Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 149
Filtrar
Mais filtros

Base de dados
País/Região como assunto
Tipo de documento
Intervalo de ano de publicação
1.
Chem Soc Rev ; 53(9): 4374-4399, 2024 May 07.
Artigo em Inglês | MEDLINE | ID: mdl-38529541

RESUMO

Membrane-based separation is one of the most energy-efficient methods to meet the growing need for a significant amount of fresh water. It is also well-known for its applications in water treatment, desalination, solvent recycling, and environmental remediation. Most typical membranes used for separation-based applications are thin-film composite membranes created using polymers, featuring a top selective layer generated by employing the interfacial polymerization technique at an aqueous-organic interface. In the last decade, various manufacturing techniques have been developed in order to create high-specification membranes. Among them, the creation of ultrathin polyamide membranes has shown enormous potential for achieving a significant increase in the water permeation rate, translating into major energy savings in various applications. However, this great potential of ultrathin membranes is greatly hindered by undesired transport phenomena such as the geometry-induced "funnel effect" arising from the substrate membrane, severely limiting the actual permeation rate. As a result, the separation capability of ultrathin membranes is still not fully unleashed or understood, and a critical assessment of their limitations and potential solutions for future studies is still lacking. Here, we provide a summary of the latest developments in the design of ultrathin polyamide membranes, which have been achieved by controlling the interfacial polymerization process and utilizing a number of novel manufacturing processes for ionic and molecular separations. Next, an overview of the in-depth assessment of their limitations resulting from the substrate membrane, along with potential solutions and future perspectives will be covered in this review.

2.
Nano Lett ; 2024 Jun 07.
Artigo em Inglês | MEDLINE | ID: mdl-38847451

RESUMO

Nanofiltration membranes with both high water permeance and selectivity are perpetually studied because of their applications in water purification. However, these two critical attributes are considered to be mutually exclusive. Here, we introduce a polar solvent, dichloromethane, in place of the apolar hexane used for decades as the organic phase for membrane interfacial polymerization synthesis to solve this dilemma. When a polar solvent as the organic phase is combined with a solvent-resistant aramid nanofibrous hydrogel film as the water phase, monomer enrichment in the reaction zone leads to a polyamide nanofiltration membrane with densely distributed nanobubble features, enhanced nanoporosity, and a loosened backbone. Benefiting from these structural features, the resulting membrane exhibits superior properties with a combination of high water permeance (52.7 L m-2 h-1 bar-1) and selectivity (water/Na2SO4, 36 bar-1; NaCl/Na2SO4, 357 bar-1), outperforming traditional nanofiltration membranes. We envision that this novel technology involving polar solvent systems and the water phase of nanofibrous hydrogel would provide new opportunities for membrane development for environmental engineering.

3.
Small ; 20(5): e2305807, 2024 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-37731008

RESUMO

Surfactant-like contaminants (SLCs) with distinctive amphiphilic structures have become a global concern in wastewater due to their toxicity and persistency. Despite extensive efforts, achieving efficient and selective SLCs removal remains challenging because of their wide range of molecular weights and complex functional group compositions. Superhydrophobic nanoparticles can potentially tackle this challenge by targeting the long oleophilic chains of SLCs. However, conventional contact angle measurements hinder hydrophobicity characterization and corresponding selectivity research because of the powder morphology of nanoparticles. Herein, the authors offered information regarding the distribution of water molecular probes in surfaces and proposed a quantitative characterization approach based on low-field nuclear magnetic resonance. Through synthesizing superhydrophobic and hydrophilic polydopamine nanospheres with similar morphologies, the selective adsorption potential of superhydrophobic nanoparticles for SLCs is systematically demonstrated. As revealed by the interaction mechanisms, the superhydrophobic surface of nanospheres increased its affinity and selectivity for SLCs adsorption by enhancing hydrophobic interactions. Superhydrophobic modification achieved ten times the adsorption capacity of sodium dodecyl benzene sulfonate, an exemplified surfactant, compared with pristine nanoparticles. By regulated self-polymerization, the superhydrophobic nanospheres are coated onto the surface of a 3D sponge and enable efficient selective SLCs adsorption from highly polluted leachate matrices with long-term stability and reusability.

4.
Environ Sci Technol ; 58(32): 14271-14281, 2024 Aug 13.
Artigo em Inglês | MEDLINE | ID: mdl-39078411

RESUMO

Sudden jump of transmembrane pressure (TMP) in membrane bioreactors (MBRs), associated with abrupt aggravation of membrane fouling, limits practical applications of MBRs and calls for effective mitigation strategies. While the TMP jump is generally related to the bacterial activity of biocakes, the mechanisms underlying the TMP jump remain unclear. Herein, we conducted various backwash protocols with different nutrient (e.g., nitrate and sodium acetate) loadings on fouled membranes in MBRs to reveal the critical role of bacterial activity of biocakes for the TMP jump. The filtration tests showed a lower TMP jump rate for the membrane backwashed with a nutrient solution (a mixture of 180 mg/L NaNO3 and 200 mg/L NaAc, averaged at 1.40 kPa/d) than that backwashed with tap water (averaged at 3.56 kPa/d), implying that TMP jump could be efficiently mitigated by providing sufficient nutrients to biocake bacteria. The characterization of biocakes showed that high-nutrient solution backwash considerably increased bacterial viability and activity, while considerably reducing biomolecule accumulation on membranes. The keystone taxa (e.g., g_Aeromonas and o_Chitinophagaceae) in the network of nutrient-enriched biocake communities were involved in nitrate reduction and biomolecule degradation. Ecological null model analyses revealed that the deterministic manner mainly shaped biocake communities with high-nutrient availability. Overall, this study highlights the significance of the bacterial activity of biocakes for TMP development and provides potential alternatives for controlling membrane fouling.


Assuntos
Reatores Biológicos , Membranas Artificiais , Pressão , Filtração , Bactérias/metabolismo
5.
Environ Sci Technol ; 58(14): 6435-6443, 2024 Apr 09.
Artigo em Inglês | MEDLINE | ID: mdl-38551393

RESUMO

Nanovoids within a polyamide layer play an important role in the separation performance of thin-film composite (TFC) reverse osmosis (RO) membranes. To form more extensive nanovoids for enhanced performance, one commonly used method is to incorporate sacrificial nanofillers in the polyamide layer during the exothermic interfacial polymerization (IP) reaction, followed by some post-etching processes. However, these post-treatments could harm the membrane integrity, thereby leading to reduced selectivity. In this study, we applied in situ self-etchable sacrificial nanofillers by taking advantage of the strong acid and heat generated in IP. CaCO3 nanoparticles (nCaCO3) were used as the model nanofillers, which can be in situ etched by reacting with H+ to leave void nanostructures behind. This reaction can further degas CO2 nanobubbles assisted by heat in IP to form more nanovoids in the polyamide layer. These nanovoids can facilitate water transport by enlarging the effective surface filtration area of the polyamide and reducing hydraulic resistance to significantly enhance water permeance. The correlations between the nanovoid properties and membrane performance were systematically analyzed. We further demonstrate that the nCaCO3-tailored membrane can improve membrane antifouling propensity and rejections to boron and As(III) compared with the control. This study investigated a novel strategy of applying self-etchable gas precursors to engrave the polyamide layer for enhanced membrane performance, which provides new insights into the design and synthesis of TFC membranes.


Assuntos
Incrustação Biológica , Nanopartículas , Osmose , Nylons/química , Gravuras e Gravação , Membranas Artificiais , Água/química
6.
Environ Sci Technol ; 58(40): 18009-18019, 2024 Oct 08.
Artigo em Inglês | MEDLINE | ID: mdl-39329389

RESUMO

Advanced reduction processes (ARPs) are promising for pollutant removal in drinking water treatment. In this study, we demonstrated highly efficient reduction of bromate, a harmful disinfection byproduct, by coupling ARPs with an iron nanoparticles-intercalated graphene oxide (GO@FeNPs) catalytic membrane. In the presence of 1.0 mM sulfite (S(IV)), the GO@FeNPs membrane/S(IV) system achieved nearly complete removal of 80 µg/L bromate in 3 min. The first-order reaction rate constant for bromate removal in this system was 420 ± 42 min-1, up to 5 orders of magnitude faster than previously reported ARPs. The GO@FeNPs catalytic membrane may offer potential advantages of nanoconfinement and facilitated electron shuttling in addition to the high surface area of the fine FeNPs, leading to the remarkable ARP performance. The GO@FeNPs membrane showed excellent stability, maintaining >97.0% bromate removal over 20 cycles of repeated runs. The membrane can also be applied for fast catalytic reduction of other oxyanions, showing >98.0% removal of nitrate and chlorate. This work may present a viable option for utilizing high-performance reductive catalytic membranes for water decontamination.


Assuntos
Bromatos , Grafite , Sulfitos , Purificação da Água , Bromatos/química , Grafite/química , Sulfitos/química , Purificação da Água/métodos , Ferro/química , Poluentes Químicos da Água/química , Nanopartículas Metálicas/química , Catálise , Membranas Artificiais , Oxirredução
7.
Environ Sci Technol ; 58(37): 16632-16641, 2024 Sep 17.
Artigo em Inglês | MEDLINE | ID: mdl-39216011

RESUMO

Conductive nanofiltration (CNF) membranes hold great promise for removing small organic pollutants from water through enhanced Donnan exclusion and electrocatalytic degradation. However, current CNF membranes face limitations in conductivity, structural stability, and nanochannel control strategies. This work addresses these challenges by introducing aniline-functionalized carbon nanotubes (NH2-CNTs) as an interlayer. NH2-CNTs enhance the dispersibility and adhesion of pristine carbon nanotubes, leading to a more conductive and stable composite nanofiltration membrane. The redesigned NH2-CNTs interlayered conductive nanofiltration (NICNF) membrane exhibits a 10-fold increase in conductivity and a high response degree (80%) with excellent cyclic stability, surpassing existing CNF membranes. The synergistic effects of enhanced Donnan exclusion, voltage switching, and electrocatalysis enable the NICNF membrane to achieve selective recovery of mixed dyes, 98.97% removal of residual wastewater toxicity, and a 5.2-fold increase in permeance compared to the commercial NF270 membrane. This research paves the way for next-generation multifunctional membranes capable of the efficient recovery and degradation of toxic organic pollutants in wastewater.


Assuntos
Filtração , Membranas Artificiais , Nanotubos de Carbono , Poluentes Químicos da Água , Nanotubos de Carbono/química , Poluentes Químicos da Água/química , Compostos de Anilina/química , Águas Residuárias/química , Purificação da Água/métodos , Condutividade Elétrica
8.
Environ Sci Technol ; 57(6): 2548-2556, 2023 02 14.
Artigo em Inglês | MEDLINE | ID: mdl-36719958

RESUMO

Surface roughness has crucial influence on the fouling propensity of thin film composite (TFC) polyamide reverse osmosis (RO) membranes. A common wisdom is that rougher membranes tend to experience more severe fouling. In this study, we compared the fouling behaviors of a smooth polyamide membrane (RO-s) and a nanovoid-containing rough polyamide membrane (RO-r). Contrary to the traditional belief, we observed more severe fouling for RO-s, which can be ascribed to its uneven flux distribution caused by the "funnel effect". Additional tracer filtration tests using gold nanoparticles revealed a more patchlike particle deposition pattern, confirming the adverse impact of "funnel effect" on membrane water transport. In contrast, the experimentally observed lower fouling propensity of the nanovoid-containing rough membrane can be explained by: (1) the weakened "funnel effect" thanks to the presence of nanovoids, which can regulate the water transport pathway through the membrane and (2) the decreased average localized flux over the membrane surface due to the increased effective filtration area for the nanovoid-induced roughness features. The current study provides fundamental insights into the critical role of surface roughness in membrane fouling, which may have important implications for the future development of high-performance antifouling membranes.


Assuntos
Nanopartículas Metálicas , Purificação da Água , Osmose , Nylons , Substâncias Húmicas , Ouro , Membranas Artificiais , Água , Filtração
9.
Environ Sci Technol ; 57(4): 1819-1827, 2023 01 31.
Artigo em Inglês | MEDLINE | ID: mdl-36652351

RESUMO

Surfactant-assisted interfacial polymerization (IP) has shown strong potential to improve the separation performance of thin film composite polyamide membranes. A common belief is that the enhanced performance is attributed to accelerated amine diffusion induced by the surfactant, which can promote the IP reaction. However, we show enhanced membrane performance for Tween 80 (a common surfactant), even though it decreased the amine diffusion. Indeed, the membrane performance is closely related to its polyamide roughness features with numerous nanovoids. Inspired by the nanofoaming theory that relates the roughness features to nanobubbles degassed during the IP reaction, we hypothesize that the surfactant can stabilize the generated nanobubbles to tailor the formation of nanovoids. Accordingly, we obtained enlarged nanovoids when the surfactant was added below its critical micelle concentration (CMC). In addition, both the membrane permeance and selectivity were enhanced, thanks to the enlarged nanovoids and reduced defects in the polyamide layer. Increasing the concentration above CMC resulted in shrunken nanovoids and deteriorated performance, which can be ascribed to the decreased stabilization effect caused by micelle formation. Interestingly, better antifouling performance was also observed for the surfactant-assisted membranes. Our current study provides mechanistic insights into the critical role of surfactant during the IP reaction, which may have important implications for more efficient membrane-based desalination and water reuse.


Assuntos
Nylons , Tensoativos , Osmose , Micelas , Membranas Artificiais
10.
Environ Sci Technol ; 57(29): 10860-10869, 2023 07 25.
Artigo em Inglês | MEDLINE | ID: mdl-37428116

RESUMO

Thin film composite polyamide (TFC) nanofiltration (NF) membranes represent extensive applications at the water-energy-environment nexus, which motivates unremitting efforts to explore membranes with higher performance. Intrusion of polyamide into substrate pores greatly restricts the overall membrane permeance because of the excessive hydraulic resistance, while the effective inhibition of intrusion remains technically challenging. Herein, we propose a synergetic regulation strategy of pore size and surface chemical composition of the substrate to optimize selective layer structure, achieving the inhibition of polyamide intrusion effective for the membrane separation performance enhancement. Although reducing the pore size of the substrate prevented polyamide intrusion at the intrapore, the membrane permeance was adversely affected due to the exacerbated "funnel effect". Optimizing the polyamide structure via surface chemical modification of the substrate, where reactive amino sites were in situ introduced by the ammonolysis of polyethersulfone substrate, allowed for maximum membrane permeance without reducing the substrate pore size. The optimal membrane exhibited excellent water permeance, ion selectivity, and emerging contaminants removal capability. The accurate optimization of selective layer is anticipated to provide a new avenue for the state-of-the-art membrane fabrication, which opens opportunities for promoting more efficient membrane-based water treatment applications.


Assuntos
Nylons , Purificação da Água , Nylons/química , Membranas Artificiais , Filtração
11.
Environ Sci Technol ; 56(4): 2605-2616, 2022 02 15.
Artigo em Inglês | MEDLINE | ID: mdl-35072469

RESUMO

The development of membranes capable of precise solute-solute separation is still in its burgeoning stage without a standardized protocol for evaluating selectivity. Three types of membrane processes with different driving forces, including pressure-driven filtration, concentration difference-driven diffusion, and electric field-driven ion migration, have been applied in this study to characterize solute-solute selectivity of a commercial nanofiltration membrane. Our results demonstrated that selectivity values measured using different methods, or even different conditions with the same method, are generally not comparable. The cross-method incomparability is true for both apparent selectivity, defined as the ratio between concentration-normalized fluxes, and the more intrinsic selectivity, defined as the ratio between the permeabilities of solutes through the active separation layer. The difference in selectivity measured using different methods possibly stems from the fundamental differences in the driving force of ion transport, the effect of water transport, and the interaction between cations and anions. We further demonstrated the difference in selectivity measured using feed solutions containing single-salt species and that containing mixed salts. A consistent protocol with standardized testing conditions to facilitate fair performance comparison between studies is proposed.


Assuntos
Filtração , Membranas Artificiais , Cátions , Difusão , Soluções
12.
Environ Sci Technol ; 56(4): 2656-2664, 2022 02 15.
Artigo em Inglês | MEDLINE | ID: mdl-35113549

RESUMO

Interlayered thin-film nanocomposite (TFNi) membranes have been shown to achieve enhanced water permeance as a result of the gutter effect. Nevertheless, some studies report impaired separation performance after the inclusion of an interlayer. In this study, we resolve the competing mechanisms of water transport in the transverse direction vs that in the normal direction. To enable easy comparison, carbon nanotube (CNT)-incorporated TFNi membranes with an identical polyamide rejection layer but different interlayer thicknesses were investigated. While increasing the thickness of the CNT interlayer facilitates water transport in the transverse direction (therefore improving the gutter effect), it simultaneously increases its hydraulic resistance in the normal direction. An optimal water permeance of 13.0 ± 0.7 L m-2 h-1 bar-1, which was more than doubled over the control membrane of 6.1 ± 0.7 L m-2 h-1 bar-1, was realized at a moderate interlayer thickness, resulting from the trade-off between these two competing mechanisms. In this study, we demonstrate reduced membrane fouling and improved fouling reversibility for a TFNi membrane over its control without an interlayer, which can be attributed to its more uniform water flux distribution. The fundamental mechanisms revealed in this study lay a solid foundation for the future development of TFNi membranes toward enhanced separation properties and antifouling ability.


Assuntos
Incrustação Biológica , Nanotubos de Carbono , Incrustação Biológica/prevenção & controle , Membranas Artificiais , Nylons , Água
13.
Environ Sci Technol ; 56(19): 14038-14047, 2022 10 04.
Artigo em Inglês | MEDLINE | ID: mdl-36150164

RESUMO

Nanofiltration (NF), highly prospective for drinking water treatment, faces a challenge in simultaneously removing emerging contaminants while maintaining mineral salts, particularly divalent cations. To overcome this challenge, NF membranes possessing small pores concomitant with highly negatively charged surfaces were synthesized via a two-step fabrication strategy. The key is to generate a polyamide active layer having a loose and carboxyl group-abundant segment on top and a dense barrier segment underneath. This was achieved by restrained interfacial polymerization between trimesoyl chloride and partly protonated piperazine to form a highly depth-heterogeneous polyamide network, followed by second amidation in an organic environment to remove untethered polyamide fragments and associate malonyl chlorides with reserved amine groups to introduce more negative charges. Most importantly, on first-principle engineering the spatial architecture of the polyamide layer, amplifying asymmetric charge distribution was paired with the thinning of the vertical structure. The optimized membrane exhibits high salt/organic rejection selectivity and water permeance superior to most NF membranes reported previously. The rejections of eight emerging contaminants were in the range of 66.0-94.4%, much higher than the MgCl2 rejection of 41.1%. This new fabrication strategy, suitable for various diacyl chlorides, along with the new membranes so produced, offers a novel option for NF in potable water systems.


Assuntos
Água Potável , Nylons , Aminas , Cátions Bivalentes , Cloretos , Membranas Artificiais , Minerais , Nylons/química , Piperazina , Estudos Prospectivos , Sais
14.
Environ Sci Technol ; 56(14): 10308-10316, 2022 Jul 19.
Artigo em Inglês | MEDLINE | ID: mdl-35767677

RESUMO

Cosolvent-assisted interfacial polymerization (IP) can effectively enhance the separation performance of thin film composite (TFC) reverse osmosis (RO) membranes. However, the underlying mechanisms regulating the formation of their polyamide (PA) rejection films remain controversial. The current study reveals two essential roles of cosolvents in the IP reaction: (1) directly promoting interfacial vaporization with their lower boiling points and (2) increasing the solubility of m-phenylenediamine (MPD) in the organic phase, thereby indirectly promoting the IP reaction. Using a series of systematically chosen cosolvents (i.e., diethyl ether, acetone, methanol, and toluene) with different boiling points and MPD solubilities, we show that the surface morphologies of TFC RO membranes were regulated by the combined direct and indirect effects. A cosolvent favoring interfacial vaporization (e.g., lower boiling point, greater MPD solubility, and/or higher concentration) tends to create greater apparent thickness of the rejection layer, larger nanovoids within the layer, and more extensive exterior PA layers, leading to significantly improved membrane water permeance. We further demonstrate the potential to achieve better antifouling performance for the cosolvent-assisted TFC membranes. The current study provides mechanistic insights into the critical roles of cosolvents in IP reactions, providing new tools for tailoring membrane morphology and separation properties toward more efficient desalination and water reuse.

15.
Environ Sci Technol ; 56(7): 4518-4530, 2022 Apr 05.
Artigo em Inglês | MEDLINE | ID: mdl-35258928

RESUMO

Conventional separation membranes suffer from evitable fouling and flux decrease for water treatment applications. Herein, a novel protocol of electro-enhanced membrane separation is proposed for the efficient treatment of microsized emulsions (∼1 µm) by rationally designing robust electroresponsive copper metallic membranes, which could mitigate oil fouling and coenhance permeance (from ∼1026 to ∼2516 L·m-2·h-1·bar-1) and rejection (from ∼87 to ∼98%). High-flux Cu membranes exhibit superior ductility and electrical conductivity, enabling promising electroactivity. Separation performance and the fouling mechanism were studied under different electrical potentials and ionic strengths. Application of negative polarization into a large-pore (∼2.1 µm) Cu membrane is favorable to not only almost completely reject smaller-sized oil droplets (∼1 µm) but also achieve antifouling and anticorrosion functions. Moreover, surfactants around oil droplets might be redistributed due to electrostatic repulsion, which effectively enhances the steric hindrance effect between neighboring oil droplets, mitigating oil coalescence and consequently membrane fouling. Furthermore, due to the screening effect of surfactants, the presence of low-concentration salts increases the adsorption of surfactants at the oil-water interface, thus preventing oil coalescence via decreasing oil-water interfacial tension. However, under high ionic strengths, the fouling mechanism converts from cake filtration to a complete blocking model due to the reduced electrostatic repulsion between the Cu membrane and oil droplets. This work would provide mechanistic insights into electro-enhanced antifouling for not only oil emulsion separation but also more water treatment applications using rationally designed novel electroresponsive membranes.

16.
Environ Sci Technol ; 56(1): 556-563, 2022 01 04.
Artigo em Inglês | MEDLINE | ID: mdl-34928146

RESUMO

In this study, we performed a direct contact membrane distillation and successfully demonstrated the non-invasive imaging of surfactant-induced wetting using optical coherence tomography. This method enabled us to investigate the wetting kinetics, which was found to follow a "three-region" relationship between the wetting rate and surfactant concentration: the (i) nonwetted region, (ii) concentration-dependent region, and (iii) concentration-independent region at low, intermediate, and high surfactant concentrations, respectively. This wetting behavior was explained by the "autophilic effect", i.e., the wetting was caused by the transfer of surfactants from the water-vapor interface to the unwetted membrane and rendered this membrane hydrophilic, and then the wetting frontier moved forward under capillary forces. At region-(i), the surfactant concentration in the water-vapor interface (Clv) was too low to make the unwetted membrane sufficiently hydrophilic; thereby, the membrane could not be wetted. At region-(ii), due to the fast adsorption of the surfactant on the newly wetted membrane, the wetting rate was determined by the advection/diffusion of surfactants from the feed stream. Consequently, the wetting rate increased with the increases in the water flux and surfactant concentration. At region-(iii), the advection/diffusion provided excess surfactants for adsorption, and thus Clv reached its upper limit (maximum surface excess) and the wetting rate leveled off.


Assuntos
Tensoativos , Purificação da Água , Cinética , Membranas Artificiais , Tomografia de Coerência Óptica
17.
Environ Sci Technol ; 56(18): 12811-12827, 2022 09 20.
Artigo em Inglês | MEDLINE | ID: mdl-36048162

RESUMO

Nanofiltration (NF) membranes have been widely applied in many important environmental applications, including water softening, surface/groundwater purification, wastewater treatment, and water reuse. In recent years, a new class of piperazine (PIP)-based NF membranes featuring a crumpled polyamide layer has received considerable attention because of their great potential for achieving dramatic improvements in membrane separation performance. Since the report of novel crumpled Turing structures that exhibited an order of magnitude enhancement in water permeance ( Science 2018, 360 (6388), 518-521), the number of published research papers on this emerging topic has grown exponentially to approximately 200. In this critical review, we provide a systematic framework to classify the crumpled NF morphologies. The fundamental mechanisms and fabrication methods involved in the formation of these crumpled morphologies are summarized. We then discuss the transport of water and solutes in crumpled NF membranes and how these transport phenomena could simultaneously improve membrane water permeance, selectivity, and antifouling performance. The environmental applications of these emerging NF membranes are highlighted, and future research opportunities/needs are identified. The fundamental insights in this review provide critical guidance on the further development of high-performance NF membranes tailored for a wide range of environmental applications.


Assuntos
Filtração , Nylons , Membranas Artificiais , Nylons/química , Piperazinas , Água
18.
Environ Sci Technol ; 56(9): 5775-5785, 2022 05 03.
Artigo em Inglês | MEDLINE | ID: mdl-35465657

RESUMO

Despite increasing sustainable water purification, current desalination membranes still suffer from insufficient permeability and treatment efficiency, greatly hindering extensive practical applications. In this work, we provide a new membrane design protocol and molecule-level mechanistic understanding of vapor transport for the treatment of hypersaline waters via a membrane distillation process by rationally fabricating more robust metal-based carbon nanotube (CNT) network membranes, featuring a superhydrophobic superporous surface (80.0 ± 2.3% surface porosity). With highly permeable ductile metal hollow fibers as substrates, the construction of a superhydrophobic (water contact angle ∼170°) CNT network layer endows the membranes with not only almost perfect salt rejection (over 99.9%) but a promising water flux (43.6 L·m-2·h-1), which outperforms most existing inorganic distillation membranes. Both experimental and molecular dynamics simulation results indicate that such an enhanced water flux can be ascribed to an ultra-low liquid-solid contact interface (∼3.23%), allowing water vapor to rapidly transport across the membrane structure via a combined mechanism of Knudsen diffusion (more dominant) and viscous flow while efficiently repelling high-salinity feed via forming a Cassie-Baxter state. A more hydrophobic surface is more in favor of not only water desorption from the CNT outer surface but superfast and frictionless water vapor transport. By constructing a new superhydrophobic triple-phase interface, the conceptional design strategy proposed in this work can be expected to be extended to other membrane material systems as well as more water treatment applications.


Assuntos
Nanotubos de Carbono , Purificação da Água , Destilação , Gases , Membranas , Vapor
19.
Environ Sci Technol ; 56(14): 10279-10288, 2022 07 19.
Artigo em Inglês | MEDLINE | ID: mdl-35802136

RESUMO

The permeance and selectivity of a reverse osmosis (RO) membrane are governed by its ultrathin polyamide film, yet the growth of this critical film during interfacial polymerization (IP) has not been fully understood. This study investigates the evolution of a polyamide nanofilm at the aqueous/organic interface over time. Despite its thickness remaining largely constant (∼15 nm) for the IP reaction time ranging from 0.5 to 60 min, the density of the polyamide nanofilm increased from 1.25 to 1.36 g cm-3 due to the continued reaction between diffused m-phenylenediamine and dangling acyl chloride groups within the formed polyamide film. This continued growth of the polyamide nanofilm led to a simultaneous increase in its crosslinking degree (from 50.1 to 94.3%) and the healing of nanosized defects, resulting in a greatly enhanced rejection of 99.2% for NaCl without sacrificing water permeance. Using humic acid as a molecular probe for sealing membrane defects, the relative contributions of the increased crosslinking and reduced defects toward better membrane selectivity were resolved, which supports our conceptual model involving both enhanced size exclusion and healed defects. The fundamental insights into the growth mechanisms and the structure-property relationship of the polyamide nanofilm provide crucial guidance for the further development and optimization of high-performance RO membranes.


Assuntos
Nylons , Água , Filtração/métodos , Membranas Artificiais , Polimerização
20.
Environ Sci Technol ; 55(13): 9181-9188, 2021 07 06.
Artigo em Inglês | MEDLINE | ID: mdl-34043321

RESUMO

Uranium extraction from seawater is a grand challenge of mounting severity as the energy demand increases with a growing global population. An amidoxime-functionalized carboxymethyl ß-cyclodextrin/graphene aerogel (GDC) is developed for highly efficient and selective uranium extraction via a facile one-pot hydrothermal process. GDC reaches equilibrium in 1 h, and the maximum adsorption capacity calculated from Langmuir model is 654.2 mg/g. Benefiting from the chelation and complexation reaction, the obtained GDC has an excellent selectivity even when the competitive cations, anions, and oil pollutants exist. In addition, the aerogel possesses great mechanical integrity and remains intact after 10 compression cycles. Meanwhile, the GDC can be easily regenerated and maintains a high reusability of 87.3% after 10 adsorption-desorption cycles. It is worthwhile to mention that GDC exhibits an excellent extraction capacity of 19.7 mg/g within 21 days in natural seawater, which is greatly desired in uranium extraction from seawater.


Assuntos
Grafite , Urânio , beta-Ciclodextrinas , Oximas
SELEÇÃO DE REFERÊNCIAS
Detalhe da pesquisa