Yongsheng Fu

Developing efficient and stable oxygen evolution reaction catalysts is crucial for practical water splitting. Herein, a mild room-temperature sulfidation strategy is employed to construct a hierarchical heterostructure composed of Fe-Co LDH nanoneedles and ultrathin Fe-CoSOH nanosheets on nickel foam. This nanoneedle-nanosheet architecture provides abundant active sites, optimized charge transfer pathways, and enhanced electrolyte wettability. Electrochemical tests show that the resulting catalyst exhibits excellent OER activity in 1.0 M KOH, requiring an overpotential of 230 mV to achieve a current density of 10 mA cm–2, with a Tafel slope of 35.37 mV dec–1. Notably, it maintains stable operation for over 600 h at a current density of 100 mA cm–2. Mechanism studies reveal that sulfur doping optimizes the electronic structure and promotes the reconstruction into the active CoOOH phase at a lower potential. Finite element simulations confirm that the hierarchical structure enhances the local electric field and reactant transport. This work provides an effective strategy for synergistically improving electrocatalytic performance through anion engineering and structural design.

High sulfur loading is essential for the practical application of lithium–sulfur (Li–S) batteries but is limited by severe polysulfide shuttling, large electrode volume changes, and sluggish Li ⁺ transport. Herein, a dual‐crosslinked binder (DCB) is constructed through hydrogen‐bonding and ionic‐pair interactions between quaternized soy protein isolate (QSPI) and poly (acrylic acid)‐based LA133. The 3D crosslinked network enhances electrode mechanical integrity and adhesion, effectively alleviating structural degradation and volume variation during cycling. Meanwhile, abundant polar functional groups provide continuous Li ⁺ coordination sites, and theoretical calculations reveal a hopping‐mediated Li ⁺ transport pathway between adjacent coordination sites, thereby promoting polysulfide conversion. As a result, the DCB simultaneously improves electrode stability and reaction kinetics. A 1.1 Ah Li–S pouch cell employing the DCB achieves a high energy density of 348 Wh kg ⁻¹ and stable cycling over 60 cycles under practical conditions with a low electrolyte/sulfur ratio of 4 µL mg _s ⁻¹ and a low N/P ratio of 1.5. This work offers an effective dual‐crosslinking strategy for regulating Li ⁺ transport and enhancing electrode stability toward practical high‐sulfur‐loading Li–S batteries.

Aqueous zinc‐ion batteries (AZIBs) have emerged as promising candidates for grid‐scale and wearable energy storage applications owing to their intrinsic safety, low cost, and high theoretical capacity of Zn anodes. However, their practical deployment remains severely constrained by the poor reversibility and structural instability of Zn anodes during cycling, which have conventionally been attributed to isolated electrochemical failures, such as dendrite growth and parasitic water‐induced side reactions. Increasing evidence reveals these degradations originate from a self‐amplifying electrochemical‐mechanical coupling process involving interfacial stress evolution. Nevertheless, a unified mechanics‐centered framework for understanding failure mechanisms in AZIBs is still lacking, while the secondary stress effects induced by mainstream modification strategies have been largely overlooked. In this review, we establish a comprehensive electrochemical‐mechanical coupling framework to systematically elucidate the multiple origins of interfacial stress, critically assess state‐of‐the‐art stress characterization techniques, and explicitly uncover the mechanical mismatch and secondary stress effects associated with widely adopted anode modification strategies. Furthermore, we reorganize stress‐regulation strategies according to the mitigation of residual, induced, and crystallization stresses, and discuss the key challenges and forward‐looking research directions, providing fundamental mechanistic insights for rational design of ultra‐stable Zn anodes to advance AZIB commercialization.

Lithium–sulfur batteries are severely limited by polysulfide shuttling and sluggish sulfur redox kinetics. Efficient catalysis in lithium–sulfur (Li–S) batteries requires not only intrinsically active catalyst materials but also catalytic interfaces with high structural exposure and electrochemical accessibility. Here, a few‐layer MoS ₂ –decorated MoO ₂ composite integrated with carbon nanotubes is developed as a functional separator coating with a high density of exposed catalytic heterointerfaces. In this composite, polar MoO ₂ strongly anchors lithium polysulfides, while highly dispersed few‐layer MoS ₂ nanoflakes provide abundant MoO ₂ –MoS ₂ heterointerfaces, accelerating polysulfide conversion. Meanwhile, the MoO ₂ –MoS ₂ junction provides balanced polysulfide adsorption and pronounced charge redistribution, thereby promoting the activation and subsequent conversion of reaction intermediates. Li ₂ S nucleation tests and in situ x‐ray diffraction further verify the accelerated kinetics of polysulfide conversion and the improved reversibility of Li ₂ S formation. As a result, Li–S cells deliver a high specific capacity of 1236 mAh g ⁻¹ at 0.2 C and retain 475 mAh g ⁻¹ after 1000 cycles at 1 C, highlighting the promise of constructing high‐density exposed catalytic heterointerfaces for high‐performance Li–S batteries.

Rechargeable magnesium batteries face instability and irregular deposition, which lead to dendritic growth, low Coulombic efficiency, and poor cycle life. In this study, we propose a perfluorinated asymmetric magnesium salt (Mg(PFBS) ₂ ) to regulate magnesium‐ion deposition and improve interfacial stability. The PFBS ^– anion tailors the solvation structure and optimizes the electric double layer (EDL), promoting Mg ²⁺ desolvation and suppressing solvent decomposition. Based on diffusion‐controlled theory, we introduce Damköhler (Da) and Wagner (Wa) numbers to elucidate the competition between electrochemical reaction kinetics and atomic/ionic diffusion governing Mg deposition behavior. Experimental and theoretical analyses indicate that PFBS ⁻ preferentially adsorbs on the Mg(002) plane, forming a Mg‐PFBS ⁻ interfacial layer that induces epitaxial growth dominated by Mg(002) orientation, significantly improving deposition uniformity. The strong electron‐withdrawing perfluorinated structure further enables preferential anion reduction, forming an inorganic‐rich, dense, and stable solid electrolyte interphase (SEI). Electrochemical measurements demonstrate that Mg||Mg symmetric cells maintain stable cycling for over 1800 h at 0.1 mA cm ⁻² and 0.05 mAh cm ⁻² , with an average Coulombic efficiency of 99.47%. Furthermore, Mg||Mo ₆ S ₈ full cells exhibit superior rate capability and long‐term cycling stability, retaining 88.6% capacity after 380 cycles at 1 C. This study offers an effective electrolyte design strategy high‐energy‐density and safe magnesium batteries.

The commercialization of aqueous zinc–metal batteries (AZMBs) is hindered by dendrite growth caused by uncontrolled Zn ²⁺ transport and side reactions involving water and anions. Here, an angstrom–scale confined ion sieve and accelerator is designed using unilamellar Ti _0.87 O ₂ nanosheets with atomic Ti vacancies (∼3.0 × 3.8 Å) and interlayer spacing (∼3.5 Å) to enable selective Zn ²⁺ (∼1.5 Å) transport while blocking H ₂ O (∼4.0 Å) and SO ₄ ²⁻ (∼5.9 Å). This design facilitates selective Zn ²⁺ ion transport with high flux and Zn/SO ₄ ²⁻ selectivity, effectively mitigating water–/anion–induced parasitic reactions at the Zn anode. Consequently, the Ti _0.87 O ₂ @Zn anode exhibits significantly suppressed dendrite growth and parasitic side reactions during repeated Zn plating/stripping, with stable cycle lives exceeding 5000 and 4000 h at 1 and 5 mA cm ⁻² , respectively. The Ah–level Ti _0.87 O ₂ @Zn//VO ₂ pouch cell retains 85.4% of its initial capacity after 300 cycles at 3 A g ⁻¹ . This strategy provides a promising interfacial design concept for improving the reversibility of aqueous Zn metal anodes and may inspire the rational design of confined ion–transport interphases for related aqueous battery systems.

Two‐dimensional (2D) nanofluidic membranes have shown great potential for precise ion transport control in osmotic energy conversion. However, relying solely on their intrinsic surface charge and size‐sieving effects is inadequate to achieve efficient selective ion transport and high energy conversion performance. Herein, we demonstrate a nano dot‐infused graphene oxide (GO) nanofluidic membrane to enhance ion permselectivity and unveil how the nano dot mediates selective cation transport. The incorporation of graphitic carbon nitride nano dots (CNNDs) introduces extra negative charges that enhance the ion selectivity of the 2D nanochannels, while the coordination interactions between Na ⁺ ions and nitrogen‐containing groups on CNNDs lower the energy barrier for Na ⁺ migration, facilitating highly efficient ion diffusion. When applied to osmotic energy generation, the GO/CNNDs membranes exhibit a remarkable cation selectivity coefficient of up to 0.95 and achieve an exceptional power density of 18.4 W m ⁻² under a 50‐fold NaCl concentration gradient, a 5.4‐fold enhancement compared to that of GO membranes. Notably, the membrane also exhibits excellent stable performance in practical complex environments and organic solvents. This work highlights the critical role of nano dots in accelerating cation transport and demonstrates the practical potential of GO/CNNDs membranes for efficient and durable osmotic energy harvesting.