Wei Ai

The practical implementation of ampere‐hour‐scale aqueous zinc metal batteries is severely hindered by hydrogen evolution corrosion and dendritic growth under high‐current operation. Although regulating electrode–electrolyte interphase water via hydrogen bonding has been recognized as an effective strategy to suppress parasitic reactions, achieving dense, and uniform zinc deposition at high current densities remains a critical challenge due to interfacial instability and stress accumulation. Here, we construct a hydrogen‐bond‐network‐regulated ionic liquid layer coupled with a rheologically adaptive polydimethylsiloxane gel to establish a water‐poor and mechanically resilient interphase. The modified hydrogen‐bond network modulates the interfacial water environment, thereby contributing to suppressing corrosion. Simultaneously, the polydimethylsiloxane gel layer provides a hydrophobic barrier against water penetration and dynamically accommodates interfacial stress, enabling dense and uniform zinc deposition under high‐rate conditions. As a result, Zn||Zn symmetric cells exhibit exceptional cycling stability exceeding 1800 h at 50 and 25 mAh cm ^{− 2} . More importantly, a 4 Ah pouch cell delivers stable cycling for 300 cycles with a cumulative capacity exceeding 1200 Ah. This work establishes a rational interphase engineering strategy for achieving durable, high‐capacity aqueous zinc metal batteries under practical high‐current conditions.

Rechargeable magnesium batteries (RMBs) have emerged as highly promising alternatives to lithium‐ion batteries because of the high volumetric capacity, natural abundance, and potentially improved safety of magnesium metal anodes. However, their practical development remains severely hindered by sluggish Mg ²⁺ transport kinetics, limited rate capability, and insufficient cycling reversibility. Carbon‐based materials, owing to their high electrical conductivity, low density, excellent chemical stability, corrosion resistance, and structural tunability, offer versatile opportunities to address these challenges and improve the electrochemical performance of RMBs. This review systematically examines the multifunctional roles of carbon‐based materials across different battery components, including their use as active hosts for Mg storage, conductive and structural supports for stabilizing electrode architectures, functional interlayers for regulating polysulfide behavior in magnesium–sulfur batteries, conductive additives, separator modifiers, and corrosion‐resistant current collectors. Particular emphasis is placed on the mechanisms by which carbon materials regulate charge transport, interfacial stability, reaction kinetics, and sulfur‐species conversion. By correlating carbon structure, surface chemistry, and dimensional architecture with electrochemical function, this review establishes structure–property–function relationships that distinguish the roles of carbon in RMBs from those in other battery chemistries. Finally, the remaining challenges and future research directions for the rational design of carbon‐based materials toward advanced RMBs are discussed.

Developing high‐performance FeS ₂ ‐based anodes for sodium‐ion batteries is impeded by sluggish kinetics, poor conductivity, and severe volume variation. Herein, we report a rationally designed FeS ₂ /SnS ₂ /rGO composite featuring a three‐dimensional hierarchical heterostructure. In this architecture, SnS ₂ nanosheets are uniformly anchored on reduced graphene oxide framework, while FeS ₂ nanoparticles are dispersed throughout the scaffold, forming interconnected electron pathways and structural robustness. More importantly, the abundant FeS ₂ ‐SnS ₂ heterointerfaces induce built‐in electric fields that regulate charge redistribution and accelerate interfacial reaction kinetics, thereby promoting surface‐dominated pseudocapacitive behavior and rapid Na ⁺ diffusion. As a result, the FeS ₂ /SnS ₂ /rGO electrode delivers a high reversible capacity of 618 mAh g ⁻¹ at 0.1 A g ⁻¹ and retains 500 mAh g ⁻¹ at 5 A g ⁻¹ , together with outstanding cycling stability (536 mAh g ⁻¹ after 400 cycles at 2 A g ⁻¹ with 99.5% retention). Furthermore, full cells paired with NaNi _1/3 Fe _1/3 Mn _1/3 O ₂ exhibit good rate capability and long‐term stability. This work demonstrates that heterointerface‐induced electric‐field regulation is an effective strategy for accelerating reaction kinetics in conversion‐type anodes.

Li–S batteries (LSBs) are promising next‐generation energy storage systems; however, their practical application is severely hindered by the shuttle effect of soluble lithium polysulfides and sluggish redox kinetics. Although separator functionalization with catalytic materials has been widely explored, the fundamental role of crystallinity in governing polysulfide conversion remains insufficiently understood. Herein, the effect of crystallinity on polysulfides regulation is systematically investigated using Co ₃ S ₄ as a model system. Amorphous Co ₃ S ₄ (A‐Co ₃ S ₄ ) and crystalline Co ₃ S ₄ (C‐Co ₃ S ₄ ) are deliberately constructed to establish a direct structure–property correlation. Compared with its crystalline counterpart, A‐Co ₃ S ₄ features a disordered atomic configuration with abundant coordination‐unsaturated sites and defect‐induced electronic states, enabling stronger polysulfides adsorption and accelerated catalytic conversion. When integrated onto a polypropylene separator, the A‐Co ₃ S ₄ ‐based interfacial layer effectively suppresses polysulfide migration, enhances interfacial charge transfer, and promotes ion transport kinetics. As a result, the A‐Co ₃ S ₄ @PP‐based cell delivers an initial capacity of 748 mAh g ⁻¹ at 1 C and maintains 537 mAh g ⁻¹ after 1000 cycles, corresponding to a low capacity decay rate of 0.02% per cycle. This work clarifies the critical role of crystallinity in polysulfide conversion and provides fundamental insights into the rational design of defect‐engineered catalytic interfaces for advanced LSBs.

Disordered dendrite growth and corrosion reactions of zinc negative electrodes remain critical challenges in aqueous zinc metal batteries. Regulating water states in shear-thickening non-Newtonian fluid electrolytes has emerged as a promising strategy to simultaneously suppress dendrite growth and corrosion for zinc negative electrodes. Herein, we design a multifunctional shear-thickening non-Newtonian fluid electrolyte, based on carboxymethyl cellulose and sulfonate silicon oxide nanoparticles, which addresses both issues through hierarchical regulation of water molecule states. Carboxymethyl cellulose converts free water into weakly bound water, thereby suppressing water-induced parasitic reactions. Concurrently, sulfonated SiO₂ nanoparticles form an integrated shear-thickening network with amylopectin and carboxymethyl cellulose while introducing abundant surface -SO₃⁻ groups that disrupt the strongly bound water layer at the zinc interface. This architecture enables localized mechanical stiffening at dendrite tips without compromising ionic conductivity. As a result, Zn | |Zn symmetric cells exhibit stable Zn plating/stripping for 900 h at 50 mA cm⁻² and 25 mAh cm⁻², and Zn | |I₂ pouch cells with a capacity of 1.5 Ah maintain stability over 200 cycles at 20 mA cm⁻². These findings offer a alternative pathway toward corrosion-resistant, mechanically adaptive aqueous and practical zinc pouch cells systems.

A molten-salt-mediated quenching strategy is reported for composition-invariant tuning of lattice strain in transition-metal sulfides. RuS ₂ catalysts with tunable tensile strain are synthesized to investigate the strain and HER activity relationship.