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1.
Proc Natl Acad Sci U S A ; 118(8)2021 02 23.
Artículo en Inglés | MEDLINE | ID: mdl-33593919

RESUMEN

Secondary organic aerosol (SOA) produced by atmospheric oxidation of primary emitted precursors is a major contributor to fine particulate matter (PM2.5) air pollution worldwide. Observations during winter haze pollution episodes in urban China show that most of this SOA originates from fossil-fuel combustion but the chemical mechanisms involved are unclear. Here we report field observations in a Beijing winter haze event that reveal fast aqueous-phase conversion of fossil-fuel primary organic aerosol (POA) to SOA at high relative humidity. Analyses of aerosol mass spectra and elemental ratios indicate that ring-breaking oxidation of POA aromatic species, leading to functionalization as carbonyls and carboxylic acids, may serve as the dominant mechanism for this SOA formation. A POA origin for SOA could explain why SOA has been decreasing over the 2013-2018 period in response to POA emission controls even as emissions of volatile organic compounds (VOCs) have remained flat.

2.
Environ Sci Technol ; 57(48): 20043-20052, 2023 Dec 05.
Artículo en Inglés | MEDLINE | ID: mdl-37992316

RESUMEN

Levoglucosan (LG) is a pyrolysis product of cellulose and hemicellulose at low combustion temperatures. However, LG release cannot be determined only by considering the contents of cellulose and hemicellulose exclusively due to the complexity of combustion processes and the physical-chemical properties of the fuel. This study detected the emission factors (EFs) of LG from 22 different solid fuel samples (including coal and biomass) by considering 18 different fuel properties and five combustion parameters. The average LGEFs during solid fuel burning varied in a range of 0.03-136 mg kg-1, with a magnitude difference of 1-4 orders. While the variations in cellulose (59.5-368 mg g-1) and hemicellulose (73.5-165 mg g-1) contents of fuel samples were only one- to 6-fold. A short combustion duration (<150 min) and a medium combustion temperature (200-400 °C) influenced by volatile and ash contents are crucial for the generation and accumulation of LG. A random forest coupled with the Akaike information criterion stepwise regression model successfully explained 96% of the total LG emission variation using three variables (ash content, cellulose content, and modified combustion efficiency). The ash content promoted coke formation and LG chain cracking by increasing the pyrolysis temperature and is considered the most important factor. The alkali metal in ash can reduce the energy barrier of intramolecular ring contraction reactions and inhibit the dehydration reactions, which led to additional heat being utilized by the competitive pathways of LG formation. This study provided a method to address the parametrization and release mechanisms of combustion source emissions.


Asunto(s)
Contaminantes Atmosféricos , Carbón Mineral , Carbón Mineral/análisis , Glucosa , Temperatura , Celulosa , Contaminantes Atmosféricos/análisis
3.
J Environ Manage ; 340: 117965, 2023 Aug 15.
Artículo en Inglés | MEDLINE | ID: mdl-37121003

RESUMEN

Straw return can improve crop yield as well as soil organic carbon (SOC) but may raise the possibility of N2O and CH4 emissions. However, few studies have compared the effects of straw return on the yield, SOC, and N2O emissions of various crops. Which management strategies are the best for balancing yield, SOC, and emission reduction for various crops needs to be clarified. A meta-analysis containing 2269 datasets collected from 369 studies was conducted to investigate the influence of agricultural management strategies on yield increase, soil carbon sequestration, and emission reduction in various crops after the straw return. Analytical results indicated that, on average, straw return increased the yield of rice, wheat, and maize by 5.04%, 8.09%, and 8.71%, respectively. Straw return increased maize N2O emissions by 14.69% but did not significantly affect wheat N2O emissions. Interestingly, straw return reduced the rice N2O emissions by 11.43% but increased the CH4 emissions by 72.01%. The recommended nitrogen application amounts for balancing yield, SOC, and emission reduction varied among the three crops, while the recommended straw return amounts were more than 9000 kg/ha. The optimal tillage and straw return strategies for rice, wheat, and maize were plow tillage combined with incorporation, rotary tillage combined with incorporation, and no-tillage combined with mulching, respectively. A straw return duration of 5-10 years for rice and maize and ≤5 years for wheat was recommended. These findings provide optimal agricultural management strategies after straw return to balance the crop yield, SOC, and emission reduction for China's three major grain crops.


Asunto(s)
Oryza , Suelo , Secuestro de Carbono , Carbono/análisis , Agricultura/métodos , Productos Agrícolas , Zea mays , Triticum/metabolismo , Grano Comestible/química , China , Óxido Nitroso/metabolismo
4.
Environ Sci Technol ; 56(11): 7163-7173, 2022 06 07.
Artículo en Inglés | MEDLINE | ID: mdl-35483018

RESUMEN

The interaction between water vapor and atmospheric aerosol leads to enhancement in aerosol water content, which facilitates haze development, but its concentrations, sources, and impacts remain largely unknown in polluted urban environments. Here, we show that the Indian capital, Delhi, which tops the list of polluted capital cities, also experiences the highest aerosol water yet reported worldwide. This high aerosol water promotes secondary formation of aerosols and worsens air pollution. We report that severe pollution events are commonly associated with high aerosol water which enhances light scattering and reduces visibility by 70%. Strong light scattering also suppresses the boundary layer height on winter mornings in Delhi, inhibiting dispersal of pollutants and further exacerbating morning pollution peaks. We provide evidence that ammonium chloride is the largest contributor to aerosol water in Delhi, making up 40% on average, and we highlight that regulation of chlorine-containing precursors should be considered in mitigation strategies.


Asunto(s)
Contaminantes Atmosféricos , Contaminación del Aire , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Contaminación del Aire/análisis , Cloruro de Amonio , China , Monitoreo del Ambiente , India , Material Particulado/análisis , Estaciones del Año
5.
Environ Sci Technol ; 56(18): 12873-12885, 2022 09 20.
Artículo en Inglés | MEDLINE | ID: mdl-36083258

RESUMEN

The light-absorbing organic aerosol (OA) constitutes an important fraction of absorbing components, counteracting major cooling effect of aerosols to climate. The mechanisms in linking the complex and changeable chemistry of OA with its absorbing properties remain to be elucidated. Here, by using solvent extraction, ambient OA from an urban environment was fractionated according to polarity, which was further nebulized and online characterized with compositions and absorbing properties. Water extracted high-polar compounds with a significantly higher oxygen to carbon ratio (O/C) than methanol extracts. A transition O/C of about 0.6 was found, below and above which the enhancement and reduction of OA absorptivity were observed with increasing O/C, occurring on the less polar and high polar compounds, respectively. In particular, the co-increase of nitrogen and oxygen elements suggests the important role of nitrogen-containing functional groups in enhancing the absorptivity of the less polar compounds (e.g., forming nitrogen-containing aromatics), while further oxidation (O/C > 0.6) on high-polar compounds likely led to fragmentation and bleaching chromophores. The results here may reconcile the previous observations about darkening or whitening chromophores of brown carbon, and the parametrization of O/C has the potential to link the changing chemistry of OA with its polarity and absorbing properties.


Asunto(s)
Contaminantes Atmosféricos , Metanol , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Carbono/análisis , Nitrógeno , Oxígeno , Material Particulado/análisis , Solventes , Agua/química
6.
Environ Res ; 211: 113107, 2022 08.
Artículo en Inglés | MEDLINE | ID: mdl-35305979

RESUMEN

The oxidation of polycyclic aromatic hydrocarbons (PAHs) determines their lifetime, toxicity and consequent environmental and climate impacts. The residential solid fuel burning composes of a substantial fraction of PAH emissions; however, their oxidation rate is yet to be explicitly understood, which is complicated by the contrasting emission factors under different combustion conditions and their subsequent evolution in the atmosphere. Here we used a plume evolution chamber using ambient oxidants to simulate the evolution of residential solid fuel burning emissions under real-world solar radiation, and then to investigate the oxidation process of the emitted PAHs. Contrasting oxidation rate of PAHs was found to be influenced by particles with or without presence of substantial amount of black carbon (BC). In the flaming burning phase, which contained 46% of BC mass fraction and 8% of organic aerosol (OA) internally mixed with BC, the larger PAHs (with 4-7 rings) was rapidly oxidized 12% for every hour of evolution under solar radiation; however, the larger PAHs from smoldering phase tended to maintain unmodified during the evolution, when 95% of OA was externally mixed with only minor fraction of BC (<5%). This may be ascribed to the complex morphology of BC, allowing more exposure for the internally-mixed OA to the oxidants; in contrast with those externally-mixed OA which was prone to be coated by condensed secondary substances. This raises an important consideration about the particle mixing state in influencing the oxidation of PAHs, particularly the coating on PAHs which may extend their lifetime and environmental impacts.


Asunto(s)
Contaminantes Atmosféricos , Hidrocarburos Policíclicos Aromáticos , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Biomasa , Monitoreo del Ambiente , Oxidantes , Hidrocarburos Policíclicos Aromáticos/análisis , Hollín
7.
J Environ Manage ; 322: 116099, 2022 Nov 15.
Artículo en Inglés | MEDLINE | ID: mdl-36058069

RESUMEN

Appropriate nitrogen (N) application increases crop yield, while its unreasonable application results in environmental problem. Determining the appropriate N application rate is the key to sustainable development. Here, the denitrification-decomposition (DNDC) model was used to analyze the effects of N fertilizer on maize yields, economic benefits, nitrate leaching, and nitrous oxide emissions in China. The N application rate for the trade-off between economy and environment at the county scale was further determined. The geodetector model was used to identify the main driving factors and their interactions of the recommended N rate in each agricultural zone. The results showed that the recommended N rate was generally high in the northwest but low in the south, consistent with the spatial patterns of yield potential. However, clay soils with clay ratios greater than 34% in southern China and sandy soils with bulk densities greater than 1.5 g cm-3 on the Huanghuaihai Plain experienced high N levels and low yields, and thus soils need to be improved. Potential grain yield was the main driving factor in most zones, yet its effects gradually weakened from north to south. The influence of soil characteristics increased from north to south. It was found that the current average N application rate of farmers in China was 249 kg N/ha, and 86.55% of counties had excessive N applications. Compared to the regional optimal N rate at a regional scale, a differentiated N application strategy at the county scale determined in this study increased maize yield and economic benefit by 10.51% and 10.85%, respectively, and reduced N2O emissions and NO3- leaching by 28.72% and 33.60%, respectively. The current research provides a scientific basis for China to formulate a win-win N management strategy for economy and environment and provides a method reference for other countries.


Asunto(s)
Fertilizantes , Nitrógeno , Agricultura/métodos , China , Arcilla , Análisis Factorial , Fertilizantes/análisis , Nitratos/análisis , Nitrógeno/análisis , Óxido Nitroso/análisis , Suelo , Zea mays
8.
J Environ Sci (China) ; 114: 136-148, 2022 Apr.
Artículo en Inglés | MEDLINE | ID: mdl-35459479

RESUMEN

The atmospheric chemistry in complex air pollution remains poorly understood. In order to probe how environmental conditions can impact the secondary organic aerosol (SOA) formation from biomass burning emissions, we investigated the photooxidation of 2,5-dimethylfuran (DMF) under different environmental conditions in a smog chamber. It was found that SO2 could promote the formation of SOA and increase the amounts of inorganic salts produced during the photooxidation. The formation rate of SOA and the corresponding SOA mass concentration increased gradually with the increasing DMF/OH ratio. The addition of (NH4)2SO4 seed aerosol accelerated the SOA formation rate and significantly shortened the time for the reaction to reach equilibrium. Additionally, a relatively high illumination intensity promoted the formation of OH radicals and, correspondingly, enhanced the photooxidation of DMF. However, the enhancement of light intensity accelerated the aging of SOA, which led to a gradual decrease of the SOA mass concentration. This work shows that by having varying influence on atmospheric chemical reactions, the same environmental factor can affect SOA formation in different ways. The present study is helpful for us to better understand atmospheric complex pollution.


Asunto(s)
Contaminantes Atmosféricos , Contaminación del Aire , Aerosoles , Contaminantes Atmosféricos/análisis , Biomasa , Oxidación-Reducción , Esmog
9.
Faraday Discuss ; 226: 239-254, 2021 Mar 01.
Artículo en Inglés | MEDLINE | ID: mdl-33241817

RESUMEN

The hygroscopicity and ability of aerosol particles to act as cloud condensation nuclei (CCN) is important in determining their lifetime and role in aerosol-cloud interactions, thereby influencing cloud formation and climate. Previous studies have used the aerosol hygroscopic properties measured at the ground to evaluate the influence on cloud formation in the atmosphere, which may introduce uncertainty associated with aerosol hygroscopicity variability with altitude. In this study, the CCN behaviour and hygroscopic properties of daily filter collections of PM2.5 from three different heights (8, 120, 260 m) on a tower in Beijing were determined in the laboratory using water, water/methanol and methanol as the atomization solvents. Whilst there was substantial temporal variability in particle concentration and composition, there was little obvious difference in aerosol CCN and hygroscopic behaviour at different heights, although the planetary boundary layer height (PBLH) reduced to below the tower height during the nighttime, suggesting that use of surface hygroscopicity measurements is sufficient for the estimation of aerosol particle activation in clouds. Additionally, the critical coating thickness (in terms of mass ratio of coating/refractory BC, MRc) defining the BC transition between being hydrophobic to hydrophilic, was determined by combining hygroscopic tandem differential mobility analyser (H-TDMA), centrifugal particle mass analyzer (CPMA) and single particle soot photometer (SP2) measurements. The MRc of 250 nm BC-containing particles increased from a background value of between 0.8 and 1.6 to around 4.6 at the onset of the growth event of nanoparticles, decreasing monotonically back to the background level as the event progressed. This indicates that large particles do not act as an effective pre-existing condensation sink of the hygroscopic vapours during the nanoparticle growth events, leading to the 250 nm BC particles requiring more coating materials to transition between being hydrophobic and hydrophilic. These findings show that large particles may be less important in suppressing the new particle formation and subsequent growth in the atmosphere.

10.
Faraday Discuss ; 226: 382-408, 2021 03 01.
Artículo en Inglés | MEDLINE | ID: mdl-33475668

RESUMEN

Organic aerosols, a major constituent of fine particulate mass in megacities, can be directly emitted or formed from secondary processing of biogenic and anthropogenic volatile organic compound emissions. The complexity of volatile organic compound emission sources, speciation and oxidation pathways leads to uncertainties in the key sources and chemistry leading to formation of organic aerosol in urban areas. Historically, online measurements of organic aerosol composition have been unable to resolve specific markers of volatile organic compound oxidation, while offline analysis of markers focus on a small proportion of organic aerosol and lack the time resolution to carry out detailed statistical analysis required to study the dynamic changes in aerosol sources and chemistry. Here we use data collected as part of the joint UK-China Air Pollution and Human Health (APHH-Beijing) collaboration during a field campaign in urban Beijing in the summer of 2017 alongside laboratory measurements of secondary organic aerosol from oxidation of key aromatic precursors (1,3,5-trimethyl benzene, 1,2,4-trimethyl benzene, propyl benzene, isopropyl benzene and 1-methyl naphthalene) to study the anthropogenic and biogenic contributions to organic aerosol. For the first time in Beijing, this study applies positive matrix factorisation to online measurements of organic aerosol composition from a time-of-flight iodide chemical ionisation mass spectrometer fitted with a filter inlet for gases and aerosols (FIGAERO-ToF-I-CIMS). This approach identifies the real-time variations in sources and oxidation processes influencing aerosol composition at a near-molecular level. We identify eight factors with distinct temporal variability, highlighting episodic differences in OA composition attributed to regional influences and in situ formation. These have average carbon numbers ranging from C5-C9 and can be associated with oxidation of anthropogenic aromatic hydrocarbons alongside biogenic emissions of isoprene, α-pinene and sesquiterpenes.


Asunto(s)
Contaminantes Atmosféricos , Material Particulado , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Beijing , Humanos , Espectrometría de Masas , Material Particulado/análisis
11.
Environ Sci Technol ; 55(9): 5677-5688, 2021 05 04.
Artículo en Inglés | MEDLINE | ID: mdl-33874721

RESUMEN

Emissions of light-absorbing black carbon (BC) and organic aerosol (OA) from biomass burning are presented as complex mixtures, which introduce challenges in modeling their absorbing properties. In this study, we chose typical residential wood burning emission and used a novel designed chamber to investigate the early stage evolution of plumes from different burning phases under real ambient conditions. The detailed mixing state between BC and OA was evaluated, on the basis of which optical modeling was performed to achieve a closure of aerosol-absorbing properties. Intensive secondary OA (SOA) formation was observed under solar radiation. OA from flaming conditions showed a higher absorptivity than from smoldering conditions, as OA is mostly internally and externally mixed with BC, respectively. For flaming (smoldering), the imaginary refractive index of OA (kOA) was initially at 0.03 ± 0.01 (0.001) and 0.15 ± 0.02 (0.05 ± 0.02) at λ = 781 and 405 nm, respectively, with a half-decay time of 2-3 h in light but a <40% decrease under dark within 5 h. The production of less-absorbing SOA in the first 1-2 h and possible subsequent photobleaching of chromophores contributed to the decrease of kOA. The enhanced abundance but decreased absorptivity of coatings on BC resulted in a relatively maintainable absorptivity of BC-containing particles during evolution.


Asunto(s)
Contaminantes Atmosféricos , Madera , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Atmósfera , Biomasa , Carbono , Humo , Hollín/análisis , Madera/química
12.
Environ Sci Technol ; 55(3): 1497-1507, 2021 02 02.
Artículo en Inglés | MEDLINE | ID: mdl-33423493

RESUMEN

Levoglucosan (LG) emitted from non-biomass burning (non-BB) sources has given rise to biased or even unreasonable source identification results when adopting LG as a distinct marker of biomass burning (BB). The estimation of LG emission and its spatiotemporal variation for various sources are the keys to reducing uncertainty. This study first developed a LG emission inventory for China from 25 sub-type sources belonging to eight categories, with a 3 km × 3 km spatial resolution and monthly distribution. The total LG emission in 2014 was 145.7 Gg. Domestic BB and open BB contributed 39.2 and 34.3% of the total emission. Non-BB sources, including municipal solid waste burning (9.7%), firework burning (9.6%), meat cooking (5.4%), domestic coal burning (1.5%), ritual item burning (0.2%), and industrial coal burning (0.1%), contributed to 26.5% of the total emission. LG emission varied spatially and temporally. Non-BB sources have a significant spatiotemporal impact on BB source contributions, even in high BB emission regions or in sowing, harvesting, and winter heating seasons. The local BB contributions have been substantially overestimated by 4.28-369% in previous studies, wherein LG was solely referred to as the BB source. By 2018, LG emission from BB might decrease to 63.9% of its total emission. This high-resolution LG emission inventory can be greatly useful for source identification studies in China. It also supports future research on the modeling of smoke aging and pollution control.


Asunto(s)
Contaminantes Atmosféricos , Material Particulado , Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Biomasa , China , Monitoreo del Ambiente , Glucosa/análogos & derivados , Material Particulado/análisis , Estaciones del Año
13.
Plant Cell Physiol ; 61(1): 118-129, 2020 Jan 01.
Artículo en Inglés | MEDLINE | ID: mdl-31532486

RESUMEN

Cyperus esculentus is probably the only plant that is known to accumulate large amounts of oil in its tubers. However, the underlying metabolic mechanism and regulatory factors involved in oil synthesis of tubers are still largely unclear. In this study, one gene encoding type I diacylglycerol acyltransferase (DGAT) (CeDGAT1) and two genes encoding type II DGAT (CeDGAT2a and CeDGAT2b) from C. esculentus were identified and functionally analyzed. All three DGAT genes were found to be expressed in tuber, root and leaf tissues. CeDGAT1 is highly expressed in roots and leaves, whereas CeDGAT2b is dominantly expressed in tubers. Furthermore, the temporal expression pattern of CeDGAT2b is well coordinated with the oil accumulation in developing tubers. When each CeDGAT was heterologously expressed in triacylglycerol (TAG)-deficient mutant of Saccharomyces cerevisiae, Arabidopsis thaliana wild type or its TAG1 mutant with AtDGAT1 disruption, only CeDGAT2b showed the ability to restore TAG biosynthesis with lipid body formation in yeast mutant, enhance seed oil production of Arabidopsis wild type and rescue multiple seed phenotypes of TAG1 mutant. In addition, CeDGAT2b was shown to have a substrate preference for unsaturated fatty acids toward TAG synthesis. Taken together, our results indicated that CeDGAT2b from C. esculentus is an actively functional protein and is most likely the major contributor to tuber oil biosynthesis containing common fatty acids, in contrast to oil-rich seeds and fruits where DGAT1 plays a more central role than DGAT2 in oil production accumulating normal fatty acids, whereas DGAT2 is a primary regulator for oil synthesis rich in unusual fatty acids.


Asunto(s)
Cyperus/genética , Diacilglicerol O-Acetiltransferasa/genética , Genes de Plantas , Aceites de Plantas/metabolismo , Tubérculos de la Planta/metabolismo , Secuencia de Aminoácidos , Arabidopsis/genética , Arabidopsis/metabolismo , Proteínas de Arabidopsis/genética , Proteínas de Arabidopsis/metabolismo , Clonación Molecular , Cyperus/metabolismo , Diacilglicerol O-Acetiltransferasa/metabolismo , Ácidos Grasos/análisis , Frutas/genética , Frutas/metabolismo , Regulación de la Expresión Génica de las Plantas , Germinación , Estructura Molecular , Hojas de la Planta/metabolismo , ARN de Planta/genética , ARN de Planta/aislamiento & purificación , Saccharomyces cerevisiae/genética , Saccharomyces cerevisiae/metabolismo , Semillas/genética , Semillas/metabolismo , Triglicéridos/metabolismo
14.
Environ Sci Technol ; 54(24): 15604-15612, 2020 12 15.
Artículo en Inglés | MEDLINE | ID: mdl-33206512

RESUMEN

Commercial shipping is considered as an important source of air pollution and cloud condensation nuclei (CCN). To assess the climatic and environmental impacts of shipping, detailed characterization of ship plumes near the point of emission and understanding of ship plume evolution further downwind are essential. This airborne measurement study presents the online characterization of particulate phase ship emissions in the region of Western Europe in 2019 prior to new international sulfur emission controls becoming enacted. More than 30 ships from both the sulfur emission control area (SECA) in the English Channel and the open sea (OS) are measured and compared. Ships within the SECA emitted much less sulfate (SO4) compared with those at OS. When shifted to a lower apparent fuel sulfur content (FSC) at similar engine loads, the peak of the fresh ship emitting the particle number size distribution shifted from around 60-80 nm in diameter to below 40 nm in diameter. The emission factors (EFs) of sulfate are predicted to decrease by around 94% after the 2020 regulation on ship sulfur emission in the open ocean. The EFs of refractory black carbon (rBC) and organic compounds (Org) do not appear to be directly affected by the lower sulfur contents. The total number concentration for condensation nuclei (CN) >2.5 nm and >0.1 µm are predicated to be reduced by 69 and 56%, respectively. Measured plume evolution results indicate that the S(IV) to S(VI) conversion rate was around 23.4% per hour at the beginning of plume evolution, and the CCN and CN >2.5 nm ratio increased with plume age primarily due to condensation and coagulation. We estimate that the new sulfur emission regulation will lead to a reduction of more than 80% in CCN from fresh ship emissions. The ship-emitted EFs results presented here will also inform emission inventories, policymaking, climate, and human health studies.


Asunto(s)
Contaminantes Atmosféricos , Navíos , Contaminantes Atmosféricos/análisis , Monitoreo del Ambiente , Europa (Continente) , Humanos , Material Particulado/análisis , Emisiones de Vehículos/análisis
15.
Geophys Res Lett ; 47(23): e2020GL090444, 2020 Dec 16.
Artículo en Inglés | MEDLINE | ID: mdl-33349736

RESUMEN

Black carbon (BC) not only warms the atmosphere but also affects human health. The nationwide lockdown due to the Coronavirus Disease 2019 (COVID-19) pandemic led to a major reduction in human activity during the past 30 years. Here, the concentration of BC in the urban, urban-industry, suburb, and rural areas of a megacity Hangzhou were monitored using a multiwavelength Aethalometer to estimate the impact of the COVID-19 lockdown on BC emissions. The citywide BC decreased by 44% from 2.30 to 1.29 µg/m3 following the COVID-19 lockdown period. The source apportionment based on the Aethalometer model shows that vehicle emission reduction responded to BC decline in the urban area and biomass burning in rural areas around the megacity had a regional contribution of BC. We highlight that the emission controls of vehicles in urban areas and biomass burning in rural areas should be more efficient in reducing BC in the megacity Hangzhou.

16.
Environ Sci Technol ; 53(24): 14212-14221, 2019 12 17.
Artículo en Inglés | MEDLINE | ID: mdl-31722174

RESUMEN

The hygroscopic properties of BC-containing particles (BCc) are important to determine their wet scavenging, atmospheric lifetime, and interactions with clouds. Such information is still lacking in the real world because of the challenges in isolating BCc from other aerosols to be directly characterized. In this study, the size-resolved chemical components of BCc including the refractory BC core and associated coatings were measured by a soot particle-aerosol mass spectrometer in suburban Nanjing. The size-resolved hygroscopicity parameter of BCc (κBCc) was obtained based on this full chemical characterization of BCc. We found increased inorganic fraction and more oxidized organic coatings with thicker coatings, which modified κBCc besides the determinant of particle size. The bulk κBCc was observed to range from 0.11 to 0.34. The size-resolved κBCc consistently showed minima at coated diameter (Dcoated) of 100 nm, parametrized as κ(x) = 0.28-0.35 × exp(-0.004 × x), x = Dcoated. Under critical supersaturations (SS) of 0.1% and 0.2%, the D50 values of BCc were 200 ± 20 and 135 ± 18 nm, respectively. On average 33 ± 16% and 59 ± 20% of BCc in number could be activated at SS = 0.1% and 0.2%, respectively. These results provide constraints on surface CCN sources for the light-absorbing BC-containing particles.


Asunto(s)
Contaminantes Atmosféricos , Hollín , Aerosoles , Carbono , Tamaño de la Partícula , Humectabilidad
17.
Environ Sci Technol ; 53(19): 11112-11121, 2019 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-31423774

RESUMEN

The size-resolved properties of atmospheric black carbon (BC) importantly determine its absorption capacity and cloud condensation nuclei (CCN) ability. This study reports comprehensive vertical profiles of BC size-related properties over the Beijing area (BJ) and Continental Europe (CE). BC mass loadings over CE were in the range of clean background over BJ. For both planetary boundary layer (PBL) and lower free troposphere, the BC mass median core diameter over BJ during the cold season was 0.21 ± 0.02 µm, larger than the warm season over BJ and CE (0.18 ± 0.01 µm), which may reflect seasonal differences in emissions. The BC coatings were positively correlated with the pollution level, with background BC having a smaller coated count median diameter (0.19 ± 0.01 µm). The modeled absorption enhancement (Eabs) due to coatings was 1.23 ± 0.14 for the background but in the PBL following a linear expression (Eabs = 0.13 × MassBC,surface + 1.26). The CCN ability of BC was significantly enhanced in the polluted PBL, due to both enlarged size and increased hygroscopicity. In polluted BJ at predicted supersaturations, ∼0.08% half of the BC number could be activated, whereas the cleaner environment needs ∼0.14%. The results here suggest that the highly coated and absorbing BC can be efficiently incorporated into clouds and can exert important indirect radiative impacts over the polluted East Asia region.


Asunto(s)
Contaminantes Atmosféricos , Aerosoles , Atmósfera , Carbono , Monitoreo del Ambiente , Europa (Continente) , Asia Oriental
18.
Anal Chem ; 90(6): 3906-3913, 2018 03 20.
Artículo en Inglés | MEDLINE | ID: mdl-29316399

RESUMEN

5-(Hydroxymethyl)-2'-deoxycytidine (5-hmdC), 5-(formyl)-2'-deoxycytidine (5-fodC), and 5-(carboxyl)-2'-deoxycytidine (5-cadC) are crucial intermediate products of the DNA demethylation pathway, which can also act as potential biomarkers reflecting the diagnosis and prognosis in multiple tumors. Detecting 5-hmdC, 5-fodC, and 5-cadC in human urine has various advantages including readily available samples and being noninvasive to patients. However, few works have reported the detection of 5-fodC and 5-cadC due to their trace amounts. Here we developed a novel magnetic hyper-cross-linked microporous polymer (HMP) material based on polyionic liquid (PIL) for the enrichment of 5-hmdC, 5-fodC, and 5-cadC. These magnetic PIL-HMP materials provided specific enrichment superiority for three modified cytidines. After enrichment, the signal intensity of 5-hmdC, 5-fodC, and 5-cadC increased 10-75-fold with lower limits of quantitation (LLOQ) of 0.049, 0.781, and 0.781 ng/mL, respectively. The recoveries were approximately 86.5-95.2% for 5-hmdC, 95.2-107.8% for 5-fodC, and 99.4-102.4% for 5-cadC under the relative standard deviation (RSD) of 0.2-10.3%. Finally, we successfully applied magnetic PIL-HMP materials coupled with high-performance liquid chromatography-electrospray ionization tandem mass spectrometry (HPLC-ESI-MS/MS) in enrichment and quantitative determination of 5-hmdC, 5-fodC, and 5-cadC in human urine of 10 breast cancer patients and 10 healthy people. We found that the level of 5-hmdC decreased in breast cancer patients ( p < 0.05), while the levels of 5-fodC and 5-cadC increased ( p < 0.05, p < 0.01). Our results demonstrated that the levels of metabolic 5-hmdC, 5-fodC, and 5-cadC in human urine are closely related to breast cancer, which could contribute to the clinical diagnosis and investigation of breast cancer and its occurrence and development mechanisms.


Asunto(s)
Neoplasias de la Mama/orina , Desoxicitidina/análogos & derivados , Desoxicitidina/orina , Líquidos Iónicos/química , Nanopartículas de Magnetita/química , Polímeros/química , Adsorción , Cromatografía Líquida de Alta Presión/métodos , Desoxicitidina/aislamiento & purificación , Disomnias , Femenino , Humanos , Extracción en Fase Sólida/métodos , Espectrometría de Masa por Ionización de Electrospray/métodos , Espectrometría de Masas en Tándem/métodos
19.
BMC Plant Biol ; 18(1): 151, 2018 Jul 24.
Artículo en Inglés | MEDLINE | ID: mdl-30041609

RESUMEN

BACKGROUND: Cyperus esculentus is unique in that it can accumulate significant amounts of oil, starch and sugar as major storage reserves in tubers with high tuber yield and therefore considered as a novel model to study carbon allocation into different storage reserves in underground sink tissues such as tubers and roots. Sucrose (Suc) plays a central role in control of carbon flux toward biosynthesis of different storage reserves; however, it remains unclear for the molecular mechanism underlying Suc metabolism in underground oil-rich storage tissues. In the present study, a comprehensive transcriptome analysis of C. esculentus oil tuber compared to other plant oil- or carbohydrate-rich storage tissues was made for the expression patterns of genes related to the Suc metabolism. RESULTS: The results revealed some species-specific features of gene transcripts in oil tuber of C. esculentus, indicating that: (i) the expressions of genes responsible for Suc metabolism are developmentally regulated and displayed a pattern dissimilar to other plant storage tissues; (ii) both of Suc breakdown and biosynthesis processes might be the major pathways associated with Suc metabolism; (iii) it was probably that Suc degradation could be primarily through the action of Suc synthase (SUS) other than invertase (INV) during tuber development. The orthologs of SUS1, SUS3 and SUS4 are the main SUS isoforms catalyzing Suc breakdown while the vacuolar INV (VIN) is the leading determinant controlling sugar composition; (iv) cytosolic hexose phosphorylation possibly relies more on fructose as substrate and uridine diphosphate glucose pyrophosphorylase (UGP) plays an important role in this pathway; (v) it is Suc-phosphate synthase (SPS) B- and C-family members rather than SPS A that are the principal contributors to SPS enzymes and play crucial roles in Suc biosynthesis pathway. CONCLUSIONS: We have successfully identified the Suc metabolic pathways in C. esculentus tubers, highlighting several conserved and distinct expressions that might contribute to sugar accumulation in this unique underground storage tissue. The specific and differential expression genes revealed in this study might indicate the special molecular mechanism and transcriptional regulation of Suc metabolism occurred in oil tubers of C. esculentus.


Asunto(s)
Cyperus/metabolismo , Aceites de Plantas/metabolismo , Tubérculos de la Planta/metabolismo , Sacarosa/metabolismo , Perfilación de la Expresión Génica , Redes y Vías Metabólicas , Transcriptoma
20.
Environ Sci Technol ; 52(12): 6912-6919, 2018 06 19.
Artículo en Inglés | MEDLINE | ID: mdl-29783837

RESUMEN

The radiative forcing of black carbon aerosol (BC) is one of the largest sources of uncertainty in climate change assessments. Contrasting results of BC absorption enhancement ( Eabs) after aging are estimated by field measurements and modeling studies, causing ambiguous parametrizations of BC solar absorption in climate models. Here we quantify Eabs using a theoretical model parametrized by the complex particle morphology of BC in different aging scales. We show that Eabs continuously increases with aging and stabilizes with a maximum of ∼3.5, suggesting that previous seemingly contrast results of Eabs can be explicitly described by BC aging with corresponding particle morphology. We also report that current climate models using Mie Core-Shell model may overestimate Eabs at a certain aging stage with a rapid rise of Eabs, which is commonly observed in the ambient. A correction coefficient for this overestimation is suggested to improve model predictions of BC climate impact.


Asunto(s)
Carbono , Hollín , Aerosoles , Modelos Teóricos , Luz Solar
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