Distinguishing homogeneous advanced oxidation processes in bulk water from heterogeneous surface reactions in organic oxidation.

Clarifying the reaction pathways at the solid-water interface and in bulk water solution is of great significance for the design of heterogeneous catalysts for selective oxidation of organic pollutants. However, achieving this goal is daunting because of the intricate interfacial reactions at the catalyst surface. Herein, we unravel the origin of the organic oxidation reactions with metal oxide catalysts, revealing that the radical-based advanced oxidation processes (AOPs) prevail in bulk water but not on the solid catalyst surfaces. We show that such differing reaction pathways widely exist in various chemical oxidation (e.g., high-valent Mn3+ and MnOX) and Fenton and Fenton-like catalytic oxidation (e.g., Fe2+ and FeOCl catalyzing H2O2, Co2+ and Co3O4 catalyzing persulfate) systems. Compared with the radical-based degradation and polymerization pathways of one-electron indirect AOP in homogeneous reactions, the heterogeneous catalysts provide unique surface properties to trigger surface-dependent coupling and polymerization pathways of a two-electron direct oxidative transfer process. These findings provide a fundamental understanding of catalytic organic oxidation processes at the solid-water interface, which could guide the design of heterogeneous nanocatalysts.

Free-standing membrane incorporating single-atom catalysts for ultrafast electroreduction of low-concentration nitrate.

The release of wastewaters containing relatively low levels of nitrate (NO3-) results in sufficient contamination to induce harmful algal blooms and to elevate drinking water NO3- concentrations to potentially hazardous levels. In particular, the facile triggering of algal blooms by ultra-low concentrations of NO3- necessitates the development of efficient methods for NO3- destruction. However, promising electrochemical methods suffer from weak mass transport under low reactant concentrations, resulting in long treatment times (on the order of hours) for complete NO3- destruction. In this study, we present flow-through electrofiltration via an electrified membrane incorporating nonprecious metal single-atom catalysts for NO3- reduction activity enhancement and selectivity modification, achieving near-complete removal of ultra-low concentration NO3- (10 mg-N L-1) with a residence time of only a few seconds (10 s). By anchoring Cu single atoms supported on N-doped carbon in a carbon nanotube interwoven framework, we fabricate a free-standing carbonaceous membrane featuring high conductivity, permeability, and flexibility. The membrane achieves over 97% NO3- removal with high N2 selectivity of 86% in a single-pass electrofiltration, which is a significant improvement over flow-by operation (30% NO3- removal with 7% N2 selectivity). This high NO3- reduction performance is attributed to the greater adsorption and transport of nitric oxide under high molecular collision frequency coupled with a balanced supply of atomic hydrogen through H2 dissociation during electrofiltration. Overall, our findings provide a paradigm of applying a flow-through electrified membrane incorporating single-atom catalysts to improve the rate and selectivity of NO3- reduction for efficient water purification.

Fluids and Electrolytes under Confinement in Single-Digit Nanopores.

Confined fluids and electrolyte solutions in nanopores exhibit rich and surprising physics and chemistry that impact the mass transport and energy efficiency in many important natural systems and industrial applications. Existing theories often fail to predict the exotic effects observed in the narrowest of such pores, called single-digit nanopores (SDNs), which have diameters or conduit widths of less than 10 nm, and have only recently become accessible for experimental measurements. What SDNs reveal has been surprising, including a rapidly increasing number of examples such as extraordinarily fast water transport, distorted fluid-phase boundaries, strong ion-correlation and quantum effects, and dielectric anomalies that are not observed in larger pores. Exploiting these effects presents myriad opportunities in both basic and applied research that stand to impact a host of new technologies at the water-energy nexus, from new membranes for precise separations and water purification to new gas permeable materials for water electrolyzers and energy-storage devices. SDNs also present unique opportunities to achieve ultrasensitive and selective chemical sensing at the single-ion and single-molecule limit. In this review article, we summarize the progress on nanofluidics of SDNs, with a focus on the confinement effects that arise in these extremely narrow nanopores. The recent development of precision model systems, transformative experimental tools, and multiscale theories that have played enabling roles in advancing this frontier are reviewed. We also identify new knowledge gaps in our understanding of nanofluidic transport and provide an outlook for the future challenges and opportunities at this rapidly advancing frontier.

Tailoring Interfaces for Enhanced Methanol Production from Photoelectrochemical CO2 Reduction.

Efficient and stable photoelectrochemical reduction of CO2 into highly reduced liquid fuels remains a formidable challenge, which requires an innovative semiconductor/catalyst interface to tackle. In this study, we introduce a strategy involving the fabrication of a silicon micropillar array structure coated with a superhydrophobic fluorinated carbon layer for the photoelectrochemical conversion of CO2 into methanol. The pillars increase the electrode surface area, improve catalyst loading and adhesion without compromising light absorption, and help confine gaseous intermediates near the catalyst surface. The superhydrophobic coating passivates parasitic side reactions and further enhances local accumulation of reaction intermediates. Upon one-electron reduction of the molecular catalyst, the semiconductor-catalyst interface changes from adaptive to buried junctions, providing a sufficient thermodynamic driving force for CO2 reduction. These structures together create a unique microenvironment for effective reduction of CO2 to methanol, leading to a remarkable Faradaic efficiency reaching 20% together with a partial current density of 3.4 mA cm-2, surpassing the previous record based on planar silicon photoelectrodes by a notable factor of 17. This work demonstrates a new pathway for enhancing photoelectrocatalytic CO2 reduction through meticulous interface and microenvironment tailoring and sets a benchmark for both Faradaic efficiency and current density in solar liquid fuel production.

Molecular Design of Functional Polymers for Silica Scale Inhibition.

Silica polymerization, which involves the condensation reaction of silicic acid, is a fundamental process with wide-ranging implications in biological systems, material synthesis, and scale formation. The formation of a silica-based scale poses significant technological challenges to energy-efficient operations in various industrial processes, including heat exchangers and water treatment membranes. Despite the common strategy of applying functional polymers for inhibiting silica polymerization, the underlying mechanisms of inhibition remain elusive. In this study, we synthesized a series of nitrogen-containing polymers as silica inhibitors and elucidated the role of their molecular structures in stabilizing silicic acids. Polymers with both charged amine and uncharged amide groups in their backbones exhibit superior inhibition performance, retaining up to 430 ppm of reactive silica intact for 8 h under neutral pH conditions. In contrast, monomers of these amine/amide-containing polymers as well as polymers containing only amine or amide functionalities present insignificant inhibition. Molecular dynamics simulations reveal strong binding between the deprotonated silicic acid and a polymer when the amine groups in the polymer are protonated. Notably, an extended chain conformation of the polymer is crucial to prevent proximity between the interacting monomeric silica species, thereby facilitating effective silica inhibition. Furthermore, the hydrophobic nature of alkyl segments in polymer chains disrupts the hydration shell around the polymer, resulting in enhanced binding with ionized silicic acid precursors compared to monomers. Our findings provide novel mechanistic insights into the stabilization of silicic acids with functional polymers, highlighting the molecular design principles of effective inhibitors for silica polymerization.

Rapid, Selective, and Chemical-Free Removal of Dissolved Silica from Water via Electrosorption: Feasibility and Mechanisms.

The unavoidable and detrimental formation of silica scale in engineered processes necessitates the urgent development of effective, economic, and sustainable strategies for dissolved silica removal from water. Herein, we demonstrate a rapid, chemical-free, and selective silica removal method using electrosorption. Specifically, we confirm the feasibility of exploiting local pH dynamics at the electrodes in flow-through electrosorption, achieved through a counterintuitive cell configuration design, to induce ionization and concomitant electrosorption of dissolved silica. In addition, to improve the feasibility of silica electrosorption under high-salinity solutions, we developed a silica-selective anode by functionalizing porous activated carbon cloths with aluminum hydroxide nanoparticles (Al(OH)3-p-ACC). The modification markedly enhances silica sorption capacity (2.8 vs 1.1 mgsilica ganode-1) and reduces the specific energy consumption (13.3 vs 19.8 kWh kgsilica-1). Notably, the modified electrode retains remarkable silica sorption capacity even in the presence of high concentrations of co-occurring ions (up to 100 mM NaCl). The mechanisms underlying the superior silica removal stability and selectivity with the Al(OH)3-p-ACC electrode are also elucidated, revealing a synergistic interaction involving outer-sphere and inner-sphere complexation between dissolved silica and Al(OH)3 nanoparticles on the electrodes. Moreover, we find that effective regeneration of the electrodes may be achieved by applying a reverse potential during discharge, although complete regeneration of the modified electrodes may necessitate alternative materials or process optimization. We recommend the adoption of feedwater-specific designs for the development of future silica-selective electrodes in electrosorption capable of meeting silica removal demands across a wide range of engineered systems.

The Future of Municipal Wastewater Reuse Concentrate Management: Drivers, Challenges, and Opportunities.

Water reuse is rapidly becoming an integral feature of resilient water systems, where municipal wastewater undergoes advanced treatment, typically involving a sequence of ultrafiltration (UF), reverse osmosis (RO), and an advanced oxidation process (AOP). When RO is used, a concentrated waste stream is produced that is elevated in not only total dissolved solids but also metals, nutrients, and micropollutants that have passed through conventional wastewater treatment. Management of this RO concentrate─dubbed municipal wastewater reuse concentrate (MWRC)─will be critical to address, especially as water reuse practices become more widespread. Building on existing brine management practices, this review explores MWRC management options by identifying infrastructural needs and opportunities for multi-beneficial disposal. To safeguard environmental systems from the potential hazards of MWRC, disposal, monitoring, and regulatory techniques are discussed to promote the safety and affordability of implementing MWRC management. Furthermore, opportunities for resource recovery and valorization are differentiated, while economic techniques to revamp cost-benefit analysis for MWRC management are examined. The goal of this critical review is to create a common foundation for researchers, practitioners, and regulators by providing an interdisciplinary set of tools and frameworks to address the impending challenges and emerging opportunities of MWRC management.

Mechanisms and models for water transport in reverse osmosis membranes: history, critical assessment, and recent developments.

Water scarcity is one of the greatest societal challenges facing humanity. Reverse osmosis (RO) desalination, a widely used membrane-based technology, has proven to be effective to augment water supply in water-stressed regions of our planet. However, progress in the design and development of RO membranes has been limited. To significantly enhance the performance of RO membranes, it is essential to acquire a deep understanding of the membrane separation and transport mechanisms. In this tutorial review, we cover the pivotal historical developments in RO technology, examine the chemical and physical properties of RO membrane materials, and critically review the models and mechanisms proposed for water transport in RO membranes. Based on recent experimental and computational findings, we conduct a thorough analysis of the key transport models-the solution-diffusion and pore-flow models-to assess their validity for accurately describing water transport in RO membranes. Our analysis involves examining the experimental evidence in favor of the solution-diffusion mechanism. Specifically, we explain whether the water content gradient within the membrane, cited as evidence for the key assumption in the solution-diffusion model, can drive a diffusive transport through RO membranes. Additionally, we review the recent molecular dynamics simulations which support the pore-flow mechanism for describing water transport in RO membranes. We conclude by providing future research directions aimed at addressing key knowledge gaps in water transport phenomena in RO membranes, with the goal of advancing the development of next-generation RO membranes.

Electrosorption Integrated with Bipolar Membrane Water Dissociation: A Coupled Approach to Chemical-free Boron Removal.

Boron removal from aqueous solutions has long persisted as a technological challenge, accounting for a disproportionately large fraction of the chemical and energy usage in seawater desalination and other industrial processes like lithium recovery. Here, we introduce a novel electrosorption-based boron removal technology with the capability to overcome the limitations of current state-of-the-art methods. Specifically, we incorporate a bipolar membrane (BPM) between a pair of porous carbon electrodes, demonstrating a synergized BPM-electrosorption process for the first time. The ion transport and charge transfer mechanisms of the BPM-electrosorption system are thoroughly investigated, confirming that water dissociation in the BPM is highly coupled with electrosorption of anions at the anode. We then demonstrate effective boron removal by the BPM-electrosorption system and verify that the mechanism for boron removal is electrosorption, as opposed to adsorption on the carbon electrodes or in the BPM. The effect of applied voltage on the boron removal performance is then evaluated, revealing that applied potentials above ∼1.0 V result in a decline in process efficiency due to the increased prevalence of detrimental Faradaic reactions at the anode. The BPM-electrosorption system is then directly compared with flow-through electrosorption, highlighting key advantages of the process with regard to boron sorption capacity and energy consumption. Overall, the BPM-electrosorption shows promising boron removal capability, with a sorption capacity >4.5 µmol g-C-1 and a corresponding specific energy consumption of <2.5 kWh g-B-1.

Precise Cation Separations with Composite Cation-Exchange Membranes: Role of Base Layer Properties.

Separation of specific ions from water could enable recovery and reuse of essential metals and nutrients, but established membrane technologies lack the high-precision selectivity needed to facilitate a circular resource economy. In this work, we investigate whether the cation/cation selectivity of a composite cation-exchange membrane (CEM), or a thin polymer selective layer on top of a CEM, may be limited by the mass transfer resistance of the underlying CEM. In our analysis, we utilize a layer-by-layer technique to modify CEMs with a thin polymer selective layer (∼50 nm) that has previously shown high selectivity toward copper over similarly sized metals. While these composite membranes have a CuCl2/MgCl2 selectivity up to 33 times larger than unmodified CEMs in diffusion dialysis, our estimates suggest that eliminating resistance from the underlying CEM could further increase selectivity twofold. In contrast, the CEM base layer has a smaller effect on the selectivity of these composite membranes in electrodialysis, although these effects could become more pronounced for ultrathin or highly conductive selective layers. Our results highlight that base layer resistance prevents selectivity factors from being comparable across diffusion dialysis and electrodialysis, and CEMs with low resistance are necessary for providing highly precise separations with composite CEMs.

Significance of Co-ion Partitioning in Salt Transport through Polyamide Reverse Osmosis Membranes.

Salt permeability of polyamide reverse osmosis (RO) membranes has been shown to increase with increasing feed salt concentration. The dependence of salt permeability on salt concentration has been attributed to the variation of salt partitioning with feed salt concentration. However, studies using various analytical techniques revealed that the salt (total ion) partitioning coefficient decreases with increasing salt concentration, in marked contrast to the observed increase in salt permeability. Herein, we thoroughly investigate the dependence of total ion and co-ion partitioning coefficients on salt concentration and solution pH. The salt partitioning is measured using a quartz crystal microbalance (QCM), while the co-ion partitioning is calculated from the measured salt partitioning using a modified Donnan theory. Our results demonstrate that the co-ion and total ion partitioning behave entirely differently with increasing salt concentrations. Specifically, the co-ion partitioning increased fourfold, while total ion partitioning decreased by 60% as the salt (NaCl) concentration increased from 100 to 800 mM. The increase in co-ion partitioning with increasing salt concentration is in accordance with the increasing trend of salt permeability in RO experiments. We further show that the dependence of salt and co-ion partitioning on salt concentration is much more pronounced at a higher solution pH. The good co-ion exclusion (GCE) model─derived from the solution-friction model─is used to calculate the salt permeability based on the co-ion partitioning coefficients. Our results show that the GCE model predicts the salt permeabilities in RO experiments relatively well, indicating that co-ion partitioning, not salt partitioning, governs salt transport through RO membranes. Our study provides an in-depth understanding of ion partitioning in polyamide RO membranes and its relationship with salt transport.

Microalgae Commercialization Using Renewable Lignocellulose Is Economically and Environmentally Viable.

Conventional phototrophic cultivation for microalgae production suffers from low and unstable biomass productivity due to limited and unreliable light transmission outdoors. Alternatively, the use of a renewable lignocellulose-derived carbon source, cellulosic hydrolysate, offers a cost-effective and sustainable pathway to cultivate microalgae heterotrophically with high algal growth rate and terminal density. In this study, we evaluate the feasibility of cellulosic hydrolysate-mediated heterotrophic cultivation (Cel-HC) for microalgae production by performing economic and environmental comparisons with phototrophic cultivation through techno-economic analysis and life cycle assessment. We estimate a minimum selling price (MSP) of 4722 USD/t for producing high-purity microalgae through Cel-HC considering annual biomass productivity of 300 t (dry weight), which is competitive with the conventional phototrophic raceway pond system. Revenues from the lignocellulose-derived co-products, xylose and fulvic acid fertilizer, could further reduce the MSP to 2976 USD/t, highlighting the advantages of simultaneously producing high-value products and biofuels in an integrated biorefinery scheme. Further, Cel-HC exhibits lower environmental impacts, such as cumulative energy demand and greenhouse gas emissions, than phototrophic systems, revealing its potential to reduce the carbon intensity of algae-derived commodities. Our results demonstrate the economic and environmental competitiveness of heterotrophic microalgae production based on renewable bio-feedstock of lignocellulose.

Origin of Limiting and Overlimiting Currents in Bipolar Membranes.

Bipolar membranes (BPMs), a special class of ion exchange membranes with the unique ability to electrochemically induce either water dissociation or recombination, are of growing interest for environmental applications including eliminating chemical dosage for pH adjustment, resource recovery, valorization of brines, and carbon capture. However, ion transport within BPMs, and particularly at its junction, has remained poorly understood. This work aims to theoretically and experimentally investigate ion transport in BPMs under both reverse and forward bias operation modes, taking into account the production or recombination of H+ and OH-, as well as the transport of salt ions (e.g., Na+, Cl-) inside the membrane. We adopt a model based on the Nernst-Planck theory, that requires only three input parameters─membrane thickness, its charge density, and pK of proton adsorption─to predict the concentration profiles of four ions (H+, OH-, Na+, and Cl-) inside the membrane and the resulting current-voltage curve. The model can predict most of the experimental results measured with a commercial BPM, including the observation of limiting and overlimiting currents, which emerge due to particular concentration profiles that develop inside the BPM. This work provides new insights into the physical phenomena in BPMs and helps identify optimal operating conditions for future environmental applications.

Ionization behavior of nanoporous polyamide membranes.

Escalating global water scarcity necessitates high-performance desalination membranes, for which fundamental understanding of structure-property-performance relationships is required. In this study, we comprehensively assess the ionization behavior of nanoporous polyamide selective layers in state-of-the-art nanofiltration (NF) membranes. In these films, residual carboxylic acids and amines influence permeability and selectivity by imparting hydrophilicity and ionizable moieties that can exclude coions. We utilize layered interfacial polymerization to prepare physically and chemically similar selective layers of controlled thickness. We then demonstrate location-dependent ionization of carboxyl groups in NF polyamide films. Specifically, only surface carboxyl groups ionize under neutral pH, whereas interior carboxyl ionization requires pH >9. Conversely, amine ionization behaves invariably across the film. First-principles simulations reveal that the low permittivity of nanoconfined water drives the anomalous carboxyl ionization behavior. Furthermore, we report that interior carboxyl ionization could improve the water-salt permselectivity of NF membranes over fourfold, suggesting that interior charge density could be an important tool to enhance the selectivity of polyamide membranes. Our findings highlight the influence of nanoconfinement on membrane transport properties and provide enhanced fundamental understanding of ionization that could enable novel membrane design.

Tailored design of nanofiltration membranes for water treatment based on synthesis-property-performance relationships.

Tailored design of high-performance nanofiltration (NF) membranes is desirable because the requirements for membrane performance, particularly ion/salt rejection and selectivity, differ among the various applications of NF technology ranging from drinking water production to resource mining. However, this customization greatly relies on a comprehensive understanding of the influence of membrane fabrication methods and conditions on membrane properties and the relationships between the membrane structural and physicochemical properties and membrane performance. Since the inception of NF, much progress has been made in forming the foundation of tailored design of NF membranes and the underlying governing principles. This progress includes theories regarding NF mass transfer and solute rejection, further exploitation of the classical interfacial polymerization technique, and development of novel materials and membrane fabrication methods. In this critical review, we first summarize the progress made in controllable design of NF membrane properties in recent years from the perspective of optimizing interfacial polymerization techniques and adopting new manufacturing processes and materials. We then discuss the property-performance relationships based on solvent/solute mass transfer theories and mathematical models, and draw conclusions on membrane structural and physicochemical parameter regulation by modifying the fabrication process to improve membrane separation performance. Next, existing and potential applications of these NF membranes in water treatment processes are systematically discussed according to the different separation requirements. Finally, we point out the prospects and challenges of tailored design of NF membranes for water treatment applications. This review bridges the long-existing gaps between the pressing demand for suitable NF membranes from the industrial community and the surge of publications by the scientific community in recent years.

Inorganic Scaling in Membrane Desalination: Models, Mechanisms, and Characterization Methods.

Inorganic scaling caused by precipitation of sparingly soluble salts at supersaturation is a common but critical issue, limiting the efficiency of membrane-based desalination and brine management technologies as well as other engineered systems. A wide range of minerals including calcium carbonate, calcium sulfate, and silica precipitate during membrane-based desalination, limiting water recovery and reducing process efficiency. The economic impact of scaling on desalination processes requires understanding of its sources, causes, effects, and control methods. In this Critical Review, we first describe nucleation mechanisms and crystal growth theories, which are fundamental to understanding inorganic scale formation during membrane desalination. We, then, discuss the key mechanisms and factors that govern membrane scaling, including membrane properties, such as surface roughness, charge, and functionality, as well as feedwater characteristics, such as pH, temperature, and ionic strength. We follow with a critical review of current characterization techniques for both homogeneous and heterogeneous nucleation, focusing on the strengths and limitations of each technique to elucidate scale-inducing mechanisms, observe actual crystal growth, and analyze the outcome of scaling behaviors of desalination membranes. We conclude with an outlook on research needs and future research directions to provide guidelines for scale mitigation in water treatment and desalination.

Molecular Simulations to Elucidate Transport Phenomena in Polymeric Membranes.

Despite decades of dominance in separation technology, progress in the design and development of high-performance polymer-based membranes has been incremental. Recent advances in materials science and chemical synthesis provide opportunities for molecular-level design of next-generation membrane materials. Such designs necessitate a fundamental understanding of transport and separation mechanisms at the molecular scale. Molecular simulations are important tools that could lead to the development of fundamental structure-property-performance relationships for advancing membrane design. In this Perspective, we assess the application and capability of molecular simulations to understand the mechanisms of ion and water transport across polymeric membranes. Additionally, we discuss the reliability of molecular models in mimicking the structure and chemistry of nanochannels and transport pathways in polymeric membranes. We conclude by providing research directions for resolving key knowledge gaps related to transport phenomena in polymeric membranes and for the construction of structure-property-performance relationships for the design of next-generation membranes.

Mining Nontraditional Water Sources for a Distributed Hydrogen Economy.

Securing decarbonized economies for energy and commodities will require abundant and widely available green H2. Ubiquitous wastewaters and nontraditional water sources could potentially feed water electrolyzers to produce this green hydrogen without competing with drinking water sources. Herein, we show that the energy and costs of treating nontraditional water sources such as municipal wastewater, industrial and resource extraction wastewater, and seawater are negligible with respect to those for water electrolysis. We also illustrate that the potential hydrogen energy that could be mined from these sources is vast. Based on these findings, we evaluate the implications of small-scale, distributed water electrolysis using disperse nontraditional water sources. Techno-economic analysis and life cycle analysis reveal that the significant contribution of H2 transportation to costs and CO2 emissions results in an optimal levelized cost of hydrogen at small- to moderate-scale water electrolyzer size. The implications of utilizing nontraditional water sources and decentralized or stranded renewable energy for distributed water electrolysis are highlighted for several hydrogen energy storage and chemical feedstock applications. Finally, we discuss challenges and opportunities for mining H2 from nontraditional water sources to achieve resilient and sustainable economies for water and energy.

Catalytic Membrane with Copper Single-Atom Catalysts for Effective Hydrogen Peroxide Activation and Pollutant Destruction.

The superior catalytic property of single-atom catalysts (SACs) renders them highly desirable in the energy and environmental fields. However, using SACs for water decontamination is hindered by their limited spatial distribution and density on engineered surfaces and low stability in complex aqueous environments. Herein, we present copper SACs (Cu1) anchored on a thiol-doped reactive membrane for water purification. We demonstrate that the fabricated Cu1 features a Cu-S2 coordination─one copper atom is bridged by two thiolate sulfur atoms, resulting in high-density Cu-SACs on the membrane (2.1 ± 0.3 Cu atoms per nm2). The Cu-SACs activate peroxide to generate hydroxyl radicals, exhibiting fast kinetics, which are 40-fold higher than those of nanoparticulate Cu catalysts. The Cu1-functionalized membrane oxidatively removes organic pollutants from feedwater in the presence of peroxide, achieving efficient water purification. We provide evidence that a dual-site cascade mechanism is responsible for in situ regeneration of Cu1. Specifically, one of the two linked sulfur atoms detaches the oxidized Cu1 while donating one electron, and an adjacent free thiol rebinds the reduced Cu(I)-S pair, retrieving the Cu-S2 coordination on the reactive membrane. This work presents a universal, facile approach for engineering robust SACs on water-treatment membranes and broadens the application of SACs to real-world environmental problems.

Synergistic Nanowire-Enhanced Electroporation and Electrochlorination for Highly Efficient Water Disinfection.

Conventional water disinfection methods such as chlorination typically involve the generation of harmful disinfection byproducts and intensive chemical consumption. Emerging electroporation disinfection techniques using nanowire-enhanced local electric fields inactivate microbes by damaging their outer structures without byproduct formation or chemical dosing. However, this physical-based method suffers from a limited inactivation efficiency under high water flux due to an insufficient contact time. Herein, we integrate electrochlorination with nanowire-enhanced electroporation to achieve a synergistic flow-through process for efficient water disinfection targeting bacteria and viruses. Electroporation at the cathode induces sub-lethal damages on the microbial outer structures. Subsequently, electrogenerated active chlorine at the anode aggravates these electroporation-induced injuries to the level of lethal damage. This sequential flow-through disinfection system achieves complete disinfection (>6.0-log) under a very high water flux of 2.4 × 104 L/(m2 h) with an applied voltage of 2.0 V. This disinfection efficiency is 8 times faster than that of electroporation alone. Further, the specific energy consumption for the disinfection by this novel process is extremely low (8 × 10-4 kW h/m3). Our results demonstrate a promising method for rapid and energy-efficient water disinfection by coupling electroporation with electrochlorination to meet vital needs for pathogen elimination.