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1.
Article in English | MEDLINE | ID: mdl-39088163

ABSTRACT

PURPOSE OF REVIEW: Intracerebral hemorrhage (ICH) is the most devastating type of stroke, causing widespread disability and mortality. Unfortunately, the acute care of ICH has lagged behind that of ischemic stroke. There is an increasing body of evidence supporting the importance of early interventions including aggressive control of blood pressure and reversal of anticoagulation in the initial minutes to hours of presentation. This review highlights scientific evidence behind a new paradigm to care for these patients called Code-ICH. RECENT FINDINGS: While numerous trials aimed at decreasing hematoma expansion through single interventions had failed to show statistically significant effects on primary outcomes, time-sensitive, multifaceted, bundled care approaches have recently shown substantial promise in improving functional outcomes in patients with ICH. The concept of Code-ICH can serve as a structural platform for the practice of acute care neurology to continuously measure its performance, reflect on best practices, advance care, and address disparities.

2.
Water Res ; 262: 122047, 2024 Jul 04.
Article in English | MEDLINE | ID: mdl-39003956

ABSTRACT

Dissolved organic matter (DOM) plays a pivotal role in drinking water treatment, influencing the performance of unit processes and final water quality (e.g. disinfection byproduct risk). Biofiltration is an effective method of reducing DOM, but currently lacks a comprehensive appreciation of the association between microbial profiles and biofiltration performance. In this study, bench-scale biofiltration units inoculated with microbial consortia from river and soil matrices were operated successively for comparing their efficacy in terms of DOM removal. The results showed that biofiltration units receiving soil microbes were significantly superior (p < 0.05) to those receiving river inoculated microbes in terms of decomposing DOM recalcitrant fractions and reducing DBP formation potential, resulting in DOC and DBP precursor removals of up to 58.4 % and 87.9 %, respectively. Characterization of the taxonomic composition revealed that differences in the microbial assembly of the two biofilter groups were subject to deterministic rather than stochastic factors. Furthermore, more complicated interspecific relationships and niche structures in soil inoculated biofilters were deciphered by co-occurrence network, providing a plausible profile on a taxonomic division of labor in DOM stepwise degradation. Accordingly, the contribution of microbial compositions was found to be of greater importance than the GAC mass and biomass attached to the media. Thus, this study has advanced the understanding of microbial-mediated DOM decomposition in biofiltration, and also provided a promising strategy for enhancing the process for water use via developing appropriate engineered consortia of bacteria.

3.
Water Res ; 262: 122146, 2024 Jul 25.
Article in English | MEDLINE | ID: mdl-39079425

ABSTRACT

The formation of flocs is crucial in the coagulation process of water treatment. However, the nature of ligand exchange on the surface of primary nanoparticles (PNPs) during floc formation requires further investigation to enhance our understanding of the coagulation mechanism. Phosphate (P) is a ubiquitous nutrient ion in aquatic surface water, in this study, the impact of P on floc growth under different pH conditions were investigated. The results revealed that floc growth patterns depended on both P dosage and pH. The mode of ligand exchange between P and in-situ formed ferric hydroxide within a pH range of 5 to 10 was further explored, and remarkable disparities in pH changes induced by P addition were observed. At lower pH levels, OH- release occurred relatively slowly, stabilizing with continued P addition. At neutral pH, OH- release was comparatively higher with P addition, while under alkaline conditions, both the quantity of OH- and its release rate decreased. It was deduced that Fe-OH21/2+ sites function as "active sites," while Fe-OH1/2- sites act as "inert sites" on the surface of PNPs formed during flocculation. These sites are crucial in the interconnections between flocs formed during coagulation and in floc growth. Analyses of Fe PNPs by Scanning Electron Microscopy (SEM) and Transmission Electron Microscopy (TEM), with and without P addition, revealed that the introduction of P inhibits or interferes with the self-crystallization of Fe PNPs through chemical coordination reactions. The results offer deeper insights into the coagulation mechanism and the transformation of Fe flocs in raw waters containing P during water treatment practices.

4.
Nat Commun ; 15(1): 6356, 2024 Jul 28.
Article in English | MEDLINE | ID: mdl-39069514

ABSTRACT

Soil dissolved organic matter (DOM) is crucial to atmospheric, terrestrial and aquatic environments as well as human life. Here, by characterizing DOM from 89 grassland soils throughout China, we reveal the spatial association between DOM geochemistry in the dry season vs annual ecosystem exchange and cancer cases. The humic-like and high molecular weight (3.4-25 kDa) fractions with lower biodegradability, decline from the northern to the southern regions of China, and are correlated with lower soil respiration and net ecosystem productivity at the continental scale. The <1.2 kDa and proteinaceous fractions could serve as a geographical indicator of nasopharyngeal cancer incidence and mortality, while the 3.4-25 kDa and humified fractions are potentially associated with pancreatic cancer cases (P < 0.05). Our findings highlight that exploiting the environmental functions of soil DOM and mitigating the negative impacts are necessary, and require actions tailored to local soil DOM conditions.


Subject(s)
Grassland , Humic Substances , Soil , China , Soil/chemistry , Humic Substances/analysis , Humans , Ecosystem , Seasons , Pancreatic Neoplasms
5.
Environ Sci Technol ; 58(27): 12281-12291, 2024 Jul 09.
Article in English | MEDLINE | ID: mdl-38939969

ABSTRACT

Significant progress has been made previously in the research and development of graphene oxide (GO) membranes for water purification, but their biofouling behavior remains poorly understood. In this study, we investigated the biofilm formation and biofouling of GO membranes with different surface microstructures in the context of filtering natural surface water and for an extended operation period (110 days). The results showed that the relatively hydrophilic and smooth Fe(OH)3/GO membrane shaped a thin and spatially heterogeneous biofilm with high stable flux. However, the ability to simultaneously mitigate biofilm formation and reduce biofouling was not observed in the weakly hydrophilic and wrinkled Fe/GO and H-Fe(OH)3/GO membranes. Microbial analyses revealed that the hydrophilicity and roughness distinguished the bacterial communities and metabolic functions. The organic matter-degrading and predatory bacteria were more adapted to hydrophilic and smooth GO surfaces. These functional taxa were involved in the degradation of extracellular polymeric substances (EPS), and improved biofilm heterogeneity. In contrast, the weakly hydrophilic and wrinkled GO surfaces had reduced biodiversity, while unexpectedly boosting the proliferation of EPS-secreting bacteria, resulting in increased biofilm formation and aggravated biofouling. Moreover, all GO membranes achieved sustainable water purification during the entire operating period.


Subject(s)
Biofilms , Biofouling , Graphite , Water Purification , Graphite/chemistry , Membranes, Artificial , Oxides/chemistry
6.
Chemosphere ; 361: 142438, 2024 Aug.
Article in English | MEDLINE | ID: mdl-38797203

ABSTRACT

In this research, the interactions of two azo dyes, Methyl Orange (MO) and Eriochrome Black T (EBT), with dissolved organic matter (DOM) in surface water were studied, emphasizing their removal using nano-filtration membranes (NF-270 and NF-90). High-Performance Size Exclusion Chromatography (HPSEC) findings indicated that the dyes' molecular weight in deionized (DI) water ranged from 500 to 15k Dalton (Da), adjusting peak intensities with Jingmi River (JM) water Beijing. Notably, when dyes were diluted in JM water, ultraviolet (UV533 & 466, and UV254), together with total organic carbon (TOC) parameters, revealed color removal rates of 99.49% (EBT), 94.2% (MO), 87.6% DOM removal, and 86% TOC removal for NF-90. The NF-90 membrane demonstrated a 75% flux decline for 50 mL permeate volume due to its finer pore structure and higher rejection effectiveness. In contrast, the NF-270 membrane showed a 60% decline in flux under the same conditions. Attenuated total reflection-Fourier transform infrared spectroscopy (ATR-FTIR) analysis of dye-treated membranes in JM water revealed that the NF-270 showed a CC bond peak at 1660 cm-1 across various samples, while analyzing NF-90, the peaks at 1400 cm-1, 1040 cm-1, 750 cm-1, and 620 cm-1 disappeared for composite sample removal. The hydrophobicity of each membrane is measured by the contact angle (CA), which identified that initial CAs for NF-270 and NF-90 were 460 and 700, respectively, that were rapidly declined but stabilized after a few seconds of processing. Overall, this investigation shows that azo dyes interact with DOM in surface waters and enhance the removal efficiency of NF membranes.


Subject(s)
Azo Compounds , Coloring Agents , Filtration , Water Pollutants, Chemical , Water Purification , Azo Compounds/chemistry , Water Pollutants, Chemical/chemistry , Water Pollutants, Chemical/analysis , Coloring Agents/chemistry , Water Purification/methods , Filtration/methods , Membranes, Artificial , Spectroscopy, Fourier Transform Infrared
7.
J Hazard Mater ; 472: 134522, 2024 Jul 05.
Article in English | MEDLINE | ID: mdl-38714057

ABSTRACT

Electro-catalytic conversion of nitrate (NO3-) to ammonia (NH3) via the Nitrate Reduction to Ammonia (NORA) process represents a promising strategy for both ammonia synthesis and environmental remediation. Despite its potential, the efficiency of low-concentration NORA is often hindered by mass transfer limitations, competing byproducts (N2 and NO2-), and side reactions such as hydrogen evolution. This study introduces a novel pulsed electro-synthesis technique that alternates the potential to periodically accumulate and transform NO2- intermediates near a Cu2O@Pd electrode, enhancing the NORA process. Compared with that under potentiostatic conditions, the Cu2O@Pd electrodes exhibited a higher NORA activity under the optimized pulsed condition, where a NH3-N Faradaic efficiency (FE) of 81.2%, a yield rate of 1.08 mg h-1 cm-2 and a selectivity efficiency (SE) of 81.5%, were achieved. In-situ characterization revealed an enhancement mechanism characterized by optimized adsorption of the key *NO intermediate, followed by the hydrogenation path "*N → *NH → *NH2→ *NH3". Further investigations indicated the electro-catalytic synergies between Pd sites and Cu species, where the Pd atoms were the reaction sites for the H adsorption while the Cu species were responsible for the NO3- activation. This research offers a novel insight into a method of enhancing low-concentration NORA.

8.
Water Res ; 256: 121539, 2024 Jun 01.
Article in English | MEDLINE | ID: mdl-38583335

ABSTRACT

Inorganic coagulants such as poly aluminum ferric chloride (Al/Fe) are applied conventionally to sewage sludge dewatering and can be retained in the sludge cake, causing its conductivity to increase and generate secondary pollution. To reduce these disadvantages, there is a need to develop alternative, more sustainable chemicals as substitutes for conventional inorganic coagulants. In the present investigation, the application of a polymeric chitosan quaternary ammonium salt (CQAS) is explored as a complete, or partial, replacement for Al/Fe in the context of sludge dewatering processes. Laboratory experiments using digested sewage sludge showed that CQAS could effectively substitute for over 80 % of the Al/Fe inorganic coagulant in the sludge dewatering process. This substitution resulted in a reduction of sludge cake conductivity by more than 50 %. Simulation of sludge dewatering curves and imaging of the sludge surface indicated that the addition of CQAS led to an increase in nanosized pores, and a decrease in the specific resistance of the sludge filter cake as the dosage of Al/Fe decreased to around 30 %. The variations of fluorescence emission, quantum yield and carboxylic and amino groups, suggested that the chelating of Al/Fe decreased due to the bridging effects of CQAS. The CQAS had different flocculation bridging effects on various EPS fractions, which varied the amount of protein chelated with Al/Fe in each fraction. This study provides new information about the benefits of replacing conventional inorganic coagulants with natural organic polymers for sewage sludge dewatering, in terms of reduced sludge cake conductivity and greater dry solids content.


Subject(s)
Chitosan , Ferric Compounds , Sewage , Sewage/chemistry , Chitosan/chemistry , Ferric Compounds/chemistry , Quaternary Ammonium Compounds/chemistry , Flocculation , Chlorides/chemistry , Waste Disposal, Fluid/methods , Aluminum/chemistry
9.
Chemosphere ; 356: 141940, 2024 May.
Article in English | MEDLINE | ID: mdl-38588894

ABSTRACT

Dissolved black carbon (DBC) is the ubiquitous component of dissolved organic matter pools with the high reactivity for disinfection byproducts formation. However, it is unknown that the influence of molecular weight (MW) of natural organic matter (NOM) on the DBC removal from potable water sources. Therefore, it was studied that the DBC removal by coagulation in the presence of the NOM with various molecular weights. The DBC removal was promoted due to the presence of NOM and the promotion degree decreased with decreasing MW of NOM. Furthermore, the removal ratio of humic-like component increased as the MW of NOM decreased, suggesting that the competition between DBC and NOM increased with decreasing MW. The functional groups after coagulation were the same with that before coagulation as the MW of NOM varied, suggesting that the molecular structure was not the key factor of influencing the DBC removal. This study will give the deep insight into the prediction of the DBC removal ratio by coagulation based on the MW of NOM in water sources.


Subject(s)
Humic Substances , Molecular Weight , Water Purification , Water Purification/methods , Humic Substances/analysis , Carbon/chemistry , Water Pollutants, Chemical/chemistry , Soot/chemistry , Drinking Water/chemistry , Disinfection , Organic Chemicals/chemistry , Organic Chemicals/isolation & purification
10.
Environ Sci Technol ; 58(13): 5899-5910, 2024 Apr 02.
Article in English | MEDLINE | ID: mdl-38502922

ABSTRACT

The established benefits of ozone on microbial pathogen inactivation, natural organic matter degradation, and inorganic/organic contaminant oxidation have favored its application in drinking water treatment. However, viable bacteria are still present after the ozonation of raw water, bringing a potential risk to membrane filtration systems in terms of biofilm accumulation and fouling. In this study, we shed light on the role of the specific ozone dose (0.5 mg-O3/mg-C) in biofilm accumulation during long-term membrane ultrafiltration. Results demonstrated that ozonation transformed the molecular structure of influent dissolved organic matter (DOM), producing fractions that were highly bioavailable at a specific ozone dose of 0.5, which was inferred to be a turning point. With the increase of the specific ozone dose, the biofilm microbial consortium was substantially shifted, demonstrating a decrease in richness and diversity. Unexpectedly, the opportunistic pathogen Legionella was stimulated and occurred in approximately 40% relative abundance at the higher specific ozone dose of 1. Accordingly, the membrane filtration system with a specific ozone dose of 0.5 presented a lower biofilm thickness, a weaker fluorescence intensity, smaller concentrations of polysaccharides and proteins, and a lower Raman activity, leading to a lower hydraulic resistance, compared to that with a specific ozone dose of 1. Our findings highlight the interaction mechanism between molecular-level DOM composition, biofilm microbial consortium, and membrane filtration performance, which provides an in-depth understanding of the impact of ozonation on biofilm accumulation.


Subject(s)
Ozone , Water Purification , Membranes, Artificial , Ultrafiltration , Biofilms
11.
Water Res ; 254: 121352, 2024 May 01.
Article in English | MEDLINE | ID: mdl-38401286

ABSTRACT

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.


Subject(s)
Sulfates , Water Purification , Flocculation , Anions , Wastewater , Cations , Water Purification/methods
12.
Water Res ; 252: 121193, 2024 Mar 15.
Article in English | MEDLINE | ID: mdl-38290239

ABSTRACT

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.


Subject(s)
Sulfates , Water Purification , Oxidation-Reduction , Autotrophic Processes , Water Purification/methods , Humic Substances/analysis
13.
Environ Sci Technol ; 58(2): 1164-1176, 2024 Jan 16.
Article in English | MEDLINE | ID: mdl-38164759

ABSTRACT

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.


Subject(s)
Dissolved Organic Matter , Soil , Humans , Grassland , Carbon , Water , China
14.
J Environ Manage ; 351: 119719, 2024 Feb.
Article in English | MEDLINE | ID: mdl-38043306

ABSTRACT

Landfill leachate properties contain important information and can be a unique indicator for the chemical and biochemical activities in landfills. In the recent decade, more landfills are experiencing elevated temperature, causing an imbalance in the decomposition of solid waste and affecting the properties of the landfill leachate. This study analyzes the properties of leachate from two landfills that were experiencing elevated temperature (ETLFs), samples were collected from both elevated temperature impacted and non-impacted areas in each landfill. The accumulation of volatile fatty acids (VFA) in leachates from elevated temperature impacted areas of both landfill sites revealed that methanogenesis was inhibited by the elevated temperature, which was further confirmed by the more acidic pH, higher H/C elemental ratio, and lower degree of aromaticity of the elevated temperature impacted leachates. Also, carbohydrates depletion indicated possible enhancement of hydrolysis and acidogenesis by elevated temperature, which was supported by compositional comparison of isolated acidic species by negative-ion electrospray ionization (ESI) Fourier transform ion cyclotron resonance mass spectrometry (FT-ICRMS) at 21 T derived from both elevated temperature impacted and non-impacted areas in the same landfill site. Furthermore, leachate organics fractionation showed that leachates not impacted by elevated temperature contain less hydrophilic fraction and more humic fraction than elevated temperature-impacted leachates for both ETLFs.


Subject(s)
Refuse Disposal , Water Pollutants, Chemical , Refuse Disposal/methods , Water Pollutants, Chemical/chemistry , Temperature , Solid Waste/analysis , Waste Disposal Facilities , Hydrogen/analysis
15.
Water Res ; 247: 120840, 2023 Dec 01.
Article in English | MEDLINE | ID: mdl-37950954

ABSTRACT

The presence of manganese(II) in drinking water sources poses a significant treatment difficulty for water utilities, thus necessitating the development of effective removal strategies. Treatment by Fe(VI), a combined oxidant and coagulant, has been identified as a potential green solution; however, its effectiveness is hampered by natural organic matter (NOM), and this underlying mechanism is not fully understood. Here, we investigated the inhibitory effect of three different types of NOM, representing terrestrial, aquatic, and microbial origins, on Mn(II) removal and floc growth during Fe(VI) coagulation. Results revealed that Fe(VI) coagulation effectively removes Mn(II), but NOM could inhibit its effectiveness by competing in oxidation reactions, forming NOM-Fe complexes, and altering floc aggregation. Humic acid was found to exhibit the strongest inhibition due to its unsaturated heterocyclic species that strongly bond to flocs and react with Fe(VI). For the first time, this study has presented a comprehensive elucidation of the atomic-level structure of Fe(VI) hydrolysis products by employing Extended X-ray Absorption Fine Structure Spectroscopy (EXAFS). Results demonstrated that NOM strengthened single-corner and double-corner coordination between FeO6 octahedrons that were consumed by Mn(II), resulting in an increased contribution of γ-FeOOH in the core-shell structure (γ-FeOOH shell and γ-F2O3 core), thereby inhibiting coagulation effects. Furthermore, NOM impeded the formation of stable manganite, resulting in more low-valence Mn(III) being incorporated in the form of an unstable intermediate. These findings provide a deeper understanding of the complex interplay between Fe coagulants, heavy metal pollution, and NOM in water treatment and offer insight into the limitations of Fe(VI) in practical applications.


Subject(s)
Manganese , Water Purification , Oxidation-Reduction , Manganese/chemistry , Water Purification/methods
16.
ACS Appl Mater Interfaces ; 15(43): 50116-50125, 2023 Nov 01.
Article in English | MEDLINE | ID: mdl-37856676

ABSTRACT

Construction of the desired morphology and nanointerface to expose the active sites and modulate the electronic structure offers an effective approach to boosting urea splitting for energy-saving hydrogen generation. Herein, we fabricate a Ni/WO3 Mott-Schottky heterojunction electrocatalyst with a hedgehog-like structure supported on Ni foam toward alkaline urea splitting. Different Ni/WO3 morphologies, such as microspheres, hedgehog-like structures, octahedrons, and cubes, were obtained when various ratios of Ni/W feeds were used. The Mott-Schottky nanointerfaces between Ni and WO3 domains are visually confirmed by high-resolution transmission electron microscopy images, which also accelerated the charge transfer rate. Benefiting from the high electrochemically active surface area and enhanced charge transferability, the optimal Ni/WO3 electrode exhibits outstanding catalytic activity toward hydrogen generation with a low overpotential of 163 mV at 100 mA cm-2 in alkaline solution and reduced cell voltage of 1.67 V when coupled with urea oxidation reaction. Theoretical calculations reveal that the Ni sites in Ni/WO3 optimize the H adsorption energy (ΔGH*) with the |ΔGH*| value of 0.097 eV, much lower than that of Ni (0.35 eV) and WO3 (0.235 eV). This work demonstrates important guidance in designing an efficient electrocatalyst for urea splitting.

17.
Environ Sci Technol ; 57(33): 12489-12500, 2023 08 22.
Article in English | MEDLINE | ID: mdl-37551789

ABSTRACT

In situ Fe(III) coprecipitation from Fe2+ oxidation is a widespread phenomenon in natural environments and water treatment processes. Studies have shown the superiority of in situ Fe(III) (formed by in situ oxidation of a Fe(II) coagulant) over ex situ Fe(III) (using a Fe(III) coagulant directly) in coagulation, but the reasons remain unclear due to the uncertain nature of amorphous structures. Here, we utilized an in situ Fe(III) coagulation process, oxidizing the Fe(II) coagulant by potassium permanganate (KMnO4), to treat phosphate-containing surface water and analyzed differences between in situ and ex situ Fe(III) coagulation in phosphate removal, dissolved organic matter (DOM) removal, and floc growth. Compared to ex situ Fe(III), flocs formed by the natural oxidizing Fe2+ coagulant exhibited more effective phosphate removal. Furthermore, in situ Fe(III) formed through accelerated oxidation by KMnO4 demonstrated improved flocculation behavior and enhanced removal of specific types of DOM by forming a more stable structure while still maintaining effective phosphate removal. Fe K-edge extended X-ray absorption fine structure spectra (EXAFS) of the flocs explained their differences. A short-range ordered strengite-like structure (corner-linked PO4 tetrahedra to FeO6 octahedra) was the key to more effective phosphorus removal of in situ Fe(III) than ex situ Fe(III) and was well preserved when KMnO4 accelerated in situ Fe(III) formation. Conversely, KMnO4 significantly inhibited the edge and corner coordination between FeO6 octahedra and altered the floc-chain-forming behavior by accelerating hydrolysis, resulting in a more dispersed monomeric structure than ex situ Fe(III). This research provides an explanation for the superiority of in situ Fe(III) in phosphorus removal and highlights the importance of atomic-level structural differences between ex situ and in situ Fe(III) coprecipitates in water treatment.


Subject(s)
Ferric Compounds , Water Purification , Ferric Compounds/chemistry , Dissolved Organic Matter , Phosphates , Oxidation-Reduction , Ferrous Compounds/chemistry , Phosphorus , Water Purification/methods
18.
Environ Sci Technol ; 57(30): 11096-11107, 2023 08 01.
Article in English | MEDLINE | ID: mdl-37467428

ABSTRACT

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.


Subject(s)
Ferric Compounds , Iron Compounds , Periplasm/metabolism , Water , Denitrification , Iron Compounds/chemistry , Iron Compounds/metabolism , Minerals/chemistry , Iron/chemistry , Oxidation-Reduction , Ferrous Compounds/chemistry , Ferrous Compounds/metabolism , Nitrogen/metabolism
19.
Water Res ; 243: 120328, 2023 Sep 01.
Article in English | MEDLINE | ID: mdl-37459797

ABSTRACT

Iron coagulants have been used extensively in drinking water treatment. This typically produces substantial quantities of insoluble iron hydrolysis products which interact with natural and anthropogenic organic substances during the coagulation process. Previous studies have shown that the removal of low molecular weight (MW) organics is relatively poor by coagulation, which leads to their presence during disinfection, with the formation of halogenated byproducts, and in treated water supplies as potentially biodegradable material. Currently, there is little knowledge about the changes that occur in the nature of coagulant flocs as they age with time and how such changes affect interactions with organic matter, especially low MW organics. To improve this deficiency, this study has investigated the variation of aged flocs obtained from two commonly used iron salts and their impact on representative organic contaminants, natural organic matter (NOM) and tetracycline antibiotic (TC), in a real surface water. It was found that aging resulted in increasing crystallization of the flocs, which can play a beneficial role in activating persulfate oxidant to remove the representative organics. Furthermore, acidification was also found to further improve the removal of low MW natural organics and tetracycline. In addition, the results showed that the low MW fractions of NOM (<1 K Dalton) were substantially removed by the aging flocs. These results are in marked contrast to the poor removal of low MW organic substances by conventional coagulation, with or without added oxidants, and show that aged flocs have a high potential of reuse for re-coagulation and activation of oxidants to reduce low MW organics, and enhance drinking water quality.


Subject(s)
Drinking Water , Water Purification , Molecular Weight , Crystallization , Flocculation , Water Purification/methods , Iron , Tetracyclines
20.
J Hazard Mater ; 457: 131736, 2023 Sep 05.
Article in English | MEDLINE | ID: mdl-37295334

ABSTRACT

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.

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