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Sustainable ferrate oxidation: Reaction chemistry, mechanisms and removal of pollutants in wastewater
2021
Dar, Afzal Ahmed | Pan, Bao | Qin, Jiani | Zhu, Qiuhui | Lichtfouse, Eric | ʻUs̲mān, Muḥammad | Wang, Chuanyi
This review is intended to evaluate the use of ferrate (Fe(VI)), being a green coagulant, sustainable and reactive oxidant, to remove micro pollutants especially pharmaceutical pollutants in contaminated water. After a brief description of advanced oxidation processes, fundamental dimensions regarding the nature, reactivity, and chemistry of this oxidant are summarized. The degradation of contaminants by Fe(VI) involves several mechanisms and reactive agents which are critically evaluated. The efficiency and chemistry of Fe(VI) oxidation differs according to the reaction conditions and activation agent, such as soluble Fe(VI) processes, which involve Fe(VI), UV light, and electro-Fe(VI) oxidation. Fe(VI) application methods (including single dose, multiple doses, chitosan coating etc), and Fe(VI) with activating agents (including sulfite, thiosulfate, and UV) are also described to degrade the micro pollutants. Besides, application of Fe(VI) to remove pharmaceuticals in wastewater are intensely studied. Electrochemical prepared Fe(VI) has more wide application than wet oxidation method. Meanwhile, we elaborated Fe(VI) performance, limitations, and proposed innovative aspects to improve its stability, such as the generation of Fe(III), synergetic effects, nanopores entrapment, and nanopores capsules. This study provides conclusive direction for synergetic oxidative technique to degrade the micro pollutants.
Show more [+] Less [-]Soot particle morphology and nanostructure with oxygenated fuels: A comparative study into cold-start and hot-start operation
2021
Verma, Puneet | Jafari, Mohammad | Zare, Ali | Pickering, Edmund | Guo, Yi | Osuagwu, Chiemeriwo Godday | Stevanovic, Svetlana | Brown, Richard | Ristovski, Zoran
This study investigates the morphology and nanostructure of soot particles during cold-start and hot-start engine operation of a diesel engine using oxygenated fuels. The soot samples were analysed using transmission electron microscopy. The oxygen content in the fuel was varied between 0 and 12%. The results showed that the primary particles during cold-start have significantly smaller size when compared to hot-start engine operation. The addition of oxygenated fuels also resulted in smaller sized primary particles. Smaller radius of gyration and higher fractal dimension of soot aggregates during cold-start would mean smaller aggregate size with a more compact structure. Shorter fringes with a higher inter-fringe spacing for cold-start would mean lower graphitisation of soot particles that could be related to higher oxidation reactivity of soot particles.
Show more [+] Less [-]Characterization of allergenicity of Platanus pollen allergen a 3 (Pla a 3) after exposure to NO2 and O3
2021
Zhou, Shumin | Wang, Xingzi | Lu, Senlin | Yao, Chuanhe | Zhang, Luying | Rao, Lanfang | Liu, Xinchun | Zhang, Wei | Li, Shuijun | Wang, Weiqian | Wang, Qingyue
Pollen allergens, widely present in the atmosphere, are the main cause of seasonal respiratory diseases that affect millions of people worldwide. Although previous studies have reported that nitrogen dioxide (NO₂) and ozone (O₃) promote pollen allergy, the specific biological processes and underlying mechanisms remain less understood. In this study, Platanus pollen grains were exposed to gaseous pollutants (NO₂ and O₃). We employed environmental electron microscopy, flow cytometry, western blot assay, enzyme-linked immunoassay, ultraviolet absorption spectrometry, circular dichroism, and protein mass spectrometry to characterise the subpollen particles (SPPs) released from pollen grains. Furthermore, we determined the immunogenicity and pathogenicity induced by Platanus pollen allergen a 3 (Pla a 3). Our results demonstrated that NO₂ and O₃ could damage the pollen cell membranes in SPPs and increase the amount of Pla a 3 allergen released into the atmosphere. Additionally, NO₂ and O₃ altered the structure of Pla a3 protein through nitrification and oxidation, which not only enhanced the immunogenicity of allergens but also increased the stability of the protein. In vivo analysis using an animal model indicated that NO₂ and O₃ greatly aggravated pollen-induced pneumonia. Thus, our study provides guidance for the prevention of pollen allergic diseases.
Show more [+] Less [-]Atmospheric ammonia and its effect on PM2.5 pollution in urban Chengdu, Sichuan Basin, China
2021
Huang, Xiaojuan | Zhang, Junke | Zhang, Wei | Tang, Guiqian | Wang, Yuesi
Controlling ammonia (NH₃) emissions has been proposed as a strategy to mitigate haze pollution. To explore the role of NH₃ in haze pollution in Sichuan Basin, where agricultural activities are intense, hourly in situ data of NH₃, as well as nitric acid and secondary inorganic aerosols (SIAs) were gathered in Chengdu from April 2017 to March 2018. We found that NH₃ had an annual mean concentration of 9.7 ± 3.5 (mean ± standard deviation) μg m⁻³, and exhibited seasonal variations (spring > summer > autumn and winter) due to changes in emission sources and meteorological conditions (particularly temperature). Chengdu's atmosphere is generally NH₃-sufficient, especially in the warm seasons, implying that the formation of SIAs is more sensitive to the availability of nitric acid. However, an NH₃ “sufficient-to-deficient” transition was found to occur during winter pollution periods, and the frequency of NH₃ deficiency increased with the aggravation of pollution. Under NH₃-deficient conditions, the nitrogen oxidation ratio increased linearly with the increase in free NH₃, implying that NH₃ contributes appreciably to the formation of nitrate and thus to high PM₂.₅ loadings. No relationships of NH₃ with fossil fuel combustion–related pollutants were found. The NH₃ emissions from farmland and livestock waste in the suburbs of Chengdu and regional transport from west of Chengdu probably contribute to the occurrence of high PM₂.₅ loading in winter and spring, respectively. These results suggest that to achieve effective mitigation of PM₂.₅ in Chengdu, local and regional emission control of NH₃ and NOx synergistically would be effective.
Show more [+] Less [-]Tracing riverine sulfate source in an agricultural watershed: Constraints from stable isotopes
2021
Liu, Jinke | Han, Guilin
The sulfate pollution in water environment gains more and more concerns in recent years. The discharge of domestic, municipal, and industrial wastewaters increases the riverine sulfate concentrations, which may cause local health and ecological problems. To better understand the sources of sulfate, this study collected water samples in a typical agricultural watershed in East Thailand. The source apportionment of sulfide was conducted by using stable isotopes and receptor models. The δ³⁴SSO₄ value of river water varied from 1.2‰ to 16.4‰, with a median value of 8.9‰. The hydrochemical data indicated that the chemical compositions of Mun river water were affected by the anthropogenic inputs and natural processes such as halite dissolution, carbonate, and silicate weathering. The positive matrix factorization (PMF) model was not suitable to trace source of riverine sulfate, because the meaning of the extracted factors seems to be vague. Based on the elemental ratio and isotopic composition, the inverse model yielded the relative contribution of sulfide oxidation (approximately 46.5%), anthropogenic input (approximately 41.5%), and gypsum dissolution (approximately 12%) to sulfate in Mun river water. This study indicates that the selection of models for source apportionment should be careful. The large contribution of anthropogenic inputs calls an urgent concern of the Thai government to establish effective management strategies in the Mun River basin.
Show more [+] Less [-]Nitrogen emission and deposition budget in an agricultural catchment in subtropical central China
2021
Zhu, Xiao | Shen, Jianlin | Li, Yong | Liu, Xuejun | Xu, Wen | Zhou, Feng | Wang, Juan | Reis, Stefan | Wu, Jinshui
The study of emissions and depositions of atmospheric reactive nitrogen species (Nᵣs) in a region is important to uncover the sources and sinks of atmospheric Nᵣs in the region. In this study, atmospheric total Nᵣs depositions including both wet-only and dry deposition were monitored simultaneously across major land-use types in a 105 km² catchment called Jinjing River Catchment (JRC) in subtropical central China from 2015 to 2016. Based on activity data and emission factors for the main Nᵣs emission sources, ammonia (NH₃) and nitrogen oxides (NOₓ) emission inventories for the catchment were also compiled. The estimated total Nᵣs deposition in JRC was 35.9 kg N ha⁻¹ yr⁻¹, with approximately 49.7 % attributed to reduced compounds (NHₓ), and 40.5 % attributed to oxidized (NOy). The total Nᵣs emission rate in JRC was 80.4 kg N ha⁻¹ yr⁻¹, with 61.5 and 18.9 kg N ha⁻¹ yr⁻¹ from NH₃ and NOₓ emissions, respectively. Livestock excretion and fertilization were the two main contributing emission sources for NH₃, while vehicle sources contributed the bulk of NOₓ emissions. The net atmospheric budgets of Nᵣs in paddy field, forest, and tea field were +3.7, −36.1, and +23.8 kg N ha⁻¹ yr⁻¹, respectively. At the catchment scale, the net atmospheric budget of Nᵣs was +47.7 kg N ha⁻¹ yr⁻¹, with +43.7 kg N ha⁻¹ yr⁻¹ of NHₓ and +4.0 kg N ha⁻¹ yr⁻¹ of NOy, indicating that the subtropical catchment was net sources of atmospheric Nᵣs. Considering that excessive atmospheric Nᵣ emissions and deposition may cause adverse effects on the environment, effects should be conducted to mitigate the Nᵣs emissions from agriculture and transportation, and increasing the area of forest is good for reducing the net positive budget of atmospheric Nᵣs in the subtropical catchments in China.
Show more [+] Less [-]Contaminated soils of different natural pH and industrial origin: The role of (nano) iron- and manganese-based amendments in As, Sb, Pb, and Zn leachability
2021
Hiller, Edgar | Jurkovič, Ľubomír | Faragó, Tomáš | Vítková, Martina | Tóth, Roman | Komárek, Michael
Soils containing a large proportion of industrial waste can pose a health risk due to high environmentally available concentrations of toxic metal(loid)s. Nano zero-valent iron (nZVI) and amorphous manganese oxide (AMO) were applied as immobilising amendments (1 wt%) to soils with different industrial origin of As and Sb, and leaching of As, Sb, Pb, and Zn was investigated using a single extraction with deionised water. The different industrial impact was reflected in the mineralogy, chemical composition and pH of these soils. Water-soluble As ratios positively correlated with pH in all experimental treatments. A significant decrease of water-soluble As ratios was observed in all nZVI-amended soils (~65–93% of the control) except for one sample with the lowest solution pH. Nano zero-valent iron was also successful in Sb immobilisation (~76–90% of the control). Highly variable results were obtained for AMO, which only led to a decrease of water-soluble As in soils with solution pH of ≥7 (~70–80% of the control), probably due to lower stability of AMO in acidic conditions. In each case, nZVI was more efficient at decreasing water-soluble As ratios than AMO. Dissolved Pb concentrations remained unchanged after the application of nZVI and AMO, and the decrease of Zn leaching using AMO was controlled mainly by soil pH increase induced by its application. According to the calculated saturation indices, tripuhyite (FeSbO₄) was predicted to be the key mineral controlling Sb solubility in mine soils. Secondary Fe (hydr)oxides either originally present or newly formed due to nZVI oxidation were instrumentally identified at different stages of their transformation and metal(loid) retention. To conclude, nZVI is suitable for application to contaminated soils at a wide pH range, while the use of AMO for decreasing As leaching is limited to soils with pH ≥ 7.
Show more [+] Less [-]Yeast biomass-induced Co2P/biochar composite for sulfonamide antibiotics degradation through peroxymonosulfate activation
2021
Peng, Yuanyuan | Tong, Wenhua | Xie, Yi | Hu, Wanrong | Li, Yonghong | Zhang, Yongkui | Wang, Yabo
Advanced oxidation processes (AOPs) based on peroxymonosulfate (PMS) activation have attracted increasing attention in recent years for organic pollutants removal. Herein, we put forward a facile method to form cobalt phosphide/carbon composite for PMS activation. Combining impregnation approach with pyrolysis treatment enabled the formation of Co₂P/biochar composites using baker’s yeast and Co²⁺ as precursors. The as-synthesized products exhibited excellent catalytic activity for sulfamethoxazole (SMX) degradation over the pH range 3.0–9.0 b y activating PMS. For example, 100% of SMX (20 mg L⁻¹) removal was achieved in 20 min with catalyst dosage of 0.4 g L⁻¹ and PMS loading of 0.4 g L⁻¹. Near zero Co²⁺ leaching was observed during catalytic reaction, which remarkably lowered the toxic risk of transition metal ion in water. Meanwhile, the reusability of catalyst could be attained by thermal treatment. SMX degradation intermediates were identified by liquid chromatography-mass spectrometry (LC-MS), which facilitated the proposal of possible SMX degradation pathways. Ecological Structure Activity Relationships (ECOSAR) analysis indicated that SMX degradation intermediates may not pose ecological toxicity to the environment. Further investigation verified that Co₂P/biochar composites could set off PMS activation not only for the degradation of SMX but also for other sulfonamides. In this study, we not only developed a facile method of utilizing environmental-benign biomass for transition metal phosphide/carbon composite formation, but also achieved highly efficient antibiotic elimination by PMS-based AOP.
Show more [+] Less [-]Mechanism of As(III) removal properties of biochar-supported molybdenum-disulfide/iron-oxide system
2021
Khan, Zulqarnain Haider | Gao, Minling | Wu, Jingjie | Bi, Ran | Mehmood, Ch Tahir | Song, Zhengguo
Sulfate (SO₄•⁻) and hydroxyl-based (HO•) radical are considered potential agents for As(III) removal from aquatic environments. We have reported the synergistic role of SO₄•⁻ and HO• radicals for As(III) removal via facile synthesis of biochar-supported SO₄•⁻ species. MoS₂−modified biochar (MoS₂/BC), iron oxide-biochar (FeOₓ@BC), and MoS₂−modified iron oxide-biochar (MoS₂/FeOₓ@BC) were prepared and systematically characterized to understand the underlying mechanism for arsenic removal. The MoS₂/FeOx@BC displayed much higher As(III) adsorption (27 mg/g) compared to MoS₂/BC (7 mg/g) and FeOx@BC (12 mg/g). Effects of kinetics, As(III) concentration, temperature, and pH were also investigated. The adsorption of As(III) by MoS₂/FeOx@BC followed the Freundlich adsorption isotherm and pseudo-second-order, indicating multilayer adsorption and chemisorption, respectively. The FTIR and XPS analysis confirmed the presence of Fe–O bonds and SO₄ groups in the MoS₂/FeOₓ@BC. Electron paramagnetic resonance (EPR) and radical quenching experiments have shown the generation of SO₄•⁻ radicals as predominant species in the presence of MoS₂ and FeOₓ in MoS₂/FeOx@BC via radical transfer from HO• to SO₄²⁻. The HO• and SO₄•⁻ radicals synergistically contributed to enhanced As(III) removal. It is envisaged that As(III) initially adsorbed through electrostatic interactions and partially undergoes oxidation, which is finally adsorbed to MoS₂/FeOx@BC after being oxidized to As(V). The MoS₂/FeOₓ@BC system could be considered a novel material for effective removal of As(III) from aqueous environments owing to its cost-effective synthesis and easy scalability for actual applications.
Show more [+] Less [-]Cd bioavailability and nitrogen cycling microbes interaction affected by mixed amendments under paddy-pak choi continued planting
2021
Li, Houfu | Abbas, Touqeer | Cai, Mei | Zhang, Qichun | Wang, Jingwen | Li, Yong | Di, Hongjie | Ṭāhir, Muḥammad
Cadmium (Cd) is the most concerning soil pollutant, and a threat to human health, especially in China. The in-situ immobilization of Cadmium by amendments is one of the most widely adopted methods to remedy soil contamination. The study was designed to evaluate the effect of organo-chemical amendments on soil Cd bioavailability and nitrogen cycling microbes under continuous planting of rice (Oryza sativa) and pak choi (Brassica chinensis L.). The experiment was carried out using four amendments, Lime, Zeolite, Superphosphate, and Biochar, at two different ratios; M1: at the ratio of 47:47:5:1, and M2 at the ratio of 71:23:5:1, respectively. Moreover, both M1 and M2 were enriched at four levels (T1: 0.5%; T2: 1%; T3: 2%; T4: 4%). Results showed that compared with CK (Cd enriched soils), the yield of rice under treatments of M1T1 and M2T1 increased by 8.93% and 8.36%, respectively. While the biomass (fresh weight) of pak choi under M1 and M2 amendments increased by 2.52–2.98 times and 0.76–2.89 times respectively, under enrichment treatments T1, T2, and T3. The total Cd concentrations in rice grains treated with M1T3 and M2T3 decreased by 89.25% and 93.16%, respectively, compared with CK. On the other hand, the total Cd concentrations in pak choi under M1T3 and M2T2 decreased by 92.86% and 90.23%, respectively. The results showed that soil pH was the main factor affecting Cd bioavailability in rice and pak choi. The Variance partitioning analysis (VPA) of rice and pak choi showed that soil pH was the most significant contributing factor. In the rice season, the contribution of soil pH (P) on Cd bioavailability was 10.14% (P = 0.102), and in the pak choi season, the contribution of soil pH was 8.38% (P = 0.133). Furthermore, the abundance of ammonia oxidation and denitrifying microorganisms had significantly correlation with soil pH and exchange Cd. In rice season, when the enrichment level of amendments increased from 0.5% (T1) to 2% (T3), the gene abundance of AOA, AOB, nirK, nirS and nosZ (І) tended to decrease. While in pak choi season, when the enrichment level increased at the level of 0.5% (T1), 1% (T2), and 2% (T3), the gene abundance of AOB, nirS, and nosZ (І) increased. Additionally, the gene abundance of AOA and nirK showed a reduction in the pak choi season contrasting to rice. And the mixed amendment M2 performed better at reducing Cd uptake than M1, which may have correlation with the ratio of lime and zeolite in them. Finally, we conclude that between these two amendments, when applied at a moderate level M2 type performed better than M1 in reducing Cd uptake, and also showed positive effects on both gene abundance and increase soil pH.
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