Demulsification with simultaneous water purification by coupling filtration and enhanced oil droplet coalescence at anode interface in an electrochemical reactor.

With the increasing demand of recycling disposal of industrial wastewater, oil-in-water (O/W) emulsion has been paid much attention in recent years owing to its high oil content. However, due to the presence of surfactant and salt, the emulsion was usually stable with complex physicochemical interfacial properties leading to increased processing difficulty. Herein, a novel flow-through electrode-based demulsification reactor (FEDR) was well designed for the treatment of saline O/W emulsion. In contrast to 53.7% for electrical demulsification only and 80.3% for filtration only, the COD removal efficiency increased to 92.8% under FEDR system. Moreover, the pore size of electrode and the applied voltage were two key factors that governed the FEDR demulsification performance. By observing the morphology of oil droplets deposited layer after different operation conditions and the behavior of oil droplets at the electrode surface under different voltage conditions, the mechanism was proposed that the oil droplets first accumulated on the surface of flow-through electrode by sieving effect, subsequently the gathered oil droplets could further coalesce with the promoting effect of the anode, leading to a high-performing demulsification. This study offers an attractive option of using flow-through electrode to accomplish the oil recovery with simultaneous water purification.

A Janus membrane with electro-induced multi-affinity interfaces for high-efficiency water purification.

Drinking water with micropollutants is a notable environmental concern worldwide. Membrane separation is one of the few methods capable of removing micropollutants from water. However, existing membranes face challenges in the simultaneous and efficient treatment of small-molecular and ionic contaminants because of their limited permselectivity. Here, we propose a high-efficiency water purification method using a low-pressure Janus membrane with electro-induced multi-affinity. By virtue of hydrophobic and electrostatic interactions between the functional interfaces and contaminants, the Janus membrane achieves simultaneous separation of diverse types of organics and heavy metals from water via single-pass filtration, with an approximately 100% removal efficiency, high water flux (>680 liters m-2 hour-1), and 98% lower energy consumption compared with commercial nanofiltration membranes. The electro-induced switching of interfacial affinity enables 100% regeneration of membrane performance; thus, our work paves a sustainable avenue for drinking water purification by regulating the interfacial affinity of membranes.

Electrically Redox-Active Membrane with Switchable Selectivity to Contaminants for Water Purification.

Membrane technology provides an attractive approach for water purification but faces significant challenges in separating small molecules due to its lack of satisfactory permselectivity. In this study, a polypyrrole-based active membrane with a switchable multi-affinity that simultaneously separates small ionic and organic contaminants from water was created. Unlike conventional passive membranes, the designed membrane exhibits a good single-pass filtration efficiency (>99%, taking 1-naphthylamine and Pb2+ as examples) and high permeability (227 L/m2/h). Applying a reversible potential can release the captured substances from the membrane, thus enabling membrane regeneration and self-cleaning without the need for additives. Advanced characterizations reveal that potential switching alters the orientation of the doped amphipathic molecules with the self-alignment of the hydrophobic alkyl chains or the disordered sulfonate anions to capture the target organic molecules or ions via hydrophobic or electrostatic interactions, respectively. The designed smart membrane holds great promise for controllable molecular separation and water purification.

Electrically Controlled Adsorptive Membranes with Tunable Affinity for Selective Chromium (VI) Separation from Water.

Ionic contaminants such as Cr(VI) pose a challenge for water purification using membrane-based processes. However, existing membranes have low permeability and selectivity for Cr(VI). Therefore, in this study, we prepared an electrically controlled adsorptive membrane (ECAM-L) by coating a loose Cl--doped polypyrrole layer on a carbon nanotube substrate, and we evaluated the performance of ECAM-L for Cr(VI) separation from water. We also used electrochemical quartz crystal microbalance measurements and molecular dynamics and density functional theory calculations to investigate the separation mechanisms. The adsorption and desorption of Cr(VI) could be modulated by varying the electrostatic interactions between ECAM-L and Cr(VI) via potential control, enabling the cyclic use of the ECAM-L without additional additives. Consequently, the oxidized ECAM-L showed high Cr(VI) removal performance (<50 µg/L) and treatment capacity (>3500 L/m2) at a high water flux (283 L/m2/h), as well as reusability after the application of a potential. Our study demonstrates an efficient membrane design for water decontamination that can selectively separate Cr(VI) through a short electric stimulus.

Sequential Demulsification through the Hydrophobic-Hydrophilic-Hydrophobic Filtration Layer toward High-Performing Oil Recovery.

Demulsification using membranes is a promising method to coalesce highly stable emulsified oil droplets for oil recovery. Nevertheless, a structure of the current filtration medium that is not efficient for oil droplet coalescence impedes rapid permeability, thereby inevitably restricting their practical applications. Herein, we report a hydrophobic-hydrophilic-hydrophobic (3H) demulsification medium that exhibits a benchmark permeability of ∼2.1 × 104 L m-2 h-1 with a demulsification efficiency of >98.0%. Remarkably, this 3H demulsification medium maintains over 90% demulsification efficiency in the oil-in-water (O/W) emulsions with a wide range of surfactant concentrations, which shows excellent applicability. Based on the combined results of quasi situ microscope images and molecular dynamics simulations, we show that the polydimethylsiloxane-modified hydrophobic layer facilitates the capture and coalescence of oil droplets, the hydrophilic inner layer assists in squeezing the coalescence of enlarged droplets, and the third hydrophobic layer accelerates the discharge of demulsified oil to sustain permeability. The sequential demulsification mechanism between this 3H filtration layer provides a general guide for designing a demulsifying membrane with high demulsification efficiency and high flux toward oil recovery.

Synergetic Oxidation of the Hydroxyl Radical and Superoxide Anion Lowers the Benzoquinone Intermediate Conversion Barrier and Potentiates Effective Aromatic Pollutant Mineralization.

Regulation of the free radical types is crucial but challenging in the ubiquitous heterogeneous catalytic oxidation for chemosynthesis, biotherapy, and environmental remediation. Here, using aromatic pollutant (AP) removal as a prototype, we identify the massive accumulation of the benzoquinone (BQ) intermediate in the hydroxyl radical (•OH)-mediated AP degradation process. Theoretical prediction and experiments demonstrate that BQ is both a Lewis acid and base because of its unique molecular and electronic structure caused by the existence of symmetrical carbonyl groups; therefore, it is hard to be electrophilically added by oxidizing •OH as a result of the high reaction energy barrier (ΔG = 1.74 eV). Fortunately, the introduction of the superoxide anion (•O2-) significantly lowers the conversion barrier (ΔG = 0.91 eV) of BQ because •O2- can act as the electron donor and acceptor simultaneously, electrophilically and nucleophilically add to BQ synchronously, and break it down. Subsequently, the breakdown products can then be further oxidized by •OH until completely mineralized. Such synergistic oxidation based on •OH and •O2- timely eliminates BQ, potentiates AP mineralization, and inhibits electrode fouling caused by high-resistance polymeric BQ; more importantly, it effectively reduces toxicity, saves energy and costs, and decreases the environmental footprint, evidenced by the life cycle assessment.

Revealing the Pore Size-Dependent Sorption Mechanism of Toluene and Cetane in Porous Carbon by Nuclear Magnetic Resonance.

The adsorption of contaminants by porous carbon has been extensively studied by conventional isotherm and kinetic methods. However, the co-adsorption behavior and sorption sites of multiple contaminants in different-sized pores remain unclear. Herein, the nuclear magnetic resonance (NMR) approach is performed to investigate the adsorption mechanism of toluene and cetane in the confined space of carbon at the molecular level. The ring current effect induces the variation in the NMR chemical shifts of in-pore adsorbed toluene and cetane, realizing the identification of pore-dependent adsorption sites for contaminant removal. Cetane has a slower adsorption kinetic but a higher binding energy than toluene, which could squeeze toluene from micropores to larger pores with increasing adsorption quantity. This leads to a stronger competitive adsorption effect in small micropores than in mesopores. Accordingly, hierarchical porous carbons are determined to be the most effective adsorbents for the adsorption of coexisting contaminants. This study not only provides an effective NMR method to reveal the adsorption mechanism in the confined space of porous carbon at the molecular level but also offers new insights into the pore size-dependent adsorption of activated carbon for petroleum contaminant treatment.

Selective Oxygen Activation to Reactive Oxygen Species on a Carbon Layer-Encapsulated CuxO Electrocatalyst for Water Purification.

In situ synthesis of reactive oxygen species (ROS) on demand via oxygen activation (OA) is significant in biological, chemical, and environmental fields. Thus, the design of OA catalysts with adequate reactivity, durability, and selectivity is critical but challenging. Here, we report a CuxO@C core@shell photoelectrode prepared by encapsulating Cu/Cu2O/CuO into a carbon layer through anodic electropolymerization (electrophoresis-coupled self-assembly of carbon quantum dots). Theoretical prediction and experiments indicate that the carbon layer can effectively facilitate optical trapping and charge transfer, thus promoting photoelectric conversion and anti-photocorrosion performance of CuxO@C. The inner CuxO core acts as an electron reservoir and continuously injects electrons into the outer carbon layer shell, and the carbon atoms adjacent to oxygen-enriched functional groups (C-O-C and -COOH) in the electron-rich carbon layer work as the reactive sites to adsorb O2 and donate electrons to the antibonding orbital [lowest unoccupied molecular orbital (π*)] of dioxygen. Optimized adsorption and hydrogenation of the critical intermediates (*O2, *OOH, and *H2O2) and thermodynamically tunable O-O bond cleavage enable O2 being selectively reduced to the superoxide anion and hydroxyl radical via the mixed multielectron processes consisting of one- and three-electron pathways. Sulfamethoxazole, an emerging refractory organic contaminant widely present in the environment, can be effectively degraded (∼100% removal) in such an electrochemical platform, benefiting from the abundant ROS generated in situ. Our findings demonstrate an innovative strategy to develop highly efficient and selective OA catalysts for practical water purification.

Facilitating Molecular Activation and Proton Feeding by Dual Active Sites on Polymeric Carbon Nitride for Efficient CO2 Photoreduction.

Photoreduction of CO2 provides an appealing way to alleviate the energy crisis and manage the global carbon balance but is limited by the high activation energy and the rate-limiting proton transfer. We now develop a dual-site strategy for high-efficiency CO2 conversion through polarizing CO2 molecules at pyridine N vacancies and accelerating the intermediate protonation by protonated pyridine N adjacent to nitrogen vacancies on polymeric carbon nitride. Our photocatalysts with atomic-level engineered active sites manifest a high CO production rate of 1835 µmol g-1 h-1 , 183 times higher than the pristine bulk carbon nitride. Theoretical prediction and experimental studies confirm that such excellent performance is attributed to the synergistic effect between vacant and protonated pyridine N in decreasing the formation energy of the key *COOH intermediates and the efficient electron transfer relay facilitated by the defect-induced shallow trap state and homogeneous charge mediators.

Protonated carbon nitride elicits microalgae for water decontamination.

Comprehending the effects of synthetic nanomaterials on natural microorganisms is critical for the development of emerging nanotechnologies. Compared to artificial inactivation of microbes, the up-regulation of biological functions should be more attractive due to the possibility of discovering unexpected properties. Herein, a nanoengineering strategy was employed to tailor g-C3N4 for the metabolic regulation of algae. We found that surface protonated g-C3N4 (P-C3N4) as a nanopolymeric elicitor enabled the reinforced biological activity of Microcystis aeruginosa and Scenedesmus for harmful substances removal. Metabolomics analysis suggested that synthetic nanoarchitectures induced moderate oxidative stress of algae, with up-regulated biosynthesis of extracellular polymeric substances (EPS) for resisting the physiological damage caused by toxic substances in water. The formation of oxidative .O2- contributed to over five-fold enhancement in the biodecomposition of harmful aniline. Our study demonstrates a synergistic biotic-abiotic platform with valuable outcomes for various customized applications.

Evaluation of degradation performance toward antiviral drug ribavirin using advanced oxidation process and its relations to ecotoxicity evolution.

The rapid spread of coronavirus disease 2019 has increased the consumption of some antiviral drugs, wherein these are discharged into wastewater, posing risks to the ecosystem and human health. Therefore, efforts are being made for the development of advanced oxidation processes (AOPs) to remediate water containing these pharmaceuticals. Here, the toxicity evolution of the antiviral drug ribavirin (RBV) was systematically investigated during its degradation via the UV/TiO2/H2O2 advanced oxidation process. Under optimal conditions, RBV was almost completely eliminated within 20 min, although the mineralization rate was inadequate. Zebrafish embryo testing revealed that the ecotoxicity of the treated RBV solutions increased at some stages and decreased as the reaction time increased, which may be attributed to the formation and decomposition of various transformation products (TPs). Liquid chromatography-mass spectrometry analysis along with density functional theory calculations helped identify possible toxicity increase-causing TPs, and quantitative structure activity relationship prediction revealed that most TPs exhibit higher toxicity than the parent compound. The findings of this study suggest that, in addition to the removal rate of organics, the potential ecotoxicity of treated effluents should also be considered when AOPs are applied in wastewater treatment.

Visualization of Electrochemically Accessible Sites in Flow-through Mode for Maximizing Available Active Area toward Superior Electrocatalytic Ammonia Oxidation.

Active chlorine species-mediated electrocatalytic oxidation is a promising strategy for ammonia removal in decentralized wastewater treatment. Flow-through electrodes (FTEs) provide an ideal platform for this strategy because of enhanced mass transport and sufficient electrochemically accessible sites. However, limited insight into spatial distribution of electrochemically accessible sites within FTEs inhibits the improvement of reactor efficiency and the reduction of FTE costs. Herein, a microfluidic-based electrochemical system is developed for the operando observation of microspatial reactions within pore channels, which reveals that reactions occur only in the surface layer of the electrode thickness. To further quantify the spatial distribution, finite element simulations demonstrate that over 75.0% of the current is accumulated in the 20.0% thickness of the electrode surface. Based on these findings, a gradient-coated method for the active layer was proposed and applied to a Ti/RuO2 porous electrode with an optimized pore diameter of ∼25 µm, whose electrochemically accessible surface area was 381.7 times that of the planar electrode while alleviating bubble entrapment. The optimized reactor enables complete ammonia removal with an energy consumption of 60.4 kWh kg-1 N, which was 24.2% and 39.9% less than those with pore diameters of ∼3 µm and ∼90 µm, respectively.

Spatiotemporal variation and risk assessment of phthalate acid esters (PAEs) in surface water of the Yangtze River Basin, China.

Spatiotemporal variation, potential sources, and risk assessment of phthalate acid esters (PAEs) in surface water of the Yangtze River Basin were investigated. Total cumulative concentrations of 15 PAEs (Σ15PAEs) ranged from 1594.47 ng·L-1 to 5155.50 ng·L-1, and the dominant components were di (2-ethylhexyl) phthalate (DEHP) (35.9-60.1%), dibutyl phthalate (DBP) (16.6-38.8%), and diisobutyl phthalate (DIBP) (6.7-18.2%). Σ15PAEs in surface water showed a trend of normal season > wet season > dry season. Σ15PAEs increased from the upstream (2341.7 ± 428.5 ng·L-1) to the mid- and downstream (3892.1 ± 842.8 and 2504.3 ± 355.9 ng·L-1, respectively), indicating the influence from production and consumptions of plasticizer-containing items. PAEs additives emission from daily necessities (28.9-62.3%) and construction and industrial production (18.7-31.2%) were the dominant sources of PAEs in this study. The risk quotient (RQ) method was employed to assess the potential ecological risk of specific components. High ecological risk of DEHP to the sensitive algae and crustacean, together with moderate ecological risk of DEHP and DIBP to the sensitive fish species were found in surface water regardless of the region and season. The spatial distribution of RQ values showed an increasing trend from the upstream to the midstream and downstream of the Yangtze River, indicating the influences from regional urbanization and industrialization levels.

Systematic Design of a Flow-Through Titanium Electrode-Based Device with Strong Oil Droplet Rejection Property for Superior Oil-in-Water Emulsion Separation Performance.

Oily wastewater treatment has been restricted by the existence of stable oil-in-water (O/W) emulsions containing micrometer-sized oil droplets. However, the strong adhesion and stacking of emulsified oil droplets on the surface of current separation media cause serious fouling of the treatment unit and the rapid decline of treatment efficiency. Herein, a novel flow-through titanium (Ti) electrode-based filtration device with remarkable oil droplet rejection property was well designed for the continuously separating O/W emulsion. In contrast to the pristine Ti foam, the permeance of the TiO2 nanoarray-coated Ti foam (NATF) increased from 2538 to 4364 L m-2 h-1 bar-1 through gravity-driven flow. Further, more than ∼70% permeability can be maintained after 6 h of O/W emulsion filtration using the current device, the value of which was markedly higher than that of conventional oil/water separation filters (less than 5%). According to the results of wettability test, the super-oil-repellent surface endowed by this nanoarray structure primarily avoided the formation of a compact oil fouling layer. When the voltage was applied, accompanied by the electrophoresis effect, redistribution of surfactant molecules on the surface of oil droplets induced by an electric field made them readily captured by the microbubbles continuously generated from the electrode, thereby rapidly migrating these bubble-adhered oil droplets far from the filtration medium.

[Selective Adsorption of Au(â ¢) by Activated Carbon Supported Polythioamides and Adsorption Mechanism].

By using in-situ synthesis of polythioamide (PTA) on activated carbon (AC), a polythioamide-modified activated carbon-based adsorbent (AC-PTA) was successfully prepared and used to study the selective adsorption effect and mechanism of Au(Ⅲ) in wastewater. The results showed that AC-PTA exhibited excellent selective adsorption to Au(Ⅲ) in the coexisting solution of multiple metal ions in a wide pH range (<5.0). The adsorption effect for Au(Ⅲ) was the best at a pH of 2 and 3; the concentration of residue Au(Ⅲ) was less than 0.1 mg·L-1, whereas other metals were barely adsorbed. The selective adsorption process for Au(Ⅲ) conformed to the pseudo-second kinetic model (R2=0.9853), the thermodynamic process conformed to the Langmuir isotherm process (R2=0.9936), and adsorption capacity was up to 2018 mg·g-1. Such advantages were mainly attributed to the coordination interaction between the -C([FY=,1]S)NH- functional groups on the AC-PTA surface and Au(Ⅲ), the electrostatic adsorption between the positive AC-PTA and negative Au(Ⅲ) complex anions, and the direct reduction of Au(Ⅲ) by AC. The successful recovery of gold was finally realized by burning the adsorbed AC-PTA at 1000℃ for 4 hours under air conditions, and solid gold with a mass fraction higher than 90.0% was obtained. This study provided the possibility for selective adsorption and recovery of low concentration Au(Ⅲ) from actual wastewater.

Removal of nickel and copper ions in strongly acidic conditions by in-situ formed amyloid fibrils.

The research investigated a novel strategy that can synchronously remove Ni2+ and Cu2+ by synthesizing amyloid fibrils under harsh conditions. The adsorption capacity of Ni2+ and Cu2+ increased by 18.5% and 34.1% respectively in the in-situ scenario as compared to that Ni2+ and Cu2+ were introduced after amyloid fibrils preparation, meantime, it avoids the generation of acidic waste liquid in the process of preparing amyloid fibrils. The adsorption behaviors of Ni2+ and Cu2+ can be well described by the pseudo-second-order kinetic model and Langmuir isotherm. The functional groups of amide, hydroxyl, and carboxyl played determining roles in the adsorption process. Moreover, when the amyloid fibrils were prepared in the presence of Ni2+ and Cu2+, i.e., the in-situ adsorption scenario, metal ions tended to occupy the functional sites, inhibit protein aggregation, and affect long amyloid fibrils synthesis accordingly. Metal ion-binding site prediction server was used to predict the binding sites of metal ions towards the protein sequence within amyloid fibrils, and the metal ion was observed to preferentially bind to a particular residue such as glutamic acid, cysteine, and serine. The amyloid fibrils be potentially valuable for the removal of heavy metals in strongly acidic wastewater such as acidic mining drainage.

Insight into the Key Role of Cr Intermediates in the Efficient and Simultaneous Degradation of Organic Contaminants and Cr(VI) Reduction via g-C3N4-Assisted Photocatalysis.

Photocatalysis provides an impetus for the synergetic removal of Cr(VI) and organic contaminants, but the generation of Cr intermediates and their potential oxidizability may be overlooked in pollutant conversion. Herein, the Cr intermediates in the Cr(VI) reduction process were emphasized in Cr(VI)/bisphenol A (BPA) by using graphitic carbon nitride as a photocatalyst. The active species for BPA photodegradation in the BPA system and Cr(VI)/BPA system suggested that the Cr(VI) reduction process indeed promotes BPA photodegradation. Electron paramagnetic resonance (EPR) of Cr complexes and in situ variable-temperature EPR analysis demonstrated Cr(V) intermediate (g = 1.978) generation in Cr(VI) reduction and its oxidization for BPA degradation in photocatalysis. By adding the electron donor Na2SO3, BPA degradation was induced in Cr(VI)/BPA solution, further confirming the positive effect of Cr(V). Moreover, the difference in BPA degradation products in the BPA/air, Cr(VI)/BPA/air, and Cr(VI)/BPA/Ar systems indirectly explained why the Cr(V) intermediate was involved in BPA degradation. Density functional theory calculations revealed that photogenerated electrons can reduce the free energy (0.98 eV) of converting Cr(VI) into Cr(V), which can facilitate the subsequent Cr(V) oxidation step for BPA degradation. This work contributes to the exploration of the Cr(VI) reduction process and the synergistic removal of organic pollutants in Cr(VI)/organics systems.

Mo,Fe-codoped metal phosphide nanosheets derived from Prussian blue analogues for efficient overall water splitting.

Designing non-precious electrocatalysts with multiple active centers and durability toward overall water splitting is of great significance for storing renewable energy. This study reports a low-cost Mo, Fe codoped NiCoPx electrocatalysts derived from Co-Fe Prussian blue analogue and following phosphorization process. Benefitted from the optimized electronic configuration, hierarchical structure and abundant active sites, the Mo,Fe-NiCoPx/NF electrode has shown competitive oxygen evolution reaction (ƞ10 = 197 mV) and hydrogen evolution reaction performance (ƞ10 = 99 mV) when the current density is 10 mA cm-2 in 1 M KOH solution. Moreover, the integrated water splitting device assembled by Mo,Fe-NiCoPx/NF as both anode and cathode only needs a voltage of 1.545 V to reach 10 mA cm-2. Density functional theory results further confirm that the Mo, Fe codoped heterostructure can synergistically optimize the d-band center and Gibbs free energy during electrocatalytic processes, thus accelerating the kinetics of electrochemical water splitting. This work demonstrates the importance of rational combination of metal doping and interface engineering for advanced catalytic materials.

Optimization of a Hierarchical Porous-Structured Reactor to Mitigate Mass Transport Limitations for Efficient Electrocatalytic Ammonia Oxidation through a Three-Electron-Transfer Pathway.

Regulation of fast three-electron-transfer processes for electrocatalytic oxidation of ammonia to nitrogen by achieving efficient generation and utilization of active sites is the optimal strategy in ammonia-containing wastewater treatment. However, the limited number of accessible active sites and sluggish interfacial mass transfer are two main bottlenecks restricting conventional ammonia oxidation configurations. Herein, we develop a macroporous Ni foam electrode integrated with vertically aligned two-dimensional mesoporous Ni2P nanosheets to create sufficient exposure of active centers. A novel ammonia oxidation reactor with the developed hierarchical porous-structured electrodes was assembled to construct an intensified microfluidic process with flow-through operation to mitigate macroscopic mass transport limitations. The confined microreaction space in the hierarchical porous reactor further promotes spontaneous nanoscale diffusion/convection of the target contaminant to high-valence Ni sites and enhances the microscopic mass transfer. The combined results of electrochemical measurements and in situ Raman spectra showed that the ammonia degradation mechanism results from direct oxidation by the high-valence Ni, significantly different from the conventional indirect active-chlorine-species-mediated oxidation. The optimized reactor achieves high-efficiency three-electron-transfer ammonia conversion with an ammonia removal efficiency of ∼70% from an initial concentration of ∼1400 mg/L and byproduct production of ∼4%, significantly superior to a conversion unit comprising a featureless Ni-based electrode in the immersed configuration, which had >50% byproduct yield. 20 days of continuous operation under variable conditions achieved >90% ammonia degradation performance and an energy consumption of 25.42 kW h kg-1 N (1 order of magnitude lower than the active-chlorine-mediated process), showing the potential of the reactor in medium-concentration ammonia-containing wastewater treatment.

Emerging graphitic carbon nitride-based membranes for water purification.

Membrane separation is a promising technology that can effectively remove various existing contaminants from water with low energy consumption and small carbon footprint. The critical issue of membrane technology development is to obtain a low-cost, stable, tunable and multifunctional material for membrane fabrication. Graphitic carbon nitride (g-C3N4) has emerged as a promising membrane material, owing to the unique structure characteristics and outstanding catalytic activity. This review paper outlined the advanced material strategies used to regulate the molecule structure of g-C3N4 for membrane separation. The presentative progresses on the applications of g-C3N4-based membranes for water purification have been elaborated. Essentially, we highlighted the innovation integration of physical separation, catalysis and energy conversion during water purification, which was of great importance for the sustainability of water treatment techniques. Finally, the continuing challenges of g-C3N4-based membranes and the possible breakthrough directions in the future research was prospected.