Physics

Abstract In recent years, halide perovskite quantum dot (PQD) solar cells have garnered more research interest, yet poor operational and environmental stability limit their commercialization. Herein, a robust all-perovskite low-dimensional (LD)/PQD heterojunction is proposed to address these issues. In particular, rationally designed 2D perovskite single crystals dissolved in optimized solvents are directly coated on the PQD matrix to drive spontaneous conformal LD prototype growth. Notably, this strategy features a heating-free procedure with negligible erosion characteristics. Benefiting from the well-matched energy-level alignment at the intimate heterojunction, interfacial charge extraction is synergistically promoted, while a defect-free 2D single-crystal layer suppresses humidity-induced degradation via effective encapsulation. With this engineered LD/PQD heterojunction, the optimized FAxCs1–xPbI3 PQD device delivers a champion efficiency of 17.6% (certified value of 16.98%), with 9-fold enhanced humidity stability versus that of the pure PQD analogue. This work provides a novel heterostructure construction paradigm and mechanistic guidance for improving the efficiency and environmental stability of PQD-based optoelectronic devices.

ABSTRACT The selective conversion of carbon dioxide (CO 2 ) into value‐added fuels and chemicals via photocatalysis is a promising route toward carbon neutrality. While conventional approaches have largely focused on thermodynamic and kinetic factors, recent advances highlight the crucial role of spin polarization in governing charge separation, intermediate stabilization, and C─C coupling pathways. This review summarizes advances over the past 5 years in understanding the role of spin polarization in photocatalytic CO 2 reduction, aiming to bridge photocatalysis with the broader field of spintronics and to guide the rational design of catalysts with enhanced selectivity toward high‐value multicarbon products. The fundamental mechanistic principle of spin polarization in photocatalytic CO 2 reduction is firstly presented, with emphasis on spin‐dependent reaction pathways. Subsequently, the influence of spin polarization on key reaction intermediates is discussed, highlighting how spin states regulate electronic structures, and reaction energetics. Building on these insights, material design strategies are systematically outlined, focusing on tailoring spin polarization to optimize electronic configurations, charge–spin dynamics, and catalytic performance. In addition, advanced characterization techniques for probing spin polarization in photocatalytic systems are also stated. Finally, current challenges and future research directions are critically discussed, providing guidance for the development of next‐generation spin‐engineered photocatalysts.

ABSTRACT Efficient alkaline hydrogen evolution reaction (HER) electrocatalysis requires simultaneously accelerating sluggish water dissociation and facile hydrogen desorption, yet integrating these kinetically incompatible steps within a single catalytic site remains fundamentally challenging. Here we report a hollow‐spherical multiphasic ruthenium (Ru)/TiO 2 /Ti 3 C 2 T x MXene heterostructure that spatially decouples the elementary HER steps through an interfacial hydrogen spillover mechanism. Through comprehensive in situ spectroscopic investigations and theoretical simulations, we demonstrate that the unconventional phase‐engineered architecture enables Ru sites to efficiently dissociate water, while the Ti 3 C 2 T x MXene surface serves as a thermodynamically favorable platform for hydrogen recombination and release. Importantly, an interfacial TiO 2 bridge acts as a relay medium that dramatically lowers the hydrogen‐transfer barrier between the distinct catalytic domains, thereby establishing a continuous dual‐site reaction pathway across the heterogeneous interfaces. Consequently, the optimized catalyst delivers an ultralow overpotential of 13 mV at 10 mA cm −2 , together with outstanding operational stability over 320 h. Moreover, the assembled anion‐exchange membrane water electrolyzer requires only 1.66 V to achieve a current density of 1 A cm −2 . This work establishes an interfacial relay strategy for regulating hydrogen spillover across heterogeneous catalytic phases and provides a general framework for constructing advanced electrocatalysts with spatially cooperative reaction pathways.

ABSTRACT Hard carbon stores lithium through mechanisms fundamentally distinct from those of graphite, offering a complementary charge‐storage pathway that can mitigate the kinetic limitations of conventional graphite anodes. Herein, we demonstrate that a physically blended graphite–hard carbon (G–HC) anode exhibits reciprocal kinetic rerouting, whereby the lithiation behaviors of graphite and hard carbon mutually regulate each other without chemical integration. In the blended electrode, the graphite staging plateau acts as an internal voltage buffer that activates polarization‐delayed lithium storage in hard carbon, while hard carbon alleviates the kinetic bottleneck associated with graphite stage‐I lithiation at high states of charge. Consequently, the optimized G–HC anode delivers a reversible capacity of ∼500 mAh g − 1 , a volumetric capacity of 695 mAh L − 1 , and excellent rate capability, retaining 351 mAh g − 1 at a 16‐fold higher current density. When coupled with an NCM811 cathode, the G–HC full cell achieves an energy density of 508 Wh kg − 1 and a power density of 3260 W kg − 1 , surpassing graphite‐based counterparts by 21.8% and 14%, respectively. These findings establish hard carbon as an active kinetic regulator rather than a simple capacity‐enhancing additive and highlight physical blending as an effective strategy for simultaneously achieving high energy and high power in lithium‐ion batteries.

ABSTRACT The design of energy materials that rely on ion transport is dominated by a diffusion‐first strategy: increase defect concentration, lower the average migration barrier, and improve microstructure. Although effective in many systems, this approach also creates disorder and spreads transport over many weak and dissipative pathways. Here we present a novel design strategy of state‐resonant transmission, in which transport is enhanced by organizing the transport landscape so that a number of highly effective channels dominate the realized flux. Using cation‐vacancy‐ordered alumina‐ceria oxide (ACO) as an architected fluorite model system and gadolinium‐doped ceria (GDC) as a diffusion‐dominated reference, we show that the ordered Ce‐Al‐Ov lattice in ACO transforms transport from broad diffusion‐like hopping into a more focused high‐flux regime. Relative to GDC, ACO exhibits contracted impedance, reduced dominant distribution of relaxation times (DRT) resistive burden, suppression of the long‐time dissipative tail, and consistently higher ionic conductivity. These results show that high transport depends not only on how many defects are introduced, but on how transport pathways are structurally organized and selectively amplified in a collective motion. This work establishes state‐resonant transmission as a practical design paradigm for next‐generation energy materials.

ABSTRACT Robust hydrogel‐elastomer integration is crucial for soft electronics and robotics but hindered by interfacial fragility. Here, we present a spatially confined in situ photopolymerization strategy to grow hydrogel coatings directly from polydimethylsiloxane (PDMS). By confining the active radicals within the solvent‐swollen elastomeric boundary, this strategy achieves a bottom‐up growth. Crucially, both experimental characterizations and molecular dynamics (MD) simulations reveal a hydrogen‐bond‐mediated discrete nucleation process during the coating formation. This localized pre‐organization serves as physical evidence of the bottom‐up growth, which constructs a dual‐anchoring interface featuring simultaneous covalent grafting and topological entanglement. The dual‐anchoring (DA) hydrogel coatings achieve high interfacial toughness, long‐term stability, and applicability to other elastomers. We further extend this protocol for fabricating patterned conductive hydrogel coatings with high‐resolution reproduction of micron‐scale features. Furthermore, it enables rapid in situ fabrication of thin‐film actuators with enhanced actuation performance. This strategy presents a convenient protocol for integrating advanced hydrogel functionalities into soft matter systems.

ABSTRACT Conventional interfacial polymerization is typically governed by rapid and disordered monomer diffusion, which limits precise regulation over through‐thickness structure and electrostatic distribution in polyamide nanofiltration membranes. Here, a reaction‐induced interfacial self‐assembly strategy is developed to regulate membrane growth dynamics and construct Janus polyamide membranes with directional ion‐transport behavior. By introducing 1,14‐dibromotetradecane into the piperazine/trimesoyl chloride interfacial polymerization system, amphiphilic quaternized intermediates are preferentially generated at the water/oil interface and reorganize the local reaction environment prior to continuous polyamide formation. This process transforms conventional diffusion‐dominated interfacial polymerization into an assembly‐regulated growth pathway, resulting in a selective layer with asymmetric through‐thickness chemistry, compact sub‐nanometer transport channels, and positively enriched bottom domains. The resulting membrane exhibits synergistic size‐sieving and localized Donnan exclusion effects for Mg 2+ /Li + separation, achieving a separation factor of 333.7 at a Mg 2+ /Li + mass ratio of 80 together with stable operation over 310 h. Molecular simulations further reveal that the asymmetric electrostatic architecture imposes substantially higher transmembrane free‐energy barriers for Mg 2+ than for Li + , thereby governing directional ion transport. This work demonstrates that transport functionality can be directly encoded during membrane formation through reaction‐field regulation, providing a feasible strategy for constructing asymmetric polyamide membranes with programmable ion‐transport properties.

ABSTRACT Filamentary wearable electronics require conductive filaments that are mechanically robust, structurally compliant, and compatible with textile integration, yet these attributes are rarely achieved simultaneously in bio‐based systems. Here, we report a collagen‐based conductive filament platform that converts native biological hierarchy into programmable wearable sensing. Collagen aggregates are used as spinnable mesoscale building units to form continuous filaments that preserve the load‐bearing advantage of the native aggregated state, yielding high tensile strength (316.2 ± 52.1 MPa) and modulus (4611.5 ± 187.8 MPa). MXene is then assembled onto the aggregate surface through rapid adsorption‐driven interfacial organization, generating a stable conductive sheath without sacrificing filament compliance. On this basis, a cucumber‐tendril‐inspired helical architecture redistributes strain through controlled untwisting, expanding the sensing window to 100% while maintaining reliable electromechanical response. The resulting helical filament exhibits stable multimodal sensing under tensile, bending, and torsional deformation, and remains functional after textile integration and wireless motion monitoring. In a complementary straight‐filament format, the same collagen@MXene platform also enables touch localization and dynamic tactile input. This work establishes a materials–interface–geometry design strategy for sustainable filamentary bioelectronics and intelligent textiles.

ABSTRACT Paper‐based sensors offer a sustainable platform for wearable electronics, yet their performance is fundamentally constrained by the intrinsic “contact‐jumping” behavior of hierarchical cellulose fibers, which causes abrupt conduction transitions, early current saturation, and an inevitable sensitivity–detection range trade‐off. Here, we introduce a stepwise conductivity‐gradient, open‐circuit‐triggered architecture that spatially reprograms pressure‐induced electron pathways within cellulose networks. By integrating in situ grown AgNPs on MXene‐modified fibers with a pressure‐activated MXene interdigitated electrode, the sensor enables cascaded pathway evolution that delays current saturation and establishes a progressively tunable piezoresistive response. Multiscale simulations and interfacial charge analyses reveal strain‐induced Ag–MXene polarization and charge delocalization, which expand available conduction channels and lower transport barriers. Benefiting from this gradient‐engineered mechanism, the sensor achieves an ultrahigh sensitivity of 1365.87 kPa −1 , a broad detection range of 0.7 Pa–203.2 kPa, a 0.7 Pa detection limit, and excellent durability over 10 000 cycles. The hierarchical network also affords strong EMI shielding and high breathability, enabling stable on‐skin operation and multifunctional sensing.

ABSTRACT The practical applications of porous piezoelectric ceramics have long been constrained by the intrinsic trade‐off between porosity and their piezoelectric and mechanical properties. Existing pore‐forming techniques, such as burnt‐out polymer spheres, still fail to achieve synergistic optimization of these properties. Here, we propose a self‐assembled pore engineering (SAP), which utilizes the density difference between reactants and products during chemical reactions to enable spontaneous pore formation. Benefiting from the synergy of SAP‐induced lattice softening, domain refinement, and significant residual stress, the fabricated porous bismuth layer‐structured Ca 0.94 Bi 4.06 Ti 4 O 15 (Bi‐CBT) ceramics with 30% porosity exhibit excellent comprehensive performance. The piezoelectric coefficient d 33 reaches 23.1 pC/N and shows a variation within ±15% over a broad temperature range of 25°C–525°C, while simultaneously possessing excellent compressive strength (558 MPa at 25°C, 276 MPa at 600°C) and low thermal conductivity (0.57 W m−1 K−1 at 25°C). More importantly, this method demonstrates broad universality across different material systems. Porous perovskite‐structured BaTiO 3 prepared via SAP achieves an ultrahigh effective electrostrictive coefficient Q eff of 0.32 m 4 /C 2 . These findings establish a versatile, low‐cost route for the scalable production of structural‐functional integrated ceramics.

ABSTRACT Interfacial modification is a widely adopted strategy for stabilizing zinc metal anodes in aqueous zinc‐ion batteries. However, most reported designs rely on strictly insoluble interphases, largely due to routine path dependence in the prevailing assumption that soluble modification layers would rapidly dissipate and lose functionality. Herein, a partially soluble zinc acetate surface modification is constructed via temperature‐controlled etching, enabling simultaneous regulation of the electrode interface and the electrolyte environment. Upon electrolyte immersion, the residual interphase homogenizes the interfacial electric field and mitigates surface corrosion, while released acetate anions which dynamically reconstruct the Zn 2+ solvation structure by partially displacing coordinated water molecules. This cooperative regulation promotes uniform Zn deposition while suppressing parasitic corrosion reactions on Zn anode. As a result, the zinc modified Zn anode delivers stable dendrite‐free plating/stripping for over 2000 h at 10 mA cm −2 and maintains reversible cycling under a 30% depth of discharge for 600 h. Full cells with an ammonium vanadate cathode exhibit a capacity retention of 67.8% after 1500 cycles at 5 A g −1 . This work demonstrates that controlled interphase solubility can be intentionally leveraged as a viable parameter for interface engineering in aqueous zinc batteries.

ABSTRACT Radiative cooling of vertical surfaces is constrained by the trade‐off between visible transparency and directional thermal emission. Existing asymmetric emitters suppress ground‐directed radiation but are opaque, preventing window integration. Here, we present a transparent asymmetric emitter (TAE) that resolves this limitation via a geometry‐mediated optical design. The TAE employs a microprism array featuring ground‐facing facets with partial silver coverage, enabling decoupled control of visible transmittance and mid‐infrared emissivity. Angle‐resolved measurements show high visible transmittance (75%) and strong anisotropic thermal response, with sky‐facing emissivity of 0.95 and near‐zero ground‐facing absorption. Controlled vacuum experiments demonstrate maximum temperature reductions of 26.4°C. Outdoor experiments using solar‐transmittance‐matched references confirm consistent cooling, with maximum temperature reductions of ∼10°C at ground temperatures of 31.5°C. A global energy model incorporating location‐specific, angle‐dependent optical properties and realistic ground temperatures is developed to capture radiative effects in vertical windows. The model predicts a latitude‐dependent trend, where energy savings are maximized in low‐latitude regions and gradually diminish toward higher latitudes. Notably, the TAE achieves energy performance comparable to the ideal limit of seasonal emissivity‐modulation technologies. As a scalable platform, the TAE establishes a viable route for integrating radiative cooling into windows without compromising daylighting.

ABSTRACT Ruthenium oxide (RuO 2 ) is a promising alternative to Ir‐based catalysts for the acidic oxygen evolution reaction (OER) owing to its high intrinsic activity, yet its practical application is hindered by rapid degradation under strongly oxidative acidic conditions. Herein, we report a dual rare‐earth co‐doping strategy to regulate Ru─O bonding through the synergistic coupling of strain and electronic effects. Incorporation of lanthanum (La) and neodymium (Nd) into the rutile RuO 2 lattice induces a 2.41% lattice expansion, resulting in elongated Ru─O bonds and weakened Ru─O covalency. These structural modifications suppress lattice oxygen activation and stabilize the oxide framework. Meanwhile, rare‐earth‐induced electronic modulation lowers the energy barrier for the *O to *OOH transition, steering OER toward a more stable adsorbate evolution mechanism (AEM) pathway. Consequently, LaNd‐RuO 2 achieves an overpotential of only 185 mV at 10 mA cm −2 in 0.5 M H 2 SO 4 and sustains stable operation for over 1200 h, significantly outperforming singly doped counterparts. A proton exchange membrane water electrolyzer employing LaNd‐RuO 2 as the anode catalyst requires only 1.81 V to reach 3 A cm −2 . This work offers an effective strategy for simultaneously enhancing the activity and durability of Ru‐based acidic OER catalysts.

ABSTRACT Bioinspired hydrogels are promising candidates for the development of multifunctional soft materials, yet the integration of anisotropic friction control, mechanical robustness, and piezoelectricity within a single material remains challenging. Here, a biomimetic hydrogel was successfully developed by incorporating lubricated piezoelectric short nanofibers, which were aligned through stretching and subsequently stabilized by ionic crosslinking to construct an anisotropic architecture. Benefiting from this design, the hydrogel simultaneously achieved high mechanical performance (strength about 42.9 MPa, toughness about 38.9 MJ·m −3 ). It also exhibited pronounced frictional anisotropy with the direction‐dependent lubrication behavior, where the friction coefficient was reduced to about 0.0087–0.0261 after incorporation of the multifunctional nanofibers, and maintained an ultralow friction coefficient (about 0.0097) throughout a continuous friction test for 3 h. Additionally, the fiber alignment enhanced the piezoelectric output by 2.3‐fold, increasing the voltage signal from about 256 mV in the unstretched state to about 600 mV under the same external excitation. Overall, this work established a simple yet effective strategy for engineering multifunctional hydrogels with coupled mechanical, anisotropic frictional, and electromechanical properties, broadening the design paradigm of bioinspired soft materials.

ABSTRACT Amino acid synthesis from nitrogen oxides (NO x ) represents a transformative frontier in sustainable C─N bond formation, converting abundant small molecules into value‐added chemicals under mild conditions. However, this process faces significant challenges due to the complex orchestration of multistep proton/electron transfers, intermediate stabilization, and selective coupling within complex reaction networks. Tandem catalysis emerges as a powerful strategy to overcome these limits by spatially integrating distinct catalytic functions for the sequential conversion of reactive intermediates. In this review, we situate NO x to amino acid synthesis within the broader landscape of chemical, microbial, and electrocatalytic routes, emphasizing the unique merits of tandem systems. It summarizes the evolution of tandem catalysts, electrodes and systems while dissecting fundamental mechanistic pathways that govern intermediates transformation. Particular emphasis is placed on rational materials engineering strategies, including alloying, defect engineering, metal‐support interactions, metal‐semiconductor coupling, and heterostructure construction, which together regulate intermediate adsorption, charge/proton transfer, and interfacial coupling kinetics. Finally, we identify persistent challenges in activity and selectivity, highlighting opportunities in operando characterization, multiscale theory, and artificial intelligence assisted discovery. By bridging fundamental mechanisms with advanced materials design, this work establishes a forward‐looking framework for efficient amino acid production via tandem catalysis.

ABSTRACT High‐capacity, large‐volume‐change anode materials offer attractive energy density but undergo pronounced volumetric swings during cycling, which can fracture the binder network, induce electrode cracking, and trigger sustained parasitic reactions and rapid capacity fade. This work reports an all‐aqueous, dual‐conductivity binder based on poly(vinyl alcohol) (PVA) and the organic mixed ionic/electronic conductor poly[3‐(potassium‐4‐butanoate)thiophene‐2,5‐diyl] (P3KBT), combined with freeze‐thaw (FT) processing to stabilize both the electrode framework and requisite interfacial interactions. FT cycles performed on the blend induce the formation of crystalline PVA domains, while P3KBT interacts with both PVA and the active material via physicochemical interactions. Collectively, these interactions create a percolated mixed ionic‐electronic conductive network. Using Fe 3 O 4 as a model high‐capacity anode active material, the PVA/P3KBT electrode delivers >96% capacity retention over 400 cycles, together with markedly enhanced adhesion, mechanical robustness, and rate capability relative to PVA controls. Cross‐sectional analysis shows that the post‐cycling thickness increase of FT‐treated electrodes (∼172%) is dramatically lower than that of non‐FT analogues (up to ∼362%), indicating more effective mitigation of pulverization and delamination. Surface characterization further reveals a more uniform, compact, and crack‐free surface for FT‐treated electrodes, consistent with suppressed side reactions and a stabilized electrode architecture.

ABSTRACT All‐inorganic perovskite solar cells are photovoltaic research hotspots due to their excellent thermal stability. To boost efficiency, ZnO is used as an electron transport material for its high mobility and energy level matching with inorganic perovskites. However, abundant surface defects on CsPbI 2 Br trigger undesirable interfacial reactions with ZnO, seriously limiting device performance and long‐term stability. Herein, a two‐birds‐with‐one‐stone interfacial modifier based on HTPT (4‐hydroxy‐6‐(trifluoromethyl)pyrimidine‐2‐thiol) is utilized. S, O, and N heteroatoms in HTPT passivate defects via multi‐site coordination, reducing reactive sites. The steric effect of CF 3 partially reduces direct contact between perovskite and ZnO, and various interfacial effects, including surface energy variation, interfacial dipole modulation, wettability, and hydrophobicity, jointly regulate the overall interface properties, constructing an effective strategy for suppressing interfacial interdiffusion and slowing interfacial degradation rates. Modified single‐junction p‐i‐n devices reach a record 17.34% efficiency with 1.32 V open‐circuit voltage and robust stability (T 80 = 864 h at 85°C, T 92 = 1000 h under maximum power point tracking (MPPT) at 30°C). P‐i‐n CsPbI 2 Br/PM6:eC9:PC61BM two‐terminal tandem cells were fabricated. The fabricated CsPbI 2 Br/organic tandem cells yield top efficiencies of 24.25% (0.08 cm 2 ) and 22.81% (1.02 cm 2 ) among p‐i‐n all‐inorganic perovskite/organic tandems and maintain decent thermal and MPPT stability.

ABSTRACT Organic electrochemical transistors (OECTs) are emerging as powerful biosensing platforms, offering high transduction efficiency, low‐voltage operation, and intrinsic compatibility with aqueous and physiological environments. Central to their recent progress is the strategic integration of biomaterials, which govern interfacial charge transfer, doping dynamics, and recognition specificity. A complete understanding of biomaterial‐enabled OECTs requires not only insights into intrinsic material chemistry but also interface engineering and device design principles that dictate signal transduction and reproducibility. In this review, we critically examine the full spectrum of biomaterials integrated into OECT biosensors (from natural macromolecules, such as proteins, nucleic acids, and polysaccharides to biocompatible polymers and synthetic engineered interfaces). Particular emphasis is placed on interfacial chemistries, including silanization and click reactions, that control receptor orientation, density, and long‐term stability. Beyond materials design, we discuss operating physics, signal transduction mechanisms, and device engineering strategies, thereby linking molecular‐scale chemistry with device‐level performance. By consolidating these interdisciplinary advances, we provide a timely roadmap for reproducible, scalable, and clinically relevant OECT biosensors. With growing demand for high‐performance and sustainable sensing platforms in precision medicine and environmental monitoring, this review highlights both key achievements and outstanding challenges that will shape the next generation of bioelectronic technologies.

ABSTRACT The increasing discharge of persistent organic dyes from industrial effluents into aquatic environments poses a serious threat to ecological systems and human health. It is essential to develop sustainable and efficient remediation technologies for the treatment. For this, we present a novel approach to green‐synthesized zinc oxide (ZnO) nanoparticles using turmeric extract as a reducing and passivating agent, followed by electrospinning for nanofiber synthesis. The integration of green‐synthesized ZnO nanoparticles with the PLA matrix as a catalyst yielded well‐defined morphologies and crystallinity, as confirmed through detailed characterization. The synthesized PLA‐ZnO nanofibers exhibited remarkable photocatalytic and piezocatalytic activities for the decolourization of anionic and cationic dyes under light and mechanical vibrations. In addition, nanofibers exhibited significant antibacterial properties against both Gram‐negative Escherichia coli (E. coli) and Gram‐positive Staphylococcus aureus (S. aureus). In our endeavor to understand the relationship between wavelength, time, and absorbance shown by PLA‐ZnO nanofibers in dye decolorization, among other variables, we studied the behavior of multiple machine learning (ML) models, including linear methods, decision‐tree‐based models, support vector regression (SVR), and a neural network regressor. Due to the exceptional efficacy of PLA‐ZnO nanofibers and ML predictions, it holds substantial promise for innovative applications in environmental remediation.

ABSTRACT Accelerating sulfur redox reaction (SRR) kinetics is important for suppressing the shuttle effect in Li–S batteries. While most efforts focus on optimizing lithium polysulfides (LiPSs) adsorption and conversion, the critical role of directional migration of Li + and polysulfide anions (S n 2− ) remains overlooked. Here, we report a 2D atomic Co‐decorated TiN/TiO 2 in‐plane heterostructure (Co‐TiN/TiO 2 ) that uniquely integrates highly catalytic Co single atoms, stabilized by strong metal–support interaction, with a heterointerface‐induced built‐in electric field (BIEF). Unlike conventional single‐atom catalysts or simple heterostructures, this design works like a “supply‐and‐removal” production line: the BIEF drives Li + toward the active sites for charge compensation while expelling S n 2− away, thereby mitigating the accumulation of LiPSs, which is consistent with the observed prevention of catalyst passivation and enhanced SRR kinetics. Consequently, the battery with Co‐TiN/TiO 2 catalyst delivers a high initial capacity of 1075 mAh g −1 at 1 C and remarkable cycling stability with a decay rate of only 0.05% per cycle over 1000 cycles. Even under high sulfur loading and lean electrolyte conditions, it maintains a high areal capacity of 4.7 mAh cm −2 and outstanding cycling performance. This work highlights the importance of coordinated ion management in designing high‐efficiency catalysts for Li–S batteries.

ABSTRACT Fe–N 4 centers are widely viewed as prospective sites for oxygen reduction reaction (ORR), yet improving their catalytic behavior through coordinated adjustments to structure and electronic properties remains difficult. Here, a C‐supported electrocatalyst with asymmetric Fe–Cu diatomic motifs is reported, in which a Fe atom bonded by S and N atoms couples with a neighboring Cu–N site (FeN 3 S–CuN 4 , denoted FeCu‐SNC). Operando spectroscopic characterizations and theoretical calculations show that stable adsorption of a hydroxyl (OH) intermediate on FeCu‐SNC produces a triply modulated Fe site with asymmetric coordination to S and Cu atoms, together with an additional hydroxyl intermediate during the catalytic process (FeCu─SN 5 –OH; the N 5 environment originates from the FeN 3 S moiety and the adjacent Cu site). This configuration generates an asymmetric surface charge distribution at the Fe center and weakens binding of reaction intermediates. Therefore, O 2 activation and conversion to the *OOH intermediate are promoted, accelerating ORR kinetics. FeCu‐SNC displays robust alkaline ORR kinetics, affording a half‐wave potential (E 1/2 ) of 0.914 V. When applied in rechargeable zinc–air batteries, it attains a maximum power output of 506 mW cm −2 . These results clarify how atomic‐ and electronic‐level modulation of heteronuclear Fe‐based diatomic sites can improve oxygen reduction catalysis.

ABSTRACT The low‑temperature application of aqueous potassium‑ion batteries is strictly limited by electrolyte freezing and unstable electrode/electrolyte interfaces. To address these challenges simultaneously, we propose a triple‑modulator electrolyte engineering strategy that introduces diethyl phosphoramidate (DEPA) as a molecular triple modulator. DEPA operates through three interconnected mechanisms. First, its ─NH 2 and ─P═O functional groups act as potent hydrogen‐bond disruptors that effectively dismantle the intrinsic tetrahedral ordering of water networks, thereby lowering the electrolyte freezing point to −40°C. Second, it actively participates in the K + solvation sheath and loosens the coordination environment, thereby lowering the desolvation energy barrier. Third, it guides the in‐situ formation of a robust, inorganic‐rich solid electrolyte interphase featuring a highly homogeneous organic‐inorganic hybrid architecture. The optimized electrolyte endows the full cell with exceptionally low‑temperature performance, delivering an initial reversible capacity of 63.1 mAh g −1 at 10 mA g −1 at −40°C. Moreover, a pouch cell with this electrolyte retains 83.2% of its initial capacity after 70 cycles at −40°C, demonstrating clear practical application potential. This work achieves synergistic “bulk‑interface” optimization through the rational design of intermolecular interactions, providing a viable molecular engineering paradigm for the development of low‐temperature‐tolerant aqueous batteries.

ABSTRACT By targeting the secondary building units (SBUs) within the metal–organic framework (MOF) structure, the polycrystalline PCN‐250 MOF membrane was modified through an in situ imidazole functionalization approach. This simple yet effective modification successfully reduced the pore size of the membrane. As a result, the imidazole‐functionalized PCN‐250 membrane achieved efficient separation of methanol‐containing mixtures, including methanol/ n ‐hexane, methanol/dimethyl carbonate, and methanol/toluene. Compared with conventional distillation, pervaporation using this membrane required only 33.4% of the energy to achieve optimal separation performance under identical operating conditions. In addition, the modified membrane achieved high flux while retaining the excellent acid resistance of the original PCN‐250 material, providing a performance advantage over other MOF membranes used in similar applications.

ABSTRACT Sodium layered transition‐metal (TM) oxides are considered promising cathode materials for sodium‐ion batteries owing to their high energy density. However, their practical application is severely hindered by detrimental phase transformations and irreversible oxygen redox at high voltages. Herein, we report a P2‐type layered oxide Na 0.67 Li 0.15 Co 0.15 Mn 0.6 Ti 0.1 O 2 (NLCMT) and decipher the dual‐functional role of Li in regulating both structural and electronic evolution. We demonstrate that electrochemically induced Li migration generates local coordination vacancies in the TM layers. These vacancies stabilize the layered framework through triggering the formation of a Na pillar‐like configuration, which effectively suppresses high‐voltage phase transitions and lattice strain accumulation. Meanwhile, the vacancy‐induced local environment enhances Co 3 d –O 2 p hybridization and facilitates adaptive ligand‐to‐metal charge transfer (LMCT). This process effectively redistributes oxygen hole density, preventing the localized accumulation of oxidized oxygen species and suppressing oxygen dimerization. Consequently, the NLCMT electrode delivers an exceptionally high discharge capacity of 197 mAh g −1 at 0.1C with remarkable reversibility. This work demonstrates an effective vacancy‐mediated strategy for developing highly reversible oxygen redox cathode materials.

ABSTRACT The efficency and stability of perovskite/organic tandem solar cells are fundamentally limited by two interconnected challenges in wide bandgap (WBG) perovskite top cells, namely high‐density surface defects and photo‐induced halide phase segregation. Both issues originate from anionic vacancies—specifically halogen vacancies—which act as shallow traps and serve as sites for ion migration, undermining device performance and stability. Herein, we demonstrate a novel ordered anion‐cation modification (OACM) approach—anionic vacancies are repaired before cation passivation. This order is determined by kinetic accessibility, where small and mobile Br − ions can easily diffuse into the lattice to fill vacancies. If a molecular passivation layer is deposited first (reversed sequence), a uniform barrier forms that blocks subsequent anion repair, significantly degrading device efficiency. By applying the OACM approach, we fabricated a 1.83 eV WBG perovskite solar cell that achieves an open‐circuit voltage of 1.33 V and a stabilized efficiency of 19.21%, while suppressing photo‐induced phase segregation. When integrated into perovskite/organic tandem devices, the stabilized top cell yields a champion efficiency of 26.20% with an improvement in storage stability. This work contributes to developing a sequence‐defined design principle for defect management in perovskite photovoltaics, transforming interface engineering from empirical trial‐and‐error into a rational, kinetically guided strategy.