The recovery of palladium (Pd) from complex acidic industrial wastewater is severely restricted by sluggish interfacial mass transfer and inherent diffusion-limited adsorption kinetics. To address this long-standing bottleneck, asymmetric N/Se-codoped resorcinol-formaldehyde nanomotors (Se-RF@NMs) were rationally fabricated via an emulsion-confined anisotropic growth strategy for photocatalytic self-propulsion-boosted Pd(II) recovey. Under light irradiation, the photoresponsive resin framework enables continuous in-situ H2O2 generation. Meanwhile, the adsorption-induced in-situ reduction of Pd(II) further accelerates catalytic H2O2 decomposition to generate oxygen microbubbles, endowing nanomotors with sustainable autonomous motion and dynamically promoting interfacial ion transport. EPR characterization confirms that photogenerated holes and reactive oxygen species sustain the cyclic H2O2 generation-decomposition system, effectively stabilizing the self-propulsion behavior of Se-RF@NMs. Benefiting from the synergistic coupling of photocatalytic self-propulsion and N/Se-based selective coordination adsorption, the optimized Se-RF@NMs achieve a superior Pd(II) adsorption capacity of 196.75 mg g−1, as well as excellent selectivity in multi-metal competitive systems and practical industrial wastewater matrices. This work elucidates a photocatalysis-driven active mass transfer enhancement mechanism, establishing a feasible paradigm to break the intrinsic diffusion limitation of conventional adsorption. It provides new insights into the rational design of intelligent self-propelled catalytic adsorbents for high-efficiency precious metal recovery in complex and harsh water environments.

Efficient uranium recovery from aqueous systems requires adsorbents that combine high interfacial affinity with recoverable macroscopic structures. Herein, bacterial cellulose-supported phosphonate-functionalized porphyrinic MOF aerogels (BC@PN-PCNs) were developed as monolithic uranium adsorbents by immobilizing PN-PCN-222, PN-PCN-223, and PN-PCN-224 within a three-dimensional bacterial cellulose network. In this architecture, the PN-PCN phase provides uranyl-binding and photoresponsive active sites, while the bacterial cellulose scaffold improves mass transport, structural integrity, and solid–liquid separation. Under weakly alkaline conditions, all BC@PN-PCN aerogels showed rapid U(VI) uptake and high adsorption capacities. At 400 ppm U(VI), BC@PN-PCN-222, BC@PN-PCN-223, and BC@PN-PCN-224 reached 1982.5, 1958.4, and 1929.4 mg g−1, respectively, far exceeding pristine bacterial cellulose. BC@PN-PCN-222 showed the best overall performance and retained more than 75% of its adsorption/desorption efficiency after four cycles. These results demonstrate an effective strategy for converting highly active MOF powders into recyclable monolithic adsorbents for uranium separation.

Gold, due to its rarity and excellent conductivity and corrosion resistance, is widely used in various electronic components. In this study, a nanocage thiourea-resorcinol-formaldehyde resin (NCTRF) adsorbent was designed and constructed to address the challenges of selective gold recovery from electronic waste. By employing monodisperse silica microspheres as a hard template along with a synchronous doping strategy, sulfur and nitrogen functional groups were uniformly introduced, yielding a material with a specific surface area of 36.9 m2 g-1 process, thiol, thiocarbonyl, and amino groups selectively capture gold ions via soft-soft interactions, accompanied by partial in situ reduction to elemental gold, thereby effectively suppressing secondary gold dissolution. Remarkably, the adsorbent exhibits an ultrahigh gold adsorption capacity of 2622 mg g-1 under hydrochloric acid solutions, along with outstanding anti-interference performance in multi-metal systems-achieving a 99.28 % gold removal rate-and excellent reusability, maintaining over 93 % recovery efficiency after five cycles. This work provides a sustainable and efficient strategy for precious metal recovery from electronic waste. and a hierarchical pore structure that promotes solute diffusion and ion transport. During the adsorption

Efficient Storage, delivery, and production of high-purity fluorinated specialty gases remain critical challenges in the semiconductor industry, where gas management directly determines the economic structure and competitiveness of chip manufacturing. Here, we report sub-angstrom pore-architecture engineering in microporous metal-organic frameworks, enabling highly efficient storage and purification of C3F6 and C3F8 at benchmark levels. By systematically tailoring linker length and terminal functional groups with sub-angstrom precision, a series of Co-based MFU-4-type materials were developed with progressively contracted pore apertures and distinct adsorption behaviors - from co-adsorption with ultrahigh storage capacity and delivery efficiency in Co-MFU-4L, to molecular size sieving in Co-MFU-4, and finally kinetic discrimination in Co-MFU-4-F for C3F6 and C3F8. Notably, the storage capacity and delivery efficiency of C3F6 on functionalized Co-MFU-4L reach 219.7 cm3 g-1 and 97%, respectively. Co-MFU-4 achieves a record C3F8 productivity (purity >99.999%) of 3.3 L g-1 from 1/99 C3F6/C3F8 mixture, as confirmed by dynamic breakthrough experiments. Molecular simulations and in situ Fourier transform infrared spectroscopy provide direct insights into the host-guest interactions. Precise pore-architecture tuning not only offers fundamental insights into the structure-property relationships at the sub-angstrom level but also demonstrates a promising route toward addressing challenges in "easy-on/off" delivery and purification of specialty gases.

Superhydrophilic catalytic self-cleaning membranes demonstrate unique advantages in emulsion separation processes. The preparation of superhydrophilic catalytic clean membranes under mild conditions is still a challenge, which is attributed to the mismatch between polymer phase transformation kinetics and catalyst growth kinetics, which makes the catalyst difficult to grow or easy to embed. Here, we report a dual-diffusion induced surface segregation for synchronous assembly strategy for the preparation of catalytic self-cleaning Prussian blue analogue membranes (PBAMs), enabling their one-step and rapid fabrication under mild conditions. Studies show that amphiphilic polyvinylpyrrolidone acts not only as a pore-forming agent but also as a bridging agent between metals and polymers during the NIPS process. The metal salt concentration can tune the size and population of Prussian blue analogue (PBA) nanoparticles. Adjusting the ratio of non-solvent to good solvent in the coagulation bath can balance the growth kinetics of the membrane with that of the PBA. The optimal superhydrophilic PBAM, exhibits a surface roughness 3.5 times that of the pristine PVDFM. It achieves a pure water permeance of 1009 L m(-2) h(-1) bar(-1), and maintains a separation efficiency of 99.9% with an emulsion permeance of 373.7 L m(-2) h(-1) bar(-1). The PBAM demonstrates high separation efficiency (>99%) and stable permeance for surfactant-stabilized various oil-in-water emulsions. The activated radicals (HO & centerdot; and SO- 4 & centerdot;) generated via PMS catalytic cleaning oxidize the pollutants adhered to the membrane surface, achieving a permeation recovery rate as high as 98%. Moreover, the membrane enables continuous and complete removal of methylene blue, with a permeance as high as 700 L m(-2) h(-1) bar(-1), demonstrating the superior emulsion separation and catalytic self-cleaning capabilities of the PBAM.

Single-atom catalysts (SACs) have demonstrated immense potential in the fields of energy and biochemical conversions. Their unique properties make them particularly efficient and selective. Characterized by their unique isolated state on supports, SACs often showcase poor synergy in the multiple molecule conversion because of the infrequent communications with others. Recently, some interesting synergetic processes of SACs in some special reactions have been found; however, to our best knowledge, the synergetic catalytic effect of SACs has not been systematically summarized. This article comprehensively overviews the basic concepts, mainstream synthetic methods, and modification strategies of SACs and emphasizes the synergetic catalysis effect in biomass conversion, CO2 reduction, and cascade reaction by itself or other media. To maximize the advantage of SACs, various synthetic methods for them, including impregnation, co-impregnation, co-precipitation, atomic layer deposition, electrochemical methods, photochemical methods, pyrolysis synthesis, spray pyrolysis method, ball-milling and chemical vapor deposition method are discussed. This review provides a comprehensive discussion concerning the dynamic interplay between precisely engineered atomic architectures and their synergistic functionalities in modulating catalytic efficacy, with focused exploration of activity enhancement strategies and operational stability optimization. Distinctively, it pioneers the establishment of comprehensive theoretical frameworks that unify SAC-driven synergistic catalytic mechanisms across three critical domains: biomass valorization, electrochemical CO2 conversion, and multi-step cascade processes. Through systematic synthesis of cutting-edge developments in coordination microenvironment modulation, inter-site electronic communication, and fundamental mechanistic studies, this work affords some interesting insight into rational design of synergistic SAC systems, thereby addressing current challenges in translating atomic-scale precision to heterogeneous catalytic performance.

Silica nanocapsules hold significant importance in agriculture, medicine and machinery owing to their high specific surface area, tunable surface properties and superior loading capacity. However, the industrial-scale production of silica nanocapsules with controllable morphology is still constrained by the challenges of precise morphology control and straightforward functional modification. To bridge this gap, we propose a novel continuous and scalable approach that integrates vapor condensation nanoemulsification with hydrolysis and condensation kinetics, enabling the controllable synthesis of functional silica nanostructures in one step. Precise control over the sample morphology (including solid spheres, nanocapsules and hollow hemispheres) and architecture (shell thickness) were achieved by tuning the concentration of silane coupling agents, condensation time and Span 80 dosage. Notably, the gyrification-inspired silica nanocapsules with wrinkled surface exhibited excellent lead removal performance (removal efficiency of 99.7%), combining high adsorption capacity (567.0 mg g-1) with rapid kinetics (20 min). This work not only provides a scalable platform for the industrial fabrication of morphology-controllable silica but also offers fundamental insights into silica growth mechanisms, thus paving the way for the design of silica functional materials in environmental and industrial applications.

ABSTRACT The energy‐free activation of ambient molecular oxygen (O2) to singlet oxygen (1O2) under neutral conditions is highly desirable for green oxidation chemistry, yet remains fundamentally limited by sluggish proton‐coupled *OOH formation and desorption. Here, we engineer an interfacial proton‐relay microenvironment between MoS2 and CuCl that enables self‐driven O2‐to‐1O2 conversion without external energy inputs. Electron‐deficient sulfur sites act as a proton reservoir by forming S‐Hads species, facilitating directional proton migration through Cu‐S‐Mo channels to activate adsorbed O2 on electron‐rich Cu sites. This coupled electron‐proton relay accelerates *OOH hydrogenation while maintaining moderate *O2/*OOH binding, effectively suppressing O─O bond cleavage and favoring a 1O2‐dominated pathway. As a result, the system achieves quantitative pollutant removal and sustained operation for over 16 h in pilot‐scale membrane filtration. This interfacial design is broadly applicable to transition metal sulfides, offering a general strategy to overcome proton‐transfer limitations and advance autonomous catalytic platforms for sustainable oxidation and environmental remediation.

Surface imprinting (SIT) and post-crosslinking imprinting (PCIT) together enable molecularly imprinted polymers (SPMIPs) with high specificity and efficient recognition. However, the use of multifunctional copolymers presents significant limitations in substrate adhesion due to their complexity. Here, we overcome this by designing an oil-mediated adhesion strategy driven by interfacial instability, firmly grafting SPMIPs onto an unmodified melamine sponge (MS). The resulting MS@SPMIPs selectively capture 2 '-deoxyadenosine (dA) via synergistic PCIT and base-complementarity effects, with 71.45% of binding sites showing high affinity and an imprinting factor of 1.95. The porous sponge architecture shortens diffusion pathways, allowing >85% dA uptake within 120 min. In spiked human urine samples, a single adsorption cycle achieves an identification efficiency of 69.8%, highlighting the advantages of geometrically precise cavities and optimized base pairing. This work demonstrates a substrate-independent integration of SIT and PCIT, advancing molecularly imprinted polymers toward practical bioseparation applications.

The topological morphology of multipod nanoparticles greatly influences their interactions with biological interfaces, exhibiting great potential for biomedical applications. However, a formidable challenge lies in balancing simple fabrication and precise structural control, as traditional formation process involving multiple steps and meticulous surface modification. Herin, a one-pot tandem self-assembly strategy based on nanoemulsion-directed anisotropic assembly and intrinsic chemistry-mediated self-assembly for the streamlined synthesis of hollow mesoporous silica multipods (MHMPs) is reported. By controlling growth time and assembly dynamics, a diversity of well-defined multipods with precise topological control is formed. The resulting MHMPs exhibit remarkable performance in Pb2+ remediation and biomedicine, achieving 86 % blood lead removal efficiency as their topology-enhanced biointeractions. Overall, this tandem self-assembly strategy provides a simplified and general route for precisely controlling multipods morphology, holding great potential for practical environmental and biomedical applications.

The highly selective separation of bioactive molecules from complex structural analogs still faces significant challenges. Herein, a novel molecularly imprinted aerogel microspheres adsorbent (BC/TA-Fe-MIPs) with a three-dimensional ordered porous structure was successfully fabricated using bacterial cellulose (BC) and tannic acid (TA) as building blocks by sequential assembly of ice-crystal-confined metal coordination crosslinking, template molecular adsorption, and glutaraldehyde covalent crosslinking, for the selective adsorption of cordycepin (COR). The results indicated that BC/TA-Fe-MIPs exhibited a high adsorption capacity (159.32 mu mol g-1 based on the Langmuir model) and an outstanding imprinting factor (2.57) toward COR. Furthermore, BC/TA-Fe-MIPs demonstrated superior selectivity for COR compared to its structural analogs, with a selectivity coefficient of 1.93 for its isomer 2 '-deoxyadenosine. XPS analysis confirmed that the recognition mechanism was primarily governed by hydrogen bonding between the phenolic hydroxyl groups of TA and COR. In addition, BC/TA-Fe-MIPs maintained over 85% of their initial capacity after five adsorption-desorption cycles and successfully enriched COR from cordyceps flower extract. All of these suggest that the BC/TA-Fe-MIPs developed in a green and easy synthesis process show great potential as a stable and selective adsorbent for the purification of cordycepin. Moreover, this work presents a feasible strategy for constructing high-performance separation materials from natural building blocks for adsorption and separation applications.

Metal-organic frameworks (MOFs) have surfaced as exceptionally promising porous materials, primarily because of their ability to form stable structures with remarkable properties. These frameworks possess numerous pores that enhance ion transport in capacitive deionization (CDI) applications. However, significant hurdles persist with MOFs, including a scarcity of active sites and complications related to water stability, which impede their broader usage. Additionally, the charge-discharge cycles that take place during operation can induce lattice distortions, a phenomenon associated with the Jahn-Teller effect that is intrinsic to MOF structures. To address this challenge, we have synthesized hybrid nanoparticles composed of MIL-101(Fe) and cellulose nanocrystals (CNCs), referred to as MCNCs, featuring a stable structure that integrates a it-conjugated framework characterized by extensive electron delocalization and a narrowed HOMO-LUMO gap. Additionally, the high density of active sites provided by C--O groups promotes efficient redox reactions, enhancing the NH4+ capture capability. The produced MCNCs polymer demonstrates remarkable electro-adsorption properties and significant structural durability, achieving an impressive specific capacitance of 119.05 F g-1 at 0.5 A g-1. Leveraging the exceptional pseudocapacitive attributes of the MCNCs, we have engineered a hybrid capacitive deionization system that not

Aerogel materials exhibit superior mechanical and adsorptive separation properties, showing considerable potential in resource recovery applications. A phosphorylated bacterial cellulose aerogel adsorbent (BC-VPA) with enhanced mechanical stability has been synthesized via a one-step process involving directional freezing and low-temperature UV polymerization, specifically designed for the selective removal of uranium from aqueous solutions. The results indicated that phosphate polymer modification leads to a more compact spatial structure within the aerogel, which is crucial for its mechanical stability and directly correlates with the polymer concentration. BC-VPA displays exceptional uranium adsorption capacity during the endothermic process. According to Langmuir model fitting, the maximum adsorption capacity of uranium by BC-VPA can reach 577.28 mg g- 1 at 298 K. Furthermore, BC-VPA exhibits high selectivity for uranium ions and excellent removal efficiency in simulated seawater adsorption tests and dynamic adsorption experiments, underscoring its practicality for potential application. By employing directional freezing and low-temperature UV polymerization, this study effectively produces aerogels with strong mechanical stability and exceptional adsorption capabilities, providing a novel technique for creating useful bacterial cellulose-based adsorbents.

In recent years, the heavy metal cadmium pollution generated during the production and recycling process of photovoltaic industries such as cadmium telluride (CdTe) solar cells has attracted high attention. Herein, a sustainable strategy for fabricating covalent organic frameworks (COFs) functionalized cellulose nanofibers aerogel was proposed by a self-assembly method, which was designed for cadmium (II) ions (Cd2+) adsorption. Environmentally compatible cellulose, derived from abundant biomass straws, can provide a macroscopic platform for integrating multi-site sulfonated covalent organic frameworks (SO3H@COFs) synthesized through a one-step method. The hierarchical structure of the cellulose aerogel encapsulating nanofibers substantially enhanced the effective adsorption of Cd2+ by generating permeation channels and abundant binding sites. The synergistic effects of electrostatic attraction, coordination, and pore-driven adsorption mechanism enhanced Cd2+ adsorption, as supported by experimental data, characterization, and density functional theory (DFT) calculations. Based on investigations conducted under varying pH conditions and in the presence of interfering metal cations, it was recommended to combine this approach with other treatment technologies as a preliminary step for optimal adsorption performance. This work provides new avenues for the design and fabrication of advanced macroscopic COFs composite materials, with promising potential for application in wastewater treatment.

To address the critical issue of pesticide loss (up to similar to 60 % of applied pesticides) caused by splash, rebound, and rain-induced runoff, which contaminates groundwater and poses risks to human health and the environment, this study presents a novel interfacial engineering strategy to enhance herbicide droplet deposition and adhesion on (super)hydrophobic leaf surfaces. This strategy utilizes the interfacial assembly of amyloid-like protein/laponite (PTB/LAP) nanocomposites to create stable oil-in-water (O/W) nanoemulsions with strong foliar affinity. Specifically, bovine serum albumin (BSA) is first adsorbed onto laponite (LAP) surfaces via hydrogen bonding; subsequent introduction of tris(2-carboxyethyl)phosphine (TCEP) reduces BSA's disulfide bonds, triggering in situ amyloid-like aggregation of surface-bound BSA (PTB) to form PTB/LAP nanocomposites. These nanocomposites significantly enhance interfacial activity, reducing aqueous surface tension to similar to 36 mN/m, and form elastic-dominated interfacial networks with excellent mechanical strength. The resulting PTB/LAP nanoemulsion remains stable (mean droplet size similar to 250 nm, polydispersity index <0.2) for over 180 days. It exhibits rapid, nanosecond-scale anchoring on leaf cuticles, yielding a 3.6-times higher retention rate than BSA/LAP emulsions under simulated heavy rainfall (150 mm per day). At an equal dosage of 2,4-D isooctyl ester, the nanoemulsion achieves 96.9 % efficacy against shepherd's purse, 2.2 times higher than conventional emulsifiable concentrates (ECs), which only achieve similar to 43.5 % efficacy. Furthermore, the PTB/LAP nanoemulsion demonstrates exceptional biocompatibility, with 100 % survival of non-target land snails after 120 h and no significant cytotoxicity or genotoxicity in CHL cell assays. This work provides an eco-friendly, scalable platform for improving pesticide efficiency, reducing environmental contamination, and advancing sustainable agriculture.

Herein, MXene/Co3O4 layered membranes with peroxymonosulfate (PMS) activation performance were fabricated by embedding porous Co3O4 nanobelt (NB) into MXene nanosheets for dyes removal. The physiochemical properties of membranes were characterized using XRD, SEM, TEM, EDS, ATR-FTIR, XPS, zeta potential measurements, contact angle measurements and ESR techniques. The Co3O4 NB not only regulates interlayer channels, but also acts as catalysts for the degradation of small molecule organic pollutants via PMS activation. The resulting layered membrane shows enhanced dye removal performance, attributed to the regulated dspacing and newly endowed excellent PMS activation performance. The separation efficiencies of MXene/Co3O4 layered membrane for dyes are over 97.5 %, the permeabilities are over 473 L m-2h-1 bar-1, and the permeability is about 2.5 times that of neat MXene membrane. Moreover, the established dynamic degradation system demonstrated a remarkable small molecular dye (e.g. Methylene blue) removal efficiency nearly 100 %, emphasizing its applicability and potential in practical applications. Additionally, the separation and catalytic degradation mechanisms of MXene/Co3O4 layered membrane for dyes were verified and analyzed through related tests and characterizations. This work provides a new dual-regulation strategy of d-spacing and catalytic performance to enhance the removal ability of layered membranes for different organic pollutants in wastewater.

Membrane fouling has always been a bottleneck restricting the development of membrane separation technology. Simple hydrophilic modification is difficult to effectively cope with serious flux attenuation. Thus, the “single defense” mechanism is not enough to build a stable barrier against oil deposition under filtration conditions. In this study, we have prepared a “multiple defense” antifouling membrane designed by integrating micro-nanosphere coating, hydrogel and hydrophilic polymer brush layer for improving the oil pollution resistance of the membrane, where tannic acid and 3-aminopropyltriethoxysilane (TA-APTES) coating is first deposited on the surface of poly(vinylidene fluoride) porous membrane and then covered with poly(sulfobetaine) zwitterionic nanohydrogel (PSBMA) by TA-Fe3+ dual autocatalysis at room temperature. Finally, poly(ethylene glycol) brush (PEG) is controllably grafted through ring-opening reaction of amino and epoxy. The membrane achieves high water permeance (more than 16000 L m−2 h−1·bar−1), high emulsion permeance (more than 2000 L m−2 h−1·bar−1) and high oil-water separation efficiency (over 99.0%). The flux almost maintains zero attenuation during long-term operation (3 h) for various stable oil-in-water emulsions and even crude oil emulsions. The membrane also has excellent underwater anti-adhesion properties for crude oil. After the membrane covered with crude oil is immersed in water, the crude oil is immediately detached from the membrane surface.

Self-propelled nanomotors exhibit significant propulsion capabilities, which can enhance the efficiency of uptake of lead pollutant at low concertation. However, a persistent challenge remains in establishing effective speed control over nanomotors, as the movement of most motors is predominantly reliant on the concentration of available fuel. To adjust the speed of a halloysite-nanotube-based nanomotor, a temperature-responsive polymer brush is chemically grown onto the halloysite nanotubes (HNTs). This modification allows for the enlargement or constriction of the HNTs cavity in response to temperature change. Chemical modification on HNTs improves the effect of lead removal by increasing the adsorption sites, making it easier for grabbing ion. The mobility and adsorption abilities of the synthesized HNTs nanomotor exhibit significant variations at approximately 45 degrees C. To further study the adsorption capacity of Pb (II) by HNTs nanomotor reached an optimal level at a pH of 5.0 and peroxide concentrations of 5.0 wt%, reaching up to 49.936 mg g- 1, with saturation occurring within 40 min. We successfully fabricated nanosized self-propelled motors, the motion of which can be reversibly controlled by a thermally responsive brake, resulting in a lead removal efficiency of 98 %. Furthermore, 90 % of the original adsorption capacity was maintained after five repetitions. We envision that such artificial responsive nano systems could have significant applications in the controllable cargo transportation. The prepared material exhibited favorable biocompatibility, providing new research insights into the design and application of nanomotors in removing of Pb (II) from the bloodstream.

The simultaneous removal of persistent organic pollutants and toxic heavy metal ions from complex wastewater remains a significant challenge. This work presents a novel dual-functional composite material (ZIF67@MT-400 N-2), obtained via in-situ growth of ZIF67 on montmorillonite (MT) followed by optimized pyrolysis (400(degrees)C under N-2 atmosphere). This composite material uniquely combines the high porosity (515.34 m(2)/g) and abundant functional hydroxyl groups of MT with the efficient catalytic metal sites of ZIF67. The obtained ZIF67@MT400 N-2 exhibited exceptional activity in activating peroxymonosulfate (PMS) for the oxidative degradation of tetracycline (TC), achieving >90 % removal (k(obs) = 0.944 min(- 1)) within 3 min. It also demonstrated universal activity against bisphenol A (BPA), sulfadiazine (SDZ), Congo red (CR), and particularly 4-nitrophenol (4-NP, 100 % in 1 min). The composite also showed outstanding adsorption removal capacities for Pb (II) (99.65 mg g(- 1)) and Cd (II) (71.80 mg g(-1)), with rapid removal rates reaching 98.85 % and 71.23 % within 120 min, respectively. Impressively, in a complex system containing TC, Pb (II), and Cd (II), ZIF67@MT-400 N-2/PMS achieved 93 % TC degradation while simultaneously adsorbing 89 % Pb (II) and 70% Cd (II), demonstrating robust anti-interference capability. The strong host-guest interaction significantly suppressed Co2+ ion leaching compared to the control (ZIF67-400 N-2), maintaining >82 % TC degradation efficiency over four consecutive cycles and persistent efficiency (>90 % TC removal) in various real water matrices (tap water, lake water). Synergistic effects of various reactive oxidative species such as & sdot;OH, & sdot;SO4- , & sdot;O-2(-) , and O-1(2) contribute to the excellent degradation activity. Toxicity assessment indicated reduced ecological risk of TC degradation intermediates. We further demonstrated the possibility of ZIF67@MT-400 N-2 for purification of practical electroplating wastewater, and showed efficient elimination of organic substances and Ni ions.

Addressing global freshwater scarcity requires developing energy-efficient water purification technologies. Capacitive deionization (CDI) has emerged as a promising electrochemical adsorption method, the performance of which is governed by electrode properties. While organic electrodes benefit from tunable molecular structures and sustainability, their application is hindered by insufficient accessible active sites and limited electron delocalization, compromising both ion capacity and kinetics. Herein, we report a molecularly engineered n-delocalized organic molecule, denoted as NHCO, which contains strategically positioned redox-active C--O and C--N functional groups and forms an ordered molecular solid through intermolecular n-n interactions, enabling its use as a high-performance CDI electrode. The NHCO electrode exhibits a narrow bandgap (2.99 eV), extended n-conjugation, and highly reversible ion coordination chemistry, synergistically enhancing the electrochemical adsorption capacity and kinetics. This synergistic effect is corroborated by a combination of experimental studies, in-situ analyses, and extensive theoretical calculations. When configured into a CDI device, it delivers an outstanding desalination capacity of 120.06 mg g-1 and a fast time-averaged desalination rate of 4.39 mg g-1 min-1 at 1.4 V, alongside exceptional regeneration stability with 99.09% capacity retention over 200 cycles. Furthermore, the assembled CDI device demonstrates high removal efficiency for organic dyes and exhibits excellent biocompatibility, underscoring its potential as a sustainable platform for advanced water purification.