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The persistent O3 pollution in the Beijing-Tianjin-Hebei (BTH) region remains unresolved, largely due to limited comprehension of O3-precursor relationship and photochemistry drivers. In this work, intraday O3 sensitivity evolution from VOC-limited (volatile organic compound) regime in the forenoon to transition regime in the late afternoon was inferred by relative incremental reactivity (RIR) in summer 2019 at Xianghe, a suburban site in BTH region, suggesting that VOC-focused control policy could combine with stringent afternoon NOx control. Then detailed impacts of VOC subgroups on O3 formation were further comprehensively quantified by parametric OH reactivity (KOH), O3 formation potential (OFP), as well as RIR weighted value and O3 formation path tracing (OFPT) approach based on photochemical box model. O3 episode days corresponded to stronger O3 formation, depicted by higher KOH (10.4 s-1), OFP (331.7 µg m-3), RIR weighted value (1.2), and F(O3)-OFPT (15.5 ppbv h-1). High proportions of isoprene and OVOCs (oxygenated VOCs) to the total KOH and the OFPT method were demonstrated whereas results of OFP and RIR-weighted presented extra great impacts of aromatics on O3 formation. The OFPT approach captured the process that has already happened and included final O3 response to the original VOC, thus reliable for replicating VOC impacts. The comparison results of the four methods showed similarities when utilizing KOH and OFPT methods, which reveals that the potential applicability of simple KOH for contingency VOC control and more complex OFPT method for detailed VOC- and source-oriented control during policy-making. To investigate propulsion of VOC-involved O3 photochemistry, atmospheric oxidation capacity (AOC) was quantified by two atmospheric oxidation indexes (AOI). Both AOIp_G (7.0 × 107 molec cm-3 s-1, potential AOC calculated by oxidation reaction rates) and AOIe_G (8.5 µmol m-3, estimated AOC given redox electron transfer for oxidation products) were stronger on O3 episode days, indicating that AOC promoted the radical cycling initiated from VOC oxidation and subsequent O3 production. Result-oriented AOIe_G reasonably characterized actual AOC inferred by good linear correlation between AOIe_G and O3 concentrations compared to process-oriented AOIp_G. Therefore, with continuous NOx abatement, AOIe_G should be considered to represent actual AOC, also O3-inducing ability.
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Poluentes Atmosféricos , Ozônio , Compostos Orgânicos Voláteis , Poluentes Atmosféricos/análise , Ozônio/análise , Compostos Orgânicos Voláteis/análise , Monitoramento Ambiental , China , OxirreduçãoRESUMO
Auxin is a class of plant hormone that plays a crucial role in the life cycle of plants, particularly in the growth response of plants to ever-changing environments. Since the auxin responses are concentration-dependent and higher auxin concentrations might often be inhibitory, the optimal endogenous auxin level must be closely controlled. However, the underlying mechanism governing auxin homeostasis remains largely unknown. In this study, a UDP-glycosyltransferase (UGT76F1) was identified from Arabidopsis thaliana, which participates in the regulation of auxin homeostasis by glucosylation of indole-3-pyruvic acid (IPyA), a major precursor of the auxin indole-3-acetic acid (IAA) biosynthesis, in the formation of IPyA glucose conjugates (IPyA-Glc). In addition, UGT76F1 was found to mediate hypocotyl growth by modulating active auxin levels in a light- and temperature-dependent manner. Moreover, the transcription of UGT76F1 was demonstrated to be directly and negatively regulated by PIF4, which is a key integrator of both light and temperature signaling pathways. This study sheds a light on the trade-off between IAA biosynthesis and IPyA-Glc formation in controlling auxin levels and reveals a regulatory mechanism for plant growth adaptation to environmental changes through glucosylation of IPyA.
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Proteínas de Arabidopsis/metabolismo , Arabidopsis/crescimento & desenvolvimento , Regulação da Expressão Gênica de Plantas , Glucose/metabolismo , Hipocótilo/crescimento & desenvolvimento , Ácidos Indolacéticos/farmacologia , Indóis/metabolismo , Arabidopsis/efeitos dos fármacos , Arabidopsis/metabolismo , Arabidopsis/efeitos da radiação , Proteínas de Arabidopsis/genética , Sequestradores de Radicais Livres/química , Sequestradores de Radicais Livres/metabolismo , Glucosiltransferases/metabolismo , Glicosilação , Hipocótilo/efeitos dos fármacos , Hipocótilo/metabolismo , Hipocótilo/efeitos da radiação , Indóis/química , Luz , Reguladores de Crescimento de Plantas/farmacologia , Plântula , TemperaturaRESUMO
Metal-organic frameworks (MOFs) have presented potential for detection of specific species and catalytic application due to their diverse framework structures and functionalities. In this work, two novel pillar-layered MOFs [Cd6(DPA)2(NTB)4(H2O)4]n·n(DPA·5DMA·H2O) (1) and [Cu2(DPA)(OBA)2]n·n(2.5DMF·H2O) (2) [DPA = 2,5-di(pyridin-4-yl)aniline, H3NTB = 4,4',4''-nitrilotribenzoic acid, H2OBA = 4,4'-oxydibenzoic acid, DMA = N,N-dimethylacetamide, DMF = N,N-dimethylformamide] were successfully synthesized and structurally characterized. Both 1 and 2 have three-dimensional framework structures. The fluorescent property of 1 makes it possible for sensing specific amino acid such as L-glutamic acid (Glu) and L-aspartic acid (Asp). While MOF 2 was found to be suitable for photocatalytic degradation of Rhodamine B (RhB) in the presence of H2O2. The results imply that MOFs are versatile and metal centers are important in determining their properties.
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Estruturas Metalorgânicas , Estruturas Metalorgânicas/química , Aminoácidos , Peróxido de Hidrogênio , Rodaminas/químicaRESUMO
Luoyang is a typical heavy industrial city in China, with a coal-dominated energy structure and serious air pollution. Following the implementation of the clean air actions, the physicochemical characteristics and sources of PM2.5 have changed. A comprehensive study of PM2.5 was conducted from October 16, 2019 to January 23, 2020 to evaluate the effectiveness of previous control measures and further to provide theory basis for more effective policies in the future. Results showed that the aerosol pollution in Luoyang in autumn and winter is still serious with the average concentration of 91.1 µg/m3, although a large reduction (46.9%) since 2014. With the contribution of nitrate increased from 12.5% to 25.1% and sulfate decreased from 16.7% to 11.2%, aerosol pollution has changed from sulfate-dominate to nitrate-dominate. High NO3-/SO42- ratio and the increasing of NO3-/SO42- ratio with the aggravation of pollution indicating vehicle exhaust playing an increasingly important role in PM2.5 pollution in Luoyang, especially in the haze processes. Secondary inorganic ions contributed significantly to the enhancement of PM2.5 during the pollution period. The high value of Cl-/Na+ and EC concentration indicate coal combustion in Luoyang is still serious. The top three contributor sources were secondary inorganic aerosols (33.3%), coal combustion (13.6%), and industrial emissions (13.4%). Close-range transport from the western and northeastern directions were more important factors in air pollution in Luoyang during the sampling period. It is necessary to strengthen the control of coal combustion and reduce vehicle emissions in future policies.
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Poluentes Atmosféricos , Poluição do Ar , Aerossóis/análise , Poluentes Atmosféricos/análise , Poluição do Ar/análise , China , Monitoramento Ambiental , Nitratos , Material Particulado/análise , Estações do Ano , Emissões de Veículos/análiseRESUMO
KEY MESSAGE: This study revealed that the Arabidopsis UGT75B1 plays an important role in modulating ABA activity by glycosylation when confronting stress environments. The cellular ABA content and activity can be tightly controlled in several ways, one of which is glycosylation by family 1 UDP-glycosyltransferases (UGTs). Previous analysis has shown UGT75B1 activity towards ABA in vitro. However, the biological role of UGT75B1 remains to be elucidated. Here, we characterized the function of UGT75B1 in abiotic stress responses via ABA glycosylation. GUS assay and qRT-PCR indicated that UGT75B1 is significantly upregulated by adverse conditions, such as osmotic stress, salinity and ABA. Overexpression of UGT75B1 in Arabidopsis leads to higher seed germination rates and seedling greening rates upon exposure to salt and osmotic stresses. In contrast, the big UGT75B1 overexpression plants are more sensitive under salt and osmotic stresses. Additionally, the UGT75B1 overexpression plants showed larger stomatal aperture and more water loss under drought condition, which can be explained by lower ABA levels examined in UGT75B1 OE plants in response to water deficit conditions. Consistently, UGT75B1 ectopic expression leads to downregulation of many ABA-responsive genes under stress conditions, including ABI3, ABI5 newly germinated seedlings and RD29A, KIN1, AIL1 in big plants. In summary, our results revealed that the Arabidopsis UGT75B1 plays an important role in coping with abiotic stresses via glycosylation of ABA.
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Ácido Abscísico/metabolismo , Proteínas de Arabidopsis/metabolismo , Arabidopsis/enzimologia , Regulação da Expressão Gênica de Plantas , Glucosiltransferases/fisiologia , Glicosiltransferases/metabolismo , Estresse Fisiológico , Arabidopsis/genética , Proteínas de Arabidopsis/genética , Catálise , Secas , Genes de Plantas , Germinação , Glucosiltransferases/genética , Glicosilação , Glicosiltransferases/genética , Pressão Osmótica , Plantas Geneticamente Modificadas/genética , Salinidade , Plântula/genética , Plântula/fisiologia , Cloreto de Sódio , Fatores de Transcrição/genética , Fatores de Transcrição/fisiologiaRESUMO
Size-segregated aerosols collected in Beijing from 2021 to 2022 were used to investigate the contribution of organic aerosols to the aerosol liquid water content (ALWC), the influencing factors of ALWC, and the concentrations and size distribution characteristics of water-soluble organic carbon (WSOC) after clean air actions. The results showed that the concentration of WSOC in particulate matter (PM)1.8 was 3.52 ± 2.43 µg/m3 during the sampling period. Obvious changes were observed in the size distribution of WSOC after clean air actions, which may be attributed to the enhancement of atmospheric oxidation capacity and the decrease in PM concentration. The contribution of organic aerosols to the ALWC in fine PM was 18.1 % during the sampling period, which was more significant at lower particles concentration and smaller particle size ranges. The ambient relative humidity (RH) and the ratio of NO3-/SO42- had an apparent influence on ALWC. The continuous increase in the nitrate proportion significantly reduced the deliquescence point of the aerosols, making them prone to hygroscopic growth at lower RH. Analysis of the relation among nitrogen oxidation ratio (sulfur oxidation ratio), ALWC and PM1.8 mass concentrations suggests that organic matter has a significant effect on the formation of secondary inorganic aerosols in the initial phase of pollution formation and plays a crucial role in aerosol pollution formation in Beijing. These results are conducive to understanding the formation mechanism of aerosols and provide scientific data and theoretical support for the formulation of more effective emission-reduction measures.
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In recent years, the situation of ozone pollution in China has become increasingly severe, with PM2.5 being the main pollutant in the atmospheric environment of several cities. Meteorological conditions, particularly temperature and humidity, have a great influence on ozone formation. Therefore, understanding and quantifying the impact of the variation in temperature and humidity on ozone level can effectively provide the theoretical basis for the government to prevent and control ozone pollution. By analyzing the relationship among the daily maximum temperature (Tmax), relative humidity (RH), and the maximum 8-h running average ozone (O3-8h) measured from January 1, 2015 to July 31, 2022, a linear positive correlation between O3-8h and Tmax was observed in the seven regions with serious ozone pollution, and the temperature penalty factor ranged from 2.1-6.0 µg·(m3·â)-1; a nonlinear correlation between O3-8h and RH was also observed, and O3-8h was the highest when RH was 55%. The sensitivity of different regions to Tmax and RH was slightly different; generally, the most suitable meteorological conditions for ozone formation were 29â ≤ Tmax< 38â and 40% ≤ RH<70%. In the Yangtze River Delta, Jiangsu-Anhui-Shandong-Henan, and the middle reaches of the Yangtze River, under extreme high temperature conditions (Tmax ≥ 35â), O3-8h stopped increasing with the increase in temperature and even dropped; simultaneously, it was often accompanied with a small increase in particulate matter. It may be related to the heterogeneous reaction of some precursors with higher water vapor content and the increase in ozone heterogeneous sink.
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Purpose: Antibiotic-resistant bacterial pneumonia poses a significant therapeutic challenge. In China, Chinese herbal compound (CHC) is commonly used to treat bacterial pneumonia. We aimed to evaluate the efficacy and safety of CHC and identify core herb combinations for the treatment of multidrug-resistant or extensively drug-resistant bacterial pneumonia. Methods: Stata 16 and TSA 0.9.5.10 beta software were used for meta-analysis and trial sequential analysis (TSA), respectively. Exploring the sources of heterogeneity through meta-regression and subgroup analysis. Results: Thirty-eight studies involving 2890 patients were included in the analyses. Meta-analysis indicated that CHC combined with antibiotics improved the response rate (RR = 1.24; 95% CI: 1.19-1.28; p < 0.0001) and microbiological eradication (RR = 1.41; 95% CI: 1.27-1.57; p < 0.0001), lowered the white blood cell count (MD = -2.09; 95% CI: -2.65 to -1.53; p < 0.0001), procalcitonin levels (MD = -0.49; 95% CI: -0.59 to -0.40; p < 0.0001), C-reactive protein levels (MD = -11.80; 95% CI: -15.22 to -8.39; p < 0.0001), Clinical Pulmonary Infection Scores (CPIS) (MD = -1.97; 95% CI: -2.68 to -1.26; p < 0.0001), and Acute Physiology and Chronic Health Evaluation (APACHE)-II score (MD = -4.08; 95% CI: -5.16 to -3.00; p < 0.0001), shortened the length of hospitalization (MD = -4.79; 95% CI: -6.18 to -3.40; p < 0.0001), and reduced the number of adverse events. TSA indicated that the response rate and microbiological eradication results were robust. Moreover, Scutellaria baicalensis Georgi, Fritillaria thunbergii Miq, Lonicera japonica Thunb, and Glycyrrhiza uralensis Fisch were identified as core CHC prescription herbs. Conclusion: Compared with antibiotic treatment, CHC + antibiotic treatment was superior in improving response rate, microbiological eradication, inflammatory response, CPIS, and APACHE-II score and shortening the length of hospitalization. Association rule analysis identified four core herbs as promising candidates for treating antibiotic-resistant bacterial pneumonia. However, large-scale clinical studies are still required. Systematic Review Registration: https://www.crd.york.ac.uk/prospero/, identifier CRD42023410587.
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Three novel fluorescent Zn(II) frameworks, namely [Zn(DPA)(NDA)]2·2DMF (1), [Zn2(DPA)(OBA)2]·2DMF·4H2O (2) and [Zn(DPA)(HNTB)]·H2O (3) (DPA = 2,5-di(pyridin-4-yl)aniline, H2NDA = 1,4-naphthalenedicarboxylic acid, H2OBA = 4,4'-oxydibenzoic acid, H3NTB = 4,4',4''-nitrilotribenzoic acid, DMF = N,N-dimethylformamide), were successfully fabricated and structurally characterized. Due to the variety of organic linkers, 1-3 exhibit varied topologies: 1 is a 4-c three-dimensional (3D) framework with {65·8} topology, 2 is a 6-c 3D net with point symbol of {44·610·8}, and 3 is a 4-c two-dimensional network that further stacks into a 3D structure by hydrogen bonding interactions with {44·62} topology. Experiments related to fluorescence show that 1-3 can be utilized to quickly identify specific anions of CrO42-/Cr2O72-, and organic molecules such as 2,4,6-trinitrophenol and benzaldehyde.
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The photolysis of NO2 is an important driving force of tropospheric ozone. The intensity of this photolysis reaction affects atmospheric oxidation and photochemical pollution process. Photolysis rate of nitrogen dioxide (JNO2) is affected by aerosols, temperature, solar zenith angle (SZA), clouds, and so on. Among them, aerosol is an important influencing factor because of its complicated and irregular change; aerosol quantitative effect on JNO2 is constructive for the coordinated control of O3 and particulate matter. In order to quantitatively assess the impact of aerosols on JNO2 in the long-term, the reconstructed JNO2 data in a suburban site in North China from 2005 to 2019 are used. We found that JNO2 and aerosol optical depth (AOD) presented logarithmic relations under different solar zenith angle (SZA) levels, the aerosol attenuation effect on JNO2 decreased as AOD increased. Two main influencing factors of JNO2, SZA, and AOD, were fitted into a quadratic polynomial to quantify the AOD effect on JNO2. The results showed that the average annual AOD effect on JNO2 in Xianghe from 2005 to 2019 was -28.6% compared to an aerosol free atmosphere; the seasonal mean AOD effect in spring, summer, autumn, and winter was -27.1% and -35.1%, -25.5% and -26.3%, respectively. During the study period, JNO2 increased with an average of 5 × 10-5 s-1 per year, while the annual average aerosol optical depth (AOD) was 0.80 ± 0.10, showing an overall downward trend. Annual mean AOD attenuation effect on JNO2 decreased over time; the decreases were larger in spring and summer, and smaller in autumn and winter.
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The atmospheric oxidation capacity (AOC) and photochemical reactivity are of increasing concern owing to their roles in photochemical pollution. The AOC and OH reactivity were evaluated based on simultaneous measurements of volatile organic compounds (VOCs), trace gases and photolysis frequency during summer and winter campaigns at a suburban site in Xianghe. The AOC exhibited well-defined seasonal and diurnal patterns, with higher intensities during the summertime and daytime than during the wintertime and nighttime, respectively. The major reductants contributing to the AOC during the summertime were CO (41%) and alkenes (41%), whereas CO (40%) and oxygenated VOCs (OVOCs) (30%) dominated the AOC during the wintertime. The dominant oxidant contributor to the AOC during the daytime was OH (≥93%), while the contributions of O3 and NO3 (≥75%) to the AOC increased during the nighttime. High values during the wintertime and an increase at night were features of the speciated OH reactivity. Inorganic compounds (NOx and CO) dominated the speciated OH reactivity (76% and 85% during the summer and winter campaigns, respectively). Among VOCs, the dominant contributors were alkenes (12%) and OVOCs (7%) during the summer and winter campaigns, respectively. The ratio of NOx- and VOC-attributed OH reactivity indicated that O3 formation occurred under a VOC-limited regime during the summertime and that aromatics had the largest potential to form O3. Isoprene and m/p-xylene were the most important contributors to the AOC, OH reactivity and O3-forming among VOCs during the summertime, biogenic sources and secondary formation and industrial production were the main sources of these species. During the wintertime, hexanal and ethylene were the key VOC species contributing to the AOC and OH reactivity, and solvent usage and traffic-related emissions were the main contributing sources. We recommend that priority measures for the control of VOC species and sources should be taken when suitable. CAPSULE: This study focused on the similarities and differences in the AOC and speciated OH reactivity during summer and winter campaigns.
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Drought is one of the most important environmental constraints affecting plant growth and development and ultimately leads to yield loss. Uridine diphosphate (UDP)-dependent glycosyltransferases (UGTs) are believed to play key roles in coping with environmental stresses. In rice, it is estimated that there are more than 200 UGT genes. However, most of them have not been identified as their physiological significance. In this study, we reported the characterization of a putative glycosyltransferase gene UGT85E1 in rice. UGT85E1 gene is significantly upregulated by drought stress and abscisic acid (ABA) treatment. The overexpression of UGT85E1 led to an enhanced tolerance in transgenic rice plants to drought stress, while the ugt85e1 mutants of rice showed a more sensitive phenotype to drought stress. Further studies indicated that UGT85E1 overexpression induced ABA accumulation, stomatal closure, enhanced reactive oxygen species (ROS) scavenging capacity, increased proline and sugar contents, and upregulated expression of stress-related genes under drought stress conditions. Moreover, when UGT85E1 was ectopically overexpressed in Arabidopsis, the transgenic plants showed increased tolerance to drought as well as in rice. Our findings suggest that UGT85E1 plays an important role in mediating plant response to drought and oxidative stresses. This work may provide a promising candidate gene for cultivating drought-tolerant crops both in dicots and monocots.
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Nucleation particle growth plays a major role in the occurrence of fine particles, yet the mechanism of new particle formation (NPF) remains ambiguous in the complex atmosphere of megacities and hinders the development of measures to mitigate PM2.5 pollution. In this study, the chemistry of ultrafine particles during the growth phase of nucleation events was investigated in urban Beijing from Nov. 15, 2018 to Jan. 15, 2019, using two scanning mobility particle spectrometers (SMPS) systems and an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). During this intense campaign, 11 NPF events were observed and the growth rate (GR) of nanoparticles ranged from 12.5 to 24.5 nm h-1. Four periodic cycles of PM2.5 episodes that included aerosol particle growth to particulate matter pollution were identified. Based on the QGR - QAMS theoretical frame that exploring the balance between the source rate of condensable vapors and the observed growth rate of nanoparticles, we clearly showed the physical and chemical evolution of nano-particle during the growth processes to ambient-atmosphere sizes (>100 nm). Generally, the modal diameter of aerosol particles grew by more than 100 nm (7 out of 11 NPF events) when the nitrate concentration and less-oxidized oxygenated organic aerosol (LO-OOA) were high; however, another class of aerosol particle growth was limited to 50-100 nm (3 out of 11 NPF events) when sulfate was high. Note that the remaining one NPF event could not be identified if it can grow up to 100 nm or not due to the unavailable of observation data during the late growth stage. By linking the aerosol growth with chemical compositions, sulfate and organics were found to be the main contributors during the initial stage of the aerosol growth, while cooking-related OA (COA) enhanced the transition stage, and nitrate and more-oxidized OOA (MO-OOA) dominated the subsequent growth of aerosol to ambient-atmosphere sizes. An important portion of aerosol growth in PM2.5 was controlled by semi-volatile organic vapors, which can partition into the externally condensed phase of the accumulation mode and coarse mode via the physical process of adsorption. Through quantifying the physical and chemical properties of aerosol particle growth, the detail processes of nucleation initiated PM2.5 pollution episodes were evaluated and provided observational evidence on the formation mechanism of winter haze pollution in the megacity of Beijing.
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Poluentes Atmosféricos , Aerossóis/análise , Poluentes Atmosféricos/análise , Pequim , Monitoramento Ambiental , Tamanho da Partícula , Material Particulado/análiseRESUMO
Plants can reduce or eliminate the damage caused by herbicides and gain herbicide resistance, which is an important theoretical basis for the development of herbicide-resistant crops at this stage. Thus, discovering novel herbicide-resistant genes to produce diverse herbicide-resistant crop species is of great value. The glycosyltransferases that commonly exist in plant kingdom modify the receptor molecules to change their physical characteristics and biological activities, and thus possess an important potential to be used in the herbicide-resistance breeding. Here, we identified a novel herbicide-induced UDP-glycosyltransferase 91C1 (UGT91C1) from Arabidopsis thaliana and demonstrated its glucosylating activity toward sulcotrione, a kind of triketone herbicides widely used in the world. Overexpression of UGT91C1 gene enhanced the Arabidopsis tolerance to sulcotrione. While, ugt91c1 mutant displayed serious damage and reduced chlorophyll contents in the presence of sulcotrione, suggesting an important role of UGT91C1 in herbicide detoxification through glycosylation. Moreover, it was also noted that UGT91C1 can affect tyrosine metabolism by reducing the sulcotrione toxicity. Together, our identification of glycosyltransferase UGT91C1, as a potential gene conferring herbicide detoxification through glucosylation, may open up a new possibility for herbicide resistant breeding of crop plants and environmental phytoremediation.
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Proteínas de Arabidopsis/metabolismo , Arabidopsis , Glicosiltransferases/metabolismo , Resistência a Herbicidas , Inativação Metabólica , Arabidopsis/efeitos dos fármacos , Arabidopsis/genética , Arabidopsis/metabolismo , Proteínas de Arabidopsis/genética , Glicosiltransferases/genética , Resistência a Herbicidas/genética , Herbicidas/metabolismo , Herbicidas/toxicidade , Inativação Metabólica/genéticaRESUMO
Nitrate-driven aerosol pollution frequently occurs during winter over the North China Plain (NCP). Extensive studies have focused on inorganic nitrate formation, but few have focused on organic nitrates in China, precluding a thorough understanding of the nitrogen cycle and nitrate aerosol formation. Here, the inorganic (NO3,inorg) and organic nitrate (NO3,org) formation regimes under aerosol liquid water (ALW) and aerosol acidity (pH) influences were investigated during winter over the NCP based on data derived from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The campaign-averaged concentration of the total nitrate was 5.3 µg m-3, with a 13% contribution from NO3,org, which exhibited a significantly decreased contribution with increasing haze episode evolution. The diurnal cycles of NO3,inorg and NO3,org were similar, with high concentrations during the nighttime at a high ALW level, revealing the important role of aqueous-phase processes. However, the correlations between the aerosol pH and NO3,inorg (R2 = 0.13, P < 0.01) and NO3,org (R2 = 0.63, P < 0.01) during polluted periods indicated a contrasting effect of aerosol pH on inorganic and organic nitrate formation. Our results provide a useful reference for smog chamber studies and promote a better understanding of organic nitrate formation via anthropogenic emissions.
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Two complexes, namely [Zn(bpeb)(sda)] (1) and [Zn(poly-bpeb)(sda)] (2), were synthesized by an organic ligand with an extensively conjugated system, bpeb = 1,4-bis[2-(3-pyridyl) vinyl]-benzene, H2sda = sulfonyldibenzoic acid and d10 metal centers Zn2+. Structural analysis revealed that compound 1 was nonporous and possessed 7-fold interpenetrated three-dimensional (3D) frameworks constructed from one-dimensional (1D) Zn-bpeb and Zn-sda chains. Interestingly, due to the short distance between the vinyl groups from two neighboring bpeb ligands, compound 1 could undergo a photochemical [2 + 2] polymerization reaction to generate 2 in a single-crystal to single-crystal (SCSC) manner under the irritation of UV. Moreover, the organic polymer in 2 could be depolymerized by heating to realize the reversible transformation from 2 to 1. Furthermore, both compounds 1 and 2 could be used as fluorescent sensors for 2,4,6-trinitrophenol (TNP) with high selectivity and sensitivity.
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A seven-year long-term comprehensive measurement of non-refractory submicron particles (NR-PM1) in autumn and winter in Beijing from 2012 to 2018 was conducted to evaluate the effectiveness of the clean air actions implemented by the Chinese government in September 2013 on aerosols from different sources and chemical processes. Results showed that the NR-PM1 concentrations decreased by 44.1% in autumn and 73.2% in winter from 2012 to 2018. Sulfate showed a much larger reduction than nitrate and ammonium in both autumn (55%) and winter (86%) and that nitrate even slightly increased by 15.8% in autumn. As a result, aerosol pollution in winter gradually changed from sulfate-rich to nitrate-rich with a sudden change after 2016 and the dominant role of nitrate in autumn was also strengthened after 2016. Among primary organic aerosol (OA) types, biomass burning OA and coal combustion OA exhibited the largest decline in autumn and winter, with reductions of 87.5% and 77.3%, respectively, while hydrocarbon-like OA (HOA) exhibited the smallest decline in both autumn (24.4%) and winter (37.1%). These significant changes in aerosol compositions were highly consistent with the much faster reduction of SO2 (75-85%) than NOx (36-59%) and were mainly due to the clean air actions rather than the impact of meteorological conditions. What's more, the enhanced atmospheric oxidizing capacity, which was indicated by increased O3, altered the chemical processes of oxygenated OA (OOA), especially in autumn. Both of less-oxidized OOA (LO-OOA) and more-oxidized OOA showed elevated contributions in OA by 4% in autumn. The increased oxygen-to-carbon ratios of LO-OOA in autumn (from 0.42 to 0.58) and winter (from 0.44 to 0.52) indicated the enhanced atmospheric oxidizing capacity strengthened photochemical reactions and resulted in the increased oxidation degree of LO-OOA. This study demonstrates the effectiveness of the clean air actions for air quality improvement in Beijing.
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Poluentes Atmosféricos , Poluição do Ar , Aerossóis/análise , Poluentes Atmosféricos/análise , Poluição do Ar/análise , Pequim , Monitoramento Ambiental , Material Particulado/análiseRESUMO
To what extent anthropogenic emissions could influence volatile organic compound (VOCs) concentrations and related atmospheric reactivity is still poorly understood. China's 70th National Day holidays, during which anthropogenic emissions were significantly reduced to ensure good air quality on Anniversary Day, provides a unique opportunity to investigate these processes. Atmospheric oxidation capacity (AOC), OH reactivity, secondary transformation, O3 formation and VOCs-PM2.5 sensitivity are evaluated based on parameterization methods and simultaneous measurements of VOCs, O3, NOx, CO, SO2, PM2.5, JO1D, JNO2, JNO3 carried out at a suburban site between Beijing and Tianjin before, during, and after the National Day holiday 2019. During the National Day holidays, the AOC, OH reactivity, O3 formation potential (OFP) and secondary organic aerosol formation potential (SOAP) were 1.6 × 107 molecules cm-3 s-1, 41.8 s-1, 299.2 µg cm-3 and 1471.8 µg cm-3, respectively, which were 42%, 29%, 47% and 42% lower than pre-National Day values and -12%, 42%, 36% and 42% lower than post-National Day values, respectively. Reactions involving OH radicals dominated the AOC during the day, but OH radicals and O3 reactions at night. Alkanes (the degree of unsaturation = 0, (D, Equation (1)) accounted for the largest contributions to the total VOCs concentration, oxygenated VOCs (OVOCs; D ≤ 1) to OH reactivity and OFP, and aromatics (D = 4) to the SOAP. O3 production was identified as VOCs-limited by VOCs (ppbC)/NOx (ppbv) ratios during the sampling campaign, with greater VOCs limitation during post- National Day and more-aged air masses during the National Day. The VOCs-sensitivity coefficient (VOCs-S) suggested that VOCs were more sensitive to PM2.5 in low-pollution domains and during the National Day holiday. This study emphasizes the importance of not only the abundance, reactivity, and secondary transformation of VOCs but also the effects of VOCs on PM2.5 for the development of effective control strategies to minimize O3 and PM2.5 pollution.
Assuntos
Poluentes Atmosféricos , Ozônio , Compostos Orgânicos Voláteis , Poluentes Atmosféricos/análise , Pequim , China , Monitoramento Ambiental , Férias e Feriados , Ozônio/análise , Compostos Orgânicos Voláteis/análiseRESUMO
Volatile organic compounds (VOCs) have vital implications for secondary pollutants, atmospheric oxidation and human health. Ambient VOCs were investigated using an online system, gas chromatography-mass spectrometry/flame ionization detector (GC-MS/FID), at a suburban site in Xianghe in the North China Plain from 6 November 2017 to 29 January 2018. Positive matrix factorization (PMF) receptor model was applied to identify the major VOC contributing sources. Four-step health risk assessment method was used to estimate risks of all risk-posing VOC species. A total of 101 VOCs were quantified, and the mean concentration of total VOCs was 61.04⯱â¯65.18 ppbv. The VOCs were dominated by alkanes (38.76%), followed by alkenes, aromatics, halocarbons, OVOCs, acetylene and acetonitrile. The results of PMF revealed that vehicle exhaust, industrial emissions, liquefied petroleum gas & natural gas, solvent utilization and secondary and long-lived species contributed 31.0%, 26.4%, 18.6%, 13.6% and 10.4%, respectively, to the total VOCs. Pollutant-specific and source-specific noncarcinogenic and carcinogenic risk estimates were conducted, which showed that acrolein and vehicle exhaust had evident noncarcinogenic risks of 4.9 and 0.9, respectively. The carcinogenic risks of specific species (1,3-butadiene, acetaldehyde, benzene, chloroform and 1,2-dichloroethane) and identified sources were above the United States Environmental Protection Agency (USEPA) acceptable level (1.0â¯×â¯10-6) but below the tolerable risk level (1.0â¯×â¯10-4). Vehicle exhaust was the largest contributor (56.2%) to noncarcinogenic risk, but solvent utilization (32.6%) to carcinogenic risk. Moreover, with the evolution of pollution levels, almost all VOC species, contributions of alkenes, aromatics, solvent utilization and vehicle exhaust, and pollutant-specific and source-specific risks increased continuously and noticeably. Collectively, our findings unraveled the importance of alkenes, aromatics, solvent utilization and vehicle exhaust in the evolution of pollution levels. Future studies should consider targeting these VOC groups and sources when focusing on effective reduction strategies and assessing public health risks.
Assuntos
Poluentes Atmosféricos/análise , Monitoramento Ambiental , Compostos Orgânicos Voláteis/análise , Poluição do Ar/estatística & dados numéricos , China , Humanos , Exposição por Inalação/estatística & dados numéricos , Medição de RiscoRESUMO
BACKGROUND: In cereal crop rice, auxin is known as an important class of plant hormone that regulates a plethora of plant growth and development. Glycosylation of auxin is known to be one of the important mechanisms mediating auxin homeostasis. However, the relevant auxin glucosyltransferase (GT) in rice still remains largely unknown. RESULTS: In this study, using known auxin glucosyltransferases from other species as queries, twelve putative auxin UDP-glycosyltransferase (UGT) genes were cloned from rice and the one showing highest sequence similarity, named as OsIAGT1, was expressed as recombinant protein. In vitro enzymatic analysis showed that recombinant OsIAGT1 was capable of catalyzing glucosylation of IAA, IBA and other auxin analogs, and that OsIAGT1 is quite tolerant to a broad range of reaction conditions with peak activity at 30 °Ð¡ and pH 8.0. OsIAGT1 showed favorite activity towards native auxins over artificially synthesized ones. Further study indicated that expression of OsIAGT1 can be upregulated by auxin in rice, and with OsIAGT1 overexpressing lines we confirmed that OsIAGT1 is indeed able to glucosylate IAA in vivo. Consistently, ectopic expression of OsIAGT1 leads to declined endogenous IAA content, as well as upregulated auxin synthesis genes and reduced expression of auxin-responsive genes, which likely leads to the reduced plant stature and root length in OsIAGT1 overexpression lines. CONCLUSION: Our result indicated that OsIAGT1 plays an important role in mediating auxin homeostasis by catalyzing auxin glucosylation, and by which OsIAGT1 regulates growth and development in rice.