Charge Tuning and Anchor Effect Achieving Stable High-Voltage Layered Metal Oxides for Sodium-Ion Battery.

Layered metal oxides (LMOs) that can stably operate at high voltage are vital to developing high-energy sodium-ion batteries (SIBs). However, the irreversible oxygen redox reaction of LMOs at the high voltage region (i.e.

Activating the high-potential V/V redox couple for an advanced NASICON sodium-ion cathode.

NaVCrTi(PO) with multi-electron redox reactions is designed for high-energy-density sodium-ion batteries. The partial Cr substitution achieves high-potential V activation, achieving an ultra-high capacity of 183.07 mA h g at 20 mA g with 89% retention after 1500 cycles at 1 A g.

Understanding the Relationship of Closed Pore Structure in Biomass- derived Hard Carbon with Cellulose Regulating Strategy.

Recycling waste biomass to pyrolytic carbon has become a development direction of sodium-ion batteries (SIBs) anodes. However, it remains a challenge to precisely control the composition and structure of biomass to modify the properties of derived carbon. Herein, a strategy of hydrolyzing cellulose in phellem with sulfuric acid is proposed, which can promote cellulose fracture, reduce the graphitization and increase the content of closed pores in hard carbon.

Heterogeneous NASICON-Type Cathode With Reversible Multielectron Reaction for High-Performance Sodium-Ion Batteries.

Na superionic conductor (NASICON)-structured compounds demonstrate great application potential by their robust framework and compositional diversity. However, they are blamed for the mediocre energy density, and achieving both multielectron reaction and good cycling stability simultaneously is challenging. Herein, a novel heterogeneous NaFe(PO)(PO)/NaVTi(PO) (NFPP/NVTP) material with stable multielectron reaction is constructed by spray drying technology.

Regulating the Pore Structure of Biomass-Derived Hard Carbon for an Advanced Sodium-Ion Battery.

Biomass-derived hard carbon materials are attractive for sodium-ion batteries due to their abundance, sustainability, and cost-effectiveness. However, their widespread use is hindered by their limited specific capacity. Herein, a type of bamboo-derived hard carbon with adjustable pore structures is developed by employing a ball milling technique to modify the carbon chain length in the precursor.

Retarded sodium alloying interface reaction for stable anode-less sodium metal batteries.

Improving the sodiophilicity of the substrate is essential to enhance the reversibility of anode-less sodium metal batteries. Here, we have prepared a sodiophilic nano-Pb coating on aluminum-based collectors by magnetron sputtering. The slow alloying kinetics between Pb and sodium allows prolonged Pb retention in the coating, endowing the coating with a durable sodiophilicity.

Lithiation Induced Hetero-Superlattice Zn/ZnLi as Stable Anode for Aqueous Zinc-Ion Batteries.

Three dimensional (3D) framework structure is one of the most effective ways to achieve uniform zinc deposition and thus inhibit the Zn dendrites growth in working Zn metallic anode. A major challenge facing for the most commonly used 3D zincophilic hosts is that the zincophilic layer tends to peel off during repeatedly cycling, making it less stable. Herein, for the first time, a hetero-superlattice Zn/ZnLi (HS-Zn/ZnLi) anode containing periodic arrangements of metallic Zn phase and zincophilic ZnLi phase at the nanoscale, is well designed and fabricated via electrochemical lithiation method.

Regulating Pseudo-Graphitic Domain and Closed Pores to Facilitate Plateau Sodium Storage Capacity and Kinetics for Hard Carbon.

Hard carbon anode demonstrates exceptional potential in sodium-ion batteries due to their cost-effectivenss and superior plateau capacity. However, the proximity of the plateau capacity to the cut-off voltage of battery operation and the premature cut-off voltage response caused by polarization at high rates greatly limit the exploitation of plateau capacities, raising big concerns about inferior rate performance of high-plateau-capacity hard carbon. In this work, a facile pre-oxidation strategy is proposed for fabricating lignin-derived hard carbon.

Exceeding Three-Electron Reactions in Polyanionic Cathode To Achieve High-Energy Density for Sodium-Ion Batteries.

Activating multielectron reactions of sodium superionic conductor (NASICON)-type cathodes toward higher energy density remains imperative to boost their application feasibility. However, multisodium storage with high stability is difficult to achieve due to the sluggish reaction kinetics, irreversible phase transitions, and negative structural degradation. Herein, a kind of NASICON-type NaVTi(PO)/C (NVTP-0.

Anion-Induced Uniform and Robust Cathode-Electrolyte Interphase for Layered Metal Oxide Cathodes of Sodium Ion Batteries.

Layer metal oxides demonstrate great commercial application potential in sodium-ion batteries, while their commercialization is extremely hampered by the unsatisfactory cycling performance caused by the irreversible phase transition and interfacial side reaction. Herein, trimethoxymethylsilane (TMSI) is introduced into electrolytes to construct an advanced cathode/electrolyte interphase by tuning the solvation structure of anions. It is found that due to the stronger interaction between ClO and TMSI than that of ClO and PC/FEC, the ClO-TMSI complexes tend to accumulate on the surface of the cathode during the charging process, leading to the formation of a stable cathode/electrolyte interface (CEI).

Thermally Healable Electrolyte-Electrode Interface for Sustainable Quasi-Solid Zinc-ion Batteries.

Quasi-solid zinc-ion batteries using hydrogel electrolytes show great potential in energy storage devices owing to their intrinsic safety, fewer side reactions and wide electrochemical windows. However, the dendrite issues on the zinc anodes cannot be fundamentally eliminated and the intrinsic anode-electrolyte interfacial interspace is rarely investigated. Here, we design a dynamically healable gelatin-based hydrogel electrolyte with a highly reversible sol-gel transition, which can construct a conformal electrode-electrolyte interface and further evolve into a stable solid-solid interface by in situ solidification.

Challenges and Strategies of Aluminum Anodes for High-Performance Aluminum-Air Batteries.

Aluminum-air battery (AAB) is a promising candidate for next-generation energy storage/conversion systems due to its cost-effectiveness and impressive theoretical energy density of 8100 Wh kg, surpassing that of lithium-ion batteries. Nonetheless, the practical applicability of AABs is hampered by the occurrence of serious self-corrosion side reactions and substantial capacity loss, resulting in suboptimal anode utilization. Consequently, improving the anode utilization to facilitate the construction of high-performance AABs have attracted widespread attention.

Revealing the closed pore formation of waste wood-derived hard carbon for advanced sodium-ion battery.

Although the closed pore structure plays a key role in contributing low-voltage plateau capacity of hard carbon anode for sodium-ion batteries, the formation mechanism of closed pores is still under debate. Here, we employ waste wood-derived hard carbon as a template to systematically establish the formation mechanisms of closed pores and their effect on sodium storage performance. We find that the high crystallinity cellulose in nature wood decomposes to long-range carbon layers as the wall of closed pore, and the amorphous component can hinder the graphitization of carbon layer and induce the crispation of long-range carbon layers.

Significantly Improving the Initial Coulombic Efficiency of TiO Anode for Sodium-Ion Batteries.

Titanium dioxide (TiO) can serve as a candidate anode material for sodium-ion batteries (SIBs) with the merits of their low cost, abundance, and environment friendliness. However, its low initial Coulombic efficiency (ICE) and sluggish sodium-ion diffusion greatly limit its further practical applications. Herein, we report a one-step prepotassiation strategy to modify commercial TiO by a spontaneous chemical reaction using potassium naphthalene (K-Nt).

Quasi-Solid-State Aluminum-Air Batteries with Ultra-high Energy Density and Uniform Aluminum Stripping Behavior.

Aqueous aluminum-air batteries are attracting considerable attention with high theoretical capacity, low-cost and high safety. However, lifespan and safety of the battery are still limited by the inevitable hydrogen evolution reaction on the metal aluminum anode and electrolyte leakage. Herein, for the first time, a clay-based quasi-solid-state electrolyte is proposed to address such issues, which has excellent compatibility and a liquid-like ionic conductivity.

Bulk-Phase Reconstruction Enables Robust Zinc Metal Anodes for Aqueous Zinc-Ion Batteries.

Aqueous zinc-ion batteries are inherently safe, but the severe dendrite growth and corrosion reaction on zinc anodes greatly hinder their practical applications. Most of the strategies for zinc anode modification refer to the research of lithium metal anodes on surface regulation without considering the intrinsic mechanisms of zinc anode. Herein, we first point out that surface modification cannot permanently protect zinc anodes due to the unavoidable surface damage during the stripping process by solid-liquid conversion.

Weak solvent chemistry enables stable aqueous zinc metal batteries over a wide temperature range from -50 to 80 °C.

The development of electrolytes with a wide temperature range, no dendrite growth and corrosion resistance is essential for the practical application of aqueous zinc metal batteries. Herein, γ-valerolactone is developed as the co-solvent to extend the operating temperature range of the aqueous electrolyte and stabilize the zinc metal anode interface. This weak solvent acts as a strong hydrogen bonding ligand and "diluent" to break the hydrogen bonds between free water molecules, thus enhancing the temperature tolerance and chemical stability of the electrolyte.

Robust and Wide Temperature-Range Zinc Metal Batteries with Unique Electrolyte and Substrate Design.

Rechargeable zinc metal batteries are promising for large-scale energy storage. However, their practical application is limited by harsh issues such as uncontrollable dendrite growth, low Coulombic efficiency, and poor temperature tolerance. Herein, a unique design strategy using γ-valerolactone-based electrolyte and nanocarbon-coated aluminum substrate was reported to solve the above problems.

Regulating solvation and interface chemistry enables advanced aluminum-air batteries.

The main challenge for developing aqueous aluminum-air batteries with high mass-specific capacity depends on the inhibition of the parasitic hydrogen evolution reaction. Herein, a regulation strategy of solvation and interface chemistry has been proposed by introducing organic methylurea (MU) and inorganic stannous chloride (SnCl) to the alkaline electrolyte, which can modulate the solvent structure and electrode/electrolyte interface and endow the aqueous aluminum-air battery with an outstanding mass-specific capacity of 2625 mA h g at 50 mA cm.

Discovering the Intrinsic Causes of Dendrite Formation in Zinc Metal Anodes: Lattice Defects and Residual Stress.

Developing a highly stable and dendrite-free zinc anode is essential to the commercial application of zinc metal batteries. However, the understanding of zinc dendrites formation mechanism is still insufficient. Herein, for the first time, we discover that the interfacial heterogeneous deposition induced by lattice defects and epitaxial growth limited by residual stress are intrinsic and critical causes for zinc dendrite formation.

A Semi-solid Zinc Powder-based Slurry Anode for Advanced Aqueous Zinc-ion Batteries.

The booming of aqueous zinc-ion batteries (AZIBs) draws the researchers' attention to issues of zinc metal anodes, such as uncontrollable dendrite growth, corrosion, and volume effects. Zinc powder anode is more suitable for the industrial application of AZIBs than the widely used zinc foil anode due to its low cost, tunability and processability. However, the related solutions are rarely studied because the above issues of zinc metal anode are more serious in zinc powder anode.

Lithiophilic Sn-Co nano-seeds sealed in a hollow carbon shell to stabilize lithium metal anodes.

A lithiophilic Sn-Co nano-seed sealed in a nitrogen-doped carbon shell is designed to stabilize lithium metal anodes, in which lithiophilic alloys can regulate lithium deposition behavior and the hollow carbon shell is beneficial to prevent agglomeration. The modified lithium anode can be stable for 1350 h and 400 h under 1 mA cm and 5 mA cm in symmetric cells. The Sn-Co@C@Li||LiFePO full cell with a low N/P ratio of 2.

A high-capacity self-sacrificial additive based on electroactive sodiated carbonyl groups for sodium-ion batteries.

A new type of high-capacity sacrificial additive (NaCO) is proposed to replenish the sodium loss in sodium ion full-cells. The HC//NaV(PO)F full-cells demonstrate significantly enhanced energy density after introducing an appropriate amount of additive.

Engineering Crystal Orientation of Cathode for Advanced Lithium-Ion Batteries: A Minireview.

Engineering crystal orientation has attracted widespread attention since it is related to the cyclability and rate performance of cathode materials for lithium-ion batteries (LIBs). Regulating the crystal directional growth with optimal exposed crystal facets is an effective strategy to improve the performance of cathode materials, but still lacks sufficient attention in research field. Herein, we briefly introduce the characterization techniques and identification methods for crystal facets, then summarize and illuminate the major methods for regulating crystal orientation and their internal mechanism.