Browse Articles

Engineering Metal‐Pocket Cooperativity in Single‐Atom COF Nanozymes for Selective Cascade Catalysis

ABSTRACT Nanozymes have emerged as robust and scalable alternatives to natural enzymes, offering high catalytic activity and structural stability. However, reproducing the exquisite selectivity of enzymatic catalysis, particularly their ability to operate with high precision in complex reaction systems, remains a central challenge. Herein, inspired by the heme–pocket architecture and cooperative regulation in cytochrome P450, we report a nanozyme multilevel programming strategy based on a single‐atom covalent organic framework (COF) platform constructed from heme‐like metal–porphyrin nodes and linkers bearing chiral amino‐acid residues, enabling selective editing of metal catalytic centers and enzyme‐mimetic pockets to control catalytic activity, chemoselectivity, and stereochemical outcomes. As a proof of concept, we employ a biomimetic chiral cascade that couples methanol dehydrogenase‐like alcohol oxidation with a chymopapain‑inspired asymmetric aldol reaction to probe and optimize metal–pocket cooperativity within the nanozyme. The programmed MnPor‐Pro‐based nanozyme delivers high product yields, excellent chemo‐ and stereoselectivity, and outstanding recyclability in the cascade reactions, indicating the effectiveness of this strategy. This work provides a rational design insight for engineering highly selective nanozymes capable of addressing complex, multistep transformations, significantly bridging the gap between artificial and natural enzymatic systems.

Local Atom Clusters Drive Supercritical Relaxor State in Lead‐Free Dielectrics for Giant Energy Storage

ABSTRACT Perovskite relaxor ferroelectrics have emerged as the leading capacitive energy‐storage materials in pulsed‐power electronics and integrated energy systems. However, conventional relaxor design strategies encounter a fundamental trade‐off, wherein increasing compositional complexity to suppress hysteresis typically weakens local polar strength, thereby hindering the simultaneous realization of ultrahigh recoverable energy density ( W rec ) and efficiency ( η ). Herein, we demonstrate that sublattice‐hierarchical local atom clustering provides an effective approach to overcoming this limitation. By combining strong A ‐site disorder with Mg/Hf‐rich nanoregions on B ‐site sublattices, we embed atomic clusters within a relaxor ferroelectric matrix to stabilize a supercritical relaxor state. Through neutron total scattering techniques and atomic‐resolution electron microscopy, we reveal that local atom clusters not only enhance lattice distortion to form ultrafine polar nanodomains but, more importantly, strengthen the local random field to enable strong and highly reversible polarization. As a result, the designed lead‐free ceramic achieves an ultrahigh W rec of 17.03 J cm −3 and an excellent η of 93.5%, resulting in a superior figure of merit up to 262. The fast‐discharging capability and robust stability against temperature, frequency, and cycling further evidence its strong application potential. These findings identify local atom clustering as a general and powerful approach for designing high‐performance dielectric ceramic capacitors.

Conformal Thermoreversible Gelatin‐Based Gel for High‐Fidelity Electrophysiological Recording and Acute Peripheral Nerve Interfacing

ABSTRACT Conformal and tissue‐adaptive bioelectronic interfacing remains a challenge for electrophysiological recording and nerve stimulation, particularly on irregular or hair‐covered surfaces where conventional electrodes fail to maintain intimate, low‐impedance contact. Here, we report a thermoreversible gelatin‐based gel that transitions from a flowable precursor to a conformal conductive interface layer upon cooling, enabling both in situ formation on skin and use as a preformed compliant interlayer between metal electrodes and neural tissue. The gel integrates a uniformly dispersed carbon nanotube network with mobile ions from sodium chloride to support coexisting ionic and electronic transport pathways, while the gelatin‐based matrix provides moisture retention and mechanical compliance. It achieves low interface impedance on hairless and hairy skin, outperforming commercial electrocardiogram gels, and electroencephalogram pastes. The gel's versatility is demonstrated across multiple modalities and species, including electrocardiography and acute peripheral nerve stimulation in rats, compound muscle action potential and sensory nerve action potential recordings in rhesus monkeys, and electroencephalography in humans. Beyond these cross‐sectional assessments, repeated short‐term recordings using the gel enable longitudinal evaluation of peripheral nerve functional recovery in nerve injury models. Together, this work establishes a tissue‐adaptive and reconfigurable strategy for achieving stable, low‐impedance bioelectronic interfacing across complex biological environments.

Innovative and Multidisciplinary Research of Materials Science at Fudan University

Extreme Bond Ionicity in Mg─Te Chalcogenides for Ultrathin Low Voltage Selector‐Only Memory beyond the Leakage Scaling Limit

ABSTRACT Conventional ovonic threshold switching (OTS) chalcogenides face a fundamental scaling limit for selector‐only memory (SOM), because aggressive thickness scaling increases leakage current and hinders reliable low voltage operation. Here, this trade‐off can be overcome by exploiting the unique materials characteristics of the Mg─Te chalcogenide system. Guided by the bonding ionicity map and supported by density functional theory calculations, Mg─Te is identified as an optimal telluride material whose highly ionic bonding is associated with deeper trap levels, a large memory window of 1.75 V, and suppressed leakage in 20 nm devices. Structural analyses and multiscale simulations suggest that the spontaneous phase separation in Mg 1 Te 3 forms MgTe‐like ordered nanodomains and Te‐rich amorphous regions, providing structural partitioning that may constrain the effective amorphous switching network and reduce stochastic switching variability. With a thin Hf interlayer, the 5 nm Mg 1 Te 3 device achieves narrow SET/RESET switching uniformity of σ  = 15/28 mV at ± 2.5 V operating voltage, representative 10 ns programming speed, and write endurance exceeding 10 10 cycles in the best‐performing device. These results highlight Mg─Te as a promising basis for highly scaled ultralow voltage SOM through the combined roles of ionic bonding, structural partitioning, and interfacial engineering.

Single‐Cell Metabolic Activity Monitoring With Microcavity Laser Emitting Cytometry

ABSTRACT Single‐cell metabolism analysis is essential for understanding cellular heterogeneity. However, the ability to track it in real time, with high precision and under physiological conditions, remains a formidable challenge. Here, we introduce a microcavity laser‐emitting cytometry for single‐cell metabolism analysis. Single cells and the biocompatible gain medium resazurin were co‐encapsulated into droplets via a microfluidic device. These droplets then flowed into the Fabry‐Pérot (F‐P) cavity, resulting in a 15‐fold reduction in the laser pump energy, effectively alleviating phototoxicity. Capitalizing on cavity‐enhanced light‐matter interactions and ultra‐narrow laser linewidths, subtle changes in resazurin concentration resulting from metabolic activity induced redox reactions within cells were transduced into quantifiable, ultra‐sensitive shifts in the lasing wavelength. This approach achieved a sensitivity of 0.382 nM per 10 pm shift. Hence, our single‐cell laser emitter enabled the quantitative characterization of metabolic kinetics at the single‐cell level, facilitating applications in cytometry for metabolic heterogeneity analysis, cell‐type discrimination, and drug efficacy quantification. This platform enables single‐cell laser emission for cell screening and pharmacological evaluation, advancing research in areas like cancer treatment and drug discovery.

Geometric Complementarity and Electrostatic Fluctuation Control in Dual‐Asymmetric Acceptors for Efficient Organic Solar Cells

ABSTRACT Asymmetric molecular design has emerged as an effective strategy for developing high‐performance acceptors for organic solar cells (OSCs). Here, we introduce a dual‐asymmetric topology strategy, in which the stereochemical configurations of both the central core and terminal groups are co‐engineered. Using this approach, we synthesized an isomeric pair, Th2Cl‐a‐2Cl and Th2Cl‐b‐2Cl and benchmarked them against the singly asymmetric a‐CH‐Th2Cl and Th2Cl‐4Cl. We find that the distinctive steric conformation of Th2Cl‐a‐2Cl promotes a geometrically complementary, interlocked packing motif within the crystal lattice. This not only reinforces the three‐dimensional network connectivity but, more importantly, gives rise to a more uniform local electrostatic environment at the molecular‐skeleton scale. As a result, Th2Cl‐a‐2Cl exhibits weaker and more balanced environment‐induced electrostatic fluctuations along the backbone, which helps reduce local electrostatic perturbations during charge transport. Consequently, PM6:Th2Cl‐a‐2Cl devices deliver a champion PCE of 20.18% with a high fill factor (FF) of 80.88%, while significantly suppressing the non‐radiative recombination loss (Δ E 3 ) to 0.190 eV. These results establish geometric complementarity and electrostatic homogeneity, achieved through topological engineering, as an effective route to improve the efficiency of OSCs.

Pathways to High‐Efficiency Perovskite‐Organic Tandem Solar Cells

ABSTRACT Perovskite‐organic tandem solar cells (POTSCs) have emerged as a promising strategy to transcend the thermodynamic Shockley–Queisser limit of single‐junction devices. This architecture uniquely combines the exceptional tunability of wide‐bandgap (WBG) perovskite front cells with narrow‐bandgap (NBG) organic rear cells. In this review, we systematically examine the critical challenges and advancements in POTSCs. For the WBG perovskite subcells, we focus on composition engineering for precise bandgap tuning, the underlying thermodynamic and kinetic mechanisms of phase segregation, energy loss pathways resulting from non‐radiative recombination, and interface regulation strategies. Regarding the organic subcells, we highlight the necessity of exact bandgap matching and summarize molecular design strategies aimed at developing highly efficient NBG materials. Finally, we discuss the tandem architecture potential for achieving high power conversion efficiencies and synergistic stability. In this synergistic configuration, the WBG perovskite layer acts as a natural UV filter to protect the organic materials from high‐energy photons, while the moisture‐insensitive organic layer provides a barrier to shield the perovskite from water and oxygen erosion. By dissecting these key aspects, this review aims to provide a comprehensive roadmap for propelling POTSC efficiencies beyond the 30% milestone.

Cilia‐Structured Lipiodol Droplets Enable Long‐Term Transarterial Embolization Therapy by Nano‐Interlocking Adhesion

ABSTRACT Transarterial embolization (TAE) offers an effective and minimally invasive therapy for unresectable hepatocellular carcinoma (HCC), one of the most lethal malignancies globally, but being limited by short‐term embolization failure for example recanalization due to weak interfacial adhesion. Herein, we report cilia‐structured lipiodol (CS‐lipiodol) droplets by self‐assembling dual‐asymmetric microparticles with hydrophilic cilia‐structured hemispheres and hydrophobic plain hemispheres at the lipiodol–water interface, enabling long‐term TAE therapy by the cilia‐mediated nano‐interlocking effect. CS‐lipiodol droplets exhibit strong interfacial adhesion and viscoelastic deformability through the nano‐interlocking effect and the Pickering‐like architecture, allowing tight and efficient occlusion across multiple in vitro embolization models. The enhanced interfacial adhesion to vascular cells and adjacent droplets confers long‐term vascular occlusion and approximately three‐fold higher in vivo embolization rates than commercial embolic agents. In the orthotopic rabbit HCC model, purely physical occlusion with CS‐lipiodol droplets induced superior tumor volume reduction. Our study provides a healthcare material platform for long‐term and vascular‐adaptive TAE therapy.

Pressure‐Resilient Electron‐Ion Networks via Multifunctional Carbon Conductive Agents for High‐Rate Solid‐State Batteries

ABSTRACT Silicon‐based all‐solid‐state batteries (ASSBs) promise high safety and energy density, yet their rate capability remains fundamentally constrained by the disruption of continuous electron‐ion transport networks induced by large volume variations. Herein, we introduce a pressure‐resilient electron‐ion network enabled by a molten‐salt‐mediated multifunctional carbon conductive agent featuring a graphene‐like stacked framework with uniformly distributed nanopores. This architecture enables synergistic electron‐ion transport (with electronic and ionic conductivities of 133.26 S cm −1 and 1.89 mS cm −1 ), accommodates large deformation (up to 91.3% strain) without structural failure and retains high elasticity under a compressive strain of 80.6%. Operando expansion and kinetic analysis reveal that the elastic network dynamically adapts to silicon volume changes, preserving interfacial integrity and continuous transport pathways. As a result, the composite silicon anode delivers high capacity of 1672.2 mA h g −1 at 3C with 76.5% retention over 300 cycles, and notably sustains 1030.0 mA h g −1 at 3C even under 20 MPa. In full cells, it achieves 76.8 mA h g −1 at 3C under 20 MPa, 2.7 times higher than those based on pristine silicon anodes. Beyond silicon, this strategy can extend to other alloy‐type anodes (e.g., Sn), offering a general paradigm for constructing pressure‐resilient electron‐ion networks toward high‐rate ASSBs.

Superelastic Subcrystalline Rare‐Earth Ceramic Nanofiber Aerogels Enable 1300°C‐Stable Upconversion Luminescence

ABSTRACT Real‐time noncontact temperature detection is critical for the reliable operation of specialized robots in extreme thermodynamic environments. Upconversion (UC) luminescent materials, owing to their temperature‐sensitive emission, offer a promising solution. However, traditional UC crystals are fundamentally limited by both severe thermal quenching above 250°C and intrinsic brittleness. Here, we break these barriers by developing a subcrystalline upconversion ceramic nanofiber aerogel through an interfacial phonon engineering strategy. Our approach embeds active rare‐earth nanocrystals within an amorphous alumina matrix, creating a tensile‐strained heterointerface that softens local phonon modes and efficiently scatters high‐frequency vibrations. This unique “phonon cage” architecture suppresses nonradiative decay pathways, enabling stable UC emission at the unprecedented temperature of 1300°C. Furthermore, the subcrystalline structure induces a higher‐order sinusoidal buckling behavior, endowing the aerogel with thermomechanical superelasticity. The aerogel fully recovers from 95% compressive strain and survives over 1000 fatigue cycles, retaining >80% of its elasticity after 100 rigorous compression cycles under 1300°C thermal load. This work paves the way for noncontact thermal sensing in extreme environments.

Multiresonant Membrane Metasurfaces for Multifunctional Molecular Absorption Sensing and Real Time Biochemical Tracking

ABSTRACT Label‐free identification and real time tracking of biochemical substances became critical for molecular diagnostics and chemical analysis, yet conventional resonant terahertz (THz) metasurface sensing relies on a single resonance, limiting spectral selectivity and dynamic capability. Here, we suggest multiresonant membrane metasurfaces and employ them for simultaneous static characteristic absorption detection and dynamic reaction monitoring within a single pixel. We consider a membrane metasurface supporting multiple quasi‐bound states in the continuum designed at target frequencies and enabling the tailoring of the field enhancement and frequency‐selective interaction with target analytes. As a proof‐of‐concept, we achieve label‐free detection of the characteristic absorption features of pefloxacin at 0.78 and 0.99 THz, and real time tracking of vitamin C oxidation and denaturation under ambient conditions. The kinetic profiles extracted from the THz amplitude evolution show excellent agreement with nonlinear reaction models (R 2 > 0.92), demonstrating quantitative biochemical tracking capabilities. Our results establish a versatile and scalable THz photonic platform that unifies static molecule identification and dynamic reaction monitoring, paving the way toward integrated on‐chip biochemical analytics and multifunctional metasurface sensors.

Targeting Nonclassical Monocytes via Artificial Cell‐Microneedles for Precision Psoriasis Therapy

ABSTRACT Current therapies for inflammatory skin diseases predominantly rely on broad systemic immunosuppression and lack precision toward defined immune‐cell subsets. Here, we identify CX3CR1 + nonclassical monocytes (NCMs) as an inflammatory monocyte subset that contributes to the amplification of psoriasiform inflammation, as supported by integrated analyses of human single‐cell transcriptomics, genetic depletion, and adoptive‐transfer models. To preferentially engage these disease‐associated NCMs, we engineer an artificial cell–microneedle platform, termed CX3@GUV‐DMF, comprising CX3CL1‐functionalized, drug‐loaded giant unilamellar vesicles (GUVs) embedded within a dissolvable hyaluronic acid (HA) microneedle array. Following intradermal insertion, surface‐presented CX3CL1 actively navigates GUVs to pathogenic CX3CR1 + NCMs, facilitating the targeted, sustained release of the loaded drug. In vivo evaluations and transcriptomic profiling demonstrate that this localized immunomodulatory strategy attenuates inflammatory myeloid activation, neutrophil infiltration, and Th17‐associated responses while promoting restoration of epidermal barrier‐associated programs. These findings establish a materials‐enabled strategy for subset‐oriented immune modulation and local inflammatory‐niche remodeling, advancing inflammatory skin therapy beyond nonspecific immunosuppression.

Programming of Complex Magnetic Profiles Enforced by 4D Printed Magnetic LCE Actuators

ABSTRACT Magnetic soft actuators enable untethered, contact‐free actuation yet they are fundamentally limited by the difficulty of programming complex, three‐dimensional (3D), spatially non‐uniform magnetic profiles. Here, we introduce a four‐dimensional (4D) printing‐enabled magnetic programming strategy that overcomes this challenge by magnetizing magnetically active liquid crystal elastomers (MLCEs) in thermally actuated target states. Digitally prescribed director architectures define deterministic 3D deformations at elevated temperature, which serve as intrinsic programming templates during magnetization under a spatially uniform magnetic field. Upon cooling, relaxation of the thermomechanical deformation transforms the initially uniform magnetization into a complex, spatially varying magnetic profile that encodes the target shape as a magnetically favoured configuration. This approach enables the recovery of thermally defined shapes at room temperature under low magnetic fields and allows bidirectional and multistate actuation via simple reversal of field direction. By integrating spatial magnetic programming with controlled geometric asymmetry, we demonstrate frequency‐tunable linear locomotion and chirality‐encoded clockwise or anticlockwise rotational motion in multimaterial soft robotic architectures. This strategy decouples magnetic profile complexity from magnetization hardware, providing a scalable, template‐free route to fully 3D magnetic programming for soft robotics and untethered actuators operating under low‐field conditions.

Review of Inorganic Separator Engineering for Next‐Generation Lithium–Sulfur Batteries: Compromise or Cornerstone?

ABSTRACT Lithium–sulfur (Li–S) batteries are promising next‐generation energy‐storage systems, but their practical application remains limited by polysulfide shuttling, sluggish redox kinetics, and interfacial instability. Separator engineering offers an effective route to regulate sulfur chemistry. This review summarizes metal compound‐based separators as active interfacial architectures that promote polysulfide adsorption and catalytic conversion while regulating ion and electron transport. To evaluate diverse separator systems, we propose a Practical Relevance Index (PRI)‐guided framework that integrates intrinsic electrochemical improvements with system‐level constraints. A localized figure of merit is further introduced to interpret performance trends without direct cross‐study ranking. Recent advances in metal oxides, sulfides, nitrides, carbides, and MXene‐based separators are discussed, with emphasis on heterostructures, defect engineering, electronic‐structure regulation, and atomic‐scale design. Particular attention is given to constraint‐aware strategies that connect interfacial chemistry with practical energy density. Finally, major challenges and future directions are outlined, including reaction‐pathway regulation, operando characterization, system integration, and scalable manufacturing. This review provides a unified framework for designing practical, high‐energy‐density Li–S batteries.

Vacuum‐Based Monolithically In Situ Integration of Quantum‐Confined CsPbBr ₃ Nanocrystals for Spectrally Stable Blue Electroluminescence

ABSTRACT Spectrally stable blue emission represents one of the most critical components of full‐color perovskite displays, which are highly attractive for display technologies. However, vapor‐deposited blue perovskite light‐emitting diodes have so far relied predominantly on Br/Cl mixed‐halide bandgap engineering, which is prone to halide migration and phase segregation under operation and therefore suffers from spectral instability. Here, we report spectrally stable vapor‐deposited, pure‐bromide blue perovskite light‐emitting diodes with spectrally stable emission achieved via a ligand‐buffered delayed nucleation (LBDN) strategy. In this method, p‐Br‐MBABr is co‐deposited as a kinetic buffer to create a ligand‐coordinated precursor state that suppresses immediate crystallization, delays nucleation, and confines subsequent crystal growth. As a result, we obtain quantum‐confined CsPbBr 3 nanocrystal films with tunable blue emission. Fully vapor‐deposited PeLEDs based on these films deliver spectrally stable pure‐blue electroluminescence. These results establish kinetic buffering as an effective route to quantum‐confined perovskites under vapor deposition and spectrally stable blue emitters for monolithically integrated full‐color perovskite displays.

Ultra‐broadband Epsilon‐Near‐Zero Ultrathin Metafilms Assembled by 2D Nanosheets Overcoming Size Limitation in Metamaterials

ABSTRACT Broadband epsilon‐near‐zero (ENZ) materials are crucial for 6G (sixth generation mobile networks) signal stability, biochemical sensor accuracy, and intelligent weapon systems. Here, the ultrathin ( d ∼10 µm) 2D metafilms achieving low‐frequency ultra‐broadband ENZ (10 kHz–1 MHz, d / λ ∼10 −10 ) are constructed via the self‐assembly of nanosheets (MXene and graphene oxide) and interface engineering. High‐resistance interfaces and wrinkles can block free carriers, suppressing long‐range plasma and Drude‐type negative dielectric response, while these carriers tend to accumulate locally at the interfaces and enhance Debye‐type positive dielectric response. These two pathways achieve the ultra‐broadband ENZ behavior via the synergistic cancellation effect between these two responses with comparable intensity and dispersion characteristics. The ENZ (|ε′|<1) with a 100‐fold ultrabroad bandwidth (10 kHz–1 MHz) is obtained, 10 kHz of ENZ also updates the low‐frequency limit of ENZ in materials. Besides, the thickness of 10 µm is achieved in metafilms, a smallest d / λ value (∼10 −10 ), overcoming the size limitation of ENZ media. The effectiveness of the ultra‐broadband ENZ is verified in electromagnetic tunneling devices, where metafilms can replace complex artificial arrays. This work establishes a new material‐genesis strategy for ultra‐broadband ENZ rather than artificial metamaterial arrays, easily applicable across the entire electromagnetic spectra.

Oxygen‐Vacancy Engineering of Na ₄ Fe ₃ (PO ₄ ) ₂ P ₂ O ₇ Enables Fast and Wide‐Temperature Sodium Storage

ABSTRACT The polyanionic cathode Na 4 Fe 3 (PO 4 ) 2 P 2 O 7 (NFPP) is regarded as a promising cathode for sodium‐ion batteries owing to its low cost, intrinsic safety, and robust framework stability. However, the strongly localized electronic structure and sluggish Na + transport kinetics impose coupled limitations on its rate capability and stability. Herein, we demonstrate a defect‐engineering strategy to activate coupled electronic‐ionic transport through the rational introduction of oxygen vacancies into NFPP. Combined experimental investigations and density functional theory calculations reveal that oxygen vacancies act as dual‐functional kinetic regulators by simultaneously reconstructing the local Fe–O electronic environment and facilitating Na + migration. The defect‐induced electronic redistribution narrows the bandgap and accelerates electron transport (over 7 times), while expanded Na + diffusion pathways and reduced migration energy barriers enable rapid ion diffusion (over 6 times). Consequently, the oxygen vacancy‐enriched NFPP cathode delivers exceptional cycling stability with 90.46% capacity retention after 7000 cycles at an ultra‐high rate of 20 C. This work establishes oxygen‐vacancy engineering as an effective strategy for coupled transport regulation in polyanionic cathodes and provides fundamental insights into defect‐mediated kinetic enhancement for advanced sodium‐ion batteries.

Fluorine‐Rich Double‐Network Interfacial Layer Enabling Dynamic Interphase Reconstruction for High‐Capacity Zinc Metal Batteries

ABSTRACT Developing large‐scale, dendrite‐free zinc (Zn) anodes is pivotal for the practical deployment of aqueous Zn‐metal batteries (AZMBs), yet maintaining interfacial stability under high‐areal‐capacity conditions remains challenging. Here, we report an adaptive artificial solid‐electrolyte interphase (ASEI) based on a single‐ion‐conducting fluorine‐rich double network (SFDN) that enables in situ dynamic reconstruction of the Zn/electrolyte interphase. The SFDN, comprising an Al(OR) 4 − ‐based (R = −CH 2 −(CF 2 ) 7 −CH 2 −) dynamic crosslinked network integrated within PVDF‐HFP matrix, delivers a high Zn 2+ transference number (0.78) and hydrophobic/zincophilic properties. During cycling, residual monomers within the SFDN fulfill a dual‐functional role: coordinating with Zn 2+ to establish a dynamic Zn(OR) 2 − ‐based network while undergoing sacrificial decomposition to form a robust ZnF 2 ‐rich inner SEI. This evolution yields a multilayered architecture that effectively suppresses water‐induced side reactions, homogenizes Zn 2+ flux, and provides self‐healing. Consequently, the SFDN@Zn anode achieves an extraordinary lifespan of over 4,000 h at 10 mA cm − 2 /10 mAh cm − 2 , and a high average Coulombic Efficiency of 99.9% at 5 mA cm − 2 . Furthermore, a ∼900 mAh Zn||I 2 pouch cell achieves a high energy density of 196 Wh kg − 1 with 97.8% capacity retention over 300 cycles. This work presents a dynamic self‐adaptive interphase engineering, offering fundamental insights into Zn‐anode stabilization, and extending to other metal‐based battery systems.

Dual Modulation of Interfacial Water Structure and Metal‐Support Interaction via Single‐Atom Sites for Industrial Hydrogen Evolution

ABSTRACT Ru‐based catalysts are promising cathodes for alkaline hydrogen evolution reaction (HER) in anion exchange membrane water electrolysis (AEMWE), yet sluggish water dissociation, overly strong Ru─H adsorption, and durability loss still limit their practical performance. Herein, we construct a controlled M─N─C (M═Fe, Co, Ni) support series for anchoring Ru particles and establish a dual‐regulation strategy that couples interfacial water activation with support‐induced Ru electronic optimization. M─N 4 coordination motifs mainly regulate the near‐surface water environment and promote water‐dissociation kinetics, while the M─N─C supports modulate the electronic structure of Ru through metal‐support interaction. The optimized Ru/Ni─N─C delivers an ultralow overpotential of 9 mV at 10 mA cm −2 and achieves 4000 mA cm −2 at 2.0 V in a practical AEMWE, with an apparent voltage increase rate of 3.1 µV h −1 over 1600 h. In situ Raman and infrared spectroscopies reveal that Ni─N 4 motifs enrich and polarize interfacial K + ‐H 2 O species, facilitating the Volmer step. Theoretical calculations further show that Ni─N 4 lowers the water dissociation barrier to 0.19 eV, while the Ni─N─C support optimizes Ru─H adsorption to −0.07 eV through metal‐support interaction. This work provides mechanistic guidance for designing efficient Ru‐based alkaline HER catalysts by integrating water‐structure regulation with support‐mediated Ru electronic modulation.