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Insight into the uptake, accumulation, and metabolism of the fungicide phenamacril in lettuce (Lactuca sativa L.) and radish (Raphanus sativus L.)
2022
Tao, Yan | Xing, Yinghui | Jing, Junjie | Yu, Pingzhong | He, Min | Zhang, Jinwei | Chen, Li | Jia, Chunhong | Zhao, Ercheng
The fungal species Fusarium can cause devastating disease in agricultural crops. Phenamacril is an extremely specific cyanoacrylate fungicide and a strobilurine analog that has excellent efficacy against Fusarium. To date, information on the mechanisms involved in the uptake, accumulation, and metabolism of phenamacril in plants is scarce. In this study, lettuce and radish were chosen as model plants for a comparative analysis of the absorption, accumulation, and metabolic characteristics of phenamacril from a polluted environment. We determined the total amount of phenamacril in the plant-water system by measuring the concentrations in the solution and plant tissues at frequent intervals over the exposure period. Phenamacril was readily taken up by the plant roots with average root concentration factor ranges of 60.8–172.7 and 16.4–26.9 mL/g for lettuce and radish, respectively. However, it showed limited root-to-shoot translocation. The lettuce roots had a 2.8–12.4-fold higher phenamacril content than the shoots; whereas the radish plants demonstrated the opposite, with the shoots having 1.5 to 10.0 times more phenamacril than the roots. By the end of the exposure period, the mass losses from the plant-water systems reached 72.0% and 66.3% for phenamacril in lettuce and radish, respectively, suggesting evidence of phenamacril biotransformation. Further analysis confirmed that phenamacril was metabolized via hydroxylation, hydrolysis of esters, demethylation, and desaturation reactions, and formed multiple transformation products. This study furthers our understanding of the fate of phenamacril when it passes from the environment to plants and provides an important reference for its scientific use and risk assessment.
Show more [+] Less [-]Elevated particle acidity enhanced the sulfate formation during the COVID-19 pandemic in Zhengzhou, China
2022
Yang, Jieru | Wang, Shenbo | Zhang, Ruiqin | Yin, Shasha
The significant reduction in PM₂.₅ mass concentration after the outbreak of COVID-19 provided a unique opportunity further to study the formation mechanism of secondary inorganic aerosols. Hourly data of chemical components in PM₂.₅, gaseous pollutants, and meteorological data were obtained from January 1 to 23, 2020 (pre-lockdown) and January 24 to February 17, 2020 (COVID-lockdown) in Zhengzhou, China. Sulfate, nitrate, and ammonium were the main components of PM₂.₅ during both the pre-lockdown and COVID-lockdown periods. Compared with the pre-lockdown period, even though the concentration and proportion of nitrate decreased, nitrate was the dominant component in PM₂.₅ during the COVID-lockdown period. Moreover, nitrate production was enhanced by the elevated O₃ concentration, which was favorable for the homogeneous and hydrolysis nitrate formation despite the drastic decrease of NO₂. The proportion of sulfate during the COVID-lockdown period was higher than that before. Aqueous-phase reactions of H₂O₂ and transition metal (TMI) catalyzed oxidations were the major pathways for sulfate formation. During the COVID-lockdown period, TMI-catalyzed oxidation became the dominant pathway for aqueous-phase sulfate formation because the elevated acidity favored the dissolution of TMI. Therefore, the enhanced TMI-catalyzed oxidation affected by the elevated particle acidity dominated the sulfate formation, resulting in the slight increase of sulfate concentration during the COVID-lockdown period in Zhengzhou.
Show more [+] Less [-]Biochar composite derived from cellulase hydrolysis apple branch for quinolone antibiotics enhanced removal: Precursor pyrolysis performance, functional group introduction and adsorption mechanisms
2022
Zou, Mengyuan | Tian, Weijun | Chu, Meile | Gao, Huizi | Zhang, Dantong
In this study, magnetic biochar (MAB) and humic acid (HA)-coated magnetic biochar produced from apple branches without and after cellulase hydrolysis (HMAB and CHMAB, respectively) were prepared and tested as adsorbents of enrofloxacin (ENR) and moxifloxacin (MFX) in aqueous solution. Compared with MAB and HMAB, novel adsorbent CHMAB possessed a superior mesoporous structure, greater graphitization degree and abundant functional groups. When antibiotic solutions ranged from 2 to 20 mg L⁻¹, the theoretical maximum adsorption capacities of CHMAB for ENR and MFX were 48.3 and 61.5 mg g⁻¹ at 35 °C with adsorbent dosage of 0.4 g L⁻¹, respectively, while those of MAB and HMAB were 39.6 and 54.4 mg g⁻¹, and 44.7 and 59.0 mg g⁻¹, respectively. The pseudo-second-order kinetic model and Langmuir model presented a better fitting to the spontaneous and endothermic adsorption process. The maximum adsorption capacity of ENR and MFX onto CHMAB was achieved at initial pH values of 5 and 8, respectively. Additionally, the adsorption capacity of ENR and MFX decreased with increasing concentrations of K⁺ and Ca²⁺ (0.02–0.1 mol L⁻¹). Synergism between the pore-filling effect, π-π electron-donor-acceptor interactions, regular and negative charge-assisted H-bonding, surface complexation, electrostatic interactions and hydrophobic interactions may dominate the adsorption process. This study demonstrated that a novel magnetic biochar composite prepared through pyrolysis of agricultural waste lignocellulose hydrolyzed by cellulase in combination with HA coating was a promising adsorbent for eliminating quinolone antibiotics from aqueous media.
Show more [+] Less [-]Water-induced release of recalcitrant polycyclic aromatic hydrocarbons from soil organic matter during microwave-assisted solvent extraction
2021
Wang, Wei | Zhang, Yanyan | Du, Wei | Tao, Shu
Polycyclic aromatic hydrocarbons (PAHs) in soil can be recalcitrant to solvent extraction after aging. We showed in this study that mixing a small amount of water in the extracting solvent during microwave-assisted extraction (MAE) can release recalcitrant PAHs, resulting in significant improvement in the analyzed concentrations. The improvement factor (F) for the total of 16 priority PAHs (∑PAH16) listed by the United States Environmental Protection Agency was 1.44–1.55 for field soils. By comparing the F values for different soil organic components, we demonstrated that the recalcitrant PAHs were primarily associated with biochar, humic acid (HA), and humin (HM), with the F values for ∑PAH16 of 1.94, 6.62, and 4.59, respectively. The results showed that the recalcitrant PAHs comprised a sequestered fraction and a desorption-limited fraction. NMR spectra showed that water worked alone at elevated temperature to promote hydrolysis of biochar and destroy the macromolecular structure, thus causing the release of the otherwise sequestered PAHs during MAE. The substantial reduction in F values for HA and HM after demineralization indicated sequestration of PAHs in organic-mineral complexes, which can be destroyed by hot water treatment. The release of the sequestered fraction was nonselective and independent of compound hydrophobicity. In comparison, the release of the desorption-limited fraction was positively affected by the hydrophobicity of PAHs and was facilitated by the presence of water in the extracting solvent. The results of this study provide important insights into the sequestration and release of recalcitrant PAHs in soil.
Show more [+] Less [-]Oxidation and sources of atmospheric NOx during winter in Beijing based on δ18O-δ15N space of particulate nitrate
2021
Zhang, Zhongyi | Guan, Hui | Xiao, Hongwei | Liang, Yue | Zheng, Nengjian | Luo, Li | Liu, Cheng | Fang, Xiaozhen | Xiao, Huayun
The determination of both stable nitrogen (δ¹⁵N–NO₃⁻) and stable oxygen (δ¹⁸O–NO₃⁻) isotopic signatures of nitrate in PM₂.₅ has shown potential for an approach of assessing the sources and oxidation pathways of atmospheric NOx (NO+NO₂). In the present study, daily PM₂.₅ samples were collected in the megacity of Beijing, China during the winter of 2017–2018, and this new approach was used to reveal the origin and oxidation pathways of atmospheric NOx. Specifically, the potential of field δ¹⁵N–NO₃⁻ signatures for determining the NOx oxidation chemistry was explored. Positive correlations between δ¹⁸O–NO₃⁻ and δ¹⁵N–NO₃⁻ were observed (with R² between 0.51 and 0.66, p < 0.01), and the underlying environmental significance was discussed. The results showed that the pathway-specific contributions to NO₃⁻ formation were approximately 45.3% from the OH pathway, 46.5% from N₂O₅ hydrolysis, and 8.2% from the NO₃+HC channel based on the δ¹⁸O-δ¹⁵N space of NO₃⁻. The overall nitrogen isotopic fractionation factor (εN) from NOx to NO₃⁻ on a daily scale, under winter conditions, was approximately +16.1‰±1.8‰ (consistent with previous reports). Two independent approaches were used to simulate the daily and monthly ambient NOx mixtures (δ¹⁵N-NOx), respectively. Results indicated that the monthly mean values of δ¹⁵N-NOx compared well based on the two approaches, with values of −5.5‰ ± 2.6‰, −2.7‰ ± 1.9‰, and −3.2‰ ± 2.2‰ for November, December, and January (2017–2018), respectively. The uncertainty was in the order of 5%, 5‰ and 5.2‰ for the pathway-specific contributions, the εN, and δ¹⁵N-NOx, respectively. Results also indicated that vehicular exhaust was the key contributor to the wintertime atmospheric NOx in Beijing (2017–2018). Our advanced isotopic perspective will support the future assessment of the origin and oxidation of urban atmospheric NOx.
Show more [+] Less [-]Aerosol water content enhancement leads to changes in the major formation mechanisms of nitrate and secondary organic aerosols in winter over the North China Plain
2021
Chen, Chunrong | Zhang, Haixu | Yan, Weijia | Wu, Nana | Zhang, Qiang | He, Kebin
In recent years, severe air pollution still frequently occurs in winter despite the effective implementation of clean air actions in China. Therefore, field measurements of particle composition and gas precursors were collected from December 1, 2018 to January 15, 2019 at an urban site in a central Chinese city to investigate the existing mechanisms of pollution. The hourly averaged PM₂.₅ concentration during the campaign was 92.7 μg m⁻³, with nitrate and organic aerosol (OA) demonstrated as the principal components. Generally, NO₂ oxidation in the daytime was observed as the major mechanism for nitrate generation, and aerosol water content (AWC) showed its influential role with the associated increases in the nitrogen oxidation and nitrate partitioning ratios. When AWC increased from dozens to hundreds of μg m⁻³ after the afternoon, nocturnal N₂O₅ hydrolysis was demonstrated as the overriding mechanism and provoked extreme contamination of nitrates. Five sources of organic aerosols (OAs) were identified: hydrocarbon-like OAs (HOAs, 16.5%), coal combustion OAs (CCOAs, 19.2%), biomass burning OAs (BBOAs, 9.9%), semi-volatile oxygenated OAs (SV–OOAs, 29.4%), and low-volatile oxygenated OAs (LV-OOAs, 25.0%). SV-OOAs and LV-OOAs were identified as gasSOAs and aqSOAs according to their sensitivities to the atmospheric oxidation capacity and AWC. In addition, aqueous-phase processing was found to be the dominant pathway for SOA formation when the AWC concentration was higher than 80 μg m⁻³. As an influential factor for nitrate and SOA formation, AWC could be greatly affected by RH and the concentrations of inorganic species. Sulfate, which was mainly contributed by anthropogenic emissions, was demonstrated to be a significant factor for active aqueous phase reactions, although SO₂ has been dramatically reduced in recent years. Above all, this study revealed the significant role of AWC in current pollution episode in winter, and will assist in establishing future measures for pollution mitigation.
Show more [+] Less [-]Insight into metabolism pathways of pesticide fomesafen in rice: Reducing cropping and environmental risks
2021
Chen, Zhao Jie | Qiao, Yu Xin | Zhang, Nan | Liu, Jintong | Yang, Hong
Fomesafen (FSA) is widely used in soybean fields for weed control. However, the persisting characteristics of FSA in the agricultural soil or water may become a hidden danger causing environmental pollution and phytotoxicity to succession crops. In this study, the growth and physiological responses of rice to FSA were investigated. It was found that the growth of rice seedlings was obviously inhibited by FSA exposure especially at over 0.1 mg L⁻¹. To gain an insight into the molecular mechanisms for the potential ecotoxicology, four libraries of rice roots and shoots exposed to FSA were created and subjected to the global RNA-sequencing (RNA-Seq) combined with HRLC-Q-TOF-MS/MS analytical technologies to comprehensively characterize the biochemical processes and catalytic reactions involved in FSA metabolism in rice. Compared with those without FSA, 499 and 450 up-regulated genes in roots and shoots with FSA were detected. Many of them were closely correlated with the tolerance to environmental stress, detoxification of xenobiotics and molecular metabolism process including cytochrome P450, glutathione S-transferases and acetyltransferase. A total of eight metabolites and fourteen conjugates in the reactive pathways of hydrolysis, substitution, reduction, methylation, glycosylation, acetylation, and malonylation were characterized by HRLC-Q-TOF-MS/MS. The relationship between the metabolized derivatives of FSA and enhanced expression the corresponding enzymatic regulators was established. This study will help understand the mechanisms and pathways of FSA metabolism and inspire the further research on FSA degradation in the paddy crops and environmental or health risks.
Show more [+] Less [-]Ferrate (VI)-mediated transformation of diethyl phthalate (DEP) in soil: Kinetics, degradation mechanisms and theoretical calculation
2021
Yu, Yao | Qi, Yumeng | Li, Chenguang | Cao, Wanming | Chen, Jing | Qu, Ruijuan | Zhou, Dongmei | Wang, Zunyao
Diethyl phthalate (DEP), as a kind of universally used plasticizer, has aroused considerable public concern owing to its wide detection, environmental stability, and potential health risks. In this work, the highly efficient removal of DEP by ferrate (VI) (Fe(VI)) was systematically explored in soil environment. The effects of the oxidant dosages, soil types, as well as the presence of coexisting cations and anions in tested soil on DEP removal were evaluated. When the dosage of Fe(VI) was 20 mM, complete removal of DEP (50 μg/g) was achieved in the tested soil after 2 min of reaction. Furthermore, the removal rate of DEP was closely related to the soil types, and the degradation rates were decreased obviously in red soil (RS), black soil (BS) and paddy soil (PS), probably due to the acidic condition and high content of organic matters. Moreover, the presence of Ca²⁺, Mg²⁺ and Al³⁺ in soil can inhibit the removal of DEP by Fe(VI), while SO₄²⁻ has an slightly promotion effect. Six oxidation intermediates were detected in the reaction process of DEP, product analysis revealed that the transformation of DEP was mainly through two pathways, including hydrolysis and hydroxylation reactions, which were probably mediated by oxygen atom transfer process of Fe(VI). Based on the frontier electron density theory calculation, two ester groups of DEP were prone to be attacked by Fe(VI), and the hydroxyl addition tended to occur at the para-position of one of the ester groups on the benzene ring. This study provides a novel approach for phthalate esters removal from soil using Fe(VI) oxidation and shows new insights into the oxidation mechanisms.
Show more [+] Less [-]Biomass utilization and production of biofuels from carbon neutral materials
2021
Srivastava, Rajesh K. | Shetti, Nagaraj P. | Reddy, Kakarla Raghava | Kwon, Eilhann E. | Nadagouda, Mallikarjuna N. | Aminabhavi, Tejraj M.
The availability of organic matters in vast quantities from the agricultural/industrial practices has long been a significant environmental challenge. These wastes have created global issues in increasing the levels of BOD or COD in water as well as in soil or air segments. Such wastes can be converted into bioenergy using a specific conversion platform in conjunction with the appropriate utilization of the methods such as anaerobic digestion, secondary waste treatment, or efficient hydrolytic breakdown as these can promote bioenergy production to mitigate the environmental issues. By the proper utilization of waste organics and by adopting innovative approaches, one can develop bioenergy processes to meet the energy needs of the society. Waste organic matters from plant origins or other agro-sources, biopolymers, or complex organic matters (cellulose, hemicelluloses, non-consumable starches or proteins) can be used as cheap raw carbon resources to produce biofuels or biogases to fulfill the ever increasing energy demands. Attempts have been made for bioenergy production by biosynthesizing, methanol, n-butanol, ethanol, algal biodiesel, and biohydrogen using different types of organic matters via biotechnological/chemical routes to meet the world’s energy need by producing least amount of toxic gases (reduction up to 20–70% in concentration) in order to promote sustainable green environmental growth. This review emphasizes on the nature of available wastes, different strategies for its breakdown or hydrolysis, efficient microbial systems. Some representative examples of biomasses source that are used for bioenergy production by providing critical information are discussed. Furthermore, bioenergy production from the plant-based organic matters and environmental issues are also discussed. Advanced biofuels from the organic matters are discussed with efficient microbial and chemical processes for the promotion of biofuel production from the utilization of plant biomasses.
Show more [+] Less [-]Monobutyl phthalate (MBP) can dysregulate the antioxidant system and induce apoptosis of zebrafish liver
2020
Jiao, Yaqi | Tao, Yue | Yang, Yang | Diogene, Tuyiringire | Yu, Hui | He, Ziqing | Han, Wei | Chen, Zhaobo | Wu, Pan | Zhang, Ying
In this paper, the acute toxicity of monobutyl phthalate (MBP), the main hydrolysis product of dibutyl phthalate, on adult zebrafish liver antioxidant system was studied. Compared the toxicity effect of MBP and DBP by histopathology and apoptosis experiments, we speculated that the toxic effects of DBP on animals may be caused by its metabolite MBP. The results indicated that the antioxidant Nrf2-Keap1 pathway was insufficient to resist MBP-induced hepatotoxicity and led to an imbalance of membrane ion homeostasis and liver damage. Decreased cell viability, significant tissue lesions and early hepatocyte apoptosis were observed in the zebrafish liver in MBP exposure at high concentration (10 mg/L). The activities of antioxidant enzymes and ATPases in zebrafish liver were inhibited with increased malondialdehyde (MDA) content and alanine aminotransferase (ALT) and aspartate aminotransferase (AST) activities. Integrated biomarker response (IBR) calculation results indicated that MBP mainly inhibited catalase (CAT) activity. Simultaneously, the expression of antioxidant-related genes (SOD, CAT, GPx, Nrf2, HO-1) was down-regulated, while apoptosis-related genes (p53, bax, cas3) were significantly up-regulated.
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