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1.
Water Res ; 254: 121355, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38430755

RESUMO

Stormwater harvesting (SWH) addresses the UN's Sustainable Development Goals (SDGs). Conventional stormwater control measures (SCMs) effectively remove particulate and colloidal contaminants from urban runoff; however, they fail to retain dissolved contaminants, particularly substances of concern like polycyclic aromatic hydrocarbons (PAHs) and heavy metals (HMs), thereby hindering the SWH applicability. Here, inspired by protein folding in nature, we reported a novel biomimetic SCM for the efficient removal of dissolved PAHs and HMs from urban runoff. Lab-scale tests were conducted together with a more mechanistic investigation on how the contaminants were removed. By integrating hydrophobic organic chains with low-cost hydrophilic flocculant matrixes, our biomimetic flocculants achieved a 1.4-9.5 times removal of all detected dissolved PAHs and HMs, while enhancing the removal of a wide-spectrum of particulate and colloidal contaminants, compared to existing SCMs. Ecotoxicity, as indicated by newborn Daphnia magna as experimental organisms, was reduced from "acute toxicity" of the original runoff sample (toxic unit of ∼2.6) to "non-toxicity" (toxic unit < 0.4) of the treated water. The improved performance is attributed to the protein-folding-like features of the bioinspired flocculants providing: (i) stronger binding to PAHs (via hydrophobic association) and HMs (via coordination), and (ii) the ability of spontaneous aggregation. The bio-inspired approach in this work holds strong promise as an alternative or supplementary component in SCM systems, and is expected to contribute to sustainable water management practices in relation to SDGs.


Assuntos
Metais Pesados , Hidrocarbonetos Policíclicos Aromáticos , Poluentes Químicos da Água , Hidrocarbonetos Policíclicos Aromáticos/análise , Poluentes Químicos da Água/química , Monitoramento Ambiental , Metais Pesados/análise
2.
Water Res ; 253: 121268, 2024 Apr 01.
Artigo em Inglês | MEDLINE | ID: mdl-38340700

RESUMO

The release of nanoplastics (NPs) into the environment is growing due to the extensive use of plastic products. Numerous studies have confirmed the negative effects of NPs on microorganisms, which poses uncertainties concerning their impact on nanofiltration (NF) membrane biofouling. This study investigated the initial cell adhesion process, NF membrane biofouling kinetic processes and bacterial responses of Pseudomonas aeruginosa (P. aeruginosa) exposed to varied NPs concentrations (0-50 mg·L-1). Transcriptome analysis demonstrated that low concentration of NPs (0.1 mg·L-1) promoted bacterial quorum sensing, energy metabolism, exopolysaccharide biosynthesis and bacterial secretion systems. Correspondingly, the polysaccharide content increased remarkably to 2.77 times the unexposed control, which served as a protective barrier for bacteria to avoid the impact of NPs-induced stress. Suppressed homologous recombination, microbial metabolic potentials and flagellar assembly were detected in bacteria exposed to a high concentration (50 mg·L-1) of NPs, mainly due to the triggered reactive oxygen species (ROS) generation, genomic DNA damage, and decreased energy production. Overall, enhanced formation of the extracellular polymeric substances (EPS) and aggravated membrane flux decline were observed when NPs interacted with the membrane surface by cell secretions (low NPs levels) or cell lysis (high NPs levels). These findings shed light on understanding the microbial metabolism mechanism and membrane biofouling propensity with NPs stress at both the molecular and gene levels.


Assuntos
Incrustação Biológica , Microplásticos , Membranas Artificiais , Percepção de Quorum , Bactérias , Biofilmes
3.
Water Res ; 254: 121352, 2024 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-38401286

RESUMO

Coagulation efficiency is heavily contingent upon a profound comprehension of the underlying mechanisms, facilitated by the evolution of coagulation theory. However, the role of anions, prevalent components in raw and wastewaters, has been relatively overlooked in this context. To address this gap, this study has investigated the impact of three common anions (i.e., chloride, sulfate, and phosphate) on Al-based coagulation. The results have shown that the influence of anions on coagulation depends predominantly on their ability to compete with hydroxyl groups throughout the entire coagulation process, encompassing hydrolysis, aggregation, and the growth of large flocs. Moreover, this competition is subject to the dual influence of both anion concentration and hydroxyl concentration (i.e., pH). The results have revealed the intricate interplay between anions and coagulants, their impact on floc structure, and their importance in optimizing coagulation efficiency and ensuring the production of high-quality water.


Assuntos
Sulfatos , Purificação da Água , Floculação , Ânions , Águas Residuárias , Cátions , Purificação da Água/métodos
4.
Water Res ; 252: 121193, 2024 Mar 15.
Artigo em Inglês | MEDLINE | ID: mdl-38290239

RESUMO

Biofiltration is an environmentally 'green' technology that is compatible with the recently proposed sustainable development goals, and which has an increasingly important future in the field of water treatment. Here, we explored the impacts of bioelectrochemical integration on a bench-scale slow rate biofiltration system regarding its performance in reclaimed water treatment. Results showed that the short-term (<3 months) integration improved the removal of natural organic matter (NOM) (approximately 8.8%). After long-term (5 months and thereafter) integration, the cathodic charge transfer resistance was found to have a significant reduction from 2662 to 1350 Ω. Meanwhile, bioelectrochemical autotrophic sulfate (SO42-) reduction (over 27.6% reduction) through the syntrophic metabolism between hydrogen oxidation strains (genus Hydrogenophaga) and sulfate-reducing microbes (genera Dethiobacter, Desulfovibrio, and Desulfomicrobium) at the cathodic region was observed. More significantly, the microbial-derived chromophoric humic substances were found to act as electron shuttles at the cathodic region, which might facilitate the process of bioelectrochemical SO42- reduction. Overall, this study provided valuable insights into the potential application of bioelectrochemical-integrated biofilter for simultaneous reduction of NOM and SO42- treating reclaimed water.


Assuntos
Sulfatos , Purificação da Água , Oxirredução , Processos Autotróficos , Purificação da Água/métodos , Substâncias Húmicas/análise
5.
Environ Sci Technol ; 58(2): 1164-1176, 2024 Jan 16.
Artigo em Inglês | MEDLINE | ID: mdl-38164759

RESUMO

Terrestrial dissolved organic matter (DOM) is critical to global carbon and nutrient cycling, climate change, and human health. However, how the spatial and compositional differences of soil DOM affect its dynamics and fate in water during the carbon cycle is largely unclear. Herein, the biodegradation of DOM from 14 spatially distributed grassland soils in China with diverse organic composition was investigated by 165 days of incubation experiments. The results showed that although the high humified fraction (high-HS) regions were featured by high humic-like fractions of 4-25 kDa molecular weight, especially the abundant condensed aromatics and tannins, they unexpectedly displayed greater DOM degradation during 45-165 days. In contrast, the unique proteinaceous and 25-100 kDa fractions enriched in the low humified fraction (low-HS) regions were drastically depleted and improved the decay of bulk DOM but only during 0-45 days. Together, DOM from the high-HS regions would cause lower CO2 outgassing to the atmosphere but higher organic loads for drinking water production in the short term than that from the low-HS regions. However, this would be reversed for the two regions during the long-term transformation processes. These findings highlight the importance of spatial and temporal variability of DOM biogeochemistry to mitigate the negative impacts of grassland soil DOM on climate, waters, and humans.


Assuntos
Matéria Orgânica Dissolvida , Solo , Humanos , Pradaria , Carbono , Água , China
6.
Water Res ; 249: 120914, 2024 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-38007899

RESUMO

The fouling of seawater reverse osmosis (SWRO) membranes remains a persistent challenge in desalination. Previous research has focused mainly on fouling separately; however, organic, inorganic, and biofouling can coexist and influence each other. Hence, in-depth study of the spatiotemporal changes in actual combined fouling in full-scale seawater desalination will provide more effective information for fouling investigation and control. In this study, we monitored (i) the operational performance of a full-scale desalination plant for 7 years and (ii) the development and characterization of membrane and spacer fouling at different locations of spiral-wound membrane modules sampled after 2.5-, 3.5-, and 7-year operation. The findings showed that (i) operational performance indicators declined with time (normalized flux 40 % reduction, salt rejection 2 % in 7 years), with a limited effect of the 20-day cleaning frequency, (ii) fouling accumulation in the membrane module mainly occurred at the feed side of the lead module and the microbial community in these area exhibited the highest diversity, (iii) the dominant microbial OTUs belonged mainly to Proteobacteria (43-70 %), followed by Bacteroidetes (10-11 %), (iv) Phylogenetic molecular ecological networks and Spearman correlation analysis revealed that Chloroflexi (Anaerolineae) and Planctomycetes were keystone species in maintaining the community structure and biofilm maturation and significantly impacted the foulant content on the SWRO membrane, even with low abundance, and that (v) fouling accumulation was composed of polysaccharides, soluble microbial products, marine humic acid-like substances, and inorganic Ca/Fe/Mg/Si dominate the fouling layer of both the membrane and spacer. Overall, variation partitioning analysis quantitatively describes the increasing contribution of biofouling over time. Ultimately, the organic‒inorganic-biofouling interaction (70 %) significantly contributed to the overall fouling of the membrane after 7 years of operation. These results can be used to develop more targeted fouling control strategies to optimize SWRO desalination plant design and operation.


Assuntos
Incrustação Biológica , Purificação da Água , Filogenia , Membranas Artificiais , Purificação da Água/métodos , Osmose , Água do Mar/química
7.
Environ Sci Technol ; 57(30): 11096-11107, 2023 08 01.
Artigo em Inglês | MEDLINE | ID: mdl-37467428

RESUMO

Denitrification-driven Fe(II) oxidation is an important microbial metabolism that connects iron and nitrogen cycling in the environment. The formation of Fe(III) minerals in the periplasmic space has a significant effect on microbial metabolism and electron transfer, but direct evidence of iron ions entering the periplasm and resulting in periplasmic mineral precipitation and electron conduction properties has yet to be conclusively determined. Here, we investigated the pathways and amounts of iron, with different valence states and morphologies, entering the periplasmic space of the denitrifier Pseudomonas sp. JM-7 (P. JM-7), and the possible effects on the electron transfer and the denitrifying ability. When consistently provided with Fe(II) ions (from siderite (FeCO3)), the dissolved Fe(II) ions entered the periplasmic space and were oxidized to Fe(III), leading to the formation of a 25 nm thick crystalline goethite crust, which functioned as a semiconductor, accelerating the transfer of electrons from the intracellular to the extracellular matrix. This consequently doubled the denitrification rate and increased the electron transport capacity by 4-30 times (0.015-0.04 µA). However, as the Fe(II) concentration further increased to above 4 mM, the Fe(II) ions tended to preferentially nucleate, oxidize, and crystallize on the outer surface of P. JM-7, leading to the formation of a densely crystallized goethite layer, which significantly slowed down the metabolism of P. JM-7. In contrast to the Fe(II) conditions, regardless of the initial concentration of Fe(III), it was challenging for Fe(III) ions to form goethite in the periplasmic space. This work has shed light on the likely effects of iron on environmental microorganisms, improved our understanding of globally significant iron and nitrogen geochemical cycles in water, and expanded our ability to study and control these important processes.


Assuntos
Compostos Férricos , Compostos de Ferro , Periplasma/metabolismo , Água , Desnitrificação , Compostos de Ferro/química , Compostos de Ferro/metabolismo , Minerais/química , Ferro/química , Oxirredução , Compostos Ferrosos/química , Compostos Ferrosos/metabolismo , Nitrogênio/metabolismo
8.
J Hazard Mater ; 457: 131736, 2023 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-37295334

RESUMO

The biological slow filtration reactor (BSFR) process has been found to be moderately effective for the removal of refractory dissolved organic matter (DOM) in the treatment of reused water. In this study, bench scale experiments were conducted using a mixture of landscape water and concentrated landfill leachate as feed water, to compare a novel iron oxide (FexO)/FeNC modified activated carbon (FexO@AC) packed BSFR, with a conventional activated carbon packed BSFR (AC-BSFR), operated in parallel. The results showed that the FexO@AC packed BSFR had a refractory DOM removal rate of 90%, operated at a hydraulic retention time (HRT) of 10 h at room temperature for 30 weeks, while under the same conditions the removal by the AC-BSFR was only 70%. As a consequence, the treatment by the FexO@AC packed BSFR substantially reduced the formation potential of trihalomethanes, and to a less extent, haloacetic acids. The modification of FexO/FeNC media raised the conductivity and the oxygen reduction reaction (ORR) efficiency of the AC media to accelerate the anaerobic digestion by consuming the electrons that are generated by anaerobic digestion itself, which lead to the marked improvement in refractory DOM removal.

9.
Water Res ; 236: 119942, 2023 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-37031529

RESUMO

Hydrophobic-modified flocculants have demonstrated considerable promise in the removal of emerging contaminants by flocculation. However, there is a lack of information about the impacts of dosing such flocculants on the performance of subsequent treatment unit(s) in the overall water treatment process. In this work, inspired by the ubiquitous protein folding phenomenon, an innovative approach using an elevated membrane cleaning temperature as the means to induce residual hydrophobic-modified chitosan flocculant (TRC), after flocculation-sedimentation, to reduce membrane fouling in a subsequent ultrafiltration was proposed; this was evaluated in a continuous flocculation-sedimentation-ultrafiltration (FSUF) process treating samples of the Yangtze River. The hydrophobic chains of TRC had similar temperature-dependent hydrophobicity to those of natural proteins. In the 40-day operation of the FSUF system with combined dosing of alum and TRC, a moderately elevated cleaning water temperature (45 °C) of both backwash with air-bubbling and soaking with sponge-scrubbing cleaning, significantly reduced reversible and irreversible fouling resistance by 49.8%∼61.3% and 73.9%∼83.3%, respectively, compared to the system using cleaning water at 25 °C. Material flow analysis, statistical analysis, instrumental characterizations, and computational simulations, showed that the enhanced fouling mitigation originated from three factors: the reduced contaminant accumulation onto membranes, the strengthened membrane-surface-modification role of TRC, and the weakened structure of the fouling material containing TRC, at the elevated cleaning temperature. Other measures of the performance, these being water purification, membrane stability and economic aspects, also confirmed the potential and feasibility of the proposed approach. This work has provided new insights into the role of hydrophobic-modified flocculants in membrane fouling control, in addition to emerging contaminant removal, in a FSUF surface water treatment process.


Assuntos
Membranas Artificiais , Purificação da Água , Floculação , Temperatura , Ultrafiltração , Interações Hidrofóbicas e Hidrofílicas , Dobramento de Proteína
10.
Environ Sci Technol ; 57(11): 4543-4555, 2023 03 21.
Artigo em Inglês | MEDLINE | ID: mdl-36877961

RESUMO

The biodegradation in the middle and downstream of slow-rate biological activated carbon (BAC) is limited by insufficient dissolved oxygen (DO) concentrations. In this study, a bubbleless aerated BAC (termed ABAC) process was developed by installing a hollow fiber membrane (HFM) module within a BAC filter to continuously provide aeration throughout the BAC system. The BAC filter without an HFM was termed NBAC. The laboratory-scale ABAC and NBAC systems operated continuously for 426 days using secondary sewage effluent as an influent. The DO concentrations for NBAC and ABAC were 0.78 ± 0.27 and 4.31 ± 0.44 mg/L, respectively, with the latter providing the ABAC with greater electron acceptors for biodegradation and a microbial community with better biodegradation and metabolism capacity. The biofilms in ABAC secreted 47.3% less EPS and exhibited greater electron transfer capacity than those in NBAC, resulting in enhanced contaminant degradation efficiency and long-term stability. The extra organic matter removed by ABAC included refractory substances with a low elemental ratio of oxygen to carbon (O/C) and a high elemental ratio of hydrogen to carbon (H/C). The proposed ABAC filter provides a valuable, practical example of how to modify the BAC technology to shape the microbial community, and its activity, by optimizing the ambient atmosphere.


Assuntos
Poluentes Químicos da Água , Purificação da Água , Filtração/métodos , Carvão Vegetal , Esgotos , Biodegradação Ambiental , Biofilmes , Purificação da Água/métodos , Poluentes Químicos da Água/análise
11.
Water Res ; 229: 119447, 2023 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-36476382

RESUMO

Pesticide concentrations in surface water occasionally exceed regulated values due to seasonal events (rainy season in high intensity agricultural areas) or intermittent discharges (leakage, spillage, or other emergency events). The need to remove pesticide compounds in these situations poses a challenge for drinking water treatment plants (DWTPs). In this work, the performance of dosing hydrophobic-modified inorganic-organic hybrid flocculants (HOC-M; lower acute toxicity than corresponding metal salt coagulants; acceptable economic costs when M=Al or Fe; prepared in large-scale quantities), for the removal of four different pesticides (each initial concentration: 0.25 µg/L) from Yangtze River water, and in mitigating membrane fouling, by an integrated flocculation-sedimentation-ultrafiltration (FSUF) process, was evaluated over a period of 40 days; the FSUF is well-established in many DWTPs. The mechanisms underlying the treatment were unveiled by employing a combination of instrumental characterizations, chemical computations, material flow analyses, and statistical analyses. Efficient pesticide removal (80.3%∼94.3%) and membrane fouling reduction (26.6%∼37.3% and 28.3%∼57.6% for reversible and irreversible membrane resistance, respectively) in the FSUF process were achieved by dosing HOC-M, whereas conventional inorganic coagulants were substantially inferior for pesticide removal (< 50%) and displayed more severe fouling development. Hydrophobic association between the pesticides and the hydrophobic organic chain of HOC-M played a predominant role in the improvement in pesticide removal; coexisting particulate/colloid inorganic minerals and natural organic matter with HOC-M adsorbed on the surface, acting as floc building materials, provided sites for the indirect combination of pesticides into flocs. The observed fouling alleviation from dosing HOC-M was ascribed to both the pre-removal of fouling-causing materials in the flocculation-sedimentation prior to UF, and a stable hydrophilization modification effect of residual HOC-M in the UF unit. The latter effect resulted from a hydrophobic association between the PVDF substrate of the membranes and the hydrophobic organic chains of the HOC-M, causing the hydrophilic ends of the HOC-M to be exposed away from the membrane surface, thereby inhibiting foulant accumulation. This work has not only demonstrated the superior performance of dosing HOC-M in the FSUF process for trace pesticide removal in DWTPs, but also clarified the underlying mechanisms.


Assuntos
Praguicidas , Purificação da Água , Ultrafiltração/métodos , Floculação , Membranas Artificiais , Purificação da Água/métodos
12.
Water Res ; 226: 119284, 2022 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-36323208

RESUMO

Previous studies have shown that the combination of biological and ozone oxidation processes can achieve a greater performance in treating natural surface water than each process individually. In this work, we designed and tested an ozonation-gravity-driven up-flow slow rate (0.01 m/h) biofiltration-ozonation (O3-GUSB-O3) process for the pre-treatment of reclaimed water prior to ultrafiltration (UF), with the aim of producing high quality drinking water and a significantly reduced degree of UF fouling. Results showed that O3 coupled with GUSB can effectively remove aromatic compounds (∼ 84.8%), dissolved organic carbon (DOC, ∼ 83.4%), and biopolymers in surface water. In addition, post-ozonation greatly contributed to the reduction of the UF membrane fouling (∼ 6 times greater flux). With regard to the disinfection by-product formation potential (DBPFP) of the final treated water, both trihalomethane formation potential (THMFP) and haloacetic acid formation potential (HAAFP) were greatly reduced (86.4% and 84.8% for THMs and HAAs, respectively). The relationship between DBPFP and various spectral indexes revealed that aromatic compounds and amino acids were more likely to generate DBPs during the disinfection stage. Among these, humic substances were more likely to generate THMs, while low molecular weight carboxylate and carbonyl organic compounds were associated with the generation of HAAs. Moreover, the dosage of O3 during the post-ozonation stage was found to influence directly the generation of DBPs. Overall, this study has conducted a detailed evaluation of a novel multi-ozone biofilter UF process for treating surface water, and the results provide a valuable basis for subsequent studies at larger scale to demonstrate the potential of the treatment process for practical applications.


Assuntos
Água Potável , Ozônio , Poluentes Químicos da Água , Purificação da Água , Ultrafiltração , Purificação da Água/métodos , Poluentes Químicos da Água/química , Ozônio/química , Desinfecção/métodos
13.
Bioresour Technol ; 362: 127838, 2022 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-36031124

RESUMO

This study innovated the concept in designing an efficient and reusable microwave (MW) absorbent through concurrent exploitation of carbon graphitization, oxygen functionalization, and carbothermal iron reduction underpinned by an endothermic co-pyrolysis of wood waste and low-dosage iron. A powerful MW assimilation was accomplished from nanoscale amorphous magnetic particles as well as graphitized microporous carbon-iron skeleton in the biochar composites. Relative to a weak magnetic loss derived from the iron phase, the graphitic carbon architecture with abundant surface functionalities (i.e., CO and CO) exhibited a strong dielectric loss, which was thus prioritized as major active sites during MW reuse. The MW-absorbing biochar demonstrated a fast, robust, and durable removal of a refractory herbicide (2,4-dichlorophenoxy acetic acid) under mild MW irradiation with zero chemical input, low electricity consumption, and negligible Fe dissolution. Overall, this study will foster carbon-neutral industrial wastewater treatment and wood waste valorization.


Assuntos
Poluentes Ambientais , Poluentes Químicos da Água , Adsorção , Carbono , Carvão Vegetal/química , Ferro/química , Micro-Ondas , Poluentes Químicos da Água/química , Madeira
14.
Environ Sci Technol ; 56(7): 4345-4355, 2022 04 05.
Artigo em Inglês | MEDLINE | ID: mdl-35319869

RESUMO

The oxidation-precipitation process of Fe(II) is ubiquitous in the environment and critically affects the fate of contaminants and nutrients in natural systems where Fe(II) is present. Here, we explored the effect of H2O2 concentration on the structure of precipitates formed by Fe(II) oxidation and compared the precipitates to those formed by Fe(III) hydrolysis. Additionally, the phosphate retention under different H2O2 concentrations was evaluated. XRD, TEM, PDA, XPS, and UV-visible absorbance spectroscopy were used to characterize the structure of the formed precipitates; UV-visible absorbance spectroscopy was also used to determine the residual phosphate and Fe(II) in solution. It was found that the predominant precipitates in Fe(II) solution changed from planar-shaped crystalline lepidocrocite (γ-FeOOH) to poor short-range order (poorly crystalline) spherical-shaped hydrous ferric oxide (HFO) with increasing H2O2 concentrations. Although the HFO precipitates formed from Fe(II) resembled those formed from Fe(III) hydrolysis, the former was larger and had clearer lattice fringes. During the formation of γ-FeOOH, both Fe(II)-Fe(III) complexes and ligand-to-metal charge transfer processes were observed, and it was found that Fe(II) was present in the planar-shaped precipitates. Fe(II) might be present in the interior of precipitates as Fe(OH)2, which could serve as a nucleus for the epitaxial growth of γ-FeOOH. In addition, the extent of phosphate retention increased with the H2O2 concentration, indicating the increased reactivity of formed precipitates with H2O2 concentration. More phosphate was retained via coprecipitation with Fe than adsorption on the preformed Fe precipitates due to the incorporation of phosphate within the structure of the formed Fe hydroxyphosphate via coprecipitation.


Assuntos
Compostos Férricos , Fosfatos , Compostos Férricos/química , Compostos Ferrosos , Peróxido de Hidrogênio , Oxirredução , Fosfatos/química
15.
Water Res ; 213: 118163, 2022 Apr 15.
Artigo em Inglês | MEDLINE | ID: mdl-35151090

RESUMO

Hydrophobically-modified chitosan (HC) has emerged as a promising flocculant for trace pharmaceutical removal from surface water. However, the variation in the characteristics of dissolved organic matter (DOM) in different water sources influences the efficacy of HC in removing pharmaceutical compounds. In this work, the flocculation performance of sequentially dosing alum and HC (alum+HC) for the treatment of five water types (three synthetic waters, and samples of two real waters collected from the Yangtze River and the Thames River), having different DOM and five representative pharmaceuticals (initial concentration: 100 ng/L), was assessed by bench-scale jar tests. The DOM characteristics were correlated quantitatively with the removal efficiencies (REs) of the pharmaceuticals. Density functional theory computations were performed to illuminate the interfacial interactions in the flocculation. Alum+HC exhibited a remarkably higher RE of all five pharmaceuticals (maximum RE: 73%-95%) from all waters compared to a conventional coagulant or flocculant (alum or polyacrylamide, respectively). In contrast to using HC alone, alum+HC also achieved a higher RE of pharmaceuticals with nearly half the HC dosage, thereby enhancing the cost-effectiveness of the alum+HC dosing system. Among the different key DOM characteristics, the surface charge and molecular weight of DOM had no evident correlation with RE(pharmaceutical), but the hydrophobic/hydrophilic nature and functional group composition of organic carbon of DOM were strongly correlated: Strongly hydrophobic fractions, with C-C & C=C functional groups (binding pharmaceuticals via hydrophobic association), were beneficial, while hydrophilic fractions with C-OH groups were less effective, for pharmaceutical removal. This work showed the enhanced performance of the alum+HC dosing combination in the removal of different pharmaceutical compounds from different waters, and filled the knowledge gap regarding the performance of hydrophobically-modified flocculants in the treatment of different surface water sources.

16.
J Hazard Mater ; 428: 128223, 2022 04 15.
Artigo em Inglês | MEDLINE | ID: mdl-35063837

RESUMO

Heteroatom doping is a promising technique to enhance biochar for effective environmental remediation. However, development of electroactive heteroatom-doped biochars, e.g., sulfur-doped biochar, has been hindered due to complex nature of non-stoichiometric biomass-derived carbon and changeable electrochemical state of dopants. Herein, we produced a series of wood waste-derived biochars with customized levels of minerals and redox-active moieties, aiming to unravel the crucial factors for sulfur doping. Calcium (Ca) in biochar was found to preferentially coordinate with sulfur to form inactive inorganic sulfur minerals (i.e., CaSO4 and CaS) with inferior catalytic reactivity. After diminishing the inherent Ca minerals beforehand, we could introduce surface phenoxyl-type radicals (C-O•) and vacancy defects on the biochar to develop an electrophilic C-S-O bonding configuration, which guaranteed a high affinity towards peroxymonosulfate (PMS, 2.08 mM g-1, 30 min) and efficient removal of bisphenol A (BPA, 91.1%, 30 min). Scavenging experiments and in-situ Raman analyses indicated that the epoxide-like C-S-O structure induced nucleophilic addition of PMS to generate surface-bound singlet oxygen (1O2, major) and hydroxyl radicals (•OH, minor) through a preservative and stoichiometric interfacial reaction. Overall, the proposed approach overcomes the major hurdles in science-informed fabrication of sulfur-doped biochar and advances its development for environmental remediation.


Assuntos
Recuperação e Remediação Ambiental , Compostos de Epóxi , Carvão Vegetal , Enxofre
17.
J Hazard Mater ; 426: 127797, 2022 03 15.
Artigo em Inglês | MEDLINE | ID: mdl-34815124

RESUMO

Public awareness of plastic pollution and its impact on the ecosystem has increased rapidly. The microplastics in raw waters and their removal during drinking water treatment is receiving growing attention, but the impact on the efficiency of ultrafiltration has not been examined previously, especially in regard to the formation potential of disinfection by-products (DBPs-FP) in effluent water. In this study, two bench-scale continuous-flow ultrafiltration systems, with and without microplastics, were operated to examine the effect of microplastics on ultrafiltration. Results showed that the microplastics not only increased microbial growth, but also affected the microbial community (e.g. families Xanthobacteraceae, Sphingomonadaceae, Leptolyngbyaceae), which can promote the production of extracellular polymeric substances and nitrogen fixation, causing rapid membrane fouling. The formation potential of THM (TCM and BDCM) and N-DBP (TCNM) species in UF permeate increased with the presence of microplastics, due to changes in water quality. Statistical analysis indicated that tyrosine-like components (C3), ammonium (NH4+-N) and tryptophan-like component (C1) can be used as indicators of the DBPs-FP. This study provides new insights into the relationship between microplastics, membrane biofouling and DBPs-FP, and the potential adverse impact of microplastics on drinking water treatment.


Assuntos
Incrustação Biológica , Microbiota , Poluentes Químicos da Água , Purificação da Água , Desinfecção , Humanos , Microplásticos , Plásticos , Poluentes Químicos da Água/análise , Poluentes Químicos da Água/toxicidade
18.
Chemosphere ; 286(Pt 3): 131888, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-34418652

RESUMO

In-situ chemical regeneration of granular activated carbon (GAC) may represent an advantageous alternative to conventional off-site thermal regeneration in water treatment applications. The performance of chemical regeneration of carbon exhausted by metaldehyde and isoproturon was investigated using rapid small-scale column tests, performed using a sequence of pesticide adsorption and chemical regeneration cycles with a novel alkaline-organic regenerant solution. A fresh regenerant solution was able to achieve 82% and 45% regeneration of carbon exhausted by metaldehyde and isoproturon, respectively. After the first regeneration, the performance declined slightly to 79%, and to 36% after the fourth regeneration. A comparison using a thermally regenerated (operational) carbon suggested that chemical regeneration was more beneficial for carbon exhausted by metaldehyde. The regenerant solution has a potential to be re-used multiple times, thereby minimizing the amount of waste chemicals generated. A series of carbon characterization tests showed that chemical regeneration did not alter the surface area, pore size distribution and surface chemistry of the carbon. As part of the evaluation, the adsorption thermodynamics of virgin and chemically regenerated carbons were determined using isothermal titration calorimetry to evaluate the adsorption behaviour of the pesticides on the carbon samples. The relatively high regeneration efficiency achieved by chemical regeneration, and minimal deleterious effect to the physico-chemical properties of the carbon, demonstrated the beneficial potential of this process as an alternative to conventional thermal regeneration of GAC.


Assuntos
Praguicidas , Poluentes Químicos da Água , Purificação da Água , Adsorção , Carvão Vegetal
19.
iScience ; 24(5): 102491, 2021 May 21.
Artigo em Inglês | MEDLINE | ID: mdl-34113827

RESUMO

Flocculation is a mainstream technology for the provision of safe drinking water but is limited due to the ineffectiveness of conventional flocculants in removing trace low-molecular-weight emerging contaminants. We described a synthesis strategy for the development of high-performance nanoflocculants (hydrophobic-organic-chain-modified metal hydroxides [HOC-M]), imitating surfactant-assembling nano-micelles, by integration of long hydrophobic chains with traditional inorganic metal (Fe/Al/Ti)-based flocculants. The core-shell nanostructure was highly stable in acidic stock solution and transformed to meso-scale coagulation nuclei in real surface water. In both jar and continuous-flow tests, HOC-M was superior over conventional flocculants in removing many contaminants (turbidity, UV254, and DOC: >95%; TP and NO3-N: >90%; trace pharmaceuticals [initial concentration: 100 ng/L]: >80%), producing flocs with better structural and dewatering properties, and lowering the environmental risk of metal leaching. The rationally designed nanoflocculants have large application potential, as a solution to increasing public concern about micro-pollutants and increasing water quality requirements.

20.
J Hazard Mater ; 411: 125167, 2021 06 05.
Artigo em Inglês | MEDLINE | ID: mdl-33858110

RESUMO

A novel process involving the simultaneous electrochemical-oxidation (EO) and electrosynthesis of ferrate has been investigated for the treatment of the commonly detected and recalcitrant pesticide, atrazine. The present study considered the electrosynthesis of ferrate, in neutral pH, using low concentration iron (Fe2+) representative of raw water levels and its subsequent effect on atrazine degradation. Ferrate synthesis was unaffected by current density (10-80 mA cm-2), indicating mass transport limitations. Synthesis was affected by the initial iron concentration, whereby 0.051, 0.108 and 0.332 mg L-1 was generated with an Fe2+ concentration of 0.5, 1.0 and 3.0 mg L-1, respectively. When operating under simultaneous EO and ferrate oxidation, atrazine degradation exceeded that of a solely EO process. From an initial concentration of 2.00 mg L-1, atrazine was degraded to 1.34, 1.05 and 0.51 mg L-1 during 10, 40 and 80 mA cm-2, characterised by pseudo-first-order kinetics. Degradation with electrochemically-generated ferrate could be described by second-order kinetics, and yielded a degradation rate constant of 23.5 M-1 s-1. The effect of natural organic matter (NOM) on atrazine degradation was also investigated. Ferrate was observed to be mostly scavenged by resorcinol, a representative NOM compound, having a second-order reaction rate constant of 9.71 × 102 M-1 s-1.

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