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1.
● Systematic information of recent progress in photocatalytic NO x removal is provided. ● The photocatalysts with special morphologies are reviewed and discussed. ● The morphology and photocatalytic NO x removal performance is related. The significant increase of NOx concentration causes severe damages to environment and human health. Light-driven photocatalytic technique affords an ideal solution for the removal of NOx at ambient conditions. To enhance the performance of NOx removal, 1D, 2D and 3D photocatalysts have been constructed as the light absorption and the separation of charge carriers can be manipulated through controlling the morphology of the photocatalyst. Related works mainly focused on the construction and modification of special morphologic photocatalyst, including element doping, heterostructure constructing, crystal facet exposing, defect sites introducing and so on. Moreover, the excellent performance of the photocatalytic NOx removal creates great awareness of the application, which has promising practical applications in NOx removal by paint (removing NOx indoor and outdoor) and pavement (degrading vehicle exhausts). For these considerations, recent advances in special morphologic photocatalysts for NOx removal was summarized and commented in this review. The purpose is to provide insights into understanding the relationship between morphology and photocatalytic performance, meanwhile, to promote the application of photocatalytic technology in NOx degradation.  相似文献   

2.
● Converting xylose to caproate under a low temperature of 20 °C by MCF was verified. ● Final concentration of caproate from xylose in a batch reactor reached 1.6 g/L. ● Changing the substrate to ethanol did not notably increase the caproate production. ● Four genera, including Bifidobacterium , were revealed as caproate producers. ● The FAB pathway and incomplete RBO pathway were revealed via metagenomic analysis. Mixed culture fermentation (MCF) is challenged by the unqualified activity of enriched bacteria and unwanted methane dissolution under low temperatures. In this work, caproate production from xylose was investigated by MCF at a low temperature (20 °C). The results showed that a 9 d long hydraulic retention time (HRT) in a continuously stirred tank reactor was necessary for caproate production (~0.3 g/L, equal to 0.6 g COD/L) from xylose (10 g/L). The caproate concentration in the batch mode was further increased to 1.6 g/L. However, changing the substrate to ethanol did not promote caproate production, resulting in ~1.0 g/L after 45 d of operation. Four genera, Bifidobacterium, Caproiciproducens, Actinomyces, and Clostridium_sensu_stricto_12, were identified as the enriched caproate-producing bacteria. The enzymes in the fatty acid biosynthesis (FAB) pathway for caproate production were identified via metagenomic analysis. The enzymes for the conversion of (Cn+2)-2,3-Dehydroxyacyl-CoA to (Cn+2)-Acyl-CoA (i.e., EC 1.3.1.8 and EC 1.3.1.38) in the reverse β-oxidation (RBO) pathway were not identified. These results could extend the understanding of low-temperature caproate production.  相似文献   

3.
● Efficient carbon methanation and nitrogen removal was achieved in AnMBR-PN/A system. ● AOB outcompeted NOB in PN section by limiting aeration and shortening SRT. ● The moderate residual organic matter of PN section triggered PD in anammox unit. ● AnAOB located at the bottom of UASB played an important role in nitrogen removal. An AnMBR-PN/A system was developed for mainstream sewage treatment. To verify the efficient methanation and subsequent chemolitrophic nitrogen removal, a long-term experiment and analysis of microbial activity were carried out. AnMBR performance was less affected by the change of hydraulic retention time (HRT), which could provide a stable influent for subsequent PN/A units. The COD removal efficiency of AnMBR was > 93% during the experiment, 85.5% of COD could be recovered in form of CH4. With the HRT of PN/A being shortened from 10 to 6 h, nitrogen removal efficiency (NRE) of PN/A increased from 60.5% to 80.4%, but decreased to 68.8% when the HRTPN/A further decreased to 4 h. Microbial analysis revealed that the highest specific ammonia oxidation activity (SAOA) and the ratio of SAOA to specific nitrate oxidation activity (SNOA) provide stable NO2-N/NH4+-N for anammox, and anammox bacteria (mainly identified as Candidatus Brocadia) enriched at the bottom of Anammox-UASB might play an important role in nitrogen removal. In addition, the decrease of COD in Anammox-UASB indicated partial denitrification occurred, which jointly promoted nitrogen removal with anammox.  相似文献   

4.
● Recent advances in the photolysis of nitrate/HNO3 are reviewed. ● Mechanisms and key factors affecting the photolysis of nitrate/HNO3 are summarized. ● Atmospheric implications and future research recommendations are provided. Nitrate is an important component of atmospheric particulate matter and affects air quality, climate, human health, and the ecosystem. Nitrate was previously considered a permanent sink for nitrogen oxides (NOx). However, this viewpoint has been challenged in recent years because growing research evidence has shown the transformation of nitrate into NOx (i.e., renoxification). The photolysis of nitrate/HNO3, especially in the particulate phase or adsorbed on particles, can be a significant renoxification process in the atmosphere. The formation and photolysis of nitrate in aerosol not only change the diurnal variation of NOx, but also provide long-distance transport of NOx in the form of nitrate, which affects local and regional atmospheric chemistry and air quality. This review summarizes recent advances in the fundamental understanding of the photolysis of nitrate/HNO3 under various atmospheric conditions, with a focus on mechanisms and key factors affecting the process. The atmospheric implications are discussed and future research is recommended.  相似文献   

5.
● SMX promotes hydrogen production from dark anaerobic sludge fermentation. ● SMX significantly enhances the hydrolysis and acidification processes. ● SMX suppresses the methanogenesis process in order to reduce hydrogen consumption. ● SMX enhances the relative abundance of hydrogen-VFAs producers. ● SMX brings possible environmental risks due to the enrichment of ARGs. The impact of antibiotics on the environmental protection and sludge treatment fields has been widely studied. The recovery of hydrogen from waste activated sludge (WAS) has become an issue of great interest. Nevertheless, few studies have focused on the impact of antibiotics present in WAS on hydrogen production during dark anaerobic fermentation. To explore the mechanisms, sulfamethoxazole (SMX) was chosen as a representative antibiotic to evaluate how SMX influenced hydrogen production during dark anaerobic fermentation of WAS. The results demonstrated SMX promoted hydrogen production. With increasing additions of SMX from 0 to 500 mg/kg TSS, the cumulative hydrogen production elevated from 8.07 ± 0.37 to 11.89 ± 0.19 mL/g VSS. A modified Gompertz model further verified that both the maximum potential of hydrogen production (Pm) and the maximum rate of hydrogen production (Rm) were promoted. SMX did not affected sludge solubilization, but promoted hydrolysis and acidification processes to produce more hydrogen. Moreover, the methanogenesis process was inhibited so that hydrogen consumption was reduced. Microbial community analysis further demonstrated that the introduction of SMX improved the abundance of hydrolysis bacteria and hydrogen-volatile fatty acids (VFAs) producers. SMX synergistically influenced hydrolysis, acidification and acetogenesis to facilitate the hydrogen production.  相似文献   

6.
● TiO2/ZSM-11 was prepared by a facile solid state dispersion method. ● Mechanism for photocatalytic degradation of dyes was investigated. ● Both experimental and MD simulations were conducted. ● Chemisorption instead of electrostatic interaction played a critical role. Photocatalytic degradation is a promising way to eliminate dye contaminants. In this work, a series of TiO2/ZSM-11 (TZ) nanocomposites were prepared using a facile solid state dispersion method. Methyl orange (MO), methylene blue (MB), and rhodamine B (RhB) were intentionally chosen as target substrates in the photocatalytic degradation reactions. Compared to pristine TiO2, negative effect was observed on MO degradation while promoted kinetics were collected on MB and RhB over TZ composites. Moreover, a much higher photocatalytic rate was interestingly achieved on RhB than MB, which indicated that a new factor has to be included other than the widely accepted electrostatic interaction mechanism to fully understand the selective photodegradation reactions. Systematic characterizations showed that TiO2 and ZSM-11 physically mixed and maintained both the whole framework and local structure without chemical interaction. The different trends observed in surface area and the photo-absorption ability of TZ composites with reaction performance further excluded both as the promotion mechanism. Instead, adsorption energies predicted by molecular dynamics simulations suggested that differences in the adsorption strength played a critical role. This work provided a deep mechanistic understanding of the selective photocatalytic degradation of dyes reactions, which helps to rationally design highly efficient photocatalysts.  相似文献   

7.
● Properties and performance relationship of CSBT photocatalyst were investigated. ● Properties of CSBT were controlled by simply manipulating glycerol content. ● Performance was linked to semiconducting and physicochemical properties. ● CSBT (W:G ratio 9:1) had better performance with lower energy consumption. ● Phenols were reduced by 48.30% at a cost of $2.4127 per unit volume of effluent. Understanding the relationship between the properties and performance of black titanium dioxide with core-shell structure (CSBT) for environmental remediation is crucial for improving its prospects in practical applications. In this study, CSBT was synthesized using a glycerol-assisted sol-gel approach. The effect of different water-to-glycerol ratios (W:G = 1:0, 9:1, 2:1, and 1:1) on the semiconducting and physicochemical properties of CSBT was investigated. The effectiveness of CSBT in removing phenolic compounds (PHCs) from real agro-industrial wastewater was studied. The CSBT synthesized with a W:G ratio of 9:1 has optimized properties for enhanced removal of PHCs. It has a distinct core-shell structure and an appropriate amount of Ti3+ cations (11.18%), which play a crucial role in enhancing the performance of CSBT. When exposed to visible light, the CSBT performed better: 48.30% of PHCs were removed after 180 min, compared to only 21.95% for TiO2 without core-shell structure. The CSBT consumed only 45.5235 kWh/m3 of electrical energy per order of magnitude and cost $2.4127 per unit volume of treated agro-industrial wastewater. Under the conditions tested, the CSBT demonstrated exceptional stability and reusability. The CSBT showed promising results in the treatment of phenols-containing agro-industrial wastewater.  相似文献   

8.
● Haze formation in China is highly correlated with iron and steel industry. ● VOCs generated in sinter process were neglected under current emission standard. ● Co-elimination removal of sinter flue gas complex pollutants are timely needed. Recent years have witnessed significant improvement in China’s air quality. Strict environmental protection measures have led to significant decreases in sulfur dioxide (SO2), nitrogen oxides (NOx), and particulate matter (PM) emissions since 2013. But there is no denying that the air quality in 135 cities is inferior to reaching the Ambient Air Quality Standards (GB 30952012) in 2020. In terms of temporal, geographic, and historical aspects, we have analyzed the potential connections between China’s air quality and the iron and steel industry. The non-target volatile organic compounds (VOCs) emissions from iron and steel industry, especially from the iron ore sinter process, may be an underappreciated index imposing a negative effect on the surrounding areas of China. Therefore, we appeal the authorities to pay more attention on VOCs emission from the iron and steel industry and establish new environmental standards. And different iron steel flue gas pollutants will be eliminated concurrently with the promotion and application of new technology.  相似文献   

9.
p- CNB and IBP were selected, to explore factors determining ozonation outcomes. ● •OH contributed only 50 % to IBP removal, compared to the 90 % for p -CNB removal. ● IBP achieved fewer TOC removal and more by-product types and quantities. ● A longer ring-opening distance existed during the degradation of IBP. ● Multiple positions on both branches of IBP were attacked, consuming more oxidants. For aromatic monomer compounds (AMCs), ozonation outcomes were usually predicted by the substituents of the benzene ring based on the electron inductive effect. However, the predicted results were occasionally unreliable for complex substituents, and other factors caused concern. In this study, p-chloronitrobenzene (p-CNB) and ibuprofen (IBP) were selected for ozonation. According to the electron inductive theory, p-CNB should be less oxidizable, but the opposite was true. The higher rates of p-CNB were due to various sources of assistance. First, the hydroxyl radical (•OH) contributed 90 % to p-CNB removal at pH 7.0, while its contribution to IBP removal was 50 %. Other contributions came from molecular O3 oxidation. Second, p-CNB achieved 40 % of the total organic carbon (TOC) removal and fewer by-product types and quantities, when compared to the results for IBP. Third, the oxidation of p-CNB started with hydroxyl substitution reactions on the benzene ring; then, the ring opened. However, IBP was initially oxidized mainly on the butane branched chain, with a chain-shortening process occurring before the ring opened. Finally, the degradation pathway of p-CNB was single and consumed fewer oxidants. However, both branches of IBP were attacked simultaneously, and three degradation pathways that relied on more oxidants were proposed. All of these factors were determinants of the rapid removal of p-CNB.  相似文献   

10.
● B[a]P, nicotine and phenanthrene molecules altered the secondary structure of Aβ42. ● β-content of the peptide was significantly enhanced in the presence of the PAHs. ● Nicotine made stable cluster with Aβ42 peptide via hydrogen bonds. ● Phenanthrene due to its small size, interfered with the Aβ42 monomer more strongly. Recent studies have correlated the chronic impact of ambient environmental pollutants like polycyclic aromatic hydrocarbons (PAHs) with the progression of neurodegenerative disorders, either by using statistical data from various cities, or via tracking biomarkers during in-vivo experiments. Among different neurodegenerative disorders, PAHs are known to cause increased risk for Alzheimer’s disease, related to the development of amyloid beta (Aβ) peptide oligomers. However, the complex molecular interactions between peptide monomers and organic pollutants remains obscured. In this work, we performed an atomistic molecular dynamics study via GROMACS to investigate the structure of Aβ42 peptide monomer in the presence of benzo[a]pyrene, nicotine, and phenanthrene. Interestingly the results revealed strong hydrophobic, and hydrogen-bond based interactions between Aβ peptides and these environmental pollutants that resulted in the formation of stable intermolecular clusters. The strong interactions affected the secondary structure of the Aβ42 peptide in the presence of the organic pollutants, with almost 50 % decrease in the α-helix and 2 %–10 % increase in the β-sheets of the peptide. Overall, the undergoing changes in the secondary structure of the peptide monomer in the presence of the pollutants under the study indicates an enhanced formation of Aβ peptide oligomers, and consequent progression of Alzheimer’s disease.  相似文献   

11.
● Monthly hospitalization expenses are sensitive to increases in PM2.5 exposure. ● The increased PM2.5 causes patients with CHD and LRI to stay longer in the hospital. ● The impact of PM2.5 on total expenses for stroke is greater in southern China. ● Males may be more sensitive to air pollution than females. Air pollution has been a severe issue in China. Exposure to PM2.5 has adverse health effects and causes economic losses. This study investigated the economic impact of exposure to PM2.5 pollution using monthly city-level data covering 88.5 million urban employees in 2016 and 2017. This study mainly focused on three expenditure indicators to measure the economic impact considering lower respiratory infections (LRIs), coronary heart disease (CHD), and stroke. The results show that a 10 µg/m3 increase in PM2.5 would cause total monthly expenses of LRIs, CHD, and stroke to increase by 0.226%, 0.237%, and 0.374%, respectively. We also found that LRI, CHD, and stroke hospital admissions increased significantly by 10%, 8.42%, and 5.64%, respectively. Furthermore, the total hospital stays of LRIs, CHDs, and strokes increased by 2.49%, 2. 51%, and 1.64%, respectively. Our findings also suggest heterogeneous impacts of PM2.5 exposures by sex and across regions, but no statistical evidence shows significant differences between the older and younger adult subgroups. Our results provide several policy implications for reducing unequal public health expenditures in overpolluted countries.  相似文献   

12.
● A crosslinked polyaniline/carbon nanotube NF membrane was fabricated. ● Electro-assistance enhanced the removal rate of the NF membrane for bisphenol A. ● Intermittent voltage-assistance can achieve nearly 100% removal of bisphenol A. ● Membrane adsorption–electro-oxidation process is feasible for micropollutant removal. Nanofiltration (NF) has attracted increasing attention for wastewater treatment and potable water purification. However, the high-efficiency removal of micropollutants by NF membranes is a critical challenge. Owing to the adsorption and subsequent diffusion, some weakly charged or uncharged micropollutants, such as bisphenol A (BPA), can pass through NF membranes, resulting in low removal rates. Herein, an effective strategy is proposed to enhance the BPA removal efficiency of a crosslinked polyaniline/carbon nanotube NF membrane by coupling the membrane with electro-assistance. The membrane exhibited a 31.9% removal rate for 5 mg/L BPA with a permeance of 6.8 L/(m2·h·bar), while the removal rate was significantly improved to 98.1% after applying a voltage of 2.0 V to the membrane. Furthermore, when BPA coexisted with humic acid, the membrane maintained 94% removal of total organic carbon and nearly 100% removal of BPA at 2.0 V over the entire filtration period. Compared to continuous voltage applied to the membrane, an intermittent voltage (2.0 V for 0.5 h with an interval of 3.5 h) could achieve comparable BPA removal efficiency, because of the combined effect of membrane adsorption and subsequent electrochemical oxidation. Density functional theory calculations and BPA oxidation process analyses suggested that BPA was adsorbed by two main interactions: π–π and hydrogen-bond interactions. The adsorbed BPA was further electro-degraded into small organic acids or mineralized to CO2 and H2O. This work demonstrates that NF membranes coupled with electro-assistance are feasible for improving the removal of weakly charged or uncharged micropollutants.  相似文献   

13.
● EPS immobilizes U(VI) via adsorption, bioreduction and desorption. ● This work provides a framework to quantify the three immobilization processes. ● The non-equilibrium adsorption of U follows pseudo-second-order kinetics. ● The equilibrium adsorption of U followed Langmuir and Freundlich isotherms. Hexavalent uranium (U(VI)) can be immobilized by various microbes. The role of extracellular polymeric substances (EPS) in U(VI) immobilization has not been quantified. This work provides a model framework to quantify the contributions of three processes involved in EPS-mediated U(VI) immobilization: adsorption, bioreduction and desorption. Loosely associated EPS was extracted from a pure bacterial strain, Klebsiella sp. J1, and then exposed to H2 and O2 (no bioreduction control) to immobilize U(VI) in batch experiments. U(VI) immobilization was faster when exposed to H2 than O2 and stabilized at 94% for H2 and 85% for O2, respectively. The non-equilibrium data from the H2 experiments were best simulated by a kinetic model consisting of pseudo-second-order adsorption (ka = 2.87 × 10−3 g EPS·(mg U)−1·min−1), first-order bioreduction (kb = 0.112 min−1) and first-order desorption (kd = 7.00 × 10−3 min−1) and fitted the experimental data with R2 of 0.999. While adsorption was dominant in the first minute of the experiments with H2, bioreduction was dominant from the second minute to the 50th min. After 50 min, adsorption was negligible, and bioreduction was balanced by desorption. This work also provides the first set of equilibrium data for U(VI) adsorption by EPS alone. The equilibrium experiments with O2 were well simulated by both the Langmuir isotherm and the Freundlich isotherm, suggesting multiple mechanisms involved in the interactions between U(VI) and EPS. The thermodynamic study indicated that the adsorption of U(VI) onto EPS was endothermic, spontaneous and favorable at higher temperatures.  相似文献   

14.
● Increased DAAO offsets 3/4 of the decrease of DAAP in 2013–2020. ● DAAO increases are mainly due to O3 concentration increase and population aging. ● Health benefit from PM2.5 reduction after 2017 is larger than that before 2017. ● Reducing PM2.5 concentration by 1% results in 0.6% reduction of DAAP. ● Reducing O3 concentration by 1% results in 2% reduction of DAAO. PM2.5 concentration declined significantly nationwide, while O3 concentration increased in most regions in China in 2013–2020. Recent evidences proved that peak season O3 is related to increased death risk from non-accidental and respiratory diseases. Based on these new evidences, we estimate excess deaths associated with long-term exposure to ambient PM2.5 and O3 in China following the counterfactual analytic framework from Global Burden Disease. Excess deaths from non-accidental diseases associated with long-term exposure to ambient O3 in China reaches to 579 (95% confidential interval (CI): 93, 990) thousand in 2020, which has been significantly underestimated in previous studies. In addition, the increased excess deaths associated with long-term O3 exposure (234 (95% CI: 177, 282) thousand) in 2013–2020 offset three quarters of the avoided excess deaths (302 (95% CI: 244, 366) thousand) mainly due to PM2.5 exposure reduction. In key regions (the North China Plain, the Yangtze River Delta and the Fen-Wei Plain), the former is even larger than the latter, particularly in 2017–2020. Health benefit of PM2.5 concentration reduction offsets the adverse effects of population growth and aging on excess deaths attributed to PM2.5 exposure. Increase of excess deaths associated with O3 exposure is mainly due to the strong increase of O3 concentration, followed by population aging. Considering the faster population aging process in the future, collaborative control, and faster reduction of PM2.5 and O3 are needed to reduce the associated excess deaths.  相似文献   

15.
● Four Ca. Brocadia species were observed during the spontaneously enrichment. ● Novel anammox species SW510 and SW773 dominated the full-scale ecosystem. ● Urease and cyanase genes were detected in the new anammox genomes. ● Functional differentiation potentially facilitated co-occurrence of anammox species. The increasing application of anammox processes suggests their enormous potential for nitrogen removal in wastewater treatment facilities. However, the functional potentials and ecological differentiation of cooccurring anammox species in complex ecosystems have not been well elucidated. Herein, by utilizing functional reconstruction and comparative genome analysis, we deciphered the cooccurring mechanisms of four Candidatus Brocadia species that were spontaneously enriched in a full-scale swine wastewater treatment system. Phylogenetic analysis indicated that species SW172 and SW745 were closely related to Ca. Brocadia caroliniensis and Ca. Brocadia sapporoensis, respectively, whereas the dominant species SW510 and SW773, with a total average abundance of 34.1%, were classified as novel species of the genus Ca. Brocadia. Functional reconstruction revealed that the novel species SW510 can encode both cytochrome cd1-type nitrite reductase and hydroxylamine oxidase for nitrite reduction. In contrast, the detected respiratory pentaheme cytochrome c nitrite reductase and acetate kinase genes suggested that SW773 likely reduced nitrite to ammonium with acetate as a carbon source. Intriguingly, the presence of genes encoding urease and cyanase indicated that both novel species can use diverse organic nitrogen compounds in addition to ammonia and nitrite as substrates. Taken together, the recovery and comparative analysis of these anammox genomes expand our understanding of the functional differentiation and cooccurrence of the genus Ca. Brocadia in wastewater treatment systems.  相似文献   

16.
● The main direct seal up carbon options and challenges are reviewed. ● Ocean-based CO2 replacement for CH4/oil exploitation is presented. ● Scale-advantage of offshore CCS hub is discussed. Carbon capture and storage (CCS) technology is an imperative, strategic, and constitutive method to considerably reduce anthropogenic CO2 emissions and alleviate climate change issues. The ocean is the largest active carbon bank and an essential energy source on the Earth’s surface. Compared to oceanic nature-based carbon dioxide removal (CDR), carbon capture from point sources with ocean storage is more appropriate for solving short-term climate change problems. This review focuses on the recent state-of-the-art developments in offshore carbon storage. It first discusses the current status and development prospects of CCS, associated with the challenges and uncertainties of oceanic nature-based CDR. The second section outlines the mechanisms, sites, advantages, and ecologic hazards of direct offshore CO2 injection. The third section emphasizes the mechanisms, schemes, influencing factors, and recovery efficiency of ocean-based CO2-CH4 replacement and CO2-enhanced oil recovery are reviewed. In addition, this review discusses the economic aspects of offshore CCS and the preponderance of offshore CCS hubs. Finally, the upsides, limitations, and prospects for further investigation of offshore CO2 storage are presented.  相似文献   

17.
● pz-UiO-66 was synthesized facilely by a solvothermal method. ● Efficient capture of copper from highly acidic solution was achieved by pz-UiO-66. ● pz-UiO-66 exhibited excellent selectivity and capacity for copper capture. ● Pyrazine-N in pz-UiO-66 was shown to be the dominant adsorption site. The selective capture of copper from strongly acidic solutions is of vital importance from the perspective of sustainable development and environmental protection. Metal organic frameworks (MOFs) have attracted the interest of many scholars for adsorption due to their fascinating physicochemical characteristics, including adjustable structure, strong stability and porosity. Herein, pz-UiO-66 containing a pyrazine structure is successfully synthesized for the efficient separation of copper from strongly acidic conditions. Selective copper removal at low pH values is accomplished by using this material that is not available in previously reported metal–organic frameworks. Furthermore, the material exhibits excellent adsorption capacity, with a theoretical maximum copper uptake of 247 mg/g. As proven by XPS and FT-IR analysis, the coordination of pyrazine nitrogen atoms with copper ions is the dominant adsorption mechanism of copper by pz-UiO-66. This work provides an opportunity for efficient and selective copper removal under strongly acidic conditions, and promises extensive application prospects for the removal of copper in the treatment for acid metallurgical wastewater.  相似文献   

18.
● A series of Cu-ZSM-5 catalysts were tested for DMF selective catalytic oxidation. ● Cu-6 nm samples showed the best catalytic activity and N2 selectivity. ● Redox properties and chemisorbed oxygen impact on DMF catalytic oxidation. ● Isolated Cu2+ species and weak acidity have effects on the generation of N2. N, N-Dimethylformamide (DMF), a nitrogen-containing volatile organic compound (NVOC) with high emissions from the spray industry, has attracted increasing attention. In this study, Cu-ZSM-5 catalysts with different CuO particle sizes of 3, 6, 9 and 12 nm were synthesized and tested for DMF selective catalytic oxidation. The crystal structure and physicochemical properties of the catalyst were studied by various characterization methods. The catalytic activity increases with increasing CuO particle size, and complete conversion can be achieved at 300–350 °C. The Cu-12 nm catalyst has the highest catalytic activity and can achieve complete conversion at 300 °C. The Cu-6 nm sample has the highest N2 selectivity at lower temperatures, reaching 95% at 300 °C. The activity of the catalysts is determined by the surface CuO cluster species, the bulk CuO species and the chemisorbed surface oxygen species. The high N2 selectivity of the catalyst is attributed to the ratio of isolated Cu2+ and bulk CuO species, and weak acidity is beneficial to the formation of N2. The results in this work will provide a new design of NVOC catalytic oxidation catalysts.  相似文献   

19.
● A novel hybrid fuel cell (F-HFC) was fabricated. ● Pollutant degradation and synchronous electricity generation occurred in F-HFC. ● BiOCl-NH4PTA photocatalyst greatly improved electron transfer and charge separation. ● Pollutant could act as substrate directly in ambient conditions without pretreatment. ● The mechanism of the F-HFC was proposed and elucidated. The development of highly efficient energy conversion technologies to extract energy from wastewater is urgently needed, especially in facing of increasing energy and environment burdens. Here, we successfully fabricated a novel hybrid fuel cell with BiOCl-NH4PTA as photocatalyst. The polyoxometalate (NH4PTA) act as the acceptor of photoelectrons and could retard the recombination of photogenerated electrons and holes, which lead to superior photocatalytic degradation. By utilizing BiOCl-NH4PTA as photocatalysts and Pt/C air-cathode, we successfully constructed an electron and mass transfer enhanced photocatalytic hybrid fuel cell with flow-through field (F-HFC). In this novel fuel cell, dyes and biomass could be directly degraded and stable power output could be obtained. About 87 % of dyes could be degraded in 30 min irradiation and nearly 100 % removed within 90 min. The current density could reach up to ~267.1 μA/cm2; with maximum power density (Pmax) of ~16.2 μW/cm2 with Rhodamine B as organic pollutant in F-HFC. The power densities were 9.0 μW/cm2, 12.2 μW/cm2, and 13.9 μW/cm2 when using methyl orange (MO), glucose and starch as substrates, respectively. This hybrid fuel cell with BiOCl-NH4PTA composite fulfills the purpose of decontamination of aqueous organic pollutants and synchronous electricity generation. Moreover, the novel design cell with separated photodegradation unit and the electricity generation unit could bring potential practical application in water purification and energy recovery from wastewater.  相似文献   

20.
● Collaborative treatment of plastics and OS was established to improve oil quality. ● PE addition successfully improved OS pyrolysis process by deploying H/Ceff ratio. ● Higher H/Ceff ratio promoted cracking to obtain more gas and light oil fractions. ● The degradation of PE and OS was promoted each other under their temperature range. Pyrolysis is an effective method to treat oily sludge (OS) due to its balance between oil recovery and nonhazardous disposal. However, tank bottom OS contains a high content of heavy fractions, which creates obstacles for pyrolysis due to the high activation energy. The incomplete cracking of macromolecules and secondary polymerization decreases the oil quality and causes coking during the operation process. This study introduced polyethylene (PE) into OS to deploy the H/Ceff ratio of feedstocks for pyrolysis. A strong interaction between OS and PE during copyrolysis could be observed from the TG/DTG curves. PE tightly participated in OS degradation, while OS also promoted PE degradation at high temperature. Apparent pits were generated in solid residues from copyrolysis, which was attributed to the uniform and violent gas release. In addition to HCN, other nitrogenous and sulphurous pollutants were inhibited. Accordingly, more gas products were attained after PE addition with more value-added compositions of alkanes and alkenes. Although the oil yield decreased after PE addition, the oil products from copyrolysis possessed higher heating values and higher contents of light fractions with short chains as well as paraffins. Consequently, copyrolysis of OS and PE significantly improved the pyrolysis process and resulted in high oil quality.  相似文献   

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