Sodium metal, with a high theoretical specific capacity of 1165 mAh g−1, is the ultimate anode for sodium batteries, yet how to deal with the inhomogeneous and dendritic sodium deposition and the infinite relative dimension change of sodium metal anodes during sodium depositing/stripping is still challenging. Here, a facile fabricated sodiuphilic 2D N‐doped carbon nanosheets (N‐CSs) are proposed as sodium host material for sodium metal batteries (SMBs) to prevent dendrite formation and eliminate volume change during cycling. Revealing from combined in situ characterization analyses and theoretical simulations, the high nitrogen content and porous nanoscale interlayer gaps of the 2D N‐CSs can not only concede dendrite‐free sodium stripping/depositing but also accommodate the infinite relative dimension change. Furthermore, N‐CSs can be easily process into N‐CSs/Cu electrode via traditional commercial battery electrode coating equipment that pave the way for large‐scale industrial applications. On account of the abundant nucleation sites and sufficient deposition space, N‐CSs/Cu electrodes demonstrate a superior cycle stability of more than 1500 h at a current density of 2 mA cm−2 with a high coulomb efficiency of more than 99.9% and ultralow nucleation overpotential, which enable reversible and dendrites‐free SMBs and shed light on further development of SMBs with even higher performance.

Ultrahigh Nitrogen Content Carbon Nanosheets for High Stable Sodium Metal Anodes

Anode-free sodium metal battery (AFSMB) promises a high energy density, but suffers from the difficulty of maintaining high cycling stability. Nonuniform sodium (Na) deposition on current collector is largely responsible for capacity decay in the cycling process of AFSMB. Here, a unique Cu3 P nanowires was constructed on copper (Cu3 P@Cu) as sodium deposition substrate by an in-situ growth method. Superior electrochemical performance of Cu3 P@Cu anode was delivered in asymmetric cells with an average Coulombic efficiency of 99.8% for over 800 cycles at 1 mA cm-2 with 1 Am h cm-2 . Symmetric cell of Cu3 P@Cu displayed a cycling lifespan of over 2000 h at 2 mA cm-2 with 1 Am h cm-2 . Cryo-TEM characterization and first principles calculation revealed that the low Na+ absorption energy and low Na+ diffusion energy barrier on Na3 P promoted the uniform Na nucleation and deposition, thus enhancing the Na surface stability. Moreover, anode-free Na3 V2 (PO4 )3 //Cu3 P@Cu full pouch cell delivered a considerable cycling capacity of ∼15 mA h in 170 cycles, demonstrating its practical feasibility. This article is protected by copyright. All rights reserved.

Anode-Free Sodium Metal Pouch Cell Using Cu3 p Nanowires In-Situ Grown on Current Collector.

Room-temperature sodium-sulfur (RT-Na/S) batteries are promising alternatives for next-generation energy storage systems with high energy density and high power density. However, some notorious issues are hampering the practical application of RT-Na/S batteries. Besides, the working mechanism of RT-Na/S batteries under practical conditions such as high sulfur loading, lean electrolyte, and low capacity ratio between the negative and positive electrode (N/P ratio), is of essential importance for practical applications, yet the significance of these parameters has long been disregarded. Herein, we comprehensively review recent advances on Na metal anode, S cathode, electrolyte, and separator engineering for RT-Na/S batteries. The discrepancies between laboratory research and practical conditions are elaborately discussed, endeavors toward practical applications are highlighted, and suggestions for the practical values of the crucial parameters are rationally proposed. Furthermore, an empirical equation to estimate the actual energy density of RT-Na/S pouch cells under practical conditions is rationally proposed for the first time, making it possible to evaluate the gravimetric energy density of the cells under practical conditions. This review aims to reemphasize the vital importance of the crucial parameters for RT-Na/S batteries to bridge the gaps between laboratory research and practical applications. This article is protected by copyright. All rights reserved.

A Critical Review on Room-Temperature Sodium-Sulfur Batteries: From Research Advances to Practical Perspectives.

<h2>Summary</h2> High-energy cryogenic batteries have been pursued throughout the past decades. Anode-free batteries offer a promising avenue to boost energy density because they comprise weightless anodes. However, their low-temperature operation is challenged by poor metal plating/stripping reversibility and unstable solid electrolyte interphase (SEI). Herein, the first low-temperature anode-free sodium battery is fabricated by simultaneous surface modification of the current collector and electrolyte design. The plasma-treated current collector (p-Al@C) possesses a sodiophilic N-doped carbon surface, enabling uniform sodium nucleation and growth; meanwhile, the optimized weak-solvation electrolyte facilitates Na+ desolvation and the formation of a B/F inorganic-contained SEI. Na||p-Al@C half cells exhibit an ultrahigh average Coulombic efficiency of 99.88%, and p-Al@C||Na3V2(PO4)3 batteries achieve an energy density of 250 Wh kg−1cathode + anode at −40°C. More interestingly, Ah-level anode-free pouch cells deliver a remarkable energy density of 110 Wh kg−1entire cell at −40°C. This work represents a critical step for low-temperature sodium batteries.

A 110 Wh kg−1 Ah-level anode-free sodium battery at −40°C

Sodium metal batteries are promising next‐generation energy storage technology by using energy‐dense and affordable Na metal anodes, yet suffering uncontrollable Na dendritic growth issues. Herein, Au nanoparticle@hollow amorphous carbon tube yolk/shell arrays (Au/HCT‐CC) is rationally designed on carbon cloth as a dynamic host. In situ transmission electron microscopy observations reveal a regulated dendrite‐free Na metal plating/stripping within the Au/HCT‐CC host. The self‐confinement of Na metal deposition in the hollow carbon can further stabilize the electrolyte/electrode interface and homogenize Na ion flux, as evidenced by rigorous experimental and theoretical characterizations, thus successfully accommodating the hurdles to Na metal anodes. When cycling in half cells, the Au/HCT‐CC electrodes deliver remarkably high coulombic efficiencies (CEs) of 99.96% over 2200 h at 5 mA cm−2. The high CE of 99.54% is preserved even under harsh cycling conditions of 10 mA cm−2 and 20 mAh cm−2 for 250 cycles. These values rival the state‐of‐the‐art electrochemical performance for Na metal anodes in literature. Finally, the practical feasibility of the new anode is demonstrated by cycling in Na3V2(PO4)3@C||Na‐Au/HCT‐CC full cells over 900 cycles with an extremely low capacity degradation rate of 0.017% per cycle.

Self‐Confinement of Na Metal Deposition in Hollow Carbon Tube Arrays for Ultrastable and High‐Power Sodium Metal Batteries

Ethylene carbonate (EC) is widely used in lithium-ion batteries due to its optimal overall performance with satisfactory conductivity, relatively stable solid electrolyte interphase (SEI), and wide electrochemical window. EC is also the most widely used electrolyte solvent in sodium ion batteries. However, compared to lithium metal, sodium metal (Na) shows higher activity and reacts violently with EC-based electrolyte (NaPF6 as solute), which leads to the failure of sodium metal batteries (SMBs). Herein, we reveal the electrochemical instability mechanism of EC on sodium metal battery, and find that the combination of EC and NaPF6 is electrically reduced in sodium metal anode during charging, resulting in the reduction of the first coulombic efficiency, and the continuous consumption of electrolyte leads to the cell failure. To address the above issues, an additive modified linear carbonate-based electrolyte is provided as a substitute for EC based electrolytes. Specifically, ethyl methyl carbonate (EMC) and dimethyl carbonate (DMC) as solvents and fluoroethylene carbonate (FEC) as SEI-forming additive have been identified as the optimal solvent for NaFP6 based electrolyte and used in Na4Fe3(PO4)2(P2O7)||Na batteries. The batteries exhibit excellent capacity retention rate of about 80% over 1000 cycles at a cut-off voltage of 4.3 V. 

Unraveling the incompatibility mechanism of ethylene carbonate-based electrolytes in sodium metal anodes

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Ultrahigh Nitrogen Content Carbon Nanosheets for High Stable Sodium Metal Anodes

Unraveling the incompatibility mechanism of ethylene carbonate-based electrolytes in sodium metal anodes