoting electrooxidation kinetics is proposed and employed to construct advanced Mn−Zn battery. The formation of carbon-protected birnessite-MnO 2 is promoted via inducing the electron-donating capability of the heterointerface between the N−C coating and the defective MnO. Moreover, density functional theory calculations also demonstrate that N−C protected birnessite-MnO 2 is more hydrophobic than pure birnessite-MnO 2 , which is beneficial to prohibiting Mn dissolution and other side reactions. As a result, the elaborate design realizes effective transformation from low valence to high valence Mn for high capacity (291 mA·h·g −1 ) and protective bamboos-like structure for rate capacity (126 mAh·g −1 at 5 A·g −1 ) and cycling stability (89% capacity retention after 2,000 cycles). The assembled flexible quasi-solid-state Mn−Zn pouch batteries display application prospects for wearable and implantable electronic devices. The atomic engineering promoting electrooxidation kinetics strategy will be instructive in activating other cathode materials and maximizing their capacity.

Aqueous zinc‐based batteries face critical stability issues at the zinc metal anode, primarily manifested as uncontrolled dendrite growth, hydrogen evolution reaction, and corrosion. To address these issues in an eco‐friendly manner, we report a biomass‐derived additive, 3‐acetylamino‐5‐acetylfuran (3A5AF), synthesized from chitin, which features abundant polar N/O functional groups. Even at an ultralow concentration (0.3 mg mL − 1 ), 3A5AF could restructure the solvation shell of Zn 2 + and establish a protective layer on the anode surface, thereby curbing undesirable side reactions and guiding the uniform deposition of zinc. This stabilization strategy endows the Zn||Zn symmetric cell with robust longevity, achieving a cycle life exceeding 2700 h under 1 mA cm − 2 and 1 mAh cm − 2 . Even when subjected to a demanding current density of 4 mA cm − 2 , the cell maintains stable operation for 2400 h. The practical utility was further confirmed in Zn||I 2 full cells, which delivered a reversible capacity of 192.6 mAh g −1 following 1000 cycles at 0.5 A g − 1 and, at 8 A g − 1 , sustained 20 000 cycles with merely a 6.1% capacity loss (93.9% retention). This work highlights the promise of sustainable biomass‐derived additives in developing high‐performance and green aqueous zinc batteries.

Lithium (Li) metal is regarded as one of the most promising anode candidates for next‐generation batteries due to its extremely high specific capacity and low redox potential. However, its application is still hindered by the uncontrolled growth of dendritic Li and huge volume fluctuation during cycles. To address these issues, flexible and self‐supporting three‐dimensional (3D) interlaced N‐doped carbon nanofibers (NCNFs) coated with uniformly distributed 2D ultrathin NiCo 2 S 4 nanosheets (denoted CNCS) were designed to eliminate the intrinsic hotspots for Li deposition. Physicochemical dual effects of CNCS arise from limited surface Li diffusivity with a higher Li affinity, leading to uniform Li nucleation and less random accumulation of Li, as confirmed by ab initio molecular dynamics simulations. Due to the unique structure, exchange current density is reduced significantly and metallic Li is further contained within the interspace between the NCNF and NiCo 2 S 4 nanosheets, preventing the formation of dendritic Li. The symmetric cell with a Li/CNCS composite anode shows a long‐running lifespan for almost 1200 h, with an exceptionally low and stable overpotential under 1 mA cm −2 /1 mAh cm −2 . A full cell coupled with a LiFePO 4 cathode at a low N/P ratio of 2.45 shows typical voltage profiles but more significantly enhanced performance than that of a LiFePO 4 cathode coupled with a bare Li anode.

Zn metals have gained the immense attention of researchers for their wide employment as the anode of high‐performance aqueous batteries. Nonetheless, the Zn anodes suffer from uncontrollable dendrite growth and parasitic side reactions, which substantially shorten the battery lifespan. This study proposes an interfacial assembly of a metal‐polyphenol coordination coating on Zn anodes to regulate Zn2+ deposition behavior. Bismush‐coordinated polyphenolic ligands (i.e., tannic acid, TA) create a functional interface that could promote Zn's uniform nucleation and plating/striping kinetics. Moreover, the artificial coating acts as a physical barrier to inhibit surface corrosion. As a consequence, the TA‐Bi‐modified Zn anodes display a small voltage hysteresis of ~38 mV at 1 mA cm−2 over 2600 h and an ultra‐long lifespan for 3100 h (~4.3 months) even at a high‐current density of 10 mA cm−2. When assembled with a vanadium‐based cathode, the full Zn‐ion batteries achieve improved electrochemical performance. A functional metal‐polyphenol coordination interface is readily assembled on the Zn surface to enable uniform and dendrite‐free Zn deposition and excellent anti‐corrosion capability. The as‐modified Zn anode exhibit ultralong lifespan over 3100 h at a high‐current density of 10 mA cm−2 and improved rate/cycling performance in practical full cells.

Silicon nanoparticles were firstly prepared from industrial waste fly ash via a solid-state and magnesiothermic reaction with molten salt. The entire progression is feasible, green, economical, and scalable. Si nanoparticles served as anode materials for lithium-ion batteries (LIBs), delivering high specific capacity of around 3173.1 mAh g −1 , and outstanding cycling stability up to 500 cycles at 1 C. The work here will shed light on the idea of transforming trash, industrial waste fly ash, to treasure, silicon nanoparticles, for sustainable energy conversion. Graphical Abstract Industrial waste fly ash derived silicon nanoparticles were firstly synthesized via a coupled solid state-magnesiothermic reaction in a molten salt, which exhibited superb Li + storage properties.

Hard carbon is regarded as the most promising anode material for sodium-ion (Na-ion) batteries, owing to its advantages of high abundance, low cost, and low operating potential. However, the rate capability and cycle life span of hard carbon anodes are far from satisfactory, severely hindering its industrial applications. Here, we demonstrate that the desolvation process defines the Na-ion diffusion kinetics and the formation of a solid electrolyte interface (SEI). The 3A zeolite molecular sieve film on the hard carbon is proposed to develop a step-by-step desolvation pathway that effectively reduces the high activation energy of the direct desolvation process. Moreover, step-by-step desolvation yields a thin and inorganic-dominated SEI with a lower activation energy for Na⁺ transport. As a result, it contributes to greatly improved power density and cycling stability for both ester and ether electrolytes. When the above insights are applied, the hard carbon anode achieves the longest life span and minimum capacity fading rate at all evaluated current densities. Moreover, with the increase in current densities, an improved plateau capacity ratio is observed. This step-by-step desolvation strategy comprehensively enhances various properties of hard carbon anodes, which provides the possibility of building practical Na-ion batteries with high power density, high energy density, and durability.