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Abstract Highly porous metal-organic framework (MOF) nanosheets have shown promising potential for efficient water sorption kinetics in atmospheric water harvesting (AWH) systems. However, the water uptake of single-component MOF absorbents remains limited due to their low water retention. To overcome this limitation, we present a strategy for fabricating vertically aligned MOF nanosheets on hydrogel membrane substrates (MOF-CT/PVA) to achieve ultrafast AWH with high water uptake. By employing directional growth of MOF nanosheets, we successfully create superhydrophilic MOF coating layer and pore channels for efficient water transportation to the crosslinked flexible hydrogel membrane. The designed composite water harvester exhibits ultrafast sorption kinetics, achieving 91.4% saturation within 15 min. Moreover, MOF-CT/PVA exhibits superior solar-driven water capture-release capacity even after 10 cycles of reuse. This construction approach significantly enhances the water vapor adsorption, offering a potential solution for the design of composite MOF-membrane harvesters to mitigate the freshwater crisis.

Abstract Chlorinated organic pollutants widely exist in aquatic environments and threaten human health. Catalytic approaches are proposed for their elimination, but sluggish degradation, incomplete dechlorination, and catalyst recovery remain extremely challenging. Here we show efficient dechlorination using ferrous oxide/graphene oxide catalytic membranes with strong nanoconfinement effects. Catalytic membranes are constructed by graphene oxide nanosheets with integrated ultrafine and monodisperse sub-5 nm nanoparticles through simple in-situ growth and filtration assembly. Density function theory simulation reveals that nanoconfinement effects remarkably reduce energy barriers of rate-limiting steps for iron (III)-sulfite complex dissociation to sulfite radicals and dichloroacetic acid degradation to monochloroacetic acid. Combining with nanoconfinement effects of enhancing reactants accessibility to catalysts and increasing catalyst-to-reactant ratios, the membrane achieves ultrafast and complete dechlorination of 180 µg L−1 dichloroacetic acid to chloride, with nearly 100% reduction efficiency within a record-breaking 3.9 ms, accompanied by six to seven orders of magnitude greater first-order rate constant of 51,000 min−1 than current catalysis. Meanwhile, the membranes exhibit quadrupled permeance of 48.6 L m−2 h−1 bar−1 as GO ones, because nanoparticles adjust membrane structure, chemical composition, and interlayer space. Moreover, the membranes show excellent stability over 20 cycles and universality for chlorinated organic pollutants at environmental concentrations.

Abstract Nanofiltration (NF) membranes are commonly supplied in spiral-wound modules, resulting in numerous drawbacks for practical applications (e.g., high operating pressure/pressure drop/costs). Vacuum-driven NF could be a promising and low-cost alternative by utilizing simple components and operating under an ultra-low vacuum pressure (

Abstract Two-dimensional (2D) materials, as adsorbents, have garnered great attention in removing heavy metal ions (HMIs) from drinking water due to their extensive exposed adsorption sites. Nevertheless, there remains a paucity of experimental research to remarkably unlock their adsorption capabilities and fully elucidate their adsorption mechanisms. In this work, exceptional lead ion (Pb2+) (a common HMI) removal capacity (up to 758 mg g−1) is achieved using our synthesized metallic 1T/1T′ phase 2D transition metal dichalcogenide (TMD, including MoS2, WS2, TaS2, and TiS2) nanosheets, which hold tremendous activated S chemisorption sites. The residual Pb2+ concentration can be reduced from 2 mg L−1 to 2 μg L−1 within 0.5 min, meeting the drinking water standards following World Health Organization guideline (Pb2+ concentrations

Abstract Flexible devices, such as soft bioelectronics and stretchable supercapacitors, have their practical performance limited by electrodes which are desired to have high conductivity and capacitance, outstanding mechanical flexibility and strength, great electrochemical stability, and good biocompatibility. Here, we report a simple and efficient method to synthesize a nanostructured conductive hydrogel to meet such criteria. Specifically, templated by a hyperconnective nanofibrous network from aramid hydrogels, the conducting polymer, polypyrrole, assembles conformally onto nanofibers through in-situ polymerization, generating continuous nanostructured conductive pathways. The resulting conductive hydrogel shows superior conductivity (72 S cm−1) and fracture strength (27.2 MPa). Supercapacitor electrodes utilizing this hydrogel exhibit high specific capacitance (240 F g−1) and cyclic stability. Furthermore, bioelectrodes of patterned hydrogels provide favorable bioelectronic interfaces, allowing high-quality electrophysiological recording and stimulation in physiological environments. These high-performance electrodes are readily scalable to applications of energy and power systems, healthcare and medical technologies, smart textiles, and so forth.

Abstract Rapid mass transfer in solid-solid reactions is crucial for catalysis. Although phoretic nanoparticles offer potential for increased collision efficiency between solids, their implementation is hindered by limited interaction ranges. Here, we present a self-driven long-range electrophoresis of organic nanocrystals facilitated by a rationally designed photogenerated outer electric field (OEF) on their surface. Employing perylene-3,4,9,10-tetracarboxylic dianhydride (PTCDA) molecular nanocrystals as a model, we demonstrate that a directional OEF with an intensity of 13.6-0.4 kV m−1 across a range of 25–200 μm. This OEF-driven targeted electrophoresis of PTCDA nanocrystals onto the microplastic surface enhances the activity for subsequent decomposition of microplastics (196.8 mg h−1) into CO2 by solid-solid catalysis. As supported by operando characterizations and theoretical calculations, the OEF surrounds PTCDA nanocrystals initially, directing from the electron-rich (0 1 1) to the hole-rich $$(11\bar{2})$$ ( 11 2 ¯ ) surface. Upon surface charge modulation, the direction of OEF changes toward the solid substrate. The OEF-driven electrophoretic effect in organic nanocrystals with anisotropic charge enrichment characteristics indicates potential advancements in realizing effective solid-solid photocatalysis.

Three-dimensional (3D) microfibrillar network represents an important structural design for various natural tissues and synthetic aerogels but achieving high mechanical properties for synthetic 3D microfibrillar networks remains challenging. Here, the authors report an ultrastrong polymeric aerogels involving self-assembled 3D networks of aramid nanofiber composites with high nodal connectivity.

Over the last few decades, developing ultra-permeable nanofiltration (UPNF) membranes has been a focus research area to support NF-based water treatment. Nevertheless, there have been ongoing debates and doubts on the need for UPNF membranes. In this work, we share our perspectives on why UPNF membranes are desired for water treatment. We analyze the specific energy consumption (SEC) of NF processes under various application scenarios, which reveals the potential of UPNF membranes for reducing SEC by 1/3 to 2/3 depending on the prevailing transmembrane osmotic pressure difference. Furthermore, UPNF membranes could potentially enable new process opportunities. Vacuum-driven submerged NF-modules could be retrofitted to existing water/wastewater treatment plants, offering lower SEC and lower cost compared to conventional NF systems. Their use in submerged membrane bioreactors (NF-MBR) can recycle wastewater into high-quality permeate water, which enables energy-efficient water reuse in a single treatment step. The ability for retaining soluble organics may further extend the application of NF-MBR for anaerobic treatment of dilute municipal wastewater. Critical analysis of membrane development reveals huge rooms for UPNF membranes to attain improved selectivity and antifouling performance. Our perspective paper offers important insights for the future development of NF-based water treatment technology, which could potentially lead to a paradigm shift in this burgeoning field.

The development of highly water-permeable membranes is key for the treatment of high salinity waters. Here the authors enhance the water permeability of a metal-organic framework nanoporous membrane via an intra-crystalline defect engineering strategy.

Fouling is a critical consideration for the design of thin-film composite (TFC) nanofiltration membranes. Traditional wisdom believes that fouling propensity is primarily dictated by membrane surface properties while porous substrates play little role (on the basis on the latter have no effect on the foulant-membrane interaction). Nevertheless, porous substrates can regulate the water transport pathways, resulting in uneven water flux distribution over the membrane surface. For the first time, we experimentally investigated the micro-scale water flux distribution for nanofiltration membranes with different substrate porosities and the impact of such flux distribution pattern on fouling. With gold nanoparticles as tracers, we demonstrated more evenly distributed water flux at increasing substrate porosity. This was found to effectively alleviate membrane fouling by eliminating localized hot spots of high flux. Furthermore, higher substrate porosity also effectively enhanced the membrane water permeance due to the optimized water transport pathways. Our study reveals the fundamental relationship between the micro-scale transport behavior and the membrane fouling propensity, which provides a firm basis for the rational design of TFC membranes toward better separation performance.

Salinity gradient power (SGP) derived from sea and fresh water through reverse electrodialysis (RED) is an emerging discipline with huge potential for carbon-free energy harvesting. SGP technology is still in an infant stage and there is a need for accurate mathematical tools to study its energy harvesting process. Previous models assume a constant salinity gradient with a continuous flow of sea water with constant salinity. In the case of recycling used sea water, such assumption is no longer valid because the salinity gradient reduces with operating time. This paper presents a generalized RED model that covers both of the continuous and recycle modes. It combines an improved kinetic battery module (KiBaM) with an electrical circuit module (ECM), for capturing the behaviors of both RED stacks operating in continuous mode (C-mode) and those in recycle mode (R-mode). To intuitively describe the compound effects of salinity variation and concentration polarization on electrical performance of the R-mode RED stack, nonlinear capacity effects (i.e., recovery effect and rate capacity effect) and self-consumed effect are introduced into the proposed model. The derivation and extraction procedures of the proposed model are included. An RED stack prototype with 50 pairs of alternating membranes is constructed for model validation. Various pulsed and constant current discharge experimental tests are performed to validate the accuracy of the proposed model.

The selective transport of water/ions through conventional forward osmosis (FO) membranes is largely impeded by solution-diffusion and internal concentration polarization (ICP). Herein, we report a novel air nanobubbles (ANBs) incorporated sandwich-structured carbon nanotube membrane (CNM) for highly permeable and stable FO desalination by taking advantage of the nanofluidic transport at the solid/liquid/vapor interface. Fluorinated multi-walled carbon nanotubes (F-MWCNTs) were assembled as the superhydrophobic interlayer between a hydrophilic cellulose acetate (CA) layer and a hydrophilic polyacrylonitrile (PAN) nanofibrous layer. The trapped ANBs in the superhydrophobic F-MWCNT layer crucially regulated the continuous water flow and effectively prevented salt diffusion. When tested with DI water as feed solution (FS) and 1 ​M NaCl as draw solution (DS), the ANBs incorporated sandwich-structured CNM achieved high water flux (158.0 ​L ​m−2 ​h−1) and ultralow reverse salt flux (0.4 ​g ​m−2 ​h−1) simultaneously, far beyond the state-of-the-art FO membranes. The PAN nanofibrous layer well protected the entrapped ANBs to allow a more durable FO performance. An ANBs-regulated nanofluidic flow model was proposed to elucidate selective water/salt transport mechanism. This work revealed the feasibility of ANBs incorporated membranes for osmosis-driven processes.

The microbial safety of swimming pool waters (SPWs) becomes increasingly important with the popularity of swimming activities. Disinfection aiming at killing microbes in SPWs produces disinfection by-products (DBPs), which has attracted considerable public attentions due to their high frequency of occurrence, considerable concentrations and potent toxicity. We reviewed the latest research progress within the last four decades on the regulation, formation, exposure, and treatment of DBPs in the context of SPWs. This paper specifically discussed DBP regulations in different regions, formation mechanisms related with disinfectants, precursors and other various conditions, human exposure assessment reflected by biomarkers or epidemiological evidence, and the control and treatment of DBPs. Compared to drinking water with natural organic matter as the main organic precursor of DBPs, the additional human inputs (i.e., body fluids and personal care products) to SPWs make the water matrix more complicated and lead to the formation of more types and greater concentrations of DBPs. Dermal absorption and inhalation are two main exposure pathways for trihalomethanes while ingestion for haloacetic acids, reflected by DBP occurrence in human matrices including exhaled air, urine, blood, and plasma. Studies show that membrane filtration, advanced oxidation processes, biodegradation, thermal degradation, chemical reduction, and some hybrid processes are the potential DBP treatment technologies. The removal efficiency, possible mechanisms and future challenges of these DBP treatment methods are summarized in this review, which may facilitate their full-scale applications and provide potential directions for further research extension. Keywords: Disinfectants, Disinfection by-products (DBP), Precursors, Human exposure, DBP treatment

The aquaporin-based biomimetic thin-film composite membrane (ABM-TFC) has demonstrated superior separation performance and achieved successful commercialization. The larger-scale production of the ABM membrane requires an appropriate balance between the performance and manufacturing cost. This study has systematically investigated the effects of proteoliposome concentration, protein-to-lipid ratio, as well as the additive on the separation performance of ABM for the purpose of finding the optimal preparation conditions for the ABM from the perspective of industrial production. Although increasing the proteoliposome concentration or protein-to-lipid ratio within a certain range could significantly enhance the water permeability of ABMs by increasing the loading of aquaporins in the selective layer, the enhancement effect was marginal or even compromised beyond an optimal point. Alternatively, adding cholesterol in the proteoliposome could further enhance the water flux of the ABM membrane, with minor effects on the salt rejection. The optimized ABM not only achieved a nearly doubled water flux with unchanged salt rejection compared to the control, but also demonstrated satisfactory filtration stability within a wide range of operation temperatures. This study provides a practical strategy for the optimization of ABM-TFC membranes to fit within the scheme of industrial-scale production.

Abstract We report a facile method for preparing silver-loaded membranes for point-of-use disinfection and disaster relief applications. A bio-inspired material, polydopamine, was coated onto a highly porous nanofibrous polyacrylonitrile substrate. We then take advantage of the redox properties of polydopamine to form silver nanoparticles in situ. These nanoparticles were uniformly distributed on the surface of nanofibers with no apparent agglomeration at a silver loading up to 4.36 wt.% (cPAN-Ag1.5). The silver-incorporated membrane cPAN-Ag1.5 achieved a high pure water flux of 130 Lm−2 h−1 at 10-cm water head, demonstrating the feasibility of energy-efficient gravity-driven filtration and eliminating the need for electrical power. The strong anti-bacterial activity and high physical rejection of the membrane led to an excellent disinfection power, with no viable bacterial cells detected in its permeate water. The membrane exhibited >7 log reduction for E. coli and >6 log reduction for B. subtilis. The strategy reported here provides an efficient and green route to synthesize point-of-use membranes. Combining their excellent permeability and disinfection effectiveness, these membranes offer an ideal solution to water supply in disaster-affected areas.

This paper focuses on a Hybrid Process that uses feed salinity dilution and osmotic power recovery from Pressure Retarded Osmosis (PRO) to achieve higher overall water recovery. This reduces the energy consumption and capital costs of conventional seawater desalination and water reuse processes. The Hybrid Process increases the amount of water recovered from the current 66.7% for conventional seawater desalination and water reuse processes to a potential 80% through the use of reclaimed water brine as an impaired water source. A reduction of up to 23% in energy consumption is projected via the Hybrid Process. The attractiveness is amplified by potential capital cost savings ranging from 8.7%–20% compared to conventional designs of seawater desalination plants. A decision matrix in the form of a customizable scorecard is introduced for evaluating a Hybrid Process based on the importance of land space, capital costs, energy consumption and membrane fouling. This study provides a new perspective, looking at processes not as individual systems but as a whole utilizing strategic co-location to unlock the synergies available in the water-energy nexus for more sustainable desalination.

In this study, polyelectrolyte assembled functionalized graphene oxide (PE-GO) membranes were fabricated through a one-step charge facilitated deposition method for high performance dye/salt separation. According to the intercalation of polydopamine (PDA) and (ionic liquid) IL functional moieties into the GO membranes, the pore size of the resulted PE-pGO and PE-iGO membrane increased from 2.69 nm to 4.13 nm and 6.54 nm, respectively. Correspondingly, a pure water flux of 13.8 ± 2.2, 36.7 ± 3.4, and 52.1 ± 6.7 L m−1 h−1 bar−1 was achieved for PE-GO, PE-pGO and PE-iGO membrane, respectively. PE-iGO membrane with the largest pore size could be operated with significant water permeability (28.3 to 38.3 L m−1 h−1 bar−1) at a low operating pressure range of 0.5–2 bar (dye concentration = 100 ppm, salt concentration = 5 g/L). More importantly, functionalities introduced to the GO nanosheets are found to impact the dye adsorption to the membrane surface. The IL intercalation promotes the elution of dye molecules from the IL moieties at elevated pH, therefore enhancing the efficiency of alkaline washing of the membrane. By contrast, the intercalation of PDA weakens such efficiency due to its strong adhesion force to the dye molecules even at the alkaline condition.