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1.
Langmuir ; 40(12): 6353-6362, 2024 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-38470331

RESUMO

The biological NO3- removal process might be accompanied by high CO2 emissions and operation costs. Capacitive deionization (CDI) has been widely studied as a very efficient method to purify water. Here, a porous carbon material with a tunable nitrogen configuration was developed. Characterization and density functional theory calculation show that nitrogenous functional groups have a higher NO3- binding energy than Cl-, SO42-, and H2PO4-. In addition, the selectivity of NO3- is improved after the introduction of micropores by using the pore template. The NO3- ion removal and selectivity of MN-C-12 are 4.57 and 3.46-5.42 times that of activated carbon (AC), respectively. The high NO3- selectivity and electrosorption properties of MN-C-12 (the highest N content and micropore area) are due to the synergistic effect of the affinity of nitrogen functional groups to NO3- and microporous ion screening. A CDI unit for the removal of nitrogen from municipal wastewater was constructed and applied to treat wastewater meeting higher discharge standards of A (N: 15 mg L-1) and B (N: 20 mg L-1) ((GB18918-2002), China). This work provides new insights into enhanced carbon materials for the selective electrosorption of wastewater by CDI technology.

2.
Small ; 19(50): e2303928, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37625020

RESUMO

The catalytic oxidation of toxic organic pollutants in water requires enhanced efficiency for commercial applications. A ZnO nanorod array grown on a carbon fiber cloth (CFC) serves as the zinc source to ensure that the Ni/ZIF-8/ZnO nanoreactor is constructed. The Ni/ZIF-8/ZnO/CFC nanoreactor efficiently activates peroxymonosulfate (PMS) for bisphenol A (BPA) degradation owing to its high density of active sites, high adsorbability, and dispersibility structure, which concentrates catalytic and adsorptive sites within a confined space. Experimental and theoretical calculations clearly show that the introduction of Ni is beneficial for improving the adsorption of BPA and the activation of PMS. The synergistic mechanism of BPA adsorption-PMS activation is also investigated, and the degradation pathway of BPA is examined. Moreover, a filter catalytic unit is constructed using Ni/ZIF-8/ZnO/CFC to achieve a continuous zero discharge of BPA, which is convenient for nanocatalyst recycling. This study aims to develop a new strategy for the removal of emerging organic pollutants from water using a system with strong adsorption and catalytic capabilities.

3.
Langmuir ; 39(25): 8760-8768, 2023 Jun 27.
Artigo em Inglês | MEDLINE | ID: mdl-37306688

RESUMO

Metal organic framework (MOF)-based adsorbents are appealing for removing low-concentration phosphates with interfering ions in wastewater purification, a new strategy developed to maintain the good activity of metal sites. Here, ZIF-67 was immobilized onto the porous surface of anion exchange resin (D-201) with a high loading amount of 22.0 wt % by a modifiable Co(OH)2 template. We observed that the removal rate of low-concentration phosphate (2 mg P/L) by ZIF-67/D-201 nanocomposites was 98.6%, and more than 90% phosphate adsorption capacity was still maintained, with 5 times molar concentration of interfering ions in the solution. Moreover, after six times of regeneration by solvothermal reaction in the ligand solution, the structure of ZIF-67 was better preserved in D-201 with more than 90% phosphate removal rate. ZIF-67/D-201 could be employed effectively in fixed-bed adsorption runs. By the analysis of experiment and characterization, we found that during the adsorption-regeneration process of ZIF-67/D-201 for phosphate, reversible structural transformation of ZIF-67 and Co3(PO4)2 occurred in D-201. In general, the study reported a new method to develop MOF adsorbents for wastewater treatment.

4.
J Environ Sci (China) ; 111: 313-323, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-34949361

RESUMO

Metal oxide/hydroxide-based nanocomposite adsorbents with porous supporting matrices have been recognized as efficient adsorbents for phosphorus recovery. Aiming at satisfying increasingly restrictive environmental requirements involving improving metal site utilization and lowering metal leakage risk, a glycol-solvothermal confined-space synthesis strategy was proposed for the fabrication of FeOOH/anion exchanger nanocomposites (Fe/900s) with enhanced metal site utilization and reduced metal leakage risk. Compared to composites prepared using alkaline precipitation methods, Fe/900s performed comparably, with a high adsorption capacity of 19.05 mg-P/g with an initial concentration of 10 mg-P/L, a high adsorption selectivity of 8.2 mg-P/g in the presence of 500 mg-SO42-/L, and high long-term resilience (with a capacity loss of ~14% after five cycles), along with substantially lower Fe loading amount (4.11 wt.%) and Fe leakage percentage. Mechanistic investigation demonstrated that contribution of the specific FeOOH sites to phosphate adsorption increased substantially (up to 50.97% under the optimal conditions), in which Fe(III)-OH was the dominant efficient species. The side effects of an excessively long reaction time, which included quaternary ammonium decomposition, FeOOH aggregation, and Fe(III) reduction, were discussed as guidance for optimizing the synthesis strategy. The glycol-solvothermal strategy provides a facile solution to environmental problems through nanocrystal growth engineering in a confined space.


Assuntos
Nanocompostos , Poluentes Químicos da Água , Adsorção , Domínio Catalítico , Compostos Férricos , Glicóis , Cinética , Fósforo , Poluentes Químicos da Água/análise
5.
J Environ Sci (China) ; 106: 105-115, 2021 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-34210426

RESUMO

Our present study was to prepare a biomass-supported adsorbents with high adsorptive capacity and high selectivity to prevent the accelerated eutrophication in water body. To this end, different metal hydroxide (La, Zr and Fe) first was successfully loaded on chitosan microspheres. Then the quaternary ammonium group with different content was introduced into the adsorbent by polymerization. By comparison of adsorption properties, chitosan-La(OH)3-quaternary ammonium-20% (CS-La-N-20%) has strong adsorption to phosphate (160 mg/g) by immobilizing nano-sized La(OH)3 within a quaternary-aminated chitosan and it maintain high adsorption in the presence of salt ions. The pH results indicated that the CS-La-N-20% would effectively sequestrate phosphate over a wide pH range between 3 and 7 without significant La3+ leaching. What's more, adsorption capacity on the introduce of positively charged quanternary-aminated groups was significantly higher than that of the unmodified adsorbents at alkaline conditions. The column adsorption capacity reached 1300 bed volumes (BV) when phosphate concentration decreased until 0.5 mg/L at 6 BV/hr. The column adsorption/desorption reveals that no significant capacity loss is observed, indicating excellent stability and repeated use property. Characterizations revealed that phosphate adsorption on CS-La-N-20% through ligand exchange (impregnated nano-La(OH)3) and electrostatic attraction (positively charged quanternary-aminated groups). All the results suggested that CS-La-N-20% can serve as a promising adsorbent for preferable phosphate removal in realistic application.


Assuntos
Quitosana , Poluentes Químicos da Água , Adsorção , Concentração de Íons de Hidrogênio , Hidróxidos , Cinética , Fosfatos
6.
J Environ Sci (China) ; 31: 226-34, 2015 May 01.
Artigo em Inglês | MEDLINE | ID: mdl-25968278

RESUMO

The presence of pharmaceuticals in aquatic environments poses potential risks to the ecology and human health. This study investigated the removal of three widely detected and abundant pharmaceuticals, namely, ibuprofen (IBU), diclofenac (DC), and sulfadiazine (SDZ), by two magnetic ion-exchange resins. The adsorption kinetics of the three adsorbates onto both resins was relatively fast and followed pseudo-second-order kinetics. Despite the different pore structures of the two resins, similar adsorption patterns of DC and SDZ were observed, implying the existence of an ion-exchange mechanism. IBU demonstrated a combination of interactions during the adsorption process. These interactions were dependent on the specific surface area and functional groups of the resin. The adsorption isotherm fittings verified the differences in the behavior of the three pharmaceuticals on the two magnetic ion-exchange resins. The presence of Cl- and SO4(2-) suppressed the adsorption amount, but with different inhibition levels for different adsorbates. This work facilitates the understanding of the adsorption behavior and mechanism of pharmaceuticals on magnetic ion-exchange resins. The results will expand the application of magnetic ion-exchange resins to the removal of pharmaceuticals in waters.


Assuntos
Diclofenaco/química , Ibuprofeno/química , Resinas de Troca Iônica/química , Sulfadiazina/química , Poluentes Químicos da Água/química , Adsorção , Antibacterianos/química , Anti-Inflamatórios não Esteroides/química , Concentração de Íons de Hidrogênio , Fenômenos Magnéticos
7.
J Hazard Mater ; 475: 134944, 2024 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-38889470

RESUMO

Although conventional nanofiltration (NF) membrane is widely applied in water treatment, it faces the challenges of insufficient selectivity toward emerging contaminants, low permeability and non-sustainable fouling control. Herein, a novel electroactive metal-organic frameworks/carbon nanotubes membrane was constructed by facile and green nanobubbles-mediated non-solvent-induced phase separation (NIPS) strategy for ultrafast antibiotics removal. It presented 3-fold to 100-fold higher permeability (101.3-105.7 L·h-1·m-2·bar-1) without compromising rejection (71.8 %-99.3 %) of common antibiotics (tetracycline, norfloxacin, sulfamethoxazole, sulfamethazine) than most commercial and state-of-the-art NF membranes. The separation mechanism was due to the synergy of loose selective layer with three-dimensional interconnected networks and UiO-66/CNTs with unique pore sieving and charge property. It also presented excellent antibiotics selectivity with high NaCl/tetracycline separation factor of 194 and CuCl2/tetracycline separation factor of 316 for remediation of antibiotics and heavy metal combined pollution. Meanwhile, it possessed efficient anti-fouling, antibacterial and electro-driven self-cleaning ability, which enabled sustainable fouling control and disinfection with short process, low energy and chemical consumption. Furthermore, potential application of UiO-66/CNTs membrane in wastewater reclamation was demonstrated by stable antibiotics rejection, efficient flux recovery and long-term stability over 260 h. This study would provide useful insights into removal of emerging contaminants from water by advanced NF membrane.


Assuntos
Antibacterianos , Membranas Artificiais , Estruturas Metalorgânicas , Nanotubos de Carbono , Poluentes Químicos da Água , Purificação da Água , Estruturas Metalorgânicas/química , Nanotubos de Carbono/química , Antibacterianos/química , Poluentes Químicos da Água/química , Purificação da Água/métodos , Desinfecção/métodos , Ácidos Ftálicos
8.
J Environ Sci (China) ; 25(7): 1291-9, 2013 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-24218839

RESUMO

The study evaluated the adsorption of two antibiotics by four engineered adsorbents (hypercrosslinked resin MN-202, macroporous resin XAD-4, activated carbon F-400, and multi-walled carbon nanotubes (MWCNT)) from aqueous solutions. The dynamic results demonstrated the dominant influence of pore size in adsorption. The adsorption amounts of antibiotics on XAD-4 were attributed to the hydrophobic effect, whereas steric hindrance or micropore-filling played a main role in the adsorption of antibiotics by F-400 because of its high microporosity. Aside from F-400, similar patterns of pH-dependent adsorption were observed, implying the importance of antibiotic molecular forms to the adsorption process for adsorbents. Increasing the ionic concentration with CaC12 produced particular adsorption characteristics on MWCNT at pH 2.0 and F-400 at pH 8.0, which were attributed to the highly available contact surfaces and molecular sieving, respectively. Its hybrid characteristics incorporating a considerable portion of mesopores and micropores made hypercross linked MN-202 a superior antibiotic adsorbent with high adsorption capacity. Furthermore, the adsorption capacity of MWCNT on the basis of surface area was more advantageous than that of the other adsorbents because MWCNT has a much more compact molecular arrangement.


Assuntos
Antibacterianos/química , Sulfadimetoxina/química , Sulfapiridina/química , Poluentes Químicos da Água/química , Adsorção , Concentração de Íons de Hidrogênio , Resinas de Troca Iônica , Nanotubos de Carbono/química , Concentração Osmolar , Poliestirenos/química , Polivinil/química , Temperatura , Eliminação de Resíduos Líquidos/instrumentação , Eliminação de Resíduos Líquidos/métodos
9.
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
10.
Water Res ; 241: 120164, 2023 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-37290197

RESUMO

Heterogeneous catalysts lag far behind their homogeneous counterparts in activating peroxymonosulfate (PMS) for water decontamination due to the low site intrinsic activity and sluggish mass transfer. The single-atom catalyst can bridge the gap between heterogeneous and homogeneous catalysts, but the difficulty to break scaling relations originating from the site monotony restricts further efficiency upgradation. Herein through modulating the crystallinity of NH2-UIO-66, a porous carbon support with ultrahigh surface area (1721.71 m2 g-1) is obtained to anchor the dual-atom FeCoN6 site, which exhibits superior turnover frequency over single-atom FeN4 and CoN4 sites (13.07 versus 9.97, 9.07 min-1). The as-synthesized composite thus outperforms the homogeneous catalytic system (Fe3++Co2+) for sulfamethoxazole (SMZ) degradation, and the catalyst-dose-normalized kinetic rate constant (99.26 L min-1 g-1) exceeds reported values by 1∼2 orders of magnitude. Moreover, only 20 mg of the catalyst can run a fluidized-bed reactor to realize continuous zero discharge of SMZ in multiple actual waters for up to 8.33 h. Unlike all reported reaction routes, the catalysis on the diatomic site follows a new surface collision oxidation path, i.e. the dispersed catalyst adsorbs PMS to generate surface-activated PMS with high potential, which collides with surrounding SMZ and directly seizes electron from it to induce pollutant oxidation. Theoretical calculation indicates that the enhanced activity of FeCoN6 site stems from the diatomic synergy, leading to stronger PMS adsorption, larger near-Fermi-level density of states and optimal global Gibbs free energy evolution. Overall, this work provides an effective strategy of constructing heterogeneous dual-atom catalyst/PMS process to achieve faster pollution control than homogeneous system, and sheds light on the interatomic synergetic mechanism for PMS activation.


Assuntos
Descontaminação , Diatomáceas , Adsorção , Carbono , Catálise , Peróxidos
11.
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
12.
Water Sci Technol ; 66(1): 193-200, 2012.
Artigo em Inglês | MEDLINE | ID: mdl-22678218

RESUMO

The aim of this study is to report on the performance of a novel non-phosphorus antiscalant, acrylic acid (AA)-allylpolyethoxy carboxylate (APEC), being developed for calcium-sulfate scale inhibition in industrial water systems. The performance of AA-APEC on calcium-sulfate scale inhibition was compared with that of the two commercial inhibitors, polyamino polyether methylene phosphonates (PAPEMP) and polyacrylic acid (PAA), containing the same polyethylene glycol segments or carboxyl functional groups as AA-APEC. The study indicated that AA-APEC could act as a highly effective calcium sulfate inhibitor, having strong ability to inhibit the precipitation of calcium sulfate at a dosage of 2 mg L(-1), showing approximately 83.6% inhibition. The results also showed that AA-APEC dosage, the solution pH, inhibiting temperature, concentration of Ca(2+), and SO(4)(2-) all play important roles in inhibiting calcium-sulfate precipitation. The precipitation thermodynamics and kinetics at different temperatures were also discussed. X-ray diffractometer (XRD) and scanning electron microscope (SEM) analysis showed that AA-APEC strongly affected the texture and the morphology of the deposited calcium sulfate. Calcium sulfate has been inhibited through stabilization by adsorption onto crystal growth sites of nascent crystals altering their morphology.


Assuntos
Acrilatos/química , Cálcio/química , Polímeros/química , Sulfatos/química , Poluentes Químicos da Água/química , Precipitação Química , Cinética , Microscopia Eletrônica de Varredura , Estrutura Molecular , Termodinâmica , Eliminação de Resíduos Líquidos/métodos , Difração de Raios X
13.
Water Res ; 220: 118635, 2022 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-35609429

RESUMO

In order to resolve the poor antibiotics rejection and serious fouling of ultrafiltration (UF) membrane during municipal wastewater reclamation, a novel anodic membrane (defective UiO-66 (D-UiO-66)/Graphite/Polyvinylidene fluoride (PVDF)) with high pure water flux (596.1 L•h - 1•m - 2•bar-1) was fabricated by incorporating defective zirconium based metal-organic framework (D-UiO-66) and conductive graphite particles into PVDF matrix and applied in the coupling of electro-oxidation and membrane filtration process. Compared to the other anodic membranes (i.e., Graphite/PVDF and UiO-66/Graphite/PVDF), D-UiO-66/Graphite/PVDF possesses superior anti-fouling and self-cleaning abilities (flux recovery=100%, model foulant: bovine serum albumin) in both intermittent and continuous supply of electric field under current density of 0.01 mA/cm2; moreover, efficient antibiotics (tetracycline, norfloxacin, tylosin and sulfamethoxazole) removal (> 96.6%) and bactericidal efficiency against E. coli and S. aureus (100%) were achieved simultaneously without the addition of chemical reagents due to the higher electrocatalytic activity of anodic membrane for oxidation of pollutants by •OH and •O2- free radicals. Three degradation pathways of antibiotics were proposed and the self-cleaning mechanism of membrane was dominated by the synergy of the partial mineralization and the reduced fouling potential of foulants after oxidation as revealed by the increase in hydrophilicity, and decrease in negative charge and molecular weight. The fabricated membrane also presents excellent electrochemical stability, separation and self-cleaning performance for treatment of municipal secondary effluent during long-term filtration with low electric energy consumption, which is promising in wastewater reclamation.


Assuntos
Grafite , Purificação da Água , Antibacterianos , Escherichia coli , Grafite/química , Membranas Artificiais , Estruturas Metalorgânicas , Ácidos Ftálicos , Staphylococcus aureus , Ultrafiltração , Águas Residuárias
14.
Chemosphere ; 287(Pt 2): 132145, 2022 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-34500330

RESUMO

Lake sediment and algal sludge with large output posed significant environmental risks. In this work, an idea of co-utilization of both solid wastes for the production of ceramsite (a sort of porous lightweight aggregates as building materials) was proposed and validated for the first time. The treatment process contained a dewatering step by a flocculation-pressure filtration method, and a sintered ceramsite preparation step. Effects of flocculant type and dosage on the dewatering performance were studied in the first step. An environmental-friendly amphoteric starch flocculant with a dosage of 12 mg/(g dried sample) was found to achieve the best dewatering performance. Effects of raw material mass ratio, sintering temperature and time in the second step were investigated. Under the optimal conditions (60 wt% of dewatered sediment; 20 wt% of dewatered algal sludge; 20 wt% of additives (fly ash: calcium oxide: kaolin = 2:1:2); sintering temperature: 1100 °C; time: 35 min), the obtained ceramsite met the Chinese National Standard as a qualified building material, with reliable environmental safety according to the leaching results for both heavy metals and microcystins. Both environmental and economic benefits of the proposed treatment were assessed. The process completely followed the rules of "reduction, harmlessness and resource utilization" for solid waste treatment and disposal; Meanwhile, the profit of the proposed ceramsite production could be more than 2.3 US dollar/m3. The co-utilization method in this work acted as a good example for the comprehensive management of solid wastes in water-rich areas.


Assuntos
Cianobactérias , Lagos , Cinza de Carvão , Misturas Complexas , Porosidade , Esgotos
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.
Environ Pollut ; 294: 118602, 2022 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-34856247

RESUMO

The polycyclic aromatic hydrocarbons (PAHs) that enter the aqueous phase usually coexist with fulvic acid (FA). Therefore, we initiated this investigation to explore the influences of FA on bacterial biofilm formation and its potential to biodegrade pyrene (PYR), using electron microscopic techniques and isobaric tags for relative and absolute quantification (iTRAQ). Our results revealed that FA stimulated biofilm formation and enhanced the biodegradation of PYR. First, FA favored the three-dimensional proliferation of bacteria, with an OD590/OD600 value of up to 14.78, and the extracellular surfaces covered by a layer of biomaterials. Distinctive intracellular morphologies of texture and organization were accompanied by reduced inter-bacterial distances of less than 0.31 µm. The biofilms formed displayed interactions between FA and surficial proteins, as noted by band shifts for the C-O and CO groups. Strikingly, FA triggered the upregulation of 130 proteins that were either operational in biofilm formation or in metabolic adjustments; with the changes supported by the increasing intensity of free amino acids and the newly generated N-O bonds. The results above revealed that the enhanced biodegradation was related to the up-regulation of the proteins functioned for ribosomal and carbon metabolism, and the ultra-structural changes in FA-induced biofilm system.


Assuntos
Carbono , Hidrocarbonetos Policíclicos Aromáticos , Benzopiranos , Biodegradação Ambiental , Biofilmes , Pirenos , Regulação para Cima
17.
Chemosphere ; 288(Pt 3): 132613, 2022 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-34678349

RESUMO

The search for nature-based tools to enhance bioremediation is essential for the sustainable restoration of contaminated ecosystems. Humic acid (HA) is an important component of organic matter in soil and water, but its effect on the microbial degradation of organic pollutants remains unclear. In this study, the biodegradation of pyrene by Mycobacterium sp. NJS-1 with and without HA was investigated. Only around 10.5% of pyrene was biodegraded in the pyrene treatment alone, whereas the addition of HA significantly enhanced biodegradation to the point where over 90% of pyrene was biodegraded. The production of 4,5-dihydropyrene-4,5-diol and phenanthrene-3,4-diol indicated the metabolic pathway via attacking of 4,5-positions of pyrene. Interestingly, 1,2-dimethoxypyrene was detected with the addition of HA, suggesting that HA induced a new ring-opening pathway involving the attack on the 1,2-positions of pyrene. The addition of HA first induced protein self-cleavage behavior with a significant increase in phenylalanine, tyrosine, and tryptophan containing large numbers of COO- groups. Furthermore, it altered the intracellular and extracellular ultrastructure of bacterial cells, promoting their growth in size and number as well as reducing the space between them. Overall, HA increased the ring-opening positions of pyrene and facilitated its interaction with bacterial cells, thus improving its biodegradability. Building upon the findings of this study to further research is conducive to the sustainable solution of environmental pollution.


Assuntos
Mycobacterium , Hidrocarbonetos Policíclicos Aromáticos , Poluentes do Solo , Biodegradação Ambiental , Ecossistema , Substâncias Húmicas/análise , Hidrocarbonetos Policíclicos Aromáticos/análise , Pirenos , Poluentes do Solo/análise
18.
Sci Total Environ ; 813: 151893, 2022 Mar 20.
Artigo em Inglês | MEDLINE | ID: mdl-34826487

RESUMO

Fe content and distribution on montmorillonite would probably enhance its sorption capacity for hydrophobic organic pollutants. Thus, Fe modified montmorillonites with different ratios of FeSO4·7H2O and Ca-montmorillonite were prepared. The results indicated that γ-Fe2O3 nanoparticles were not only generated at the montmorillonite surfaces, but that the γ-Fe2O3 also extended the edges of montmorillonite surfaces. The sorption capacities for pyrene were enhanced and even reached 834.79 µg g-1 with increase in ferrous iron content, but were then suppressed due to aggregation of γ-Fe2O3 on montmorillonite surfaces. Furthermore, pyrene was directly observed on γ-Fe2O3-montmorillonite surfaces with a lattice spacing parameter of approximately 0.27 nm, indicating that a new phase that mainly contained pyrene was generated during the sorption process. Additionally, after regenerating the γ-Fe2O3-montmorillonite composites, they could be reused for at least 5 cycles. It is therefore proposed that the prepared γ-Fe2O3-montmorillonite could be exploited as a potential green composite for remediation of hydrophobic organic pollutants in soil and sediment.


Assuntos
Bentonita , Nanopartículas , Adsorção , Ferro , Pirenos , Solo
19.
Sci Total Environ ; 753: 142079, 2021 Jan 20.
Artigo em Inglês | MEDLINE | ID: mdl-32911176

RESUMO

A high incidence of harmful algal bloom in eutrophic surface waters causes many environmental problems. Thermophilic aerobic composting enables effective treatment and disposal of algal sludge that remains after the dewatering of algae slurries, and provides a value-added organic fertiliser. Previous studies have either only dealt with the composting of a single waste component or were conducted at a lab-/pilot-scale; however, this work is a comprehensive assessment of full-scale mechanized thermophilic aerobic co-composting of algal sludge and other typical biomass-based wastes, including chicken faeces and rice straw, in a water-rich rural area in the Tai lake basin, China. With the optimised feedstock material mass ratio (6.0:1.8:1.0 for straw:algae:faeces; initial C/N ratio of 20; and initial moisture of 60 wt%), the co-composting process effectively achieved the reduction, harmlessness, and reuse of waste. The moisture content (28.36 wt% of wet weight), organic matter content (57.91 wt% of dried weight), total nutrient content (6.59 wt% for TN + TP + TK of dried weight), and heavy metal contents as well as the pH of the final product fully met the Chinese National Agricultural Organic Fertiliser Standard requirements. The reduction rates of microcystin and toxic volatile fatty acid contents were higher than 99.5%, and the seed germination index of the product was 114.5%. A notable economic benefit with a gross profit margin of 167-434% of the process was highlighted. Investigation of the associated mechanisms, including statistical analysis, spectral characterisation, micro-morphological observation, and microbial community analysis, revealed that a decreased particle sizes with a looser structure and an efficient humification effect, resulting from the work of several identified dominant microbial species, contributed to the high product quality. The current study provided a demonstration of the promising full-scale co-composting technology for comprehensive management of the environment in water-rich rural areas and the construction of a sustainable watershed.


Assuntos
Compostagem , Cianobactérias , Animais , China , Fezes , Gado , Esgotos , Solo
20.
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.

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