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1.
J Environ Manage ; 365: 121638, 2024 Aug.
Article in English | MEDLINE | ID: mdl-38959766

ABSTRACT

In the sludge dewatering process, a formidable challenge arises due to the robust interactions between extracellular polymeric substances (EPS) and bound water. This study introduces a novel, synergistic conditioning method that combines iron (Fe2+)/peroxymonosulfate (PMS) and polyacrylamide (PAM) to significantly enhance sludge dewatering efficiency. The application of the Fe2+/PMS-PAM conditioning method led to a substantial reduction in specific filtration resistance (SFR) by 82.75% and capillary suction time (CST) by 80.44%, marking a considerable improvement in dewatering performance. Comprehensive analyses revealed that pre-oxidation with Fe2+/PMS in the Fe2+/PMS-PAM process effectively degraded EPS, facilitating the release of bound water. Subsequently, PAM enhanced the flocculation of fine sludge particles resulting from the advanced oxidation processes (AOPs). Furthermore, analysis based on the Extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory demonstrated shifts in interaction energies, highlighting the breakdown of energy barriers within the sludge and a transition in surface characteristics from hydrophilic (3.79 mJ m-2) to hydrophobic (-61.86 mJ m-2). This shift promoted the spontaneous aggregation of sludge particles. The innovative use of the Flory-Huggins theory provided insights into the sludge filtration mechanism from a chemical potential perspective, linking these changes to SFR. The introduction of Fe2+/PMS-PAM conditioning disrupted the uniformity of the EPS-formed gel layer, significantly reducing the chemical potential difference between the permeate and the water in the gel layer, leading to a lower SFR and enhanced dewatering performance. This thermodynamic approach significantly enhances our understanding of sludge dewatering and conditioning. These findings represent a paradigm shift, offering innovative strategies for sludge treatment and expanding our comprehension of dewatering and conditioning techniques.


Subject(s)
Acrylic Resins , Iron , Sewage , Waste Disposal, Fluid , Sewage/chemistry , Iron/chemistry , Acrylic Resins/chemistry , Waste Disposal, Fluid/methods , Flocculation , Peroxides/chemistry , Oxidation-Reduction , Filtration
2.
Bioresour Technol ; 406: 131011, 2024 Jun 18.
Article in English | MEDLINE | ID: mdl-38901751

ABSTRACT

Predicting thermodynamic adhesion energies was a critical strategy for mitigating membrane fouling. This study utilized a backpropagation (BP) neural network model to predict the thermodynamic adhesion energies associated with membrane fouling in a planktonic anammox MBR. Acid-base (ΔGAB), electrostatic double layer (ΔGEL), and Lifshitz-van der Waals (ΔGLW) energies were selected as output variables, the training dataset was collected by the advanced Derjaguin-Landau-Verwey-Overbeek (XDLVO) method. Optimization results identified "7-10-3″ as the optimal network structure for the BP model. The prediction results demonstrated a high degree of fit between the predicted and experimental values of thermodynamic adhesion energy (R2 ≥ 0.9278), indicating a robust predictive capability of the model in this study. Overall, the study presented a practical BP neural network model for predicting thermodynamic adhesion energies, significantly enhancing the prediction tool for adhesive fouling behavior in anammox MBRs.

3.
Chemosphere ; 358: 142132, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38670505

ABSTRACT

The escalation of industrial activities has escalated the production of pharmaceutical and dyeing effluents, raising significant environmental issues. In this investigation, a hybrid approach of Fenton-like reactions and adsorption was used for deep treatment of these effluents, focusing on effects of variables like hydrogen peroxide concentration, catalyst type, pH, reaction duration, temperature, and adsorbent quantity on treatment effectiveness, and the efficacy of acid-modified attapulgite (AMATP) and ferric iron (Fe(III))-loaded AMATP (Fe(III)-AMATP) was examined. Optimal operational conditions were determined, and the possibility of reusing the catalysts was explored. Employing Fe3O4 as a heterogeneous catalyst and AMATP for adsorption, CODCr was reduced by 78.38-79.14%, total nitrogen by 71.53-77.43%, and phosphorus by 97.74-98.10% in pharmaceutical effluents. Similarly, for dyeing effluents, Fe(III)-AMATP achieved 79.87-80.94% CODCr, 68.59-70.93% total nitrogen, and 79.31-83.33% phosphorus reduction. Regeneration experiments revealed that Fe3O4 maintained 59.48% efficiency over three cycles, and Fe(III)-AMATP maintained 62.47% efficiency over four cycles. This work offers an economical, hybrid approach for effective pharmaceutical and dyeing effluent treatment, with broad application potential.


Subject(s)
Ferric Compounds , Hydrogen Peroxide , Industrial Waste , Magnesium Compounds , Silicon Compounds , Waste Disposal, Fluid , Water Pollutants, Chemical , Waste Disposal, Fluid/methods , Water Pollutants, Chemical/chemistry , Ferric Compounds/chemistry , Adsorption , Silicon Compounds/chemistry , Magnesium Compounds/chemistry , Hydrogen Peroxide/chemistry , Catalysis , Iron/chemistry , Phosphorus/chemistry , Nitrogen/chemistry , Coloring Agents/chemistry , Hydrogen-Ion Concentration , Water Purification/methods
4.
Small ; : e2400205, 2024 Apr 26.
Article in English | MEDLINE | ID: mdl-38676331

ABSTRACT

The conventional membranes used for separating oil/water emulsions are typically limited by the properties of the membrane materials and the impact of membrane fouling, making continuous long-term usage unachievable. In this study, a filtering electrode with synchronous self-cleaning functionality is devised, exhibiting notable antifouling ability and an extended operational lifespan, suitable for the continuous separation of oil/water emulsions. Compared with the original Ti foam, the in situ growth of NiTi-LDH (Layered double hydroxide) nano-flowers endows the modified Ti foam (NiTi-LDH/TF) with exceptional superhydrophilicity and underwater superoleophobicity. Driven by gravity, a rejection rate of over 99% is achieved for various emulsions containing oil content ranging from 1% to 50%, as well as oil/seawater emulsions. The flux recovery rate exceeds 90% after one hundred cycles and a 4-h filtration period. The enhanced separation performance is realized through the "gas bridge" effect during in situ aeration and electrochemical anodic oxidation. The internal aeration within the membrane pores contributes to the removal of oil foulants. This study underscores the potential of coupling foam metal filtration materials with electrochemical technology, providing a paradigm for the exploration of novel oil/water separation membranes.

5.
J Hazard Mater ; 469: 133973, 2024 May 05.
Article in English | MEDLINE | ID: mdl-38452683

ABSTRACT

Efficient oil-water separation has always been a research hotspot in the field of environmental studies. Employing a one-step hydrothermal approach, NiFe-layered double hydroxides (LDH) nanosheets were synthesized on nickel foam substrates. The resulting NiFe-LDH/NF membrane exhibited rejection rates exceeding 99% across six diverse oil-water mixtures, concurrently demonstrating a remarkable ultra-high flux of 1.4 × 106 L·m-2·h-1. This flux value significantly surpasses those documented in existing literature, maintaining stable performance over 1000 manual filtration cycles. These breakthroughs stem from the synergistic interplay among the three-dimensional channels of the nickel foam, the nanosheets, and the hydration layer. By leveraging the pore size of the foam to enhance the functionality of the hydration layer, the conventional trade-off between permeability and selectivity was transformed into a balanced force relationship between the hydration layer and the oil phase. The operational and failure mechanisms of the hydration layer were examined using the prepared NiFe-LDH/NF membrane, validating the correlation between oil phase viscosity and density with hydration layer rupture. Additionally, an extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory was employed to investigate changes in interaction energy, further reinforcing the study's findings. This research contributes novel insights and assistance to the comprehension and application of hydration layers in other membrane studies dedicated to oil-water separation.

6.
Sci Total Environ ; 920: 171124, 2024 Apr 10.
Article in English | MEDLINE | ID: mdl-38382609

ABSTRACT

While microalgal-bacterial membrane bioreactors (microalgal-bacterial MBRs) have risen as an important technique in the realm of sustainable wastewater treatment, the membrane fouling caused by free microalgae is still a significant challenge to cost-effective operation of the microalgal-bacterial MBRs. Addressing this imperative, the current study investigated the influence of magnesium ion (Mg2+) addition on the biological dynamics and membrane fouling characteristics of the laboratory-scale submerged microalgal-bacterial MBRs. The results showed that Mg2+, important in augmenting photosynthetic process, yielded a biomass concentration of 2.92 ± 0.06 g/L and chlorophyll-a/MLSS (mixed liquor suspended solids) of 33.95 ± 1.44 mg/g in the RMg (Mg2+ addition test group). Such augmentation culminated in elevated total nitrogen and phosphorus removal efficiencies, clocking 81.73 % and 80.98 % respectively in RMg. Remarkably, despite the enhanced microalgae activity and concentration in RMg, the TMP growth rate declined by a significant 46.8 % compared to R0. Detailed characterizations attributed reduced membrane fouling of RMg to a synergy of enlarged floc size and reduced EPS contents. This transformation is intrinsically linked to the bridging action of Mg2+ and its role in creating a non-stressed ecological environment for the microalgal-bacterial MBR. In conclusion, the addition of Mg2+ in the microalgal-bacterial MBR appears an efficient approach, improving the efficiency of pollutant treatment and mitigating fouling, which potentially revolutionizes cost-effective applications and propels the broader acceptance of microalgal-bacterial MBRs. It also of great importance to promote the development and application of microalgal-bacterial wastewater treatment technology.


Subject(s)
Biofouling , Microalgae , Wastewater , Biofouling/prevention & control , Membranes, Artificial , Bioreactors/microbiology , Bacteria , Sewage
7.
Small ; 20(25): e2310799, 2024 Jun.
Article in English | MEDLINE | ID: mdl-38213014

ABSTRACT

In the evolving landscape of water treatment, membrane technology has ascended to an instrumental role, underscored by its unmatched efficacy and ubiquity. Diverse synthesis and modification techniques are employed to fabricate state-of-the-art liquid separation membranes. Click reactions, distinguished by their rapid kinetics, minimal byproduct generation, and simple reaction condition, emerge as a potent paradigm for devising eco-functional materials. While the metal-free thiol-ene click reaction is acknowledged as a viable approach for membrane material innovation, a systematic elucidation of its applicability in liquid separation membrane development remains conspicuously absent. This review elucidates the pre-functionalization strategies of substrate materials tailored for thiol-ene reactions, notably highlighting thiolation and introducing unsaturated moieties. The consequential implications of thiol-ene reactions on membrane properties-including trade-off effect, surface wettability, and antifouling property-are discussed. The application of thiol-ene reaction in fabricating various liquid separation membranes for different water treatment processes, including wastewater treatment, oil/water separation, and ion separation, are reviewed. Finally, the prospects of thiol-ene reaction in designing novel liquid separation membrane, including pre-functionalization, products prediction, and solute-solute separation membrane, are proposed. This review endeavors to furnish invaluable insights, paving the way for expanding the horizons of thiol-ene reaction application in liquid separation membrane fabrication.

8.
Sci Bull (Beijing) ; 69(1): 125-140, 2024 Jan 15.
Article in English | MEDLINE | ID: mdl-37957069

ABSTRACT

Transition metal carbides/nitrides/carbonitrides, commonly referred to as MXenes, have gained widespread attention since their discovery in 2011 as a promising family of two-dimensional (2D) materials. Their impressive chemical, electrical, thermal, mechanical, and biological properties have fueled a surge in research focused on the synthesis and application of MXenes in various fields, including membrane-based separation. By engineering the materials and membrane structures, MXene-based membranes have demonstrated remarkable separation performance and added functionalities, such as antifouling and photocatalytic properties. In this review, we aim to have a timely and critical review of research on their fabrication strategy and performance in advanced molecular separation and ion exchange, beginning with a brief introduction of the preparation and physicochemical properties of MXenes. Finally, outlooks and future works are outlined with the aims to provide valuable insights and guidance for advancing membranes' applications in different separation domains.

9.
Sci Total Environ ; 913: 169644, 2024 Feb 25.
Article in English | MEDLINE | ID: mdl-38159758

ABSTRACT

Light profoundly modulates the algal-bacterial membrane bioreactor (algal-bacterial MBR) performance. Yet, its outdoor deployment grapples with the inherent diurnal cycle of sunlight, engendering suboptimal light conditions. The adaptability of such systems to these fluctuating light conditions and their implications for practical outdoor applications remained an under-explored frontier. In response, this study meticulously scrutinized two laboratory-scale algal-bacterial MBRs under varying light regimes: a 24-h continuous and a 12-h cyclic illumination. Over 70 days, continuous illumination was observed to yield superior biomass production and total nitrogen and total phosphorus removal efficiencies compared to its cyclic counterpart. Contrarily, when focusing on membrane fouling, the 12-h cyclic illumination exhibited lower membrane fouling. The spectral analyses coupled with adhesion ability evaluation, traced the enhanced membrane fouling under continuous illumination to the elevated organics and heightened adhesive properties of the flocs. Given the tangible benefits of reduced membrane fouling and the potential harnessing of solar radiation, the 12-h cyclic illumination emerges as an economically astute operational paradigm for algal-bacterial MBRs. The significance of this study is to promote the application of algal-bacterial MBR in sewage treatment and provide robust support for the development of green technology in the future.


Subject(s)
Photoperiod , Sewage , Sewage/microbiology , Membranes, Artificial , Bioreactors/microbiology , Bacteria
10.
Chemosphere ; 341: 140064, 2023 Nov.
Article in English | MEDLINE | ID: mdl-37673189

ABSTRACT

Effectuating optimal wastewater treatment via algae-bacterial symbiosis (ABS) systems necessitates the precise selection of aeration intensity. This study pioneers an in-depth investigation into the interplay of aeration intensity on the microalgal-bacterial consortia's self-flocculation efficacy and the overall treatment performance within ABS systems. The research provides evidence for a direct association between aeration intensity and biomass proliferation, indicating enhanced pollutant removal efficiency with escalated intensities (1.0 and 1.5 L min-1), though the variance lacks statistical significance. The peak self-flocculation efficacy of the microalgal-bacterial consortium (82.39% at 30 min) was manifested at an aeration intensity of 1.0 L min-1. The meticulous analysis of biomass properties showed the complexity of self-flocculation capacity in the consortium, which involves a dynamic interplay of several pivotal factors, including floc size, zeta potential, and EPS content. In situations where these factors pose conflicting influences, the determining factor emerges as the dominant influencer. In this study, the optimal aeration intensity was identified as 1 L min-1, shedding light on the critical threshold for ABS system operation. This study not only enriches the understanding of microalgal-bacterial wastewater treatment mechanisms but also fosters innovative strategies to enhance the performance of such systems.


Subject(s)
Environmental Pollutants , Microalgae , Flocculation , Symbiosis , Biological Assay , Biomass
11.
J Colloid Interface Sci ; 650(Pt A): 775-783, 2023 Nov 15.
Article in English | MEDLINE | ID: mdl-37441970

ABSTRACT

To gain a thorough understanding of interfacial behaviors such as adhesion and flocculation controlling membrane fouling, it is necessary to simulate the actual membrane surface morphology and quantify interfacial interactions. In this work, a new method integrating the rough membrane morphology reconstruction technology (atomic force microscopy (AFM) combining with triangulation technique), the surface element integration (SEI) method, the extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory, the compound Simpson's approach, and the computer programming was proposed. This new method can exactly mimic the real membrane surface in terms of roughness and shape, breaking the limitation of previous fractal theory and Gaussian method where the simulated membrane surface is only statistically similar to the real rough surface, thus achieving a precise description of the interfacial interactions between sludge foulants and the real membrane surface. This method was then applied to assess the antifouling propensity of a polyvinylidene fluoride (PVDF) membrane modified with Ni-ZnO particles (NZPs). The simulated results showed that the interfacial interactions between sludge foulants in a membrane bioreactor (MBR) and the modified PVDF-NZPs membrane transformed from an attractive force to a repulsive force. The phenomenon confirmed the significant antifouling propensity of the PVDF-NZPs membrane, which is highly consistent with the experimental findings and the interfacial interactions described in previous literature, suggesting the high feasibility and reliability of the proposed method. Meanwhile, the original programming code of the quantification was also developed, which further facilitates the widespread use of this method and enhances the value of this work.

12.
Water Res ; 243: 120353, 2023 Sep 01.
Article in English | MEDLINE | ID: mdl-37482001

ABSTRACT

The optimization of membrane bioreactors (MBRs) involves a critical challenge in structural design for mitigation of membrane fouling. To address this issue, a three-dimensional computational fluid dynamics (CFD) model was utilized in this study to simulate the hydrodynamic characteristics of a flat sheet (FS) MBR. The optimization of the membrane module configuration and operating conditions was performed by investigating key parameters that altered the shear stress and liquid velocity. The mixed liquor suspended solids (MLSS) concentration was found to increase the shear stress, leading to a more uniform distribution of shear stress. By optimizing the appropriate bubble diameter to 5 mm, the shear stress on the membrane surface was optimized with relatively uniform distribution. Additionally, extending the side baffle length dramatically improved the uniformity of the shear stress distribution on each membrane. A novel in-situ aeration method was also discovered to promote turbulent kinetic energy by 200 times compared with traditional aeration modes, leading to a more uniform bubble streamline. As a result, the novel in-situ aeration method demonstrated superior membrane antifouling potential in the MBR. This work provides a new approach for the structural design and optimization of MBRs. The innovative combination of the CFD model, optimization techniques, and novel in-situ aeration method has provided a substantial contribution to the advancement of membrane separation technology in wastewater treatment.


Subject(s)
Hydrodynamics , Waste Disposal, Fluid , Waste Disposal, Fluid/methods , Membranes, Artificial , Bioreactors , Stress, Mechanical
13.
Environ Res ; 234: 116420, 2023 10 01.
Article in English | MEDLINE | ID: mdl-37327838

ABSTRACT

This study investigated the combined effects of polymeric aluminum chloride (PAC) and polyacrylamide (PAM) on sludge dewatering, aiming to unveil underlying mechanisms. Co-conditioning with 15 mg g-1 PAC and 1 mg g-1 PAM achieved optimal dewatering, reducing specific filtration resistance (SFR) of co-conditioned sludge to 4.38 × 1012 m-1kg-1, a mere 48.1% of raw sludge's SFR. Compared with the CST of raw sludge (36.45 s), sludge sample can be significantly reduced to 17.7 s. Characterization tests showed enhanced neutralization and agglomeration in co-conditioned sludge. Theoretical calculations revealed elimination of interaction energy barriers between sludge particles post co-conditioning, converting sludge surface from hydrophilic (3.03 mJ m-2) to hydrophobic (-46.20 mJ m-2), facilitating spontaneous agglomeration. Findings explain improved dewatering performance. Based on Flory-Huggins lattice theory, connection between polymer structure and SFR was established. Raw sludge formation triggered significant change in chemical potential, increasing bound water retention capacity and SFR. In contrast, co-conditioned sludge exhibited thinnest gel layer, reducing SFR and significantly improving dewatering. These findings represent a paradigm shift, shedding new light on fundamental thermodynamic mechanisms of sludge dewatering with different chemical conditioning.


Subject(s)
Sewage , Waste Disposal, Fluid , Aluminum Chloride , Flocculation , Polymers/chemistry , Filtration , Thermodynamics , Water/chemistry
14.
Chemosphere ; 315: 137791, 2023 Feb.
Article in English | MEDLINE | ID: mdl-36623602

ABSTRACT

The oily water treatment is becoming one of the hottest topics due to that increase of offshore oil transportation and the various accident oil leakages. In this study, a functional TiO2-ABS composite membrane was generated through the three-dimensional (3D) printing strategy for the first time and was conducted to simulated oily water treatment. The TiO2-ABS composite membrane demonstrated a significant promotion in hydrophilicity and oleophobicity which were evidenced by the water contact angle of 14.8° and the underwater oil contact angle of 144.7°, respectively. The optimal modified membrane had both exceedingly high flux (1.8 × 105 L m-2·h-1) and oil rejection rate (99.5%). Moreover, the results of filtration cycles of 10 days and extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory demonstrated that the modified membranes took possession of excellent stability and antifouling property. What was more, the TiO2-ABS composite membrane revealed over 99% rejection to all five types of oil/water systems. The interestingly experimental results indicated that the prepared membrane possessed a broad development trend and application prospect in the field of oily water treatment.


Subject(s)
Acrylonitrile , Butadienes , Styrene , Titanium , Oils
15.
Chemosphere ; 310: 136817, 2023 Jan.
Article in English | MEDLINE | ID: mdl-36241107

ABSTRACT

Although protein is an important membrane foulant in the water body that may be significantly affected by the coexisting common cation magnesium (Mg2+), the effect of Mg2+ on protein fouling is rarely reported. In this context, this study selected bovine serum albumin (BSA) as the model foulant, and investigated its fouling characteristics at different Mg2+ concentrations (0-100 mM). Filtration tests showed that the protein fouling can be significantly mitigated by adding Mg2+, and the specific filtration resistance (SFR) of pure BSA (3.56 × 1014 m kg-1) was at least 5 times that of BSA-Mg2+ solutions (0.5-100 mM). In addition, an optimal Mg2+ concentration exists, which can achieve the lowest BSA SFR. A series of characterizations indicated that the main contributors to the differences in BSA SFR were the changes in BSA adhesion capacity and the thickness and structure of the foulant layer. Basically, the above results were attributed to the hydration repulsion effect of Mg2+, which prevented tight adhesion of foulants to the membrane. Moreover, the lowest BSR SFR at 1 mM Mg2+ was achieved not only by the hydration repulsion effect but also by the particle size compression due to the conformational change of BSA molecules. This combined effect led to the lowest foulant retention on the membrane surface and delivered to the lowest SFR. This study conducts a thorough inspection into the specific effect of Mg2+ on protein fouling and provides a fresh insight into protein fouling control in the UF process.


Subject(s)
Ultrafiltration , Water Purification , Ultrafiltration/methods , Magnesium/pharmacology , Membranes, Artificial , Serum Albumin, Bovine/chemistry , Ions
16.
Chemosphere ; 309(Pt 1): 136734, 2022 Dec.
Article in English | MEDLINE | ID: mdl-36209866

ABSTRACT

While magnesium cation (Mg2+) universally coexists with natural organic matter (NOM) in the water environment, influence of Mg2+ on NOM fouling in membrane filtration process is still unclear. This work was therefore performed to investigate effects of Mg2+ on NOM (sodium alginate (SA) as a model substance) fouling and role of Ca2+ in mitigating fouling from Mg2+ in the ultrafiltration (UF) water treatment process. Filtration tests showed two interesting fouling phenomena: (1) membrane fouling caused by combination of Mg2+ and SA maintained at a high value with the increased Mg2+ concentration; (2) the high fouling property of Mg2+ can be significantly improved by the prominent addition of calcium cation (Ca2+). It was found that changes of foulant morphology played essential roles through thermodynamic mechanisms represented by the Flory-Huggins lattice theory. Density functional theory (DFT) calculation showed that the combination of SA and Mg2+ tends to coordinate two terminal carboxyl groups in SA, beneficial to stretching alginate chains and forming a stable gel network at low doses. In addition, intramolecular coordination is difficult to occur between SA and Mg2+ due to the high hydration repulsion radius of Mg2+. Therefore, a dense and thick gel network remained even under high Mg2+concentration. Furthermore, due to the higher binding affinity of Ca2+ over Mg2+, high doses of Ca2+ trigger a transition of the stable SA-Mg2+ gel network to other configurations where flocculation and aggregation occur, thereby reducing the specific filtration resistance. The proposed thermodynamic mechanism satisfactorily explained the above interesting fouling behaviors, facilitating to development of new solutions to control membrane fouling.


Subject(s)
Ultrafiltration , Water Purification , Magnesium , Calcium/chemistry , Membranes, Artificial , Density Functional Theory , Alginates/chemistry , Calcium, Dietary , Cations
17.
Sci Total Environ ; 853: 158650, 2022 Dec 20.
Article in English | MEDLINE | ID: mdl-36089022

ABSTRACT

While ethylenediamine tetramethylenephosphonic acid (EDTMPA) has been emerged as a stronger chelating agent than ethylene diamine tetraacetic acid (EDTA) for fouling mitigation, and transparent exopolymer particles (TEP) is a major foulant in membrane-based water treatment process, effects of EDTMPA on TEP fouling and the underlying mechanism have been not yet studied. In this study, Flory-Huggins lattice theory was combined with density functional theory (DFT) technology to explore this subject at molecular level. Filtration experiments showed a unimodal pattern of specific filtration resistance (SFR) of TEP sample with Ca2+ concentration in range of 0-3 mM. For the TEP sample with the peak SFR value at 1.5 mM Ca2+, continuous addition of EDTMPA (from 0 to 100 mg·L-1) resulted in a sustained decrease in SFR. Energy dispersive spectroscopy (EDS) mapping characterization showed the continuing decline of calcium content in the TEP layer with increase of EDTMPA addition, indicating that EDTMPA successfully captured Ca2+ from alginate­calcium ligation (TEP), and then disintegrated the TEP structure. DFT simulation showed that Ca2+ preferentially coordinated with the terminal carboxyl groups of alginate chains to form a coordination configuration that is conducive to stretch the three-dimensional polymer network. Such a network corresponded to an extremely high SFR according to Flory-Huggins theory. EDTMPA addition caused disintegration of the coordination configuration of Ca2+ binding to terminal carboxyl groups, which further resulted in collapse and flocculation of TEP gel network structure, thus leading to a continuous SFR decrease. This work provided deep thermodynamic insights into effects of EDTMPA on TEP-associated fouling at molecular level, facilitating to better understanding and mitigation of membrane fouling.


Subject(s)
Extracellular Polymeric Substance Matrix , Water Purification , Membranes, Artificial , Calcium/chemistry , Edetic Acid , Filtration , Alginates/chemistry , Polymers/chemistry , Ethylenediamines , Chelating Agents , Ethylenes
18.
Sci Total Environ ; 842: 156912, 2022 Oct 10.
Article in English | MEDLINE | ID: mdl-35753486

ABSTRACT

While transparent exopolymer particles (TEP) is a major foulant, and ethylene diamine tetraacetic acid (EDTA) is a strong chelating agent frequently used for fouling mitigation in membrane-based water treatment processes, little has been known about TEP-associated membrane fouling affected by EDTA. This work was performed to investigate roles of EDTA addition in TEP (Ca-alginate gel was used as a TEP model) associated fouling. It was interestingly found that, TEP had rather high specific filtration resistance (SFR) of 2.49 × 1015 m-1·kg-1, and SFR of TEP solution firstly decreased and then increased rapidly with EDTA concentration increase (0-1 mM). A series of characterizations suggested that EDTA took roles in SFR of TEP solution by means of changing TEP microstructure. The rather high SFR of TEP layer can be attributed to the big chemical potential gap during filtration described by the extended Flory-Huggins lattice theory. Initial EDTA addition disintegrated TEP structure by EDTA chelating calcium in TEP, inducing reduced SFR. Continuous EDTA addition decreased solution pH, resulting into no effective chelating and accumulation of EDTA on membrane surface, increasing SFR. It was suggested that factors increasing homogeneity of TEP gel will increase SFR, and vice versa. This study revealed the thermodynamic mechanism of TEP fouling behaviors affected by EDTA, and also demonstrated the importance of EDTA dosage and pH adjustment for TEP-associated fouling control.


Subject(s)
Alginates , Water Purification , Alginates/chemistry , Edetic Acid , Ethylenes , Filtration , Membranes, Artificial
19.
Sci Total Environ ; 836: 155579, 2022 Aug 25.
Article in English | MEDLINE | ID: mdl-35508249

ABSTRACT

Fouling behaviors of polysaccharides vary with their structure, while the mechanisms underlying this phenomenon remain unexplored. This work was carried out to explore the thermodynamic fouling mechanisms of polysaccharides with different structure. Carrageenan and xanthan gum were selected as the model polysaccharides with structure of straight and branch chains, respectively. Batch filtration experiments showed that xanthan gum solution corresponded to a more rapid flux decline trend, and specific filtration resistance (SFR) of xanthan gum (2.32 × 1015 m-1 kg-1) was over 10 times than that of carrageenan (2.21 × 1014 m-1 kg-1). It was found that, xanthan gum possessed a more disordered structure and a rather higher viscosity (15.03 mPa·s V.S. 1.98 mPa·s for carrageenan). Calculation of extended Derjaguin-Landau-Verwey-Overbeek (XDLVO) theory showed higher adhesion energy of xanthan gum (-42.82 my m-2 V.S. -23.26 mJ m-2 for carrageenan). Scanning electron microscopy (SEM) analyses showed that xanthan gum gel layer had a more homogenous structure and rigid polymer backbone, indicating better mixing with water to form a gel. As verified by heating experiments, such a structure tended to contain more bound water. According to this information, Flory-Huggins lattice theory was introduced to build a bridge between polymeric structure and SFR. It was revealed that branch structure corresponded to higher chemical potential change during gel layer formation, and higher ability to carry bound water, resulting in higher filtration resistance during filtration process. This work revealed the fundamental thermodynamic mechanism of membrane fouling caused by polysaccharides with different structure, deepening understanding of membrane fouling.


Subject(s)
Filtration , Membranes, Artificial , Carrageenan , Molecular Structure , Polymers/chemistry , Polysaccharides , Water
20.
Sci Total Environ ; 820: 153252, 2022 May 10.
Article in English | MEDLINE | ID: mdl-35066039

ABSTRACT

While transparent exopolymer particles (TEP) has high fouling potential, its underlying fouling mechanisms have not yet been well revealed. In current work, fouling characteristics of TEP under different Ca2+ concentrations (0 to 1.5 mM) were investigated. TEP quantification and filtration tests showed that TEP contents increased with Ca2+ concentration, while TEP's specific filtration resistance (SFR) under the influence of Ca2+ concentration presented a unimodal pattern. The peak of TEP's SFR reached at Ca2+ concentration of 1 mM when SA concentration was 0.3 g·L-1. A series of characterizations suggested that microstructure transformation of TEP particles was the main contributor to the resistance variations of TEP solution. The optical microscope observation showed that above and below the critical Ca2+ concentration (1 mM when SA concentration is 0.3 g·L-1 in this study), the formed TEP existed in the form of c-TEP (average particle size is 0.24 µm) and p-TEP (average particle size is 1.05 µm), respectively. Thermodynamic analysis showed that the adhesion ability of c-TEP (-249,989 and - 303,692 kT) was more than 19 times than that of p-TEP (-12,905 kT), which would accelerate foulant layer formation. In addition, below the critical value, the increased SFR with Ca2+ concentration could be explained by integrating Flory-Huggins lattice theory with the preferential intermolecular coordination. Above the critical value, the decreased SFR can be attributed to the formation of a "large-size crack structure" cake layer from the p-TEP. This study revealed fundamental mechanisms of membrane fouling caused by TEP, greatly deepening understanding of TEP fouling, and facilitating to development of effective fouling control strategies.


Subject(s)
Extracellular Polymeric Substance Matrix , Water Purification , Filtration , Membranes, Artificial , Thermodynamics
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