RESUMEN
The assimilation of antibiotic resistance genes (ARGs) by pathogenic bacteria poses a severe threat to public health. Here, we reported a dual-reaction-site-modified CoSA/Ti3C2Tx (single cobalt atoms immobilized on Ti3C2Tx MXene) for effectively deactivating extracellular ARGs via peroxymonosulfate (PMS) activation. The enhanced removal of ARGs was attributed to the synergistic effect of adsorption (Ti sites) and degradation (Co-O3 sites). The Ti sites on CoSA/Ti3C2Tx nanosheets bound with PO43- on the phosphate skeletons of ARGs via Ti-O-P coordination interactions, achieving excellent adsorption capacity (10.21 × 1010 copies mg-1) for tetA, and the Co-O3 sites activated PMS into surface-bond hydroxyl radicals (â¢OHsurface), which can quickly attack the backbones and bases of the adsorbed ARGs, resulting in the efficient in situ degradation of ARGs into inactive small molecular organics and NO3. This dual-reaction-site Fenton-like system exhibited ultrahigh extracellular ARG degradation rate (k > 0.9 min-1) and showed the potential for practical wastewater treatment in a membrane filtration process, which provided insights for extracellular ARG removal via catalysts design.
Asunto(s)
Antibacterianos , Genes Bacterianos , Antibacterianos/farmacología , Cobalto , Titanio/farmacología , Adsorción , Aguas Residuales , Farmacorresistencia Microbiana/genéticaRESUMEN
Investigating the fate of persistent organic pollutants in water distribution systems (WDSs) is of great significance for preventing human health risks. The role of iron corrosion scales in the migration and transformation of organics in such systems remains unclear. Herein, we determined that hydroxyl (â¢OH), chlorine, and chlorine oxide radicals are generated by Fenton-like reactions due to the coexistence of oxygen vacancy-related Fe(II) on goethite (a major constituent of iron corrosion scales) and hypochlorous acid (HClO, the main reactive chlorine species of residual chlorine at pH â¼ 7.0). â¢OH contributed mostly to the decomposition of atrazine (ATZ, model compound) more than other radicals, producing a series of relatively low-toxicity small molecular intermediates. A simplified kinetic model consisting of mass transfer of ATZ and HClO, â¢OH generation, and ATZ oxidation by â¢OH on the goethite surface was developed to simulate iron corrosion scale-triggered residual chlorine oxidation of organic compounds in a WDS. The model was validated by comparing the fitting results to the experimental data. Moreover, the model was comprehensively applicable to cases in which various inorganic ions (Ca2+, Na+, HCO3-, and SO42-) and natural organic matter were present. With further optimization, the model may be employed to predict the migration and accumulation of persistent organic pollutants under real environmental conditions in the WDSs.
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Contaminantes Químicos del Agua , Cinética , Radicales Libres/química , Contaminantes Químicos del Agua/química , Oxidación-Reducción , Hierro/química , Compuestos de Hierro/química , Minerales/químicaRESUMEN
Clay minerals are ubiquitous in subsurface environments and have long been recognized as having a limited or negligible impact on the fate of arsenic (As) due to their negatively charged surfaces. Here, we demonstrate the significant role of kaolinite (Kln), a pervasive clay mineral, in enhancing As(V) immobilization during ferrous iron (Fe(II)) oxidation at near-neutral pH. Our results showed that Fe(II) oxidation alone was not capable of immobilizing As(V) at relatively low Fe/As molar ratios (≤2) due to the generation of Fe(III)-As(V) nanocolloids that could still migrate easily as truly dissolved As did. In the presence of kaolinite, dissolved As(V) was significantly immobilized on the kaolinite surfaces via forming Kln-Fe(III)-As(V) ternary precipitates, which had large sizes (at micrometer levels) to reduce the As mobility. The kaolinite-induced heterogeneous pathways for As(V) immobilization involved Fe(II) adsorption, heterogeneous oxidation of adsorbed Fe(II), and finally heterogeneous nucleation/precipitation of Fe(III)-As(V) phases on the edge surfaces of kaolinite. The surface precipitates were mixtures of amorphous basic Fe(III)-arsenate and As-rich hydrous ferric oxide. Our findings provide new insights into the role of clay minerals in As transformation, which is significant for the fate of As in natural and engineered systems.
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Arseniatos , Caolín , Oxidación-Reducción , Caolín/química , Arseniatos/química , Hierro/química , Compuestos Ferrosos/química , AdsorciónRESUMEN
In this study, Ru(III) ions were utilized to activate periodate (PI) for oxidation of trace organic pollutants (TOPs, e.g., carbamazepine (CBZ)). The Ru(III)/PI system can significantly promote the oxidation of CBZ in a wide initial pH range (3.0-11.0) at 1 µM Ru(III), showing much higher performance than transition metal ions (i.e., Fe(II), Co(II), Zn(II), Fe(III), Cu(II), Ni(II), Mn(II), and Ce(III)) and noble metal ion (i.e., Ag(I), Pd(II), Pt(II), and Ir(III)) activated PI systems. Probe experiments, UV-vis spectra, and X-ray absorption near-edge structure (XANES) spectra confirmed high-valent Ru-oxo species (Ru(V)=O) as the dominant oxidant in the process. Because of the dominant role of Ru(V)=O, the Ru(III)/PI process exhibited a remarkable selectivity and strong anti-interference in the oxidation of TOPs in complex water matrices. The Ru(V)=O species can undertake 1-e- and 2-e- transfer reactions via the catalytic cycles of Ru(V)=O â Ru(IV) â Ru(III) and Ru(V)=O â Ru(III), respectively. The utilization efficiency of PI in the Ru(III)/PI process for the oxidation of TOPs can approach 100% under optimal conditions. PI stoichiometrically transformed into IO3- without production of undesired iodine species (e.g., HOI and I2). This study developed an efficient and environmentally benign advanced oxidation process for rapid removal of TOPs and enriched understandings on reactivity of Ru(V)=O and Ru catalytic cycles.
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Contaminantes Ambientales , Compuestos Férricos , Metales , Oxidación-Reducción , Agua/químicaRESUMEN
Pyrolysis of oily sludge (OS) is a feasible technology to match the principle of reduction and recycling; however, it is difficult to confirm the feasible environmental destination and meet the corresponding requirements. Therefore, an integrated strategy of biochar-assisted catalytic pyrolysis (BCP) of OS and residue utilization for soil reclamation is investigated in this study. During the catalytic pyrolysis process, biochar as a catalyst intensifies the removal of recalcitrant petroleum hydrocarbons at the expense of liquid product yield. Concurrently, biochar as an adsorbent can inhibit the release of micromolecular gaseous pollutants (e.g. HCN, H2S, and HCl) and stabilize heavy metals. Due to the assistance of biochar, pyrolysis reactions of OS are more likely to occur and require a lower temperature to achieve the same situation. During the soil reclamation process, the obtained residue as a soil amendment can not only provide a carbon source and mineral nutrients but can also improve the abundance and diversity of microbial communities. Thus, it facilitates the plant germination and the secondary removal of petroleum hydrocarbons. The integrated strategy of BCP of OS and residue utilization for soil reclamation is a promising management strategy, which is expected to realize the coordinated and benign disposal of more than one waste.
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Petróleo , Suelo , Suelo/química , Aguas del Alcantarillado/química , Pirólisis , Carbón Orgánico , Aceites , HidrocarburosRESUMEN
Liquid-liquid extraction (LLE) using ionic liquids (ILs)-based methods to remove perfluoroalkyl chemicals (PFACs), such as perfluorooctanoic acid (PFOA) and perfluorooctane sulfonic acid (PFOS), from wastewater, is an important strategy. However, the lack of physicochemical and LLE data limits the selection of the most suitable ILs for the extraction of PFACs. In this work, 1763 ILs for PFACs extraction from water were systematically screened using COSMOtherm to estimate the infinite dilution activity coefficient (lnγ∞)of PFOA and PFOS in water and ILs. To evaluate the accuracy of COSMOtherm, 8 ILs with various lnγ∞ values were selected, and their extraction efficiency (E) and distribution coefficient (Dexp) were measured experimentally. The results showed that the predicted lnγ∞ decreased as the increase of experimental extraction efficiency of PFOA or PFOS, while the tendency of predicted distribution coefficient (Dpre) was consistent with the experimental (Dexp) results. This work provides an efficient basis for selecting ILs for the extraction of PFACs from wastewater.
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Ácidos Alcanesulfónicos , Fluorocarburos , Líquidos Iónicos , Aguas Residuales , Caprilatos , AguaRESUMEN
Vacuum ultraviolet (VUV) photolysis is recognized as an environmental-friendly treatment process. Nitrate (NO3-) and natural organic matter (NOM) are widely present in water source. We investigated trichloronitromethane (TCNM) formation during chlorination after VUV photolysis, because TCNM is an unregulated highly toxic disinfection byproduct. In this study: (1) we found reactive nitrogen species that is generated under VUV photolysis of NO3- react with organic matter to form nitrogen-containing compounds and subsequently form TCNM during chlorination; (2) we found the mere presence of 0.1 mmol/L NO3- can result in the formation of up to 63.96 µg/L TCNM; (3) we found the changes in pH (6.0-8.0), chloride (1-4 mmol/L), and bicarbonate (1-4 mmol/L) cannot effectively diminish TCNM formation; and, (4) we established the quantitative structure-activity relationship (QSAR) model, which indicated a linear relationship between TCNM formation and the Hammett constant (σ) of model compounds; and, (5) we characterized TCNM precursors in water matrix after VUV photolysis and found 1161 much more nitrogen-containing compounds with higher aromaticity were generated. Overall, this study indicates more attention should be paid to reducing the formation risk of TCNM when applying VUV photolysis process at scale.
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Contaminantes Químicos del Agua , Purificación del Agua , Relación Estructura-Actividad Cuantitativa , Vacio , Contaminantes Químicos del Agua/análisis , Halogenación , Desinfección , Compuestos de Nitrógeno , Agua/química , Nitrógeno/química , Rayos UltravioletaRESUMEN
Electrochemical advanced oxidation processes (EAOPs) are promising technologies for perfluorooctanoic acid (PFOA) degradation, but the mechanisms and preferred pathways for PFOA mineralization remain unknown. Herein, we proposed a plausible primary pathway for electrochemical PFOA mineralization using density functional theory (DFT) simulations and experiments. We neglected the unique effects of the anode surface and treated anodes as electron sinks only to acquire a general pathway. This was the essential first step toward fully revealing the primary pathway applicable to all anodes. Systematically exploring the roles of valence band holes (h+), hydroxyl radicals (HOâ¢), and H2O, we found that h+, whose contribution was previously underestimated, dominated PFOA mineralization. Notably, the primary pathway did not generate short-chain perfluoroalkyl carboxylic acids (PFCAs), which were previously thought to be the main degradation intermediates, but generated other polyfluorinated alkyl substances (PFASs) that were rapidly degraded upon formation. Also, we developed a simplified kinetic model, which considered all of the main processes (mass transfer with electromigration included, surface adsorption/desorption, and oxidation on the anode surface), to simulate PFOA degradation in EAOPs. Our model can predict PFOA concentration profiles under various current densities, initial PFOA concentrations, and flow velocities.
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Fluorocarburos , Contaminantes Químicos del Agua , Caprilatos/química , Ácidos Carboxílicos , Electrodos , Fluorocarburos/análisis , Oxidación-Reducción , Contaminantes Químicos del Agua/química , Técnicas ElectroquímicasRESUMEN
Point-of-use (POU) devices with satisfying mercury (Hg) removal performance are urgently needed for public health and yet are scarcely reported. In this study, a thiol-laced metal-organic framework (MOF)-based sponge monolith (TLMSM) has been investigated for Hg(II) removal as the POU device for its benchmark application. The resulting TLMSM was characterized by remarkable chemical resistance, mechanical stability, and hydroscopicity (>2100 wt %). Importantly, the TLMSM has exhibited high adsorption capacity (â¼954.7 mg g-1), fast kinetics (kf â¼ 1.76 × 10-5 ms-1), broad working pH range (1-10), high selectivity (Kd > 5.0 × 107 mL g-1), and excellent regeneration capability (removal efficiency >90% after 25 cycles). The high applicability of TLMSM in real-world scenarios was verified by its excellent Hg(II) removal performance in various real water matrices (e.g., surface waters and industrial effluents). Moreover, a fixed-bed column test demonstrated that â¼1485 bed volumes of the feeding streams (â¼500 µg L-1) can be effectively treated with an enrichment factor of 12.6, suggesting the great potential of TLMSM as POU devices. Furthermore, the principal adsorption complexes (e.g., single-layer -S-Hg-Cl and double-layer -S-Hg-O-Hg-Cl and -S-Hg-O-Hg-OH) formed during the adsorption process under a wide range of pH were synergistically and systematically unveiled using advanced tools. Overall, this work presents an applicable approach by tailoring MOF into a sponge substrate to achieve its real application in heavy metal removal from water, especially for Hg(II).
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Mercurio , Estructuras Metalorgánicas , Contaminantes Químicos del Agua , Adsorción , Cinética , Compuestos de Sulfhidrilo , Agua , Contaminantes Químicos del Agua/análisisRESUMEN
The redox behavior of metal active sites determines the rate of heterogeneous catalysis in peroxymonosulfate activation. Previous reports focused on the construction of catalysts for accelerating interfacial electron transfer. In this work, a new strategy was proposed for facilitating valence cycles of Cu+/Cu2+ by using pollutants. The 2.5Cu/CeO2/PMS system was capable of achieving the efficient removal of pollutants, including tetracycline, oxytetracycline, and rhodamine B, in a wide pH working range. In the presence of tetracycline, a Cu-N bond was formed between the -NH2 group of tetracycline and the Cu site of the catalyst, showing that the coordination of Cu active sites changed to CuO4N1. The charge of CuO4N1 active sites rearranged, making it easier to obtain electrons and promote the PMS oxidation, thereby accelerating the reduction of Cu2+ to Cu+ and PMS activation. The PMS activation system showed excellent sustainability and selectivity for the removal of organic pollutants. This study provides a novel routine to promote peroxymonosulfate activation by utilizing pollutants to accelerate the redox behavior of metal species.
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Cobre , Contaminantes Ambientales , Cobre/química , Oxidación-Reducción , Peróxidos/química , TetraciclinaRESUMEN
This study compares the environmental impacts of a centralized natural gas combined cycle (NGCC) and a distributed natural gas-fired combined heat and power (CHP) energy system in the United States. We develop an energy-balance model in which each energy system supplies the electric, heating, and cooling demands of 16 commercial building types in 16 climate zones of the United States. We assume a best-case scenario where all the CHP's heat and power are allocated toward building demands to ensure robust results. We quantify the greenhouse gas (GHG) emissions, conventional air pollutants (CAPs), and natural gas (NG) consumption. In most cases, the decentralized CHP system increases GHG emissions, decreases CAP emissions, and decreases NG consumption relative to the centralized NGCC system. Only fuel-cell CHPs were able to simultaneously reduce GHG, CAP, and NG consumption relative to the NGCC-based system. The results suggest that despite their energy efficiency benefits, standard distributed CHP-based systems typically do not have enough benefits compared to an NGCC-based system to justify a reorganization of existing infrastructure systems. Because fuel-cell CHPs can also use hydrogen as a fuel source, they are compatible with decarbonized energy systems and may aid in the transition toward a cleaner energy economy.
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Contaminantes Atmosféricos , Contaminación del Aire , Contaminantes Atmosféricos/análisis , Contaminación del Aire/análisis , Objetivos , Efecto Invernadero , Calor , Gas Natural/análisis , Estados UnidosRESUMEN
Nanomaterial adsorbents (NAs) have shown promise to efficiently remove toxic metals from water, yet their practical use remains challenging. Limited understanding of adsorption mechanisms and scaling up evaluation are the two main obstacles. To fully realize the practical use of NAs for metal removal, we review the advanced tools and chemical principles to identify mechanisms, highlight the importance of adsorption capacity and kinetics on engineering design, and propose a systematic engineering scenario for full-scale NA implementation. Specifically, we provide in-depth insight for using density functional theory (DFT) and/or X-ray absorption fine structure (XAFS) to elucidate adsorption mechanisms in terms of active site verification and molecular interaction configuration. Furthermore, we discuss engineering issues for designing, scaling, and operating NA systems, including adsorption modeling, reactor selection, and NA regeneration, recovery, and disposal. This review also prioritizes research needs for (i) determining NA microstructure properties using DFT, XAFS, and machine learning and (ii) recovering NAs from treated water. Our critical review is expected to guide and advance the development of highly efficient NAs for engineering applications.
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Nanoestructuras , Contaminantes Químicos del Agua , Purificación del Agua , Adsorción , Agua , Contaminantes Químicos del Agua/análisisRESUMEN
Hydrophobic membranes used in membrane distillation (MD) systems are often subject to wetting during long-term operation. Thus, it is of great importance to fully understand factors that influence the wettability of hydrophobic membranes and their impact on the overall separation efficiency that can be achieved in MD systems. This Critical Review summarizes both fundamental and applied aspects of membrane wetting with particular emphasis on interfacial interaction between the membrane and solutes in the feed solution. First, the theoretical background of surface wetting, including the relationship between wettability and interfacial interaction, definition and measurement of contact angle, surface tension, surface free energy, adhesion force, and liquid entry pressure, is described. Second, the nature of wettability, membrane wetting mechanisms, influence of membrane properties, feed characteristics and operating conditions on membrane wetting, and evolution of membrane wetting are reviewed in the context of an MD process. Third, specific membrane features that increase resistance to wetting (e.g., superhydrophobic, omniphobic, and Janus membranes) are discussed briefly followed by the comparison of various cleaning approaches to restore membrane hydrophobicity. Finally, challenges with the prevention of membrane wetting are summarized, and future work is proposed to improve the use of MD technology in a variety of applications.
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Destilación , Purificación del Agua , Interacciones Hidrofóbicas e Hidrofílicas , Membranas Artificiales , HumectabilidadRESUMEN
The sluggish regeneration rate of FeII and low operating pH still restrict the wider application of classical Fenton process (FeII/H2O2) for practical water treatment. To overcome these challenges, we exploit the Mn-CNH co-catalyst to construct a solid-liquid interfacial Fenton reaction and accelerate the FeIII/FeII redox cycle at the interface for sustainably generating â¢OH from H2O2 activation. The Mn-CNH co-catalyst exhibits an excellent regeneration rate of FeII (â¼65%) and a high tetracycline removal rate (Kobs) of 0.0541 min-1, which is 19.0 times higher than that of the FeII/H2O2 system (0.0027 min-1) at a near-neutral pH (pH ≈ 5.8), and it also attains 100% degradation of sulfamethoxazole, rhodamine B, and methyl orange. The cyclic mechanism of FeIII/FeII is further elucidated in an atomic scale by combining characterizations and density functional theory calculations, including FeaqIII specific adsorption and the electron-transfer process. Mn active sites can accumulate electrons from the matrix and adsorb FeaqIII to form Mn-Fe bonds at the solid-liquid interface, which accelerate electron transfer from Mn-CNH to FeaqIII and promote the regeneration of FeII at a wide pH range with a lower energy barrier. The regeneration rate of FeII in the Mn-CNH/FeII/H2O2 system outperforms the benchmark Fenton system and other typical metal nanomaterials, which has great potential to be widely applied in actual environment remediation.
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Compuestos Férricos , Peróxido de Hidrógeno , Catálisis , Concentración de Iones de Hidrógeno , Oxidación-ReducciónRESUMEN
Fresh water microplastic pollution is of pressing concern globally, but its distribution and sources in reservoirs are poorly documented. Danjiangkou Reservoir is the second largest reservoir in China and is divided into the Han Reservoir and Dan Reservoir. In this work, microplastic abundances and morphological characteristics of the reservoir were investigated. The microplastic abundance of 15 main tributaries of the reservoir was also measured. The vertical distribution (in water column and sediment), horizontal distribution (in Han Reservoir and Dan Reservoir) and source of microplastics were analyzed. Microplastics accumulated in the middle layer of the reservoir, and the size and color of the microplastic particles changed from the surface to the bottom, which implies that surveys of surface water are not enough to determine the microplastic contamination for deep water reservoirs. In the surface water, the microplastic abundance in the Han Reservoir was lower than that in the Dan Reservoir (p < 0.05), but microplastic abundance did not differ significantly in the intermediate and bottom water. Tributaries were one of the main sources of microplastics for Han Reservoir but not for Dan Reservoir. Agricultural cultivation in the hydro-fluctuation belt might be an important source of microplastics in the Dan Reservoir, which should be given additional attention. The results of this study can provide valuable information for developing microplastic sampling strategies in deep water reservoirs. Further studies are recommended to investigate the process through which microplastics in the hydro-fluctuation belt enter the reservoir and the sinking behavior of microplastics in the reservoir.
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Microplásticos , Contaminantes Químicos del Agua , China , Monitoreo del Ambiente , Plásticos , Contaminantes Químicos del Agua/análisisRESUMEN
Fertilizer drawn forward osmosis (FDFO) was proposed to extract fresh water from flowback and produced water (FPW) from shale gas extraction for irrigation, with fertilizer types and membrane orientations assessed. The draw solution (DS) with NH4H2PO4 displayed the best performance, while the DS with (NH4)2HPO4 resulted in the most severe membrane fouling. The DS with KCl and KNO3 led to substantial reverse solute fluxes. The FDFO operation where the active layer of the membrane was facing the feed solution outperformed that when the active layer was facing the DS. The diluted DS and diluted FPW samples were used for irrigation of Cherry radish and Chinese cabbage. Compared to deionized water, irrigation with the diluted DS (total dissolved solid (TDS) = 350 mg·L-1) promoted plant growth. In contrast, inhibited plant growth was observed when FPW with high salinity (TDS = 5000 mg·L-1) and low salinity (TDS = 1000 mg·L-1) was used for irrigation of long-term (8-week) plant cultures. Finally, upregulated genes were identified to illustrate the difference in plant growth. The results of this study provide a guide for efficient and safe use of FPW after FDFO treatment for agricultural application.
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Fertilizantes , Purificación del Agua , Fertilizantes/análisis , Membranas Artificiales , Gas Natural , Ósmosis , AguaRESUMEN
Mercury (Hg) removal is crucial to the safety of water resources, yet it lacks an effective removal technology, especially for emergency on-site remediation. Herein, multilayered oxygen-functionalized Ti3C2 (Ti3C2Ox) (abbreviated as M-Ti3C2) nanosheets were prepared to remove Hg(II) from water. The M-Ti3C2 has demonstrated ultrafast adsorption kinetics (the concentration decreased from 10â¯400 to 33 µg L-1 in 10 s), impressively high capacity (4806 mg g-1), high selectivity, and broad working pH range (3-12). The density functional theory (DFT) calculations and experimental characterizations unveil that this exceptional Hg(II) removal is owing to the distinct interaction (e.g., adsorption coupled with catalytic reduction). Specifically, Ti atoms on the {001} facets of M-Ti3C2 prefer to adsorb Hg(II) in the form of HgClOH, which subsequently undergoes homolytic cleavage to form radical species (e.g., â¢OH and â¢HgCl). Immediately, the â¢HgCl radicals dimerize and form crystalline Hg2Cl2 on the edges of M-Ti3C2. Up to â¼95% of dimeric Hg2Cl2 can be efficiently recovered via facile thermal treatment. Notably, owing to the adsorbed â¢OH and energy released during the distinct interaction, M-Ti3C2 has been oxidized to TiO2/C nanocomposites. And the TiO2/C nanocomposites have shown to have better performance on the photocatalytic degradation of organic pollutants than Degussa P25. These exceptional features coupled with mercuric recyclable nature make M-Ti3C2 an outstanding candidate for rapid/urgent Hg(II) removal and recovery.
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Mercurio , Titanio , Adsorción , Catálisis , AguaRESUMEN
Sulfide is a toxic and corrosive odorant generated in various sludge treatment and disposal systems. We developed an electrochemical pretreatment (EPT) approach to eliminate sludge sulfide production without adding chemicals. Biochemical sulfide potential (BSP) test was used to evaluate the effectiveness of EPT on sludge sulfide production. The sulfide control was effective with EPT, and we determined the underlying mechanism of EPT. EPT which was operated at 12 V for 720 s eliminated 99% of dissolved sulfide and 100% of gaseous H2S(g). In comparison, the dissolved sulfide reached 104 ± 1 mg S/L in the control BSP test. A sulfur mass balance analysis in the BSP test showed that 90% of the produced sulfide was removed via metal precipitation. Metal distribution results confirmed that metals (i.e., Fe, Mn, and Ni) in the sludge became soluble after EPT and were released from their residual and organically bound fractions. EPT which was operated at 15 V solubilized around 73, 92, and 72% of Fe, Mn, and Ni, and these metals precipitated the sulfide that was produced from biological sulfate reduction. Sludge analysis revealed that EPT disintegrated sludge flocs and disrupted metal-binding functional groups. Specifically, reduction of 17% CâO functional groups in the sludge was found, which could be associated with metal release. The impact of oxidants (e.g., chlorine) generated from EPT on sulfide oxidation was minimal. The findings of this study broadened up our understanding of the electrochemical process for sulfide control during saline sludge digestion.
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Aguas del Alcantarillado , Eliminación de Residuos Líquidos , Cloruros , Sulfuros , AzufreRESUMEN
Efficient elimination of antibacterial activity of halogenated antibiotics by dehalogenation pretreatment is desired for a biochemical treatment process. In this study, crystalline cobalt phosphide nanosheet arrays on a Ti plate (C-CoP/Ti) are fabricated by a simple electrodeposition and phosphorization process. The crystalline structure greatly promotes atomic hydrogen (H*) generation. Moreover, the nanosheet arrays can provide abundant active sites and accelerate electron transfer and mass transport. As a result, the dehalogenation rate of florfenicol (FLO, an emerging organic pollutant) on C-CoP/Ti is 11.1, 2.97, and 13.6 times higher than that on amorphous CoP/Ti, Pd/Ti, and bare Ti, respectively. The C-CoP/Ti electrode achieves 97.4% dehalogenation of FLO (20 mg L-1) within 30 min at -1.2 V (vs Ag/AgCl). Nearly 100% of Cl and 20% of F are broken away within 120 min, showing the highest electrocatalytic defluorination efficiency reported so far. Both experimental results and theoretical calculations reveal that the dehalogenation of FLO on C-CoP/Ti is synergistically accomplished via direct reduction of electron transfer and indirect reduction of H*. This study develops a highly efficient non-noble metal electrode material for dehalogenation of halogenated organic compounds.
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Tianfenicol , Electrodos , Halogenación , Tianfenicol/análogos & derivados , TitanioRESUMEN
Recently, the UV/free chlorine process has gained attention as a promising technology for destroying refractory organic contaminants in the aqueous phase. We have developed a kinetic model based on first-principles to describe the kinetics and mechanisms of the oxidation of organic contaminants in the UV/free chlorine process. Substituted benzoic acid compounds (SBACs) were chosen as the target parent contaminants. We determined the second-order rate constants between SBACs and reactive chlorine species (RCS; including [Formula: see text], [Formula: see text] and [Formula: see text]) by fitting our model to the experimental results. We then predicted the concentration profiles of SBACs under various operational conditions. We analyzed the kinetic data and predicted concentration profiles of reactive radicals ([Formula: see text] and RCS), we found that [Formula: see text] was the dominant radicals for SBACs destruction. In addition, we established quantitative structure activity relationships (QSARs) that can help predict the second-order rate constants for SBACs destruction by each type of reactive radicals using SBACs Hammett constants. Our first-principles-based kinetic model has been verified using experimental data. Our model can facilitate a design for the most cost-effective application of the UV/free chlorine process. For example, our model can determine the optimum chlorine dosage and UV light intensity that result in the lowest energy consumption.