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1.
• Activated carbon was proposed to be an efficient accelerant for molded red mud catalyst. • The surface acidity and reducibility were highly improved, as well as the pore structure. • The enrichment of the surface Fe2+ and the adsorbed oxygen account for the improvement. Our previous study proved that the acid-pretreatment process could efficiently activate red mud (RM) for the selective catalytic reduction (SCR) of NOx. However, in terms of the molding process, which is the key step determining whether it can be applied in large-scale industrial, the surface acidity and reducibility of catalyst always decreased dramatically, and part of surface area and pore structure were lost. In this study, we prepared monolithic honeycomb red mud (MHRM) catalysts with activated carbon (AC) as an accelerant and investigated the effect of AC on the MHRM. The results showed that the MHRM with 3 wt.% of AC (MHRM-AC3) exhibited the best SCR performance, and kept more than 80% NOx conversion in the range of 325°C–400°C. Compared with the MHRM, MHRM-AC1, and HMRM-AC5, the MHRM-AC3 has more mesoporous and macroporous structures, which can provide more adsorption active sites. The AC significantly improved NH3 adsorption and surface reducibility, which was mainly due to the increase of the surface acid sites (especially the Brönsted acid sites), the concentration of Fe(II), and the surface adsorbed oxygen. The presence of more Fe(II) enriched the surface oxygen vacancies, as well as the surface adsorbed oxygen, due to the charge imbalance and unsaturated chemical bond. And surface adsorbed oxygen exhibited more active than lattice oxygen owing to its higher mobility, which was conducive to NOx reduction in the SCR reaction.  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.
• Pt/CZL exhibits the optimum catalytic performance for HC and NOx elimination. • The strong PM-Ce interaction favors the oxygen mobility and DOSC. • Pd/CZL shows higher catalytic activity for CO conversion due to more Olatt species. • Great oxygen mobility at high temperature broadens the dynamic operation window. • The relationship between DOSC and catalytic performance is revealed. The physicochemical properties of Pt-, Pd- and Rh- loaded (Ce,Zr,La)O2 (shorted for CZL) catalysts before/after aging treatment were systematically characterized by various techniques to illustrate the relationship of the dynamic oxygen storage/release capacity and redox ability with their catalytic performances for HC, NOx and CO conversions. Pt/CZL catalyst exhibits the optimum catalytic performance for HC and NOx elimination, which mainly contribute to its excellent redox ability and dynamic oxygen storage/release capacity (DOSC) at lower temperature due to the stronger PM (precious metals)-support interaction. However, the worse stability of Pt-O-Ce species and volatile Pt oxides easily result in the dramatical decline in catalytic activity after aging. Pd/CZL shows higher catalytic activity for CO conversion by reason of more Olatt species as the active oxygen for CO oxidation reaction. Rh/CZL catalyst displays the widest dynamic operation window for NOx elimination as a result of greater oxygen mobility at high temperature, and the ability to retain more Rh-O-Ce species after calcined at 1100°C effectively restrains sintering of active RhOx species, improving the thermal stability of Rh/CZL catalyst.  相似文献   

4.
• K+ hinder the structural degradation of Cu/SAPO-34 under humid condition<100°C. • K+ on Cu/SAPO-34 brings lower acidity and inferior SCR activity at high temperature. • Fe/Beta was used to compensate the low activity of Cu/SAPO-34 at high temperature. • The hybrid catalysts with KCu/SAPO-34 and Fe/Beta show a great potential for using. K ions were introduced onto Cu/SAPO-34 catalysts via the ion-exchange process in order to improve their stability under low-temperature hydrothermal aging. The changes in structure and copper-species contents of these catalysts upon hydrothermal aging were probed in order to investigate their effects on selective catalytic reduction (SCR) activity. For the fresh Cu/SAPO-34 catalysts, K ions had little influence on the chabazite framework but effected their acidities by exchanging with acid sites. After hydrothermal aging, the structural integrity and amount of active sites decreased on pure Cu/SAPO-34. While the K-loaded catalysts showed improved chabazite structure, acidity, and active site conservation with increasing K loading. However, although the 0.7 wt% K catalyst maintained the same crystallinity, active site abundance, and low-temperature SCR activity as the fresh catalyst upon aging, an apparent decrease in SCR activity at high temperature was observed because of the inevitable decrease in the number of Brönsted acid sites. To compensate for the activity disadvantage of K-loaded Cu/SAPO-34 at high temperature, Fe/Beta catalysts were co-employed with K-loaded Cu/SAPO-34, and a wide active temperature window of SCR activity was obtained. Thus, our study reveals that a combined system comprising Fe/Beta and K-loaded Cu/SAPO-34 catalysts shows promise for the elimination of NOx in real-world applications.  相似文献   

5.
•CeOx/GF-EP process had the better degradation efficiency than GF-EP process. •CeOx/GF-EP process had the flexible application in the pH range from 5.0 to 9.0. •CeOx could enhance surface hydrophilicity and reduce the charge-transfer resistance. •The interfacial electron transfer process was revealed. E-peroxone (EP) was one of the most attractive AOPs for removing refractory organic compounds from water, but the high energy consumption for in situ generating H2O2 and its low reaction efficiency for activating O3 under acidic conditions made the obstacles for its practical application. In this study, cerium oxide was loaded on the surface of graphite felt (GF) by the hydrothermal method to construct the efficient electrode (CeOx/GF) for mineralizing carbamazepine (CBZ) via EP process. CeOx/GF was an efficient cathode, which led to 69.4% TOC removal in CeOx/GF-EP process with current intensity of 10 mA in 60 min. Moreover, CeOx/GF had the flexible application in the pH range from 5.0 to 9.0, TOC removal had no obvious decline with decrease of pH. Comparative characterizations showed that CeOx could enhance surface hydrophilicity and reduce the charge-transfer resistance of GF. About 5.4 mg/L H2O2 generated in CeOx/GF-EP process, which was 2.1 times as that in GF-EP process. The greater ozone utility was also found in CeOx/GF-EP process. More O3 was activated into hydroxyl radicals, which accounted for the mineralization of CBZ. An interfacial electron transfer process was revealed, which involved the function of oxygen vacancies and Ce3+/Ce4+ redox cycle. CeOx/GF had the good recycling property in fifth times’ use.  相似文献   

6.
• 90% total COD, 95.3% inert COD and 97.2% UV254 were removed. • High R2 values (over 95%) for all responses were obtained with CCD. • Operational cost was calculated to be 0.238 €/g CODremoved for total COD removal. • Fenton oxidation was highly-efficient method for inert COD removal. • BOD5/COD ratio of leachate concentrate raised from 0.04 to 0.4. The primary aim of this study is inert COD removal from leachate nanofiltration concentrate because of its high concentration of resistant organic pollutants. Within this framework, this study focuses on the treatability of leachate nanofiltration concentrate through Fenton oxidation and optimization of process parameters to reach the maximum pollutant removal by using response surface methodology (RSM). Initial pH, Fe2+ concentration, H2O2/Fe2+ molar ratio and oxidation time are selected as the independent variables, whereas total COD, color, inert COD and UV254 removal are selected as the responses. According to the ANOVA results, the R2 values of all responses are found to be over 95%. Under the optimum conditions determined by the model (pH: 3.99, Fe2+: 150 mmol/L, H2O2/Fe2+: 3.27 and oxidation time: 84.8 min), the maximum COD removal efficiency is determined as 91.4% by the model. The color, inert COD and UV254 removal efficiencies are determined to be 99.9%, 97.2% and 99.5%, respectively, by the model, whereas the total COD, color, inert COD and UV254 removal efficiencies are found respectively to be 90%, 96.5%, 95.3% and 97.2%, experimentally under the optimum operating conditions. The Fenton process improves the biodegradability of the leachate NF concentrate, increasing the BOD5/COD ratio from the value of 0.04 to the value of 0.4. The operational cost of the process is calculated to be 0.238 €/g CODremoved. The results indicate that the Fenton oxidation process is an efficient and economical technology in improvement of the biological degradability of leachate nanofiltration concentrate and in removal of resistant organic pollutants.  相似文献   

7.
• 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   

8.
• An in situ electron-induced deNOx process with CNT activated by DBD was achieved. • Carbon atoms on CNT surface were verified to be excited by plasma in DBD-CNT system. • Reactions between NOx and excited C result in synergistic effect of DBD-CNT system. In this study, a new in situ electron-induced process is presented with carbon nanotubes (CNTs) as a reduction agent activated by dielectric barrier discharge (DBD) for nitrogen oxide (NOx) abatement at low temperature (<407 K). Compared with a single DBD system and a DBD system with activated carbon (DBD-AC), a DBD system with carbon nanotubes (DBD-CNT) showed a significant promotion of NOx removal efficiency and N2 selectivity. Although the O2 content was 10%, the NOx conversion and N2 selectivity in the DBD-CNT system still reached 64.9% and 81.9% at a specific input energy (SIE) of 1424 J/L, and these values decreased to 16.8%, 31.9% and 43.2%, 62.3% in the single DBD system and the DBD-AC system, respectively. X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM) were utilized to investigate surface changes in the CNTs after activation by DBD to explore the NOx reduction abatement mechanism of this new process. Furthermore, the outlet gas components were also observed via Fourier transform infrared spectroscopy (FTIR) to help reveal the NOx reduction mechanism. Experimental results verified that carbon atoms excited by DBD and the structure of CNTs contributed to the synergistic activity of the DBD-CNT system. The new deNOx process was accomplished through in situ heterogenetic reduction reactions between the NOx and carbon atoms activated by the plasma on the CNTs. In addition, further results indicated that the new deNOx process exhibited acceptable SO2 tolerance and water resistance.  相似文献   

9.
• 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   

10.
• 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   

11.
• ORP value from −278.71 to −379.80 mV showed indiscernible effects on methane yield. • Fe(II) and Fe(III) promoted more degradation of proteins and amino acids than Fe0. • The highest enrichment of Geobacter was noted in samples added with Fe0. • Cysteine was accumulated during iron enhanced anaerobic sludge digestion. • Both iron content and valence were important for methane production. This study compared effects of three different valent iron (Fe0, Fe(II) and Fe(III)) on enhanced anaerobic sludge digestion, focusing on the changes of oxidation reduction potential (ORP), dissolved organic nitrogen (DON), and microbial community. Under the same iron dose in range of 0−160 mg/L after an incubation period of 30 days (d), the maximum methane production rate of sludge samples dosed with respective Fe0, Fe(II) and Fe(III) at the same concentration showed indiscernible differences at each iron dose, regardless of the different iron valence. Moreover, their behavior in changes of ORP, DON and microbial community was different: (1) the addition of Fe0 made the ORP of sludge more negative, and the addition of Fe(II) and Fe(III) made the ORP of sludge less negative. However, whether being more or less negative, the changes of ORP may show unobservable effects on methane yield when it ranged from −278.71 to −379.80 mV; (2) the degradation of dissolved organic nitrogen, particularly proteins, was less efficient in sludge samples dosed with Fe0 compared with those dosed with Fe(II) and Fe(III) after an incubation period of 30 d. At the same dose of 160 mg/L iron, more cysteine was noted in sludge samples dosed with Fe(II) (30.74 mg/L) and Fe(III) (27.92 mg/L) compared with that dosed with Fe0 (21.75 mg/L); (3) Fe0 particularly promoted the enrichment of Geobacter, and it was 6 times higher than those in sludge samples dosed with Fe(II) and Fe(III) at the same dose of 160 mg/L iron.  相似文献   

12.
• A new pulsed switching peroxi-coagulation (PSPC) system was developed. • The ECT for 2,4-D removal in the PSPC was lower than that in the EF. • The iron consumption for 2,4-D removal in the PSPC was lower than that in the PC. The aim of this study was to develop a new pulsed switching peroxi-coagulation system to control hydroxyl radical (?OH) production and to enhance 2,4-Dichlorophenoxyacetic acid (2,4-D) degradation. The system was constructed with a sacrifice iron anode, a Pt anode, and a gas diffusion cathode. Production of H2O2 and Fe2+ was controlled separately by time delayers with different pulsed switching frequencies. Under current densities of 5.0 mA/cm2 (H2O2) and 0.5 mA/cm2 (Fe2+), the ?OH production was optimized with the pulsed switching frequency of 1.0 s (H2O2):0.3 s (Fe2+) and the ratio of H2O2 to Fe2+ molar concentrations of 6.6. Under the optimal condition, 2,4-D with an initial concentration of 500 mg/L was completely removed in the system within 240 min. The energy consumption for the 2,4-D removal in the system was much lower than that in the electro-Fenton process (68±6 vs. 136±10 kWh/kg TOC). The iron consumption in the system was ~20 times as low as that in the peroxi-coagulation process (196±20 vs. 3940±400 mg/L) within 240 min. The system should be a promising peroxi-coagulation method for organic pollutants removal in wastewater.  相似文献   

13.
• AOA and comammox bacteria can be more abundant and active than AOB/NOB at WWTPs. • Coupled DNRA/anammox and NOx-DAMO/anammox/comammox processes are demonstrated. • Substrate level, SRT and stressors determine the niches of overlooked microbes. • Applications of overlooked microbes in enhancing nitrogen removal are promising. Nitrogen-cycling microorganisms play key roles at the intersection of microbiology and wastewater engineering. In addition to the well-studied ammonia oxidizing bacteria, nitrite oxidizing bacteria, heterotrophic denitrifiers, and anammox bacteria, there are some other N-cycling microorganisms that are less abundant but functionally important in wastewater nitrogen removal. These microbes include, but not limited to ammonia oxidizing archaea (AOA), complete ammonia oxidation (comammox) bacteria, dissimilatory nitrate reduction to ammonia (DNRA) bacteria, and nitrate/nitrite-dependent anaerobic methane oxidizing (NOx-DAMO) microorganisms. In the past decade, the development of high-throughput molecular technologies has enabled the detection, quantification, and characterization of these minor populations. The aim of this review is therefore to synthesize the current knowledge on the distribution, ecological niche, and kinetic properties of these “overlooked” N-cycling microbes at wastewater treatment plants. Their potential applications in novel wastewater nitrogen removal processes are also discussed. A comprehensive understanding of these overlooked N-cycling microbes from microbiology, ecology, and engineering perspectives will facilitate the design and operation of more efficient and sustainable biological nitrogen removal processes.  相似文献   

14.
• Nano CaO2 is evaluated as a remediation agent for 2,4-DCP contaminated groundwater. • 2,4-DCP degradation mechanism by different Fe2+ concentration was proposed. • 2,4-DCP was not degraded in the system for solution pH>10. • The 2,4-DCP degradation area is inconsistent with the nano CaO2 distribution area. This study evaluates the applicability of nano-sized calcium peroxide (CaO2) as a source of H2O2 to remediate 2,4-dichlorophenol (2,4-DCP) contaminated groundwater via the advanced oxidation process (AOP). First, the effect and mechanism of 2,4-DCP degradation by CaO2 at different Fe concentrations were studied (Fenton reaction). We found that at high Fe concentrations, 2,4-DCP almost completely degrades via primarily the oxidation of •OH within 5 h. At low Fe concentrations, the degradation rate of 2,4-DCP decreased rapidly. The main mechanism was the combined action of •OH and O2•−. Without Fe, the 2,4-DCP degradation reached 13.6% in 213 h, primarily via the heterogeneous reaction on the surface of CaO2. Besides, 2,4-DCP degradation was significantly affected by solution pH. When the solution pH was>10, the degradation was almost completely inhibited. Thus, we adopted a two-dimensional water tank experiment to study the remediation efficiency CaO2 on the water sample. We noticed that the degradation took place mainly in regions of pH<10 (i.e., CaO2 distribution area), both upstream and downstream of the tank. After 28 days of treatment, the average 2,4-DCP degradation level was ≈36.5%. Given the inadequacy of the results, we recommend that groundwater remediation using nano CaO2: (1) a buffer solution should be added to retard the rapid increase in pH, and (2) the nano CaO2 should be injected copiously in batches to reduce CaO2 deposition.  相似文献   

15.
• Bi doping in TiO2 enhanced the separation of photo-generated electron-hole. • The performance of photocatalytic degradation of MC-LR was improved. • Coexisting substances have no influence on algal removal performance. • The key reactive oxygen species were h+ and OH in the photocatalytic process. The increase in occurrence and severity of cyanobacteria blooms is causing increasing concern; moreover, human and animal health is affected by the toxic effects of Microcystin-LR released into the water. In this paper, a floating photocatalyst for the photocatalytic inactivation of the harmful algae Microcystis aeruginosa (M. aeruginosa) was prepared using a simple sol-gel method, i.e., coating g-C3N4 coupled with Bi-doped TiO2 on Al2O3-modified expanded perlite (CBTA for short). The impact of different molar ratios of Bi/Ti on CBTA was considered. The results indicated that Bi doping in TiO2 inhibited photogenerated electron-hole pair recombination. With 6 h of visible light illumination, 75.9% of M. aeruginosa (initial concentration= 2.7 × 106 cells/L) and 83.7% of Microcystin-LR (initial concentration= 100 μg/L) could be removed with the addition of 2 g/L CBTA-1% (i.e., Bi/Ti molar ratio= 1%). The key reactive oxygen species (ROSs) in the photocatalytic inactivation process are h+ and OH. The induction of the Bi4+/Bi3+ species by the incorporation of Bi could narrow the bandgap of TiO2, trap electrons, and enhance the stability of CBTA-1% in the solutions with coexisting environmental substances.  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.
• Orange tree residuals biochar had a better ability to adsorb ammonia. • Modified tea tree residuals biochar had a stronger ability to remove phosphorus. • Partially-modified biochar could remove ammonia and phosphorus at the same time. • The real runoff experiment showed an ammonia nitrogen removal rate of about 80%. • The removal rate of total phosphorus in real runoff experiment was about 95%. Adsorption of biochars (BC) produced from cash crop residuals is an economical and practical technology for removing nutrients from agricultural runoff. In this study, BC made of orange tree trunks and tea tree twigs from the Laoguanhe Basin were produced and modified by aluminum chloride (Al-modified) and ferric sulfate solutions (Fe-modified) under various pyrolysis temperatures (200°C–600°C) and residence times (2–5 h). All produced and modified BC were further analyzed for their abilities to adsorb ammonia and phosphorus with initial concentrations of 10–40 mg/L and 4–12 mg/L, respectively. Fe-modified Tea Tree BC 2h/400°C showed the highest phosphorus adsorption capacity of 0.56 mg/g. Al-modified Orange Tree BC 3h/500°C showed the best performance for ammonia removal with an adsorption capacity of 1.72 mg/g. FTIR characterization showed that P = O bonds were formed after the adsorption of phosphorus by modified BC, N-H bonds were formed after ammonia adsorption. XPS analysis revealed that the key process of ammonia adsorption was the ion exchange between K+ and NH4+. Phosphorus adsorption was related to oxidation and interaction between PO43– and Fe3+. According to XRD results, ammonia was found in the form of potassium amide, while phosphorus was found in the form of iron hydrogen phosphates. The sorption isotherms showed that the Freundlich equation fits better for phosphorus adsorption, while the Langmuir equation fits better for ammonia adsorption. The simulated runoff infiltration experiment showed that 97.3% of ammonia was removed by Al-modified Orange tree BC 3h/500°C, and 92.9% of phosphorus was removed by Fe-modified Tea tree BC 2h/400°C.  相似文献   

18.
• The Large scale Urban Consumption of energY model was updated and coupled with WRF. • Anthropogenic heat emissions altered the precipitation and its spatial distribution. • A reasonable AHE scheme could improve the performance of simulated PM2.5. • AHE aggravated the O3 pollution in urban areas. Anthropogenic heat emissions (AHE) play an important role in modulating the atmospheric thermodynamic and kinetic properties within the urban planetary boundary layer, particularly in densely populated megacities like Beijing. In this study, we estimate the AHE by using a Large-scale Urban Consumption of energY (LUCY) model and further couple LUCY with a high-resolution regional chemical transport model to evaluate the impact of AHE on atmospheric environment in Beijing. In areas with high AHE, the 2-m temperature (T2) increased to varying degrees and showed distinct diurnal and seasonal variations with maxima in night and winter. The increase in 10-m wind speed (WS10) and planetary boundary layer height (PBLH) exhibited slight diurnal variations but showed significant seasonal variations. Further, the systematic continuous precipitation increased by 2.1 mm due to the increase in PBLH and water vapor in upper air. In contrast, the precipitation in local thermal convective showers increased little because of the limited water vapor. Meanwhile, the PM2.5 reduced in areas with high AHE because of the increase in WS10 and PBLH and continued to reduce as the pollution levels increased. In contrast, in areas where prevailing wind direction was opposite to that of thermal circulation caused by AHE, the WS10 reduced, leading to increased PM2.5. The changes of PM2.5 illustrated that a reasonable AHE scheme might be an effective means to improve the performance of PM2.5 simulation. Besides, high AHE aggravated the O3 pollution in urban areas due to the reduction in NOx.  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.
• 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   

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