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1.
Environ Sci Technol ; 58(26): 11791-11801, 2024 Jul 02.
Artículo en Inglés | MEDLINE | ID: mdl-38871647

RESUMEN

The effect of aqueous solution chemistry on the ionic hydration structure and its corresponding nanofiltration (NF) selectivity is a research gap concerning ion-selective transport. In this study, the hydration distribution of two typical monovalent anions (Cl- and NO3-) under different aqueous solution chemical conditions and the corresponding transmembrane selectivity during NF were investigated by using in situ liquid time-of-flight secondary ion mass spectrometry in combination with molecular dynamics simulations. We demonstrate the inextricable link between the ion hydration structure and the pore steric effect and further find that ionic transmembrane transport can be regulated by breaking the balance between the hydrogen bond network (i.e., water-water) and ion hydration (i.e., ion-water) interactions of hydrated ion. For strongly hydrated (H2O)nCl- with more intense ion-water interactions, a higher salt concentration and coexisting ion competition led to a larger hydrated size and, thus, a higher ion rejection by the NF membrane, whereas weakly hydrated (H2O)nNO3- takes the reverse under the same conditions. Stronger OH--anion hydration competition resulted in a smaller hydrated size of (H2O)nCl- and (H2O)nNO3-, showing a lower observed average hydration number at pH 10.5. This study deepens the long-overlooked understanding of NF separation mechanisms, concerning the hydration structure.


Asunto(s)
Filtración , Agua/química , Iones , Simulación de Dinámica Molecular , Soluciones , Aniones/química
2.
Environ Sci Technol ; 58(9): 4450-4458, 2024 Mar 05.
Artículo en Inglés | MEDLINE | ID: mdl-38386650

RESUMEN

Calcium salt precipitation is an effective solution to wastewater fluoride pollution. The purity and precipitation efficiency of calcium fluoride is critical for its removal and recovery. This study aimed to reveal the role of coexisting sulfates in the precipitation of calcium fluoride. A low sulfate concentration promoted calcium fluoride precipitation. The size of calcium fluoride-aggregated particle clusters increased from 750 to 2000 nm when the molar ratio of sulfate to fluoride was increased from 0 to 3:100. Sulfate doped in the calcium fluoride crystals neutralized the positive charge of the calcium fluoride. Online atomic force microscopy measurements showed that sulfate reduced the repulsive force between calcium fluoride crystals and increased the adhesion force from 1.62 to 2.46 nN, promoting the agglomeration of calcium fluoride crystals. Sulfate improved the precipitation efficiency of calcium fluoride by promoting agglomeration; however, the purity of calcium fluoride was reduced by doping. Sulfate reduced the induction time of calcium fluoride crystallization and improved the nucleation rate of calcium fluoride. Sulfate should be retained to improve the precipitation of calcium fluoride and to avoid its loss from the effluents. However, it is necessary to separate sulfate from fluoride to obtain high-purity calcium fluoride. Therefore, sulfate concentration regulation in high-fluoride wastewater is key to achieving the efficient removal and recovery of fluoride ions.


Asunto(s)
Fluoruro de Calcio , Fluoruros , Fluoruros/química , Aguas Residuales , Sulfatos/química , Contaminación Ambiental , Calcio
3.
Environ Sci Technol ; 58(6): 2984-2997, 2024 Feb 13.
Artículo en Inglés | MEDLINE | ID: mdl-38306608

RESUMEN

Most aquatic plants applied to ecological restoration have demonstrated a clonal growth pattern. The risk-spreading strategy plays a crucial role in facilitating clonal plant growth under external environmental stresses via clonal integration. However, the effects of different concentrations of nanoplastics (NPs) on the growth traits of clonal aquatic plants are not well understood. Therefore, this study aimed to investigate the impact of NPs exposure on seedlings of parent plants and connected offspring ramets. A dose response experiment (0.1, 1, and 10 mg L-1) showed that the growth of Eichhornia crassipes (water hyacinth) was affected by 100 nm polystyrene nanoplastics after 28 days of exposure. Tracer analysis revealed that NPs are accumulated by parent plants and transferred to offspring ramets through stolon. Quantification analysis showed that when the parent plant was exposed to 10 mg L-1 NPs alone for 28 days, the offspring ramets contained approximately 13 ± 2 µg/g NPs. In the case of connected offspring ramets, leaf and root biomass decreased by 24%-51% and 32%-51%, respectively, when exposed to NP concentrations ranging from 0.1 to 10 mg L-1. Excessive enrichment of NPs had a detrimental effect on the photosynthetic system, decreasing the chlorophyll content and nonphotochemical quenching. An imbalance in the antioxidant defense systems, which were unable to cope with the oxidative stress caused by NP concentrations, further damaged various organs. The root system can take up NPs and then transfer them to the offspring through the stolon. Interference effects of NPs were observed in terms of root activity, metabolism, biofilm composition, and the plant's ability to purify water. However, the risk-spreading strategy employed by parent plants (interconnected offspring ramets) offered some relief from NP-induced stress, as it increased their relative growth rate by 1 to 1.38 times compared to individual plants. These findings provide substantial evidence of the high NP enrichment capacity of E. crassipes for ecological remediation. Nevertheless, we must also remain aware of the environmental risk associated with the spread of NPs within the clonal system of E. crassipes, and contaminated cloned individuals need to be precisely removed in a timely manner to maintain normal functions.


Asunto(s)
Microplásticos , Fotosíntesis , Humanos , Clorofila , Biomasa , Plantas/metabolismo
4.
Environ Sci Technol ; 58(6): 2891-2901, 2024 Feb 13.
Artículo en Inglés | MEDLINE | ID: mdl-38308618

RESUMEN

Direct interspecies electron transfer (DIET) provides an innovative way to achieve efficient methanogenesis, and this study proposes a new approach to upregulate the DIET pathway by enhancing quorum sensing (QS). Based on long-term reactor performance, QS enhancement achieved more vigorous methanogenesis with 98.7% COD removal efficiency. In the control system, methanogenesis failure occurred at the accumulated acetate of 7420 mg of COD/L and lowered pH of 6.04, and a much lower COD removal of 41.9% was observed. The more significant DIET in QS-enhancing system was supported by higher expression of conductive pili and the c-Cyts cytochrome secretion-related genes, resulting in 12.7- and 10.3-fold improvements. Moreover, QS enhancement also improved the energy production capability, with the increase of F-type and V/A-type ATPase expression by 6.3- and 4.2-fold, and this effect probably provided more energy for nanowires and c-Cyts cytochrome secretion. From the perspective of community structure, QS enhancement increased the abundance of Methanosaeta and Geobacter from 54.3 and 17.6% in the control to 63.0 and 33.8%, respectively. Furthermore, the expression of genes involved in carbon dioxide reduction and alcohol dehydrogenation increased by 0.6- and 7.1-fold, respectively. Taken together, this study indicates the positive effects of QS chemicals to stimulate DIET and advances the understanding of the DIET methanogenesis involved in environments such as anaerobic digesters and sediments.


Asunto(s)
Electrones , Percepción de Quorum , Anaerobiosis , Transporte de Electrón , Citocromos/metabolismo , Metano , Reactores Biológicos
5.
J Am Chem Soc ; 145(3): 1759-1768, 2023 Jan 25.
Artículo en Inglés | MEDLINE | ID: mdl-36607337

RESUMEN

Integrating different reaction sites offers new prospects to address the difficulties in single-atom catalysis, but the precise regulation of active sites at the atomic level remains challenging. Here, we demonstrate a sodium-directed photon-induced assembly (SPA) strategy for boosting the atomic utilization efficiency of single-atom catalysts (SACs) by constructing multifarious Au sites on TiO2 substrate. Na+ was employed as the crucial cement to direct Au single atoms onto TiO2, while the light-induced electron transfer from excited TiO2 to Au(Na+) ensembles contributed to the self-assembly formation of Au nanoclusters. The synergism between plasmonic near-field and Schottky junction enabled the cascade electron transfer for charge separation, which was further enhanced by oxygen vacancies in TiO2. Our dual-site photocatalysts exhibited a nearly 2 orders of magnitude improvement in the hydrogen evolution activity under simulated solar light, with a striking turnover frequency (TOF) value of 1533 h-1 that exceeded other Au/TiO2-based photocatalysts reported. Our SPA strategy can be easily extended to prepare a wide range of metal-coupled nanostructures with enhanced performance for diverse catalytic reactions. Thus, this study provides a well-defined platform to extend the boundaries of SACs for multisite catalysis through harnessing metal-support interactions.

6.
Appl Environ Microbiol ; 89(12): e0166223, 2023 12 21.
Artículo en Inglés | MEDLINE | ID: mdl-38047646

RESUMEN

IMPORTANCE: Antibiotics can induce dose-dependent hormetic effects on bacterial cell proliferation, i.e., low-dose stimulation and high-dose inhibition. However, the underlying molecular basis has yet to be clarified. Here, we showed that sulfonamides play dual roles as a weapon and signal against Comamonas testosteroni that can modulate cell physiology and phenotype. Subsequently, through investigating the hormesis mechanism, we proposed a comprehensive regulatory pathway for the hormetic effects of Comamonas testosteroni low-level sulfonamides and determined the generality of the observed regulatory model in the Comamonadaceae family. Considering the prevalence of Comamonadaceae in human guts and environmental ecosystems, we provide critical insights into the health and ecological effects of antibiotics.


Asunto(s)
Hormesis , Sulfonamidas , Humanos , Sulfonamidas/farmacología , Ecosistema , Percepción de Quorum , Sulfanilamida/farmacología , Antibacterianos/farmacología
7.
Environ Sci Technol ; 57(32): 12083-12093, 2023 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-37530558

RESUMEN

Demulsification using membranes is a promising method to coalesce highly stable emulsified oil droplets for oil recovery. Nevertheless, a structure of the current filtration medium that is not efficient for oil droplet coalescence impedes rapid permeability, thereby inevitably restricting their practical applications. Herein, we report a hydrophobic-hydrophilic-hydrophobic (3H) demulsification medium that exhibits a benchmark permeability of ∼2.1 × 104 L m-2 h-1 with a demulsification efficiency of >98.0%. Remarkably, this 3H demulsification medium maintains over 90% demulsification efficiency in the oil-in-water (O/W) emulsions with a wide range of surfactant concentrations, which shows excellent applicability. Based on the combined results of quasi situ microscope images and molecular dynamics simulations, we show that the polydimethylsiloxane-modified hydrophobic layer facilitates the capture and coalescence of oil droplets, the hydrophilic inner layer assists in squeezing the coalescence of enlarged droplets, and the third hydrophobic layer accelerates the discharge of demulsified oil to sustain permeability. The sequential demulsification mechanism between this 3H filtration layer provides a general guide for designing a demulsifying membrane with high demulsification efficiency and high flux toward oil recovery.

8.
Environ Sci Technol ; 57(32): 12117-12126, 2023 08 15.
Artículo en Inglés | MEDLINE | ID: mdl-37525979

RESUMEN

Regulation of the free radical types is crucial but challenging in the ubiquitous heterogeneous catalytic oxidation for chemosynthesis, biotherapy, and environmental remediation. Here, using aromatic pollutant (AP) removal as a prototype, we identify the massive accumulation of the benzoquinone (BQ) intermediate in the hydroxyl radical (•OH)-mediated AP degradation process. Theoretical prediction and experiments demonstrate that BQ is both a Lewis acid and base because of its unique molecular and electronic structure caused by the existence of symmetrical carbonyl groups; therefore, it is hard to be electrophilically added by oxidizing •OH as a result of the high reaction energy barrier (ΔG = 1.74 eV). Fortunately, the introduction of the superoxide anion (•O2-) significantly lowers the conversion barrier (ΔG = 0.91 eV) of BQ because •O2- can act as the electron donor and acceptor simultaneously, electrophilically and nucleophilically add to BQ synchronously, and break it down. Subsequently, the breakdown products can then be further oxidized by •OH until completely mineralized. Such synergistic oxidation based on •OH and •O2- timely eliminates BQ, potentiates AP mineralization, and inhibits electrode fouling caused by high-resistance polymeric BQ; more importantly, it effectively reduces toxicity, saves energy and costs, and decreases the environmental footprint, evidenced by the life cycle assessment.


Asunto(s)
Radical Hidroxilo , Superóxidos , Oxidación-Reducción , Benzoquinonas/química , Benzoquinonas/metabolismo
9.
Environ Sci Technol ; 57(2): 1134-1143, 2023 01 17.
Artículo en Inglés | MEDLINE | ID: mdl-36602374

RESUMEN

In situ synthesis of reactive oxygen species (ROS) on demand via oxygen activation (OA) is significant in biological, chemical, and environmental fields. Thus, the design of OA catalysts with adequate reactivity, durability, and selectivity is critical but challenging. Here, we report a CuxO@C core@shell photoelectrode prepared by encapsulating Cu/Cu2O/CuO into a carbon layer through anodic electropolymerization (electrophoresis-coupled self-assembly of carbon quantum dots). Theoretical prediction and experiments indicate that the carbon layer can effectively facilitate optical trapping and charge transfer, thus promoting photoelectric conversion and anti-photocorrosion performance of CuxO@C. The inner CuxO core acts as an electron reservoir and continuously injects electrons into the outer carbon layer shell, and the carbon atoms adjacent to oxygen-enriched functional groups (C-O-C and -COOH) in the electron-rich carbon layer work as the reactive sites to adsorb O2 and donate electrons to the antibonding orbital [lowest unoccupied molecular orbital (π*)] of dioxygen. Optimized adsorption and hydrogenation of the critical intermediates (*O2, *OOH, and *H2O2) and thermodynamically tunable O-O bond cleavage enable O2 being selectively reduced to the superoxide anion and hydroxyl radical via the mixed multielectron processes consisting of one- and three-electron pathways. Sulfamethoxazole, an emerging refractory organic contaminant widely present in the environment, can be effectively degraded (∼100% removal) in such an electrochemical platform, benefiting from the abundant ROS generated in situ. Our findings demonstrate an innovative strategy to develop highly efficient and selective OA catalysts for practical water purification.


Asunto(s)
Oxígeno , Purificación del Agua , Especies Reactivas de Oxígeno/química , Peróxido de Hidrógeno/química , Carbono
10.
Environ Sci Technol ; 57(6): 2566-2574, 2023 02 14.
Artículo en Inglés | MEDLINE | ID: mdl-36719078

RESUMEN

The desalination performance of flow electrode capacitive deionization (FCDI) is determined by the ion adsorption on the powdered activated carbon (PAC) and the electron transfer between the current collector and PAC. However, a comprehensive understanding of rate-limiting steps is lacking, let alone to enhance FCDI desalination by regulating the PAC characteristics. This study showed that the electron transfer between PAC and the current collector on the anode side was the rate-limiting step of FCDI desalination. Compared with W900, the desalination performance of FCDI decreased by 95% when W1200 with weak electron transfer ability was used as a flow electrode. The PAC selected in this study transferred electrons directly through the conductive carbon matrix in FCDI and was mainly affected by graphitization. The desalination performance of FCDI was improved by 20 times when the graphitization degree of PAC increased from 0.69 to 1.03. The minimum energy required for electrons to escape from the PAC surface was reduced by the high degree of graphitization, from 4.27 to 3.52 eV, thus improving the electron transfer capacity of PAC on the anode side. This study provides a direction for the optimization of flow electrodes and further promotes the development of FCDI.


Asunto(s)
Cloruro de Sodio , Purificación del Agua , Carbón Orgánico , Electrones , Electrodos
11.
Environ Sci Technol ; 57(36): 13658-13668, 2023 09 12.
Artículo en Inglés | MEDLINE | ID: mdl-37647171

RESUMEN

Ionic contaminants such as Cr(VI) pose a challenge for water purification using membrane-based processes. However, existing membranes have low permeability and selectivity for Cr(VI). Therefore, in this study, we prepared an electrically controlled adsorptive membrane (ECAM-L) by coating a loose Cl--doped polypyrrole layer on a carbon nanotube substrate, and we evaluated the performance of ECAM-L for Cr(VI) separation from water. We also used electrochemical quartz crystal microbalance measurements and molecular dynamics and density functional theory calculations to investigate the separation mechanisms. The adsorption and desorption of Cr(VI) could be modulated by varying the electrostatic interactions between ECAM-L and Cr(VI) via potential control, enabling the cyclic use of the ECAM-L without additional additives. Consequently, the oxidized ECAM-L showed high Cr(VI) removal performance (<50 µg/L) and treatment capacity (>3500 L/m2) at a high water flux (283 L/m2/h), as well as reusability after the application of a potential. Our study demonstrates an efficient membrane design for water decontamination that can selectively separate Cr(VI) through a short electric stimulus.


Asunto(s)
Polímeros , Pirroles , Adsorción , Agua
12.
Environ Sci Technol ; 2023 Jan 10.
Artículo en Inglés | MEDLINE | ID: mdl-36630187

RESUMEN

Antibacterial modification is a chemical-free method to mitigate biofouling, but surface accumulation of bacteria shields antibacterial groups and presents a significant challenge in persistently preventing membrane biofouling. Herein, a great synergistic effect of electrorepulsion and quaternary ammonium (QA) inactivation on maintaining antibacterial activity against biofouling has been investigated using an electrically conductive QA membrane (eQAM), which was fabricated by polymerization of pyrrole with QA compounds. The electrokinetic force between negatively charged Escherichia coli and cathodic eQAM prevented E. coli cells from reaching the membrane surface. More importantly, cathodic eQAM accelerated the detachment of cells from the eQAM surface, particularly for dead cells whose adhesion capacity was impaired by inactivation. The number of dead cells on the eQAM surface was declined by 81.2% while the number of live cells only decreased by 49.9%. Characterization of bacteria accumulation onto the membrane surface using an electrochemical quartz crystal microbalance revealed that the electrorepulsion accounted for the cell detachment rather than inactivation. In addition, QA inactivation mainly contributed to minimizing the cell adhesion capacity. Consequently, the membrane fouling was significantly declined, and the final normalized water flux was promoted higher than 20% with the synergistic effect of electrorepulsion and QA inactivation. This work provides a unique long-lasting strategy to mitigate membrane biofouling.

13.
Environ Sci Technol ; 57(45): 17640-17648, 2023 11 14.
Artículo en Inglés | MEDLINE | ID: mdl-37906121

RESUMEN

Membrane technology provides an attractive approach for water purification but faces significant challenges in separating small molecules due to its lack of satisfactory permselectivity. In this study, a polypyrrole-based active membrane with a switchable multi-affinity that simultaneously separates small ionic and organic contaminants from water was created. Unlike conventional passive membranes, the designed membrane exhibits a good single-pass filtration efficiency (>99%, taking 1-naphthylamine and Pb2+ as examples) and high permeability (227 L/m2/h). Applying a reversible potential can release the captured substances from the membrane, thus enabling membrane regeneration and self-cleaning without the need for additives. Advanced characterizations reveal that potential switching alters the orientation of the doped amphipathic molecules with the self-alignment of the hydrophobic alkyl chains or the disordered sulfonate anions to capture the target organic molecules or ions via hydrophobic or electrostatic interactions, respectively. The designed smart membrane holds great promise for controllable molecular separation and water purification.


Asunto(s)
Polímeros , Purificación del Agua , Polímeros/química , Pirroles , Filtración , Electricidad , Iones
14.
Environ Sci Technol ; 57(43): 16695-16706, 2023 10 31.
Artículo en Inglés | MEDLINE | ID: mdl-37844151

RESUMEN

Electrocatalytic hydrogenation is acknowledged as a promising strategy for chlorophenol dechlorination. However, the widely used Pd catalysts exhibit drawbacks, such as high costs and low selectivity for phenol hydrosaturation. Herein, we demonstrate the potential and mechanism of Ru in serving as a Pd substitute using 2,4,6-trichlorophenol (TCP) as a model pollutant. Up to 99.8% TCP removal efficiency and 99% selectivity to cyclohexanol, a value-added compound with an extremely low toxicity, were achieved on the Ru electrode. In contrast, only 66% of TCP was removed on the Pd electrode, with almost no hydrosaturation selectivity. The superiority of Ru over Pd was especially noteworthy in alkaline conditions or the presence of interfering species such as S2-. The theoretical simulation demonstrates that Ru possesses a hydrodechlorination energy barrier of 0.72 eV, which is comparable to that on Pd. Meanwhile, hydrosaturation requires an activation energy of 0.69 eV on Ru, which is much lower than that on Pd (0.92 eV). The main reaction mechanism on Ru is direct electron transfer, which is distinct from that on Pd (indirect pathway via atomic hydrogen, H*). This work thereby provides new insights into designing cost-effective electrocatalysts for halogenated phenol detoxification and resource recovery.


Asunto(s)
Clorofenoles , Hidrogenación , Electrones , Fenol , Transporte de Electrón
15.
Environ Sci Technol ; 57(12): 5003-5012, 2023 03 28.
Artículo en Inglés | MEDLINE | ID: mdl-36931868

RESUMEN

The adsorption of contaminants by porous carbon has been extensively studied by conventional isotherm and kinetic methods. However, the co-adsorption behavior and sorption sites of multiple contaminants in different-sized pores remain unclear. Herein, the nuclear magnetic resonance (NMR) approach is performed to investigate the adsorption mechanism of toluene and cetane in the confined space of carbon at the molecular level. The ring current effect induces the variation in the NMR chemical shifts of in-pore adsorbed toluene and cetane, realizing the identification of pore-dependent adsorption sites for contaminant removal. Cetane has a slower adsorption kinetic but a higher binding energy than toluene, which could squeeze toluene from micropores to larger pores with increasing adsorption quantity. This leads to a stronger competitive adsorption effect in small micropores than in mesopores. Accordingly, hierarchical porous carbons are determined to be the most effective adsorbents for the adsorption of coexisting contaminants. This study not only provides an effective NMR method to reveal the adsorption mechanism in the confined space of porous carbon at the molecular level but also offers new insights into the pore size-dependent adsorption of activated carbon for petroleum contaminant treatment.


Asunto(s)
Carbón Orgánico , Tolueno , Tolueno/química , Porosidad , Espectroscopía de Resonancia Magnética , Adsorción , Ácido Ascórbico
16.
Environ Sci Technol ; 57(21): 7913-7923, 2023 05 30.
Artículo en Inglés | MEDLINE | ID: mdl-37188658

RESUMEN

Antiviral transformation products (TPs) generated during wastewater treatment are an environmental concern, as their discharge, in considerable amounts, into natural waters during a pandemic can pose possible risks to the aquatic environment. Identification of the hazardous TPs generated from antivirals during wastewater treatment is important. Herein, chloroquine phosphate (CQP), which was widely used during the coronavirus disease-19 (COVID-19) pandemic, was selected for research. We investigated the TPs generated from CQP during water chlorination. Zebrafish (Danio rerio) embryos were used to assess the developmental toxicity of CQP after water chlorination, and hazardous TPs were estimated using effect-directed analysis (EDA). Principal component analysis revealed that the developmental toxicity induced by chlorinated samples could be relevant to the formation of some halogenated TPs. Fractionation of the hazardous chlorinated sample, along with the bioassay and chemical analysis, identified halogenated TP387 as the main hazardous TP contributing to the developmental toxicity induced by chlorinated samples. TP387 could also be formed in real wastewater during chlorination in environmentally relevant conditions. This study provides a scientific basis for the further assessment of environmental risks of CQP after water chlorination and describes a method for identifying unknown hazardous TPs generated from pharmaceuticals during wastewater treatment.


Asunto(s)
COVID-19 , Contaminantes Químicos del Agua , Animales , Desinfección/métodos , Cloro/análisis , Pez Cebra , Contaminantes Químicos del Agua/toxicidad , Contaminantes Químicos del Agua/análisis , Tratamiento Farmacológico de COVID-19 , Agua
17.
J Environ Sci (China) ; 126: 734-741, 2023 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-36503798

RESUMEN

Bioaugmented sand filtration has attracted considerable attention because it can effectively remove contaminants in drinking water without additional chemical reagent addition. In this study, a synthesized chemical manganese dioxide (MnO2)-coated quartz sand (MnQS) and biogenic manganese oxide (BioMnOx) composite system was proposed to simultaneously remove typical pharmaceutical contaminants and Mn2+. We demonstrated a manganese-oxidizing bacterium, Pseudomonas sp. QJX-1, could oxidize Mn2+ to generate BioMnOx using humic acids (HA) as sole carbon source. The coaction of MnQS, QJX-1, and the generated BioMnOx in simultaneously removing caffeine and Mn2+ in the presence of HA was evaluated. We found a synergistic effect between them. MnQS and BioMnOx together significantly increased the caffeine removal efficiency from 32.8% (MnQS alone) and 21.5% (BioMnOx alone) to 61.2%. Meanwhile, Mn2+ leaked from MnQS was rapidly oxidized by QJX-1 to regenerate reactive BioMnOx, which was beneficial for continuous contaminant removal and system stability. Different degradation intermediates of caffeine oxidized by MnQS and BioMnOx were detected by LC-QTOF-MS analysis, which implied that caffeine was oxidized by a different pathway. Overall, this work promotes the potential application of bioaugmented sand filtration in pharmaceutical removal in the presence of natural organic matter in drinking water.


Asunto(s)
Agua Potable , Compuestos de Manganeso , Manganeso , Sustancias Húmicas , Carbono , Bacterias , Arena , Preparaciones Farmacéuticas
18.
Environ Microbiol ; 24(2): 894-904, 2022 02.
Artículo en Inglés | MEDLINE | ID: mdl-35072982

RESUMEN

Superoxide and other reactive oxygen species (ROS) shape microbial communities and drive the transformation of metals and inorganic/organic matter. Taxonomically diverse bacteria and phytoplankton produce extracellular superoxide during laboratory cultivation. Understanding the physiological reasons for extracellular superoxide production by aerobes in the environment is a crucial question yet not fully solved. Here, we showed that iron-starving Arthrobacter sp. QXT-31 (A. QXT-31) secreted a type of siderophore [deferoxamine (DFO)], which provoked extracellular superoxide production by A. QXT-31 during carbon sources-level fluctuation. Several other siderophores also demonstrated similar effects to A. QXT-31. RNA-Seq data hinted that DFO stripped iron from iron-bearing proteins in electron transfer chain (ETC) of metabolically active A. QXT-31, resulting in electron leakage from the electron-rich (resulting from carbon sources metabolism by A. QXT-31) ETC and superoxide production. Considering that most aerobes secrete siderophore(s) and undergo carbon sources-level fluctuation, the superoxide-generation pathway is likely a common pathway by which aerobes produce extracellular superoxide in the environment, thus influencing the microbial community and cycling of elements. Our results pointed that the ubiquitous siderophore might be the potential driving force for the microbial generation of superoxide and other ROS and revealed the important role of iron physiology in microbial ROS generation.


Asunto(s)
Arthrobacter , Sideróforos , Arthrobacter/genética , Arthrobacter/metabolismo , Carbono/metabolismo , Hierro/metabolismo , Sideróforos/metabolismo , Superóxidos/metabolismo
19.
Environ Sci Technol ; 56(13): 9417-9427, 2022 07 05.
Artículo en Inglés | MEDLINE | ID: mdl-35737437

RESUMEN

Long-term exposure to excessive iodine via drinking water presents health risks. Moderate oxidation of iodide (I-) to iodine (I2) has a better iodine removal effect than excessive oxidation to iodate (IO3-). This study combines computational and experimental methods to construct a heterogeneous interface with synchronous I- moderate oxidation and I2 adsorption to increase the total iodine removal. Compared to other forms of crystal manganese dioxide (MnO2), theoretical calculations predict that MnO2 with a γ-crystal structure has the lowest adsorption energy, that is, -1.20 eV, and a slight overlap between the conduction and valence bands, which favors electron transfer between I- and Mn(IV) and I2 adsorption. Thus, γ-type MnO2 was designed by adjusting the precursor Mn sources and hydrothermal reaction conditions. The liquid chromatography-inductively coupled plasma-mass spectrometry and high-performance liquid chromatography confirmed that the total iodine concentration in water decreased from 173.7 to 36.3 µg/L after 2 h, with 200 mg/L γ-MnO2 dosage lower than the national standard of 0.1 mg/L. A minute proportion of I- in water was converted to IO3- (approximately 1.1 µg/L). The current I- adsorbent performed better than previously reported ones. During iodine removal, most of the I- migrated from water to the surface of γ-MnO2, and the ratio of I- to I2 was determined to be 1:0.6 by X-ray photoelectron spectroscopy. This study evaluates iodine species transformation and an optimum strategy for heterogeneous interface design; it is promising for treating high-iodine groundwater.


Asunto(s)
Yodo , Compuestos de Manganeso , Adsorción , Yoduros/química , Yodo/química , Oxidación-Reducción , Óxidos/química , Agua/química
20.
Environ Sci Technol ; 56(13): 9722-9731, 2022 Jul 05.
Artículo en Inglés | MEDLINE | ID: mdl-35737582

RESUMEN

Active chlorine species-mediated electrocatalytic oxidation is a promising strategy for ammonia removal in decentralized wastewater treatment. Flow-through electrodes (FTEs) provide an ideal platform for this strategy because of enhanced mass transport and sufficient electrochemically accessible sites. However, limited insight into spatial distribution of electrochemically accessible sites within FTEs inhibits the improvement of reactor efficiency and the reduction of FTE costs. Herein, a microfluidic-based electrochemical system is developed for the operando observation of microspatial reactions within pore channels, which reveals that reactions occur only in the surface layer of the electrode thickness. To further quantify the spatial distribution, finite element simulations demonstrate that over 75.0% of the current is accumulated in the 20.0% thickness of the electrode surface. Based on these findings, a gradient-coated method for the active layer was proposed and applied to a Ti/RuO2 porous electrode with an optimized pore diameter of ∼25 µm, whose electrochemically accessible surface area was 381.7 times that of the planar electrode while alleviating bubble entrapment. The optimized reactor enables complete ammonia removal with an energy consumption of 60.4 kWh kg-1 N, which was 24.2% and 39.9% less than those with pore diameters of ∼3 µm and ∼90 µm, respectively.

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