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1.
• The NPs aggregation in the electrolyte solution is consistent with the DLVO theory. • In NaNO3 and low Ca(NO3)2, EPS alleviates the NPs aggregation by steric repulsion. • In high Ca(NO3)2, EPS accelerates the NPs aggregation by exopolysaccharide bridging. • Ag2S NPs have stronger stability compared with Cit-Ag NPs in aqueous systems. Extracellular polymeric substances (EPS) in activated sludge from wastewater treatment plants (WWTPs) could affect interactions between nanoparticles and alter their migration behavior. The influence mechanisms of silver nanoparticles (Ag NPs) and silver sulfide nanoparticles (Ag2S NPs) aggregated by active EPS sludge were studied in monovalent or divalent cation solutions. The aggregation behaviors of the NPs without EPS followed the Derjaguin-Landau-Verwey-Overbeek (DLVO) theory. The counterions aggravated the aggregation of both NPs, and the divalent cation had a strong neutralizing effect due to the decrease in electrostatic repulsive force. Through extended DLVO (EDLVO) model analysis, in NaNO3 and low-concentration Ca(NO3)2 (<10 mmol/L) solutions, EPS could alleviate the aggregation behaviors of Cit-Ag NPs and Ag2S NPs due to the enhancement of steric repulsive forces. At high concentrations of Ca(NO3)2 (10‒100 mmol/L), exopolysaccharide macromolecules could promote the aggregation of Cit-Ag NPs and Ag2S NPs by interparticle bridging. As the final transformation form of Ag NPs in water environments, Ag2S NPs had better stability, possibly due to their small van der Waals forces and their strong steric repulsive forces. It is essential to elucidate the surface mechanisms between EPS and NPs to understand the different fates of metal-based and metal-sulfide NPs in WWTP systems.  相似文献   

2.
• CeO2 doping significantly improved low-temperature NH3-SCR activity on FeTiOx. • The crystallinity of FeTiOx was decreased dramatically after CeO2 doping. • Unique Ce-O-Fe structure in FeCe0.2TiOx accounted for its superior redox property. • Facile activation of NH3 to-NH2 on FeCe0.2TiOx promoted the DeNOx efficiency. FeTiOx has been recognized as an environmental-friendly and cost-effective catalyst for selective catalytic reduction (SCR) of NOx with NH3. Aimed at further improving the low-temperature DeNOx efficiency of FeTiOx catalyst, a simple strategy of CeO2 doping was proposed. The low-temperature (<250℃) NH3-SCR activity of FeTiOx catalyst could be dramatically enhanced by CeO2 doping, and the optimal composition of the catalyst was confirmed as FeCe0.2TiOx, which performed a NOx conversion of 90% at ca. 200℃. According to X-ray diffraction (XRD), Raman spectra and X-ray absorption fine structure spectroscopy (XAFS) analysis, FeCe0.2TiOx showed low crystallinity, with Fe and Ce species well mixed with each other. Based on the fitting results of extended X-ray absorption fine structure (EXAFS), a unique Ce-O-Fe structure was formed in FeCe0.2TiOx catalyst. The well improved specific surface area and the newly formed Ce-O-Fe structure dramatically contributed to the improvement of the redox property of FeCe0.2TiOx catalyst, which was well confirmed by H2-temperature-programmed reduction (H2-TPR) and in situ XAFS experiments. Such enhanced redox capability could benefit the activation of NO and NH3 at low temperatures for NOx removal. The detailed reaction mechanism study further suggested that the facile oxidative dehydrogenation of NH3 to highly reactive-NH2 played a key role in enhancing the low-temperature NH3-SCR performance of FeCe0.2TiOx catalyst.  相似文献   

3.
• Challenges in sampling of NH3 sources for d15N analysis are highlighted. • Uncertainties in the isotope-based source apportionment of NH3 and NH4+ are outlined. • Characterizing dynamic isotopic fractionation may reduce uncertainties of NHx science. Agricultural sources and non-agricultural emissions contribute to gaseous ammonia (NH3) that plays a vital role in severe haze formation. Qualitative and quantitative contributions of these sources to ambient PM2.5 (particulate matter with an aerodynamic equivalent diameter below 2.5 µm) concentrations remains uncertain. Stable nitrogen isotopic composition (δ15N) of NH3 and NH4+15N(NH3) and δ15N(NH4+), respectively) can yield valuable information about its sources and associated processes. This review provides an overview of the recent progress in analytical techniques for δ15N(NH3) and δ15N(NH4+) measurement, sampling of atmospheric NH3 and NH4+ in the ambient air and their sources signature (e.g., agricultural vs. fossil fuel), and isotope-based source apportionment of NH3 in urban atmosphere. This study highlights that collecting sample that are fully representative of emission sources remains a challenge in fingerprinting δ15N(NH3) values of NH3 emission sources. Furthermore, isotopic fractionation during NH3 gas-to-particle conversion under varying ambient field conditions (e.g., relative humidity, particle pH, temperature) remains unclear, which indicates more field and laboratory studies to validate theoretically predicted isotopic fractionation are required. Thus, this study concludes that lack of refined δ15N(NH3) fingerprints and full understanding of isotopic fractionation during aerosol formation in a laboratory and field conditions is a limitation for isotope-based source apportionment of NH3. More experimental work (in chamber studies) and theoretical estimations in combinations of field verification are necessary in characterizing isotopic fractionation under various environmental and atmospheric neutralization conditions, which would help to better interpret isotopic data and our understanding on NHx (NH3 + NH4+) dynamics in the atmosphere.  相似文献   

4.
• The combination of NaOH and nitrite was used to control harmful gas in sewers. • Hydrogen sulfide and methane in airspace were reduced by 96.01% and 91.49%. • Changes in sewage quality and greenhouse effect by chemical dosing were negligible. • The strong destructive effects on biofilm slowed down the recovery of harmful gases. • The cost of the method was only 3.92 × 10−3 $/m3. An innovative treatment method by the combination of NaOH and nitrite is proposed for controlling hydrogen sulfide and methane in gravity sewers and overcome the drawbacks of the conventional single chemical treatment. Four reactors simulating gravity sewers were set up to assess the effectiveness of the proposed method. Findings demonstrated hydrogen sulfide and methane reductions of about 96.01% and 91.49%, respectively, by the combined addition of NaOH and nitrite. The consumption of NaNO2 decreased by 42.90%, and the consumption rate of NaOH also showed a downward trend. Compared with a single application of NaNO2, the C/N ratio of wastewater was increased to about 0.61 mg COD/mg N. The greenhouse effect of intermediate N2O and residual methane was about 48.80 gCO2/m3, which is far lower than that of methane without control (260 gCO2/m3). Biofilm was destroyed to prevent it from entering the sewage by the chemical additives, which reduced the biomass and inhibited the recovery of biofilm activity to prolong the control time. The sulfide production rate and sulfate reduction rate were reduced by 92.32% and 85.28%, respectively. Compared with conventional control methods, the cost of this new method was only 3.92 × 10−3 $/m3, which is potentially a cost-effective strategy for sulfide and methane control in gravity sewers.  相似文献   

5.
• The optimum SCR activity was realized by tuning the acid pretreatment. • Optimized catalysts showed NOx conversion above 90%. • The NH3 and NO adsorption capacity of Al-O3-Fe is stronger than Fe-O3-Fe. • The formation of almandine consumes Fe3+ and Al3+ and weakens their interaction. Red mud (RM), as an alkaline waste, was recently proved to be a promising substitute for the SCR catalyst. Dealkalization could improve the acidity and reducibility of red mud, which were critical for SCR reaction. However, the dealkalization effect depended on the reaction between acid solution and red mud. In this study, we realized the directional control of the chemical state of active sites through tuning the acid pretreatment (dealkalization) process. The pretreatment endpoint was controlled at pH values of 3–5 with diluted nitric acid. When the pH values of red mud were 3 and 5 (CRM-3 and CRM-5), activated catalysts showed NOx conversion above 90% at 275°C–475°C. The high initial reaction rate, Ce3+/(Ce3+ + Ce4+) ratio, and surface acidity accounted for the excellent SCR performance of CRM-5 catalyst. Meanwhile, more Fe3+ on the CRM-3 surface improved the NH3 adsorption. There was a strong interaction between Al and Fe in both CRM-5 and CRM-3 catalysts. DFT results showed that the adsorption capacity of the Al-O3-Fe for NH3 and NO is stronger than that of Fe-O3-Fe, which enhanced the NOx conversion of the catalyst. However, the almandine was formed in CRM-4, consumed part of Fe3+ and Al3+, and the interaction between Al and Fe was weakened. Also, deposited almandine on the catalyst surface covered the active sites, thus leading to lower NH3-SCR activity.  相似文献   

6.
• 4-chlorophenol biodegradation could be enhanced in Fe2O3 coupled anaerobic system. • Metabolic activity and electron transport could be improved by Fe2O3 nanoparticles. • Functional microbial communities could be enriched in coupled anaerobic system. • Possible synergistic mechanism involved in enhanced dechlorination was proposed. Fe2O3 nanoparticles have been reported to enhance the dechlorination performance of anaerobic systems, but the underlying mechanism has not been clarified. This study evaluated the technical feasibility, system stability, microbial biodiversity and the underlying mechanism involved in a Fe2O3 nanoparticle-coupled anaerobic system treating 4-chlorophenol (4-CP) wastewater. The results demonstrated that the 4-CP and total organic carbon (TOC) removal efficiencies in the Fe2O3-coupled up-flow anaerobic sludge blanket (UASB) were always higher than 97% and 90% during long-term operation, verifying the long-term stability of the Fe2O3-coupled UASB. The 4-CP and TOC removal efficiencies in the coupled UASB increased by 42.9±0.4% and 27.5±0.7% compared to the control UASB system. Adding Fe2O3 nanoparticles promoted the enrichment of species involved in dechlorination, fermentation, electron transfer and acetoclastic methanogenesis, and significantly enhanced the extracellular electron transfer ability, electron transport activity and conductivity of anaerobic sludge, leading to enhanced 4-CP biodegradation performance. A possible synergistic mechanism involved in enhanced anaerobic 4-CP biodegradation by Fe2O3 nanoparticles was proposed.  相似文献   

7.
• Forward osmosis (FO) coupled with chemical softening for CCI ROC minimization • Effective removal of scale precursor ions by lime-soda ash softening • Enhanced water recovery from 54% to 86% by mitigation of FO membrane scaling • High-purity CaCO3 was recovered from the softening sludge • Membrane cleaning efficiency of 88.5% was obtained by EDTA for softened ROC Reverse osmosis (RO) is frequently used for water reclamation from treated wastewater or desalination plants. The RO concentrate (ROC) produced from the coal chemical industry (CCI) generally contains refractory organic pollutants and extremely high-concentration inorganic salts with a dissolved solids content of more than 20 g/L contributed by inorganic ions, such as Na+, Ca2+, Mg2+, Cl, and SO42. To address this issue, in this study, we focused on coupling forward osmosis (FO) with chemical softening (FO-CS) for the volume minimization of CCI ROC and the recovery of valuable resources in the form of CaCO3. In the case of the real raw CCI ROC, softening treatment by lime-soda ash was shown to effectively remove Ca2+/Ba2+ (>98.5%) and Mg2+/Sr2+/Si (>80%), as well as significantly mitigate membrane scaling during FO. The softened ROC and raw ROC corresponded to a maximum water recovery of 86% and 54%, respectively. During cyclic FO tests (4 × 10 h), a 27% decline in the water flux was observed for raw ROC, whereas only 4% was observed for softened ROC. The cleaning efficiency using EDTA was also found to be considerably higher for softened ROC (88.5%) than that for raw ROC (49.0%). In addition, CaCO3 (92.2% purity) was recovered from the softening sludge with an average yield of 5.6 kg/m3 treated ROC. This study provides a proof-of-concept demonstration of the FO-CS coupling process for ROC volume minimization and valuable resources recovery, which makes the treatment of CCI ROC more efficient and more economical.  相似文献   

8.
• Size and shape-dependent MnFe2O4 NPs were prepared via a facile method. • Ligand-exchange chemistry was used to prepare the hydrophilic MnFe2O4 NPs. • The catalytic properties of MnFe2O4 NPs toward dye degradation were fully studied. • The catalytic activities of MnFe2O4 NPs followed Michaelis–Menten behavior. • All the MnFe2O4 NPs exhibit selective degradation to different dyes. The magnetic nanoparticles that are easy to recycle have tremendous potential as a suitable catalyst for environmental toxic dye pollutant degradation. Rationally engineering shapes and tailoring the size of nanocatalysts are regarded as an effective manner for enhancing performances. Herein, we successfully synthesized three kinds of MnFe2O4 NPs with distinctive sizes and shapes as catalysts for reductive degradation of methylene blue, rhodamine 6G, rhodamine B, and methylene orange. It was found that the catalytic activities were dependent on the size and shape of the MnFe2O4 NPs and highly related to the surface-to-volume ratio and atom arrangements. Besides, all these nanocatalysts exhibit selectivity to different organic dyes, which is beneficial for their practical application in dye pollutant treatment. Furthermore, the MnFe2O4 NPs could be readily recovered by a magnet and reused more than ten times without appreciable loss of activity. The size and shape effects of MnFe2O4 nanoparticles demonstrated in this work not only accelerate further understanding the nature of nanocatalysts but also contribute to the precise design of nanoparticles catalyst for pollutant degradation.  相似文献   

9.
• DPAA sorption data was found to fit the Freundlich equation. Kf was significantly positive correlated with oxalate-extractable Fe2O3. • Ligand exchange was the main mechanism for DPAA sorption on soils. • Bidentate binuclear and monodentate mononuclear DPAA bonds were identified. Diphenylarsinic acid (DPAA) is a phenyl arsenic compound derived from chemical warfare weapons. Macroscopic and microscopic work on DPAA sorption will provide useful information in predicting the partitioning and mobility of DPAA in the soil-water environment. Here, batch experiments and extended X-ray absorption fine structure (EXAFS) spectroscopy were used to investigate the sorption mechanisms of DPAA. The DPAA sorption data from 11 soil types was found to fit the Freundlich equation, and the sorption capacity, Kf, was significantly and positively correlated with oxalate-extractable Fe2O3. The Kf values of eight of the 11 untreated soils (1.51–113.04) significantly decreased upon removal of amorphous metal (hydr)oxides (0.51–13.37). When both amorphous and crystalline metal (hydr)oxides were removed from the untreated soils, the Kf values either decreased or slightly increased (0.65–3.09). Subsequent removal of soil organic matter from these amorphous and crystalline metal (hydr)oxide-depleted samples led to further decreases in Kf to 0.02–1.38, with only one exception (Sulfic Aquic-Orthic Halosols). These findings strongly suggest that ligand exchange reactions with amorphous metal (hydr)oxides contribute most to DPAA sorption on soils. EXAFS data provide further evidence that DPAA primarily formed bidentate binuclear (2C) and monodentate mononuclear (1V) coring-sharing complexes with As-Fe distances of 3.34 and 3.66 Å, respectively, on Fe (hydr)oxides. Comparison of these results with earlier studies suggests that 2C and 1V complexes of DPAA may be favored under low and high surface coverages, respectively, with the formation of 1V bonds possibly conserving the sorption sites or decreasing the steric hindrance derived from phenyl substituents.  相似文献   

10.
• BiVO4/Fe3O4/rGO has excellent photocatalytic activity under solar light radiation. • It can be easily separated and collected from water in an external magnetic field. • BiVO4/Fe3O4/0.5% rGO exhibited the highest RhB removal efficiency of over 99%. • Hole (h+) and superoxide radical (O2) dominate RhB photo-decomposition process. • The reusability of this composite was confirmed by five successive recycling runs. Fabrication of easily recyclable photocatalyst with excellent photocatalytic activity for degradation of organic pollutants in wastewater is highly desirable for practical application. In this study, a novel ternary magnetic photocatalyst BiVO4/Fe3O4/reduced graphene oxide (BiVO4/Fe3O4/rGO) was synthesized via a facile hydrothermal strategy. The BiVO4/Fe3O4 with 0.5 wt% of rGO (BiVO4/Fe3O4/0.5% rGO) exhibited superior activity, degrading greater than 99% Rhodamine B (RhB) after 120 min solar light radiation. The surface morphology and chemical composition of BiVO4/Fe3O4/rGO were studied by scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, UV–visible diffuse reflectance spectroscopy, Fourier transform infrared spectroscopy, and Raman spectroscopy. The free radicals scavenging experiments demonstrated that hole (h+) and superoxide radical (O2) were the dominant species for RhB degradation over BiVO4/Fe3O4/rGO under solar light. The reusability of this composite catalyst was also investigated after five successive runs under an external magnetic field. The BiVO4/Fe3O4/rGO composite was easily separated, and the recycled catalyst retained high photocatalytic activity. This study demonstrates that catalyst BiVO4/Fe3O4/rGO possessed high dye removal efficiency in water treatment with excellent recyclability from water after use. The current study provides a possibility for more practical and sustainable photocatalytic process.  相似文献   

11.
12.
• The feasibility of facile fabrication of capacitor from floc sludge is discussed. • The porous carbon composites are obtained by acidification and KOH activation. • The as-prepared 3D structure has large surface area and optimal pore size. • Admirable specific capacitance and outstanding cycling stability are obtained. In this paper, floc sludge was transformed into porous carbon matrix composites by acidification and KOH activation at high temperature and used as an electrode material for application in capacitors. The effects of different treatment processes on the electrochemical properties of sludge materials were compared. The results of electrochemical tests showed that the sludge electrode exhibited excellent energy storage performance after HNO3 acidification and KOH activation with a mass ratio of 3:1 (KOH/C). The specific capacitance of the sludge electrode reached 287 F/g at a current density of 1 A/g. In addition, the sludge electrode material showed excellent cycle stability (specific capacity retained at 93.4% after 5000 cycles at 5 A/g). Based on XRD, FTIR, SEM, TEM, and BET surface analysis, the morphology of sludge electrode materials can be effectively regulated by chemical pretreatment. The best-performing material showed a 3D porous morphology with a large specific surface area (2588 m2/g) and optimal pore size distribution, improving ion channels and charge conductivity. According to the life cycle assessment of floc sludge utilization, it reduced the resource consumption and toxicity risk by more than 90% compared with ordinary sludge disposal processes. This work provided a cost-effective and eco-friendly sludge reuse method and demonstrated the application potential of sludge-based materials in high-performance supercapacitors.  相似文献   

13.
• Comprehensive mitigation of gas emissions from swine manure was investigated. • Additives addition for mitigation of gas from the manure has been developed. Sargassum horneri, seaweed masking strategy controlled gas by 90%-100%. • Immediate reduction in emitted gas and improving air quality has been determined. • Microbial consortium with seaweed completely controlled gas emissions by 100%. Gas emissions from swine farms have an impact on air quality in the Republic of Korea. Swine manure stored in deep pits for a long time is a major source of harmful gas emissions. Therefore, we evaluated the mitigation of emissions of ammonia (NH3), hydrogen sulfide (H2S) and amine gases from swine manure with biological products such as seaweed (Sargassum horneri) and a microbial consortium (Bacillus subtilis (1.2 × 109 CFU/mL), Thiobacillus sp. (1.0 × 1010 CFU/mL) and Saccharomyces cerevisiae (2.0 × 109 CFU/mL)) used as additives due to their promising benefits for nutrient cycling. Overall, seaweed powder masking over two days provided notable control of over 98%-100% of the gas emissions. Furthermore, significant control of gas emissions was especially pronounced when seaweed powder masking along with a microbial consortium was applied, resulting in a gas reduction rate of 100% for NH3, amines and H2S over 10 days of treatment. The results also suggested that seaweed powder masking and a microbial consortium used in combination to reduce the gas emissions from swine manure reduced odour compared with that observed when the two additives were used alone. Without the consortium, seaweed decreased total volatile fatty acid (VFA) production. The proposed novel method of masking with a microbial consortium is promising for mitigating hazardous gases, simple, and environmentally beneficial. More research is warranted to determine the mechanisms underlying the seaweed and substrate interactions.  相似文献   

14.
Factors impacting indoor-outdoor relations are introduced. Sulfate seems a fine tracer for other non-volatile species. Particulate nitrate and ammonium desorb during outdoor-to-indoor transport. OC load increases during the transport due to sorption of indoor SVOCs. Outdoor PM2.5 influences both the concentration and composition of indoor PM2.5. People spend over 80% of their time indoors. Therefore, to assess possible health effects of PM2.5 it is important to accurately characterize indoor PM2.5 concentrations and composition. Controlling indoor PM2.5 concentration is presently more feasible and economic than decreasing outdoor PM2.5 concentration. This study reviews modeling and measurements that address relationships between indoor and outdoor PM2.5 and the corresponding constituent concentrations. The key factors in the models are indoor-outdoor air exchange rate, particle penetration, and deposition. We compiled studies that report I/O ratios of PM2.5 and typical constituents (sulfate (SO42-), nitrate (NO3-), ammonium (NH4+), elemental carbon (EC), and organic carbon (OC), iron (Fe), copper (Cu), and manganese (Mn)). From these studies we conclude that: 1) sulfate might be a reasonable tracer of non-volatile species (EC, Fe, Cu, and Mn) and PM2.5 itself; 2) particulate nitrate and ammonium generally desorb to gaseous HNO3 and NH3 when they enter indoors, unless, as seldom happens, they have strong indoor sources; 3) indoor-originating semi-volatile organic compounds sorb on indoor PM2.5, thereby increasing the PM2.5 OC load. We suggest further studies on indoor-outdoor relationships of PM2.5 and constituents so as to help develop standards for healthy buildings.  相似文献   

15.
• Aquatic plants are more likely to absorb TiO2 NPs that are beneficial to them. • Ag NPs inhibited the growth of aquatic plants under both 5- and 60-day exposure. • CeO2 NPs had positive/negative impact on plant in 5/60-day exposure, respectively. • TiO2 NPs presence could enhance the photosynthesis and increase the plant biomass. • The ENPs changed plant activity, which resulted in changes of wetland performance. Engineered nanoparticles (ENPs) threaten the environment through wastewater discharging. Generally, constructed wetlands (CWs) are efficient methods for ENPs removal. However, the biotoxicity of ENPs on plants in CWs is unclear. Here, we investigated the distribution and bio-impacts of different ENPs (Ag NPs, TiO2 NPs, and CeO2 NPs) in plants under 5- and 60-day exposure to 1 and 50 mg/L concentrations. Results showed that ENPs appeared in the vascular bundle and mesophyll cell space, which induced the variation in antioxidase activities (e.g., superoxide dismutase [SOD], peroxidase [POD], and catalase [CAT] activities) as well as overproduction of malondialdehyde (MDA). Additionally, Ag NPs inhibited photosynthesis rate and root activity during two exposure phases. CeO2 NPs had positive and negative impacts on plants in 5- and 60-day exposure, respectively. Inversely, TiO2 NPs enhanced photosynthesis and root activity under 60-day exposure. Finally, the contents of the C, N, and P elements in plants fluctuated in response to ENPs stress. All results have a positive correlation with the wetland performance under ENPs exposure except for TiO2 NPs treatment. Overall, our study systematically reveals aquatic plants' responses to ENPs and provides a reference for building ecological treatment systems to purify wastewater containing ENPs.  相似文献   

16.
• A novel Z-scheme Si-SnO2-TiOx with SnO2 as electron mediator is first constructed. • Transparent and conductive SnO2 can pass light through and promote charge transport. • VO from SnO2 and TiOx improve photoelectrochemical performances. • Efficient photocatalytic degradations originate from the Z scheme construction. Z-scheme photocatalysts, with strong redox ability, have a great potential for pollutants degradation. However, it is challenging to construct efficient Z-scheme photocatalysts because of their poor interfacial charge separation. Herein, by employing transparent and conductive SnO2 as electron mediator to pass light through and promote interfacial charge transportation, a novel Z-scheme photocatalyst Si-SnO2-TiOx (1<x<2) was constructed. The Z-scheme photocatalyst displayed an order of magnitude higher photocurrent density and a 4-fold increase in open-circuit potential compared to those of Si. Moreover, the onset potential shifted negatively for approximately 2.2 V. Benefiting from these advantages, this Z-scheme Si-SnO2-TiOx exhibited efficient photocatalytic performance toward phenol degradation and mineralization. 75% of the phenol was degraded without bias potential and 70% of the TOC was removed during phenol degradation. Other typical pollutants such as bisphenol A and atrazine could also be degraded without bias potential. Introducing a transparent and conductive electron mediator to construct Z-scheme photocatalyst gives a new sight to the improvement of photocatalytic performance in Z scheme.  相似文献   

17.
• A V2O5/TiO2 granular catalyst for simultaneous removal of NO and chlorobenzene. • Catalyst synthesized by vanadyl acetylacetonate showed good activity and stability. • The kinetic model was established and the synergetic activity was predicted. • Both chlorobenzene oxidation and SCR of NO follow pseudo-first-order kinetics. • The work is of much value to design of multi-pollutants emission control system. The synergetic abatement of multi-pollutants is one of the development trends of flue gas pollution control technology, which is still in the initial stage and facing many challenges. We developed a V2O5/TiO2 granular catalyst and established the kinetic model for the simultaneous removal of NO and chlorobenzene (i.e., an important precursor of dioxins). The granular catalyst synthesized using vanadyl acetylacetonate precursor showed good synergistic catalytic performance and stability. Although the SCR reaction of NO and the oxidation reaction of chlorobenzene mutually inhibited, the reaction order of each reaction was not considerably affected, and the pseudo-first-order reaction kinetics was still followed. The performance prediction of this work is of much value to the understanding and reasonable design of a catalytic system for multi-pollutants (i.e., NO and dioxins) emission control.  相似文献   

18.
• Bi2O3 cannot directly activate PMS. • Bi2O3 loading increased the specific surface area and conductivity of CoOOH. • Larger specific surface area provided more active sites for PMS activation. • Faster electron transfer rate promoted the generation of reactive oxygen species. 1O2 was identified as dominant ROS in the CoOOH@Bi2O3/PMS system. Cobalt oxyhydroxide (CoOOH) has been turned out to be a high-efficiency catalyst for peroxymonosulfate (PMS) activation. In this study, CoOOH was loaded on bismuth oxide (Bi2O3) using a facile chemical precipitation process to improve its catalytic activity and stability. The result showed that the catalytic performance on the 2,4-dichlorophenol (2,4-DCP) degradation was significantly enhanced with only 11 wt% Bi2O3 loading. The degradation rate in the CoOOH@Bi2O3/PMS system (0.2011 min1) was nearly 6.0 times higher than that in the CoOOH/PMS system (0.0337 min1). Furthermore, CoOOH@Bi2O3 displayed better stability with less Co ions leaching (16.4% lower than CoOOH) in the PMS system. These phenomena were attributed to the Bi2O3 loading which significantly increased the conductivity and specific surface area of the CoOOH@Bi2O3 composite. Faster electron transfer facilitated the redox reaction of Co (III) / Co (II) and thus was more favorable for reactive oxygen species (ROS) generation. Meanwhile, larger specific surface area furnished more active sites for PMS activation. More importantly, there were both non-radical (1O2) and radicals (SO4•, O2•, and OH•) in the CoOOH@Bi2O3/PMS system and 1O2 was the dominant one. In general, this study provided a simple and practical strategy to enhance the catalytic activity and stability of cobalt oxyhydroxide in the PMS system.  相似文献   

19.
• UV/O3 process had higher TAIC mineralization rate than O3 process. • Four possible degradation pathways were proposed during TAIC degradation. • pH impacted oxidation processes with pH of 9 achieving maximum efficiency. • CO32– negatively impacted TAIC degradation while HCO3 not. • Cl can be radicals scavenger only at high concentration (over 500 mg/L Cl). Triallyl isocyanurate (TAIC, C12H15N3O3) has featured in wastewater treatment as a refractory organic compound due to the significant production capability and negative environmental impact. TAIC degradation was enhanced when an ozone(O3)/ultraviolet(UV) process was applied compared with the application of an independent O3 process. Although 99% of TAIC could be degraded in 5 min during both processes, the O3/UV process had a 70%mineralization rate that was much higher than that of the independent O3 process (9%) in 30 min. Four possible degradation pathways were proposed based on the organic compounds of intermediate products identified during TAIC degradation through the application of independent O3 and O3/UV processes. pH impacted both the direct and indirect oxidation processes. Acidic and alkaline conditions preferred direct and indirect reactions respectively, with a pH of 9 achieving maximum Total Organic Carbon (TOC) removal. Both CO32– and HCO3 decreased TOC removal, however only CO32– negatively impacted TAIC degradation. Effects of Cl as a radical scavenger became more marked only at high concentrations (over 500 mg/L Cl). Particulate and suspended matter could hinder the transmission of ultraviolet light and reduce the production of HO· accordingly.  相似文献   

20.
•Bio-RD-PAO can effectively and extensively remove organohalides. •Bio-RD alone effectively dehalogenate the highly-halogenated organohalides. •PAO alone is efficient in degrading the lowly-halogenated organohalides. •The impacts of PAO on organohalide-respiring microbial communities remain elusive. •Bio-RD-PAO provides a promising solution for remediation of organohalide pollution. Due to the toxicity of bioaccumulative organohalides to human beings and ecosystems, a variety of biotic and abiotic remediation methods have been developed to remove organohalides from contaminated environments. Bioremediation employing organohalide-respiring bacteria (OHRB)-mediated microbial reductive dehalogenation (Bio-RD) represents a cost-effective and environmentally friendly approach to attenuate highly-halogenated organohalides, specifically organohalides in soil, sediment and other anoxic environments. Nonetheless, many factors severely restrict the implications of OHRB-based bioremediation, including incomplete dehalogenation, low abundance of OHRB and consequent low dechlorination activity. Recently, the development of in situ chemical oxidation (ISCO) based on sulfate radicals (SO4·) via the persulfate activation and oxidation (PAO) process has attracted tremendous research interest for the remediation of lowly-halogenated organohalides due to its following advantages, e.g., complete attenuation, high reactivity and no selectivity to organohalides. Therefore, integration of OHRB-mediated Bio-RD and subsequent PAO (Bio-RD-PAO) may provide a promising solution to the remediation of organohalides. In this review, we first provide an overview of current progress in Bio-RD and PAO and compare their limitations and advantages. We then critically discuss the integration of Bio-RD and PAO (Bio-RD-PAO) for complete attenuation of organohalides and its prospects for future remediation applications. Overall, Bio-RD-PAO opens up opportunities for complete attenuation and consequent effective in situ remediation of persistent organohalide pollution.  相似文献   

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