Composite solid-state electrolytes (CSEs) for lithium metal batteries (LMBs) are considered one of the most promising electrolytes due to the combination of high ionic conductivity from inorganic fillers and flexibility from the polymer matrix. However, low ionic conductivity and poor interfacial stability have hindered the further development of CSEs. Herein, a Li-doping strategy is employed to introduce Li+ into the lattice of hollow multi-shell (HoMS) Fe2O3 microspheres, yielding a functionalized Li50-Fe2O3 filler. This structure not only provides rapid diffusion channels for Li+ but also enhances the anchoring of anions (e.g. TFSI-) on the surface due to the accompanying oxygen vacancies and the mixed Fe2+/Fe3+ valence states, which promote LiTFSI dissociation. By incorporating Li50-Fe2O3 into the poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) matrix, a CSE (PLiFe) with high ionic conductivity is fabricated. The PLiFe achieves a Li+ transference number of 0.50 and an ionic conductivity of 1.07 mS cm-1. Additionally, the PLiFe induces the formation of a dual-layer SEI structure at the Li metal interface with an inorganic-rich inner layer and an organic-rich outer layer, which significantly enhances the interfacial stability. The assembled NCM811|PLiFe|Li battery retains 75% of its capacity after 200 cycles at 1 C. This study provides a novel approach for the design of CSEs with enhanced ionic conductivity and interfacial stability through ion-doping-induced tuning of HoMS structures.

Constructing vertically aligned, penetrating metal-organic framework (MOFs) gas transfer pathways within mixed matrix membranes (MMMs) is an effective strategy for optimizing gas transport under low filler loading (<= 25 wt.%). Herein, we developed a novel "stack-polymerize-section" process to construct vertically aligned ZIF-8 pathways in MMMs by tailoring the density and channel size of PAN@ZIF-8 NFM for optimizing CO2 ultrafast and in-parallel transport. The designed XLPEO/PAN@ZIF-8 MMM exhibits excellent performance far exceeding the 2019 McKeown upper bound, with CO2 permeability and CO2/N2 selectivity of 369.2 Barrer and 90.0, respectively. Meanwhile, a novel parallel computational model that synergistically integrates the Maxwell model with resistance-based (RB) model methodology was proposed to introduce the interfacial resistance coefficient derived from polymer-MOFs interface heterogeneous concentration gradients. This work demonstrates the potential of vertically aligned MOFs channels for high-performance gas separation, providing a scalable and controllable fabrication pathway for maximizing the efficiency of MOFs in membrane technology.

Saline droplet evaporation constitutes a fundamental physicochemical phenomenon with critical applications in separation technologies, desalination processes, and crystal engineering. This investigation elucidates circulation mechanisms during saline droplet evaporation through systematic examination of various geometrical configurations and thermal conditions. A computational fluid dynamics approach validated through optical visualization and infrared thermal imaging revealed distinct circulation regimes governed by the interplay between Rayleigh convection and Marangoni effects. At ambient conditions, droplets exhibited predominantly Rayleighdriven convection, with contact angles below 90 degrees generating peripheral deposition patterns while angles exceeding 90 degrees produced centralized crystal accumulation due to non-uniform evaporation flux distribution. Temperature modulation induced substantial flow pattern transitions at specific critical thresholds, with thermal Marangoni effects overriding Rayleigh convection when temperature differences exceeded 0.94 K for droplets with 120 degrees contact angles. Circulation transitions manifested more prominently in droplets with larger contact angles, characterized by progressive transformation from Rayleigh-driven clockwise flows to thermal Marangonidriven counterclockwise patterns. Interfacial heat transfer coefficients exhibited deterministic influence on circulation dominance, with values below 10 W/m2 & sdot;K maintaining Rayleigh-dominated flow and values between 100-1000 W/m2 & sdot;K establishing thermal Marangoni dominance. A comprehensive phase diagram correlating dimensionless Rayleigh and Marangoni numbers to circulation patterns was developed, providing predictive capability for flow regime transitions under varying evaporation conditions. The established quantitative relationships between thermal parameters and circulation mechanisms enable precise control of crystal deposition morphologies through interfacial thermal regulation.

2D layered double hydroxide (LDH) composite membrane in gas separation was limited by insufficient orientation control accuracy and interface incompatibility with the organic substrate. In this study, we proposed a molecular-level channel engineering strategy to construct an LDH composite membrane by synergistically integrating vertical orientation, interlayer ion intercalation, and surface chemisorption sites. Specifically, LDH was induced hydrothermally to grow vertically along the (003) crystal plane on hydrophilic HPAN substrate, forming straight-through transfer channels with low tortuosity. Furthermore, the interlayer spacing was precisely adjusted to 0.306 nm by Cl- intercalation instead of CO32- to sieve H-2 and CO2. Concurrently, polyethyleneimine (PEI) was covalently grafted on LDH surface to further enhance H-2/CO2 selectivity by CO2 chemosorption. This multiple synergistic mechanism achieves simultaneous improvements of H-2 permeance and H-2/CO2 selectivity. The prepared LDH(Cl-)/PEI-HPAN membranes exhibited a H-2 permeance of 707 GPU and a H-2/CO2 selectivity of 78.5, representing increasements of 244% and 185%, compared with the pristine LDH-HPAN membrane, exceeding the 2008 Robeson upper bound. This membrane integrates the anti-swelling stability of Cl- (weak hydration) and the mechanical robustness of PEI hydrophobic chains, providing a new paradigm for 2D material membranes with high separation performances and ease of scalable preparation for industrial hydrogen purification.

Simultaneously regulating the local electronic microenvironment of dual phases in heterostructures remains a significant challenge. Herein, we propose a lattice-inherited single-atom strategy to construct Re-doped MoS2/MoP dual phases, where Re atoms remain atomically dispersed throughout the MoS2 to MoP transformation. This strategy enables concurrent regulation of the diffusion of MoS2 and catalytic MoP phases, thereby overcoming the intrinsic adsorption, diffusion, and catalytic limitations of individual phases in conventional dual-phase heterostructures. DFT calculations reveal that, in Re-MoS2, Re incorporation induces reconfiguration of surface S 3p orbitals, weakening Li-S orbital overlap and lowering Li+ diffusion barrier. In Re-MoP, unpaired delocalized electrons upshift the d-band center and strengthen interfacial charge coupling, thereby accelerating polysulfide redox kinetics. Meanwhile, the dual-phase distribution of Re atoms enhances the built-in electric field, promoting directional polysulfide migration toward catalytic domains. Structurally, the constructed hetero-nanotube catalysts, featuring ultrathin Re-doped MoS2/MoP coaxially encapsulating carbon nanotubes, ensure intimate face-to-face contact and efficient electron transport. The cell exhibits remarkable cycling stability (0.035% decay over 1000 cycles at 5 C) and achieves a high areal capacity of 9.16 mAh cm-2 at 10.59 mg cm-2 sulfur loading. This work opens a new avenue for enhancing heterostructure synergistic effects, extending beyond Li-S batteries to other multi-electron-transfer systems.

The sluggish redox kinetics and severe shuttle effect of lithium polysulfides (LiPSs) remain critical challenges for practical lithium-sulfur (Li-S) batteries. Herein, we report a dual-site catalytic architecture featuring asymmetrically coordinated Mo single atoms (Mo-P3N1) and Mo atomic clusters co-anchored on an N, P-doped carbon matrix (Mo-NPC/Mo AC). Distinct from conventional symmetric M-N4 single-atom structures, the introduction of P coordination breaks the geometric symmetry and induces electronic polarization of Mo centers, leading to an upshifted d-band center and enhanced LiPSs adsorption capability. Comprehensive synchrotron X-ray absorption spectroscopy combined with wavelet transform analysis directly confirms the coexistence of atomically dispersed Mo sites and Mo-Mo coordinated clusters. Through electrochemical kinetic analysis and density functional theory calculations, we reveal a directionally decoupled catalytic mechanism: Mo-NPC single atoms predominantly accelerate the rate-determining solid-state conversion of Li2S4 to Li2S during discharge, while Mo atomic clusters effectively lower the energy barrier for Li2S decomposition during charge. This full redox-cycle-oriented synergistic catalysis significantly reduces polarization and accelerates sulfur conversion kinetics. Benefiting from the integrated effects of electronic structure modulation, dual-site catalytic cooperation, and hierarchical porous confinement, Li-S batteries employing Mo-NPC/Mo AC functionalized separators deliver an initial specific capacity of 1081 mAh g- 1 at 1C, with a low capacity decay rate of 0.074% per cycle over 650 cycles, together with remarkable rate capability up to 4C. This work establishes a mechanistically clarified dual-site catalytic model for regulating the complete sulfur redox pathway and provides new insights into rational catalyst design for high-performance Li-S batteries.

Covalent organic framework (COF) membranes have attracted considerable attention in electrochemical energy storage systems owing to their ordered pore architectures and tunable surface chemistry. However, their intrinsic two-dimensional planar structure and strong it-it stacking interactions render them inherently brittle and difficult to process into flexible free-standing membranes, severely limiting their practical applications. Herein, we report that sulfonic acid functionalization enables fabrication of the free-standing COF membrane (m-TpBDSA), while non-sulfonated analogues yield only non-processable powders (TpBD) under identical conditions. Structural investigations reveal that sulfonic acid groups induce the framework twisting, which weakens interlayer it-it stacking and facilitates strain dissipation, enabling the free-standing COF membrane to achieve tensile strength of 50 MPa and bending curvatures up to 3500 m-1. Beyond enabling processability, the high-density sulfonic acid groups establish continuous hydrogen-bonding networks within sub-nanometer channels that promote rapid proton migration through the Grotthuss mechanism, endowing the membrane with a proton conductivity of 332 mS cm-1. The sulfonated COF membrane achieves an energy efficiency of 70 % in vanadium flow battery at a high current density of 500 mA cm-2. These findings provide insights into both membrane formation mechanisms and proton transport behavior, establishing a foundation for designing flexible, high-performance COF membranes for advanced electrochemical energy storage.

Solid-state lithium metal batteries (SSLMBs) are promising next-generation energy storage system. Poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) is potential electrolyte material due to the high thermal stability and membrane processibility. Yet PVDF-HFP based electrolytes are plagued by low ionic conductivity. Solid inorganic fillers have been adopted to create interfacial transportation pathway between fillers and polymer. However, only out surface facilitates Li+ transportation, resulting in a limited ionic conductivity improvement. Herein, multi-transportation pathway is designed in PVDF-HFP by multi-shelled hollow microsphere (MSHM) Fe2O3. The unique MSHM Fe2O3 architecture creates multi-transportation pathway along its out surface and inner multi-shells, and the hollow reservoir could confine anions and solvents to release desolvated Li+. Thus, more efficient Li+ are transported through multi-transportation pathway to accelerate Li+ migration and lower the migration energy barrier to 0.133 eV. The PVDF-HFP-MSHM Fe2O3 electrolyte shows a high ionic conductivity of 1.87 mS cm(-1) at 30 degrees C. And the high voltage NCM622||Li cell demonstrates an initial specific capacity of 179.4 mAh g(-1) at 1C with a capacity retention of 94.4% after 250 cycles. This work presents a hierarchical multi-shelled architecture engineering to construct multi-transportation pathway in polymer electrolytes, which paves a new avenue to advance the electrolyte for SSLMBs.

The trade-off between chemical stability and proton selective conduction greatly influences energy efficiency and cycling stability of vanadium redox flow batteries (VRFBs). Herein, the electron-withdrawing side chain protective engineering was proposed. Owing to the electron-withdrawing effect of the trifluoromethyl and carboxylic acid contained side chain, the sulfonic acid groups (-SO3H) were located on the main chain benzene ring with enhanced proton dissociation ability, the electrostatic potential of benzene hydrogen atoms increased to repel vanadium ions, and the HOMO-LUMO gap was enlarged for excellent oxidation energy barrier, simultaneously improving H+/Vn+ selectivity and chemical stability of the sulfonated poly(arylene) membrane (SPTPC). Both low area resistance (0.2 Omega cm2) and vanadium permeability (1.1 & times; 10-9 cm2 s-1) led to high H+/Vn+ selectivity (5.54 & times; 1010 mS s cm-3) in the SPTPC membrane. The corresponding VRFB achieved high energy efficiency of 80 % @280 mA cm-2, extremely low discharge capacity decay rate of 0.027 % and long-term stable operation of 7000 charge-discharge cycles at 200 mA cm-2. A degradation mechanism was proposed that attributed the excellent cycling stability to the preferential degradation of electron-withdrawing side chain as a sacrifice structure.

Halide perovskite nanocrystals (NCs) are promising optoelectronic materials owing to their tunable structural and chemical characteristics across the visible spectral range. Introducing magnetic transition-metal ions can endow them with additional optical and magnetic functionalities. However, achieving efficient and controllable Mn2+ doping in size-confined and ensemble-uniform CsPbBr3 NCs remains challenging, which limits systematic investigations of exciton-dopant-ion interactions. Here, we report a ligand-mediated interfacial ion shuttling (LMIS) strategy that enables efficient Mn2+ incorporation into size-confined CsPbBr3 NCs under ambient conditions. In this process, oleic acid/oleylamine ligand pairs act as dynamic coordination shuttles to promote the transport of MnX2 species across the water-toluene interface, thereby enabling interfacial dopant delivery. LMIS enables comparative studies of photophysical processes across different confinement dimensionalities and doping regimes, while maintaining high photoluminescence efficiency and allowing scale-up over more than two orders of magnitude. On the basis of this controllable doping platform, the energy transfer between host exciton emission and Mn2+ dopant emission can be regulated, leading to stable single-component white-light emission with CIE coordinates of (0.33, 0.32). These results suggest that LMIS may serve as a practical route for controlled dopant incorporation and photophysical modulation in confined perovskite nanostructures.

Metal–organic framework (MOF)-poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) nanofiber membrane-based quasi-solid electrolytes (QSEs) for lithium metal batteries (LMBs) suffer from Li dendrite growth and unstable interface towards high-voltage cathode. Herein, a dual metal MOF-based QSE (PHZZS) is constructed by in situ growth of Zn/Co-MOF on PVDF-HFP nanofiber membrane, followed by in situ polymerization of poly(ethylene glycol) diacrylate/succinonitrile/lithium bis(trifluoromethanesulfonyl)imide (PEGDA/SN/LiTFSI) precursor. The Zn/Co-MOF improves precursor wetting and infiltration, enabling uniform formation of the PEGDA network. Meanwhile, Zn/Co Lewis acid sites and the porous structure in Zn/Co-MOF collectively confine SN and TFSI− migration, promoting LiTFSI dissociation to enhance Li+ conduction. The restricted anion migration further alleviates interfacial concentration polarization and local current crowding, leading to more uniform Li deposition and enhanced interfacial stability toward high-voltage cathodes. Thus, PHZZS delivers an ionic conductivity of 1.78 mS cm−1 at 27 °C and enables stable Li||Li cycling for 2400h. LFP||Li and NCM811||Li cells retain 99% and 75% of their initial discharge capacities, respectively, after 400 cycles at 0.5C, while the NCM811||Li pouch cell maintains a specific capacity of 192 mAh g−1 after 50 cycles at 0.1C. This study provides a viable strategy for designing MOF-based QSEs that combine fast Li+ transport with high-voltage stability.

Rubidium resources exhibit considerable application potential in high-tech fields. However, conventional technologies for rubidium extraction are severely constrained by the selectivity in the presence of competing ions. Herein, we propose a microscale synergistic evaporation-adsorption-crystallization process, termed the "Fiber Evadsorber" (FE), for the effective extraction of rubidium from saline water. In the developed FE system, the fiber matrix can not only facilitate interfacial evaporation but also acts as a support for potassium copper hexacyanoferrate (KCuFC). Driven by capillary effect, the saline water solution is continuously transported upward through the narrow interstices between adjacent fibers. The continuous interfacial evaporation concentrates the saline solution, thereby enabling the sequential and spatially separable precipitation of rubidium and competing ions, which is governed by their inherent solubility differences and initial concentrations in the feed solution. This unique design could enable the sequential crystallization and spatial separation of target and interfering ions based on discrepancies in their solubility and concentration. This process effectively mitigates the interference from competing ions. Furthermore, Rb+ can be selectively captured in a specific region of FE, which significantly enhances the overall separation efficiency. The results demonstrated that under optimized heated air-enhanced evaporation conditions (temperature: 55.5 degrees C; relative humidity (RH): 12%; 0.85 m/s wind speed, and 420 m3/h airflow), the separation factor of Rb+ relative to competing ions using KCuFC with the optimized loading amount significantly improved to 595.0 +/- 0.9 in a feed solution containing 10 g/L Na+ and 10 mg/L Rb+. These findings verify the technical feasibility of the proposed microscale approach, highlighting its strong potential for Rb+ extraction from saline water.

Interfacial evaporation is recognized as a promising sustainable desalination technology, yet its energy efficiency remains bottlenecked by the intrinsically high enthalpy of water evaporation. Here, we engineer a covalent organic framework (COF)-based membrane with a hierarchical micrometer-to-angstrom architecture to precisely regulate water behavior for efficient activation and evaporation. With competitive interface/solution nucleation kinetics, confined interfacial growth of COF on vertical microchannels drives a re-entrant crystallinity transition, yielding uniform COF lattices with ordered water-binding sites. Critically, experimental and theoretical investigations reveal that angstrom-scale hydrophobic/hydrophilic motifs within the COF synergistically promote activated water states featuring weak hydration and rapid diffusion behavior, thereby maximizing intermediate water domains and reducing the evaporation enthalpy to only 30% of that of bulk water. Consequently, the engineered membrane achieves a high rate of 2.98 kg m-2 h-1 under a moderate thermal gradient (45 °C/25 °C) and maintains stable performance over 240 h of continuous operation. This work establishes a paradigm for manipulating water activation via angstrom-scale texturing in porous materials, paving the way for energy-efficient desalination and beyond.

Current H2-selective polymer membranes face an inescapable permeability-selectivity trade-off. We report a hydrogen-bond crosslinking strategy mediated by pyrophosphoric acid (PPA) to engineer chain packing in unprotonatable 6FDA-TFMB polyimides (PI) for ultra-selective H2 separation. Through molecular design, rigid non-coplanar 6FDA-TFMB PI featuring trifluoromethyl side groups was subsequently incorporated with hydroxyl-rich PPA. Collaborative simulation-experimental validation confirmed that the hydrogen-bond (C═O···H-O) crosslinking between PI and PPA in the PI2-PPA1-60°C membrane achieved 4% compression of polymer chain spacing (d-spacing from 3.95 to 3.69 Å) compared to pristine PI, constructing a hierarchically graded chain-spacing architecture with 2.18-5.17 Å gradient distribution. This engineering structure endowed the PI2-PPA1-60°C membrane with extremely high H2 permeability (167.24 Barrer), while achieving efficient molecular sieving, elevating H2/CH4 and H2/N2 selectivity to 708.51 and 443.56 respectively (PI-H2/CH4: 95.34; H2/N2: 40.59). The breakthrough separation performance surpassed the 2015 Robeson upper bound, providing an engineerable supramolecular solution to decouple the permeability-selectivity conflict in membrane technology.

Nitrogen-doped carbon (NC) is widely employed as a conductive matrix in Li-S batteries, yet its intrinsic catalytic contribution is often overlooked when combined with metal compounds. Herein, we propose a hierarchical microreactor architecture that integrates conductive and catalytic functions through an intimately coupled Mo2C@NC interface. Density functional theory calculations demonstrate that coupling NC with Mo2C induces pronounced electron redistribution of N atoms, with pyridinic N exhibiting the strongest charge transfer from Mo2C, making the p-band center closest to the Fermi level, thereby endowing superior LiPSs adsorption activity. Guided by this insight, a phase-inversion strategy is employed using pyridinic-N-rich polyacrylonitrile (PAN) and MoO3 precursors to construct a cross-linked MoO3@PAN network, which is subsequently transformed into Mo2C@NC microreactors after carbonization. In this structure, Mo2C nanowires are uniformly confined within pyridinic-N-rich carbon shells, forming a zero-distance conductive-catalytic interface that enables efficient electron transfer from Mo2C to NC. This integrated microreactor provides continuous electron pathways, abundant catalytic sites, and unobstructed ion transport, effectively avoiding pore blockage commonly encountered in conventional composite cathodes. Consequently, the Mo2C@NC cathode exhibits high cycling stability over 1000 cycles at 2.0 C with a low decay rate of 0.052% per cycle. Even at 4.0 C, it retains 790.6 mAh g-1 for over 400 cycles with only 0.027% fading per cycle.

Metal organic frameworks (MOFs)-based mixed matrix membranes (MMMs) exhibit great prospect for He/CH4 separation. However, it is still restricted by interfacial incompatibility-induced low filler loading and selectivity loss. This study proposed an interface fusion strategy by 6FDA-TFMB (PI) functionalized CF3-UiO-66 through NH2-UiO-66 bridging to achieve dual regulation of interface compatibility and molecular sieving. Crucially, this interface fusion strategy allowed a substantial increase in filler loading to 20 wt.%, representing a 100% improvement over unfunctionalized CF3-UiO-66. The covalent bond formed between the amino group and the dianhydride improved the interfacial compatibility. The -CF3 group on the UiO-66 reduced the pore size of UiO-66 and weaken the adsorption of CH4. The dual synergistic effect made the resultant MMMs exhibited excellent He permeability (165.2 Barrer) and He/CH4 selectivity (394.1), representing improvements of 81.14% and 319.7%, respectively, compared with pristine 6FDA-TFMB membrane, approaching to the 2008 Robenson upper bound, surpassing most of the reported PI based membranes for He/CH4 separation. This synergistic architecture not only validated the interface fusion engineering but also provided a foundation for designing efficient He/CH4 separation materials with tailored microscopic properties.

The trade-off between permeability and selectivity remains a major challenge in developing nanofiltration membranes for the treatment of antibiotic-contaminated wastewater. Herein, we present an acetic acid activation method to reconstruct the morphology and pore size of polyamide membranes. The acetic acid induces swelling of the polyamide network and dissolves oligomers, thereby generating additional free volume, and creating new interconnections within the polymer matrix. This process simultaneously reduces the thickness of the selective layer from 81.6 nm to 40.8 nm while maintaining its structural integrity. Molecular simulations reveal a strong affinity between acetic acid and polyamide chains, which drives polymer swelling and increases free volume. Following treatment with dilute acetic acid, the water permeance of the polyamide membrane increased from 15.9 L center dot m- 2 center dot h- 1 center dot bar- 1 to 21.5 L center dot m- 2 center dot h- 1 center dot bar- 1. This work outlines a potential approach to fabricating high-flux nanofiltration membranes, enabling efficient antibiotics separation and sustainable wastewater purification.

Covalent organic frameworks (COFs) are regarded as disruptive membrane materials owing to their versatile functionalities, high stability and ordered nanochannels. However, a major obstacle to the application of COFbased membranes in gas separation is the inherent size difference between their pore sizes and target gas molecules. Herein, we employed a confined cross-linking strategy to graft CO2-philic poly-ethyleneimine (PEI) onto carboxylic acid-type iCOF membranes, constructing a gradient wedge-shaped pore wall structure to enhance H2 separation. High-density carboxyl group-containing iCOF nanosheets were prepared via an improved singlephase solution method and assembled into membranes. 1-ethyl-3-(3-dimethylami-nopropyl) carbodiimide/N-Hydroxysuccinimide (EDC/NHS) coupling chemistry was used to functionalize iCOF membranes with PEI. The introduction of a large number of amino groups via PEI enhances CO2 adsorption by 81.4%. Meanwhile, the grafting of PEI reduces defects or pinholes on the membrane surface and improves the mechanical properties and stability. As a result, the PEI-functionalized iCOF@PEI-4 membrane exhibits a H2 permeance of 1103 GPU and an H2/CO2 selectivity of 21.3, positioning its performance among advanced membranes and surpassing the 2008 Robeson upper bound. Customized structural design of iCOF membranes through tailored functionalization may provide insights for designing molecularly selective COF membranes.

Recovering fuel-cell-grade hydrogen from low-quality syngas is vital for decarbonization, yet optimizing hybrid membrane-pressure swing adsorption (PSA) systems remains hindered by the disconnect between mainstream process simulators and dynamic PSA tools. To address this, we developed a high-fidelity cross-platform framework by deeply embedding a MATLAB-constructed dynamic PSA solver into UniSim Design via an automation interface. Leveraging this architecture for granular techno-economic assessment, a hybrid membrane-PSA process was optimized using response surface methodology (RSM), revealing critical trade-offs between separation efficiency and productivity. Under optimal conditions, the system yields 5614.04 Nm(3)/h of fuel-cell-grade hydrogen (99.9993% purity, CO < 0.2 ppm) with an overall recovery of 90.34% and a specific cost (SC) of 3.025 USD/kg H-2. The resulting efficiency and cost-competitiveness confirm the viability of this hybrid technology as a reliable engineering paradigm for achieving distributed energy security and carbon neutrality goals.

Polyurea membranes exhibit exceptional acid-base tolerance due to their densely cross-linked structure and extensive hydrogen-bonding network, making them attractive for separations under extreme pH conditions. However, the tightly associated network also leads to limited free volume, resulting in low water permeability that hinders practical applications. Herein, we report a permeance-enhanced polyurea nanofiltration membrane fabricated via coordination-induced structural reconstruction. By introducing Zr4+ into the polyurea network, coordination interactions with urea groups partially disrupt interchain hydrogen bonding, leading to network loosening and additional free volume. As a result, the water permeance is increased by 21% without compromising selectivity. Meanwhile, incorporation of Zr4+ enhances membrane hydrophilicity and surface positive charge, which therefore improves antifouling properties and promotes the rejection of heavy metal ions. Importantly, the reconstructed membrane retains excellent acid resistance, maintaining a stable salt rejection above 95% over 720 h. This work provides a simple yet effective strategy to overcome the permeability-stability trade-off in polyurea membranes and offers new insights into coordination-mediated regulation of polymer network structures for high-performance separations under harsh conditions.