
Abrikosov vortex motion in type-II superconductors generates finite resistance under applied current, limiting practical use. Traditional suppression via defect engineering is complex and hard to reproduce. Here, we show that interfacial engineering-specifically, tuning the penetration depth (λ) mismatch between an Nb superconducting channel and its capping layer-offers an alternative control of vortex dynamics and re-entrant behavior. Nb microstrips capped with Ta, V, or Cu reveal that force balance-induced vortex pinning yields a re-entrant, dissipationless state in Nb/Ta under magnetic fields of 1.64 T and currents above 0.5 mA, whereas Nb/V and Nb/Cu lack this effect. The phenomenon is strongly anisotropic, appearing only for a magnetic field along the in-plane y-axis and becoming asymmetric under field reversal above 0.8 mA, leading to nonreciprocal behavior. Force analysis shows a ∼0.56 meV/nm pinning energy per vortex, indicating an interface-controlled mechanism that is far weaker yet highly tunable compared to defect-based pinning.
Conventional anticounterfeiting based on structural color relies on human vision for authentication, which introduces subjective bias and ambiguity, particularly for individuals with color vision deficiencies. Here, we propose a strategy that overcomes this limitation by integrating hue-programmable bilayer heterostructures with machine-vision authentication, wherein optical information is encrypted by structural color and objectively decrypted via a smartphone-based pattern recognition system. To realize this strategy, we design bilayer heterogeneous photonic crystals (BHPCs) comprising monolayers of polystyrene nanospheres with diameters of 400 nm and 500 nm, fabricated by gas-liquid interface self-assembly and tape-assisted transfer. The BHPCs uniquely access a magenta hue sector unattainable by either monolayer, offer a large angular extension, and enable dual-region authentication. We elucidate its diffraction mechanism as incoherent spectral superposition, validated by experiment and simulation. This approach eliminates subjective color perception bias, avoids expensive spectrometers, and allows user-defined encryption levels. The work provides a new paradigm for high-security, machine-readable anticounterfeiting and offers design insights for PC-based displays and sensors.
Freshwater scarcity has become an urgent global issue. Bioinspired fog harvesting is a promising route to freshwater supply, whereas conventional bioinspired surfaces merely optimize partial procedures independently, severely restricting fog harvesting efficiency. Herein, inspired by cactus spines, Sarracenia trichomes, spider silk, and leaf veins, we rationally designed a multi-bioinspired patterned surface (MBPS) featuring nanoneedles, wettability-gradient microchannels, and vein-like networks to synergistically regulate the entire harvesting process. Specifically, once a continuous water film forms within the microchannels, fog droplets effectively captured by dense nanoneedles, upon contacting the hydrophilic pattern, are rapidly drawn into the microchannels and directionally transported toward the designated collection area via the interconnected network under the combined effect of multiple driving forces. This unique harvesting mode synergizes fog capture, droplet coalescence, and transport, endowing the MBPS with a high efficiency of 2.52 g cm-2 h-1 as well as excellent cyclic stability. Such multi-effect synergy further facilitates efficient fog harvesting.
Decoupling the intrinsically coupled electrical and thermal transport remains a central challenge for achieving high-performance thermoelectrics. Herein, we report a defect-modulated transport-decoupling strategy in anisotropic Bi2Te3/Sb2Te3 (BT/ST) heterojunction nanomaterials with silver nanowires. By guiding defect evolution at the BT/ST phase boundaries, nanopore-containing heterointerfaces are constructed. Combined spatially resolved EELS observations and HRTEM/IFFT suggest that nanopores are preferentially associated with dislocation-rich heterogeneous interfacial regions. These engineered nanopores and heterogeneous interfaces effectively suppress phonon transport, leading to an ultralow lattice thermal conductivity of ∼0.13 W m-1 K-1 at 600K. Meanwhile, the two-dimensional nanoplate framework provides anisotropic transport characteristics, while silver nanowires provide additional conductive pathways and modify the interfacial electronic transport, enabling enhanced electrical conductivity while preserving a high Seebeck coefficient. As a result, the electrical and thermal transport processes are spatially regulated. The optimized BT/ST nanoheterojunctions containing 2 vol % AgNWs exhibits a peak ZT⊥ of 0.74, corresponding to a substantial ∼174% enhancement compared with the pristine matrix. More importantly, the combination of suppressed phonon transport and preserved electrical transport parallel to the SPS pressing direction yields a high S∥ of 169 μV K-1 and an outstanding peak ZT∥ of 1.25 at 600 K. This work demonstrates that controllable nanopore construction and directional electrical pathway engineering are effective for realizing anisotropic carrier-phonon decoupling in high-performance thermoelectric materials.
Ammonium salt-based top-interface passivation is effective for inverted perovskite solar cells, yet how the head-group conformation governs the passivation mechanism remains unresolved. Herein, using 9H-fluoren-9-amine hydrochloride (FAMACl) and aminodiphenylmethane hydrochloride (DPMACl) as a comparative pair, we reveal that structural differences in the head groups drive fundamentally distinct passivation pathways. The rigid, conjugated structure of FAMACl enables strong chemical passivation through coordination with undercoordinated Pb2+ defects, but introduces unfavorable energy level alignment that limits efficiency gains. In contrast, the flexible DPMACl architecture generates a substantial molecular dipole moment, which induces a strong interfacial electric field that optimizes energy level alignment and suppresses nonradiative recombination via field-effect passivation, delivering a champion power conversion efficiency of 26.02%. This work establishes a direct link between the conformational flexibility of ammonium head-groups and their passivation functionality, offering a new molecular design principle for high-performance perovskite photovoltaics.
The all-inorganic CsPbI2Br material shows promise for indoor photovoltaics but suffers from a severe open-circuit voltage (Voc) deficit under low light due to defect-mediated recombination. Here, we introduce 3,4-thiophenedicarboxylic anhydride (TDA) into the precursor solution to synergistically retard crystallization and passivate defects. Density functional theory and synergistic experiments confirm that TDA strongly coordinates with PbI2, outcompeting DMSO and increasing the activation energy for CsPbI2Br nucleation. This yields CsPbI2Br films with larger grains, enhanced crystallinity, and reduced trap density. Residual TDA molecules can passivate uncoordinated Pb2+ at grain boundaries, suppressing nonradiative recombination. Using a dopant-free P3HT hole-transport layer, the optimized device achieves a champion power conversion efficiency (PCE) of 17.33% with a remarkable Voc of 1.42 V under standard illumination. Under 1000 lux LED indoor light, the device delivers a PCE of 36.22%. More importantly, TDA-optimized devices can retain 90% of initial efficiency after 1500 h in ambient air and 90% after 1000 h at 85 °C. This work provides a facile strategy to overcome the Voc deficit and instability of CsPbI2Br indoor photovoltaics.
Ultrasound-enabled catalytic strategies offer a non-invasive route for antibacterial therapy but are typically limited to non-centrosymmetric piezoelectric materials. Herein, we developed ultrasound-assisted flexocatalysis as a symmetry-independent approach for reactive oxygen species (ROS) generation using ternary copper antimony disulfide (CuSbS2, CSS) nanocrystals synthesized via a hot-injection method, and engineered an all-in-one synergistic catalytic platform integrated with multiple catalytic activities, including flexocatalytic, photocatalytic, and oxidase-/peroxidase-like nanozymatic activities to promote antibacterial treatment. As a result, rapid and efficient antibacterial performance is achieved, with inhibition efficiencies up to 97.0% against Escherichia coli, 98.73% against Pseudomonas aeruginosa, and 97.8% against Staphylococcus aureus within 30 min, enabling synergistic ROS production under mechanical, optical, and enzymatic stimulations. Besides, CSS exhibited high catalytic activity toward organic pollutant degradation, achieving over 97% rhodamine B removal within 40 min. This work sheds light on the rational design of centrosymmetric chalcogenide nanomaterials as versatile flexocatalysts, paving the way for their application in advanced antibacterial and biomedical catalytic systems.
Random lasing (RL) from perovskites is highly attractive for achieving speckle-free imaging owing to its low spatial coherence. However, the intrinsic instability of perovskites limits their practical applications. Here, to overcome this, we encapsulate different metal-halide perovskites in a hydrophobic poly (methyl methacrylate) matrix and fabricate core-shell perovskite composite fibers via coaxial electrospinning. The composite exhibits a uniform distribution of perovskites, resulting in single- and dual-color emitting perovskite fibers. The dual-emissive fibers demonstrate remarkable water resistance, maintaining emission after 9 days. Their emission persists even under combined thermal stress (50 °C) and UV exposure in water for up to 40 min. Notably, the green-emitting core-shell fibers exhibit stable RL behavior in diverse environments, including air, water, and an acidic medium (pH = 3), highlighting their robustness in extreme conditions. Furthermore, RL from these fibers enables speckle-free imaging with an ultralow speckle contrast (K = 0.008), compared to a conventional CW laser.
High-concentration glycerol, the clinical standard for red blood cell (RBC) cryopreservation, requires laborious deglycerolization and causes significant hemolysis, whereas trehalose is biocompatible but poorly permeable to the RBC membrane. Herein, we report a tardigrade-inspired, glycerol-free strategy for RBC cryopreservation based on a conserved CAHS-derived peptide motif. Systematic sequence analysis identified a minimal CAHS-motif that possesses an intrinsic helical propensity and adopts a stabilized amphipathic α-helical conformation under dehydration-mimicking conditions. Under the 4 °C loading condition, CAHS-motif and trehalose co-incubation was associated with increased membrane fluidity and increased intracellular trehalose accumulation while maintaining low pre-freeze hemolysis. In parallel, the CAHS-motif acts synergistically with trehalose to suppress ice-associated damage during freezing and thawing. Under the combined effect, RBCs cryopreserved with the CAHS-motif and trehalose formulation achieved a post-thaw recovery of 89.0 ± 0.6% and excellent blood compatibility (99.0 ± 0.7%), outperforming the conventional glycerol-based method. Post-thaw RBCs retained normal morphology, volume, and key functional activities in vitro and effectively corrected anemia in an APH-induced hemolytic anemia mouse model without detectable pro-inflammatory responses. These results establish a clinically relevant, bioinspired platform for high-recovery RBC cryopreservation and highlight the translational potential of extremophile-derived motifs in transfusion medicine.
Premature cracking during free hot deformation (FHD) of n-type Bi2Te2.7Se0.3 limits the attainable strain, thereby interrupting dynamic recrystallization (DRX) and capping (0001) basal-texture development. Here, we identify this crack-limited DRX bottleneck through thermomechanical compression and interrupted-deformation evidence, and then eliminate it using hot extrusion (HE), where the inherently triaxial compressive stress state suppresses crack initiation and propagation. Crack-free extrusion enables near-complete DRX and a near-ideal (0001) basal texture, while retaining ∼10 nm amorphous nanodomains, which contribute to reducing lattice thermal conductivity without degrading electrical transport. The optimized alloy is tougher-95.8 MPa in bending and 138.4 MPa in compression (+62%/+48% vs FHD)-and reaches zT ≈ 1.20 at 343 K. Importantly, under strictly identical single-stage micro-TEC assembly and test boundaries (identical p-legs; only n-legs varied), the extruded n-legs increase ΔTmax to an outstanding 75.8 K at Th ≈ 300 K, which is among the highest values reported for Bi2Te3-based TECs under comparable testing conditions. These results establish crack-free hot extrusion as a scalable route to remove the fracture-imposed DRX ceiling in layered brittle thermoelectrics and to translate microstructural gains into device-level cooling performance.
Subarachnoid hemorrhage (SAH) remains a devastating stroke subtype with high morbidity and mortality, largely due to complex early brain injury (EBI) within the first 72 h involving cerebral vasospasm (CVS), oxidative stress, and neuroinflammation. Existing therapies such as nimodipine offer limited protection and fail to address multiple injury pathways. Here, we report a SPARC-targeted albumin-based zinc sulfide nanoparticle (ZnS/BSA NPs) designed for lesion-specific delivery and multi-mechanistic therapy for SAH. We demonstrate that SPARC is significantly upregulated in both human and rat SAH brains, enabling active targeting of injured vasculature and crossing the blood-brain barrier (BBB). ZnS/BSA NPs exhibit good colloidal stability in serum-containing medium and pH-responsive release of Zn2+ and H2S. Mechanistically, Zn2+ suppresses Ca2+ influx/CaMKII activation to alleviate CVS; H2S activates NRF2/HO-1 to scavenge reactive oxygen/nitrogen species (RONS) and inhibits NF-κB/NLRP3 signaling to shift microglia from M1 to M2 polarization. Additionally, the NPs inhibit Caspase-1/GSDMD-mediated pyroptosis in microglia and suppress both Caspase-1/GSDMD-mediated pyroptosis and Bax/Caspase-3-mediated apoptosis in neurons, thereby preserving BBB integrity and reducing brain edema. In a rat SAH model, ZnS/BSA NPs significantly improved learning, memory, and motor function, outperforming nimodipine. This work highlights SPARC as a viable druggable target and represents a "targeted, multi-mechanistic" nanotherapeutic paradigm for EBI after SAH.
Hypertrophic scar (HS) is a fibrotic disorder caused by imbalanced tissue repair after skin injury. Its core features include persistent inflammation and excessive collagen deposition. Current clinical treatments are limited by poor efficacy, severe local adverse reactions, and low transdermal delivery efficiency of topical drugs. In this study, a pH-responsive borax-dextran hydrogel (TA/5-FU@BDHs) co-loaded with triamcinolone acetonide (TA) and 5-fluorouracil (5-FU) was developed for transdermal treatment of HS. First, (2-hydroxypropyl)-β-cyclodextrin (HP-β-CD) was used to prepare HP-β-CD@TA/5-FU inclusion complexes, taking advantage of its hydrophobic cavity to encapsulate TA and 5-FU, thereby enhancing the aqueous solubility and stability of the two drugs. The inclusion complexes were encapsulated into a borax-cross-linked dextran hydrogel, forming a composite carrier for pH-responsive drug release and efficient transdermal delivery. The physicochemical properties of the inclusion complexes and hydrogel were systematically characterized by particle size and zeta potential analysis, storage stability testing, X-ray diffraction (XRD), differential scanning calorimetry (DSC), scanning electron microscopy (SEM), and swelling and degradation behavior assessment. It enabled rapid drug release in the weakly acidic HS microenvironment, significantly promoting transdermal absorption and cellular uptake. In vitro and in vivo studies demonstrated that TA/5-FU@BDHs induced macrophage polarization from M1 to M2 phenotype by modulating inflammatory mediators, exerting anti-inflammatory effects. Meanwhile, it inhibited abnormal activation of hypertrophic scar fibroblasts (HSFs) and downregulated the expression of fibrosis-related proteins. In summary, TA/5-FU@BDHs enable precise pH-responsive release, effectively ameliorate the core pathological processes of HS via macrophage polarization, and exert anti-inflammatory and antifibrotic effects. This system provides a safe, effective, and clinically translatable strategy for transdermal local treatment of HS.
Mechanical cues play a critical role in musculoskeletal homeostasis and disease pathophysiology, where excessive loading induces tissue damage and promotes inflammation. Aging further exacerbates this process, particularly in age-related diseases, such as osteoarthritis (OA). Although both hyper-mechanical loading and aging are known to contribute to chronic inflammation in OA and other age-related diseases, their combined effects remain poorly modeled in vitro. Here, we developed a dynamic 3D culture platform integrating gelatin hydrogels, human bone marrow-derived mesenchymal stromal cell (MSC) spheroids, and a compressive bioreactor to recapitulate joint-like mechanical environments. Gelatin hydrogel-encapsulated MSC spheroids maintained mechanical stability under repeated loading (10-20 kPa) while preserving cell viability and spreading. Aged MSC spheroids exhibited metabolic reprogramming toward glycolysis, elevated secretion of pro-inflammatory cytokines (IL-6 and IL-8), and increased PIEZO1 expression. Compressive loading further amplified inflammatory signaling and promoted M1-like macrophage polarization, particularly in aged donor-derived MSCs, modeling key features of inflammaging. Dexamethasone suppressed inflammatory cytokine secretion and promoted M2-like macrophage polarization, whereas tocilizumab modulated immune responses without reducing cytokine production. This platform establishes a donor-specific, mechanobiological model of inflammaging for precision therapeutic screening in osteoarthritis and related diseases.
With the rapid evolution of high-power electronics driven by advanced communication technologies and artificial intelligence, efficient thermal management has become a critical challenge. Hexagonal boron nitride (h-BN)/polymer composites, which integrate the flexibility of polymers with high thermal conductivity, low dielectric constant, and electrical insulation of inorganic fillers, are promising candidates for electronic packaging and communication systems. However, inefficient micro/nanoscale interfacial heat transport and weak interfacial bonding severely limit simultaneous improvements in thermal conductivity and mechanical robustness. Here, we demonstrate an edge-selective hydroxylation strategy that overcomes this limitation. Edge hydroxyl groups bridge the filler-matrix interface via hydrogen bonding interactions, markedly decreasing interfacial thermal resistance by 24.5%, while reducing the intrinsic thermal conductivity of BNNS by only 4.1%. Both molecular dynamics simulations and experimental results consistently show that the significantly enhanced interfacial coupling enables the edge-hydroxylated boron nitride nanosheets/polyvinyl alcohol (BNNS-OH/PVA) films to achieve a high in-plane thermal conductivity of 45.8 W m-1 K-1 and a tensile strength of 47.2 MPa, while maintaining low dielectric constant and loss for high electromagnetic wave transparency. These findings establish interfacial bridging as an effective route to simultaneously optimize heat transport and mechanical performance, offering a viable pathway for thermal management in next-generation high-power electronics and communication devices.
Porphyrin metal-organic frameworks (PMOFs) are recognized for their significant potential as photocatalysts active under visible light due to their adjustable structural attributes and extensive π-conjugated porphyrin core. In this study, the photocatalytic efficacy of aluminum-based porphyrin MOFs (Al-PMOFs) modified with four non-noble metals (Co2+, Cu2+, Zn2+, and Ni2+) is systematically examined. Among the evaluated materials, Al-PMOF(Co) exhibited the highest photoactivity toward CO2 reduction to formic acid. Through systematic variation of the cobalt loading (0.25-15 wt %), the 8 wt % incorporation level was identified as the best-performing among those investigated. The photocatalytic activity of Al-PMOF(Co)_8 was 1.6-fold higher than that of pristine Al-PMOF. Theoretical simulations enhanced through an active learning approach identified the critical descriptors governing photocatalytic performance, including band gap characteristics, band edge positions, charge separation, and carrier effective masses under operando conditions. These findings demonstrate the importance of cobalt incorporation for improving charge separation and enhancing photocatalytic CO2 reduction, providing useful guidelines for the rational design of highly efficient photocatalysts for sustainable carbon conversion.
The modulation of ferromagnetic order in 2D carbon materials has attracted increasing attention for the development of next-generation spintronic devices and multifunctional information storage technologies. In particular, the graphdiyne (GDY) family has been regarded as more suitable for spintronics owing to its tunable electronic structure and intrinsic semiconductor behavior. However, the effective magnetic introduction methods and their applications in specific devices have always been a challenge for the development of such materials. Here, this study presents a nitrogen-substituted derivative of GDY, triphenyl-substituted triazine graphdiyne (TPTG), as an ideal platform for inducing transition-metal iron (Fe) atoms to modulate the electronic state, resulting in the coexistence of room-temperature ferromagnetism and a semiconductor energy band. Subsequent spin-polarized density functional theory calculations further reveal that the observed ferromagnetism arises from pronounced localized magnetic moments together with electron transfer between carbon atoms and Fe ions. Moreover, by employing a transfer strategy suitable for this material system, thin films were successfully transferred onto a silicon substrate to construct an Fe-doped TPTG-based electronic device. Such a device exhibits typical artificial synaptic behavior under optical stimulation and demonstrates nonvolatile memory characteristics after illumination is removed, enabling the transition from short-term plasticity (STP) to long-term plasticity (LTP). The coexistence of ferromagnetism and semiconducting properties not only makes GDY-based materials promising candidates for exploring physical phenomena but also offers opportunities for the development of carbon-based neuromorphic devices.
Surface protection is critical for advanced systems such as marine equipment and medical implants, where fouling and microbial deposition cause irreversible degradation. However, developing protective coatings that integrate multifunctionality (e.g., amphiphobicity and antifouling), environmental compatibility, and durability remains challenging. Inspired by beetle cuticle architecture, a bioinspired spontaneous interfacial reconfiguration strategy was introduced to construct a multifunctional coating that synergizes low-surface-energy enrichment with bioactive molecular interactions. Following this strategy, a bio-based amphiphobic and antibacterial coating (PCGBF@GT) was fabricated via a rapid, environmentally benign UV-curing process (within 5 min). Spontaneous migration of fluorinated segments in the castor oil-derived resin provides robust amphiphobicity and fouling resistance. Meanwhile, the incorporation of glycidyl methacrylate-modified tannic acid (GT) introduces hydrogen-bonding interactions and positive zeta potential, stabilizing the interface and enabling broad-spectrum antibacterial activity against Escherichia coli (99.92 ± 0.90%) and Staphylococcus aureus (99.83 ± 0.06%). This work demonstrates a sustainable, bioinspired pathway toward high-performance protective coatings for marine and biomedical applications.
Hydrogel-based adsorbents have emerged as versatile materials for environmental remediation and sensing owing to their tunable chemistries, hydrated networks, and compatibility with multifunctional nanomaterials. However, conventional static hydrogels remain constrained by diffusion-limited mass transport, slow adsorption kinetics, and limited integration of pollutant detection with remediation. This review highlights the emerging shift from passive adsorption toward dynamic and actuatable hydrogels as adaptive sense-respond-act material systems capable of accelerated pollutant capture, real-time monitoring, and autonomous regeneration. We first discuss static hydrogel design principles, including polymer composition, nanomaterial incorporation, and structural architectures that govern adsorption capacity, selectivity, kinetics, and reusability. We then examine dynamic hydrogel platforms, including intrinsically stimuli-responsive networks, extrinsically actuated composites, and shape-programmed architectures that actively enhance mass transport and interfacial exposure. Particular emphasis is placed on emerging systems that integrate sensing with decontamination, positioning actuatable hydrogels as adaptive environmental interfaces and soft robotic materials. A comparative discussion of static and dynamic systems evaluates their performance, practical limitations, and translational potential for water remediation, resource recovery, and integrated sensing technologies. Finally, challenges in scalability, stability, and system integration are critically assessed, and future directions are proposed toward autonomous, intelligent hydrogel platforms for next-generation environmental technologies.
Understanding the correlation between heterointerface engineering and electromagnetic (EM) properties in hybrid materials, including metal-organic frameworks, is critical to advancing next-generation high-performance electromagnetic wave (EMW) absorbers. As the first demonstration of an all-MOF heterostructure film that achieves both high-performance EM absorption and thermal management, herein, a heterostructured MOF film, NUS-8@Cu3(HHTP)2, was fabricated by hybridizing the solution-processable MOF NUS-8 with the highly conductive MOF Cu3(HHTP)2. This prototypical heterostructure NUS-8@Cu3(HHTP)2 was found to exhibit effective modulation of its dielectric loss behavior. The optimal composite exhibits a notable minimum reflection loss (RLmin) of -42.9 dB and an ultra-wide effective absorption bandwidth (EAB) of 8.47 GHz at 2.5 mm, setting up new benchmarks over conductive MOFs and MOF composites reported thus far. When the optimized NUS-8@Cu3(HHTP)2 composite was incorporated into an epoxy matrix, a stable and robust EMW absorbing patch featuring an RLmin of -33.2 dB and an EAB of 6.38 GHz was achieved. Of particular importance is that NUS-8@Cu3(HHTP)2 epoxy composites demonstrate an enhanced thermal conductivity, eliciting efficient heat dissipation for reliable use in thermally demanding environments. Put simply, this work introduces a new strategy for designing high-performance EM absorbers through heterostructure engineering.
Selective scavenging of hazardous oxoanions and toxic gas sequestration rank among the most demanding sustainable environmental remediation, wherein astutely functionalized metal-organic framework (MOF)-based reconfigurable composites can lead to practical waste management. Herein, we developed a robust noninterpenetrated MOF, CSMCRI-24 (CSMCRI = Central Salt & Marine Chemicals Research Institute) containing cationic [Ni2(μ2-OH)(CO2)2]+ secondary building units, nitrogen-rich channels, and flanked -NO2 group-decked pores. Building on its wide range of pH stability, high porosity, and the presence of exchangeable counter anions, the activated framework (24a) acts as a dual-functional platform for selective and reversible uptake of three oxoanions (CrO42-, MnO4-, and ReO4-) followed by their bi-phasic visible colorimetric transitions. Importantly, the maximum adsorption capacities of these oxoanions surpass that of contemporary materials, and the MOF demonstrates ultrafast adsorption kinetics with above 95% removal efficiencies even in the co-existence of 50-fold excess of competing anions. Potential applicability of this charged MOF is highlighted from its unaltered oxoanion scavenging performance for different water matrices as well as steady removal efficiency during continuous-flow fixed-bed column experiments under practical operating conditions. The framework further enables reversible H2S sequestration with concurrent naked-eye colorimetric detection, highlighting the versatility of task-specific pore functionality. Aiming at practical deployment, an in situ-engineered MOF-based ionic sponge is fabricated, which provides a robust and regenerable platform for visible and reversible scavenging of toxic oxoanions and H2S. Complementing a battery of experimental pieces of evidence, in-depth density functional theory calculations elucidate the molecular-level interactions of oxoanions and H2S with the pore-aligned MOF functionality, providing mechanistic insights into the adsorption and sequestration of these hazardous analytes. Collectively, the present work demonstrates a viable pathway for translating task-specific, site-integrated cationic MOFs into programmable ionic sponges, providing a multifunctional platform for sustainable water purification, toxic gas remediation, and nuclear waste management.