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1.
Chemosphere ; 364: 143095, 2024 Aug 13.
Artículo en Inglés | MEDLINE | ID: mdl-39146995

RESUMEN

The presence of organic compounds on the particulate matter (PM) or aerosols can arise from the condensation of gaseous organic compounds on the existing aerosols, or from organic precursors to form secondary organic aerosols (SOA) through photochemistry. The objective of this study is to characterize organic constituents on aerosols relevant to their emission sources and the key compounds revealing the evolution of aerosols with the use of a novel analytical technique. A time-of-flight mass spectrometry (TOFMS) coupled with comprehensive two-dimensional gas chromatography (GC×GC) was developed using a flow type of modulator instead of a thermal type as a prelude to field applications without the need for cryogen. The methodology of GC×GC-TOFMS is discussed in this study in detail. Since the coarse PM (PM10-2.5) may exhibit with a relatively high OC content compared to PM2.5, the GC×GC results have been obtained by analyzing PM10 samples collected in parallel with OC/EC analysis of PM2.5 samples at the Lulin Atmospheric Background Station (LABS, 23.47°N, 120.87°E, 2862 m ASL) as the high-mountain background site in East Asia. We found that the organic analytes were in a majority in the range of 12-30 carbon numbers falling in the category of semi-volatile organic compounds (SVOCs) with 43 compounds of alcohol, aldehyde, ketone, and ester varieties if excluding alkanes. Intriguingly, trace amounts of plasticizers and phosphorus flame retardants such as phthalates (PAEs) and triphenyl phosphate (TPP) were also found, likely originating from regions involved in open burning of household solid waste in Southeast Asia or e-waste recycling in southern China and along the long-range transport route. Compounds such as these are unique to the specific sources, demonstrating the wide spread of these hazardous compounds in the environment.

2.
Environ Pollut ; 358: 124496, 2024 Oct 01.
Artículo en Inglés | MEDLINE | ID: mdl-38964642

RESUMEN

Biomass burning play a key role in the global carbon cycle by altering the atmospheric composition, and affect regional and global climate. Despite its importance, a very few high-resolution records are available worldwide, especially for recent climate change. This study analyzes levoglucosan, a specific tracer of biomass burning emissions, in a 38-year ice core retrieved from the Shulehe Glacier No. 4, northeastern Tibetan Plateau. The levoglucosan concentration in the Shulehe Glacier No. 4 ice core ranged from 0.1 to 55 ng mL-1, with an average concentration of 8 ± 8 ng mL-1. The concentrations showed a decreasing trend from 2002 to 2018. Meanwhile, regional wildfire activities in Central Asian also exhibited a declining trend during the same period, suggesting the potential correspondence between levoglucosan concentration of the Shulehe Glacier No. 4 ice core and the fire activity of Central Asia. Furthermore, a positive correlation also exists between the levoglucosan concentration of the Shulehe Glacier No. 4 ice core and the wildfire counts in Central Asia from 2002 to 2018. While backward air mass trajectory analysis and fire spots data showed a higher distribution of fire counts in South Asia compared to Central Asia, but the dominance of westerly circulation in the northern TP throughout the year. Therefore, the levoglucosan in the Shulehe Glacier No. 4 provides clear evidence of Central Asian wildfire influence on Tibetan Plateau glaciers through westerlies. This highlights a great importance of ice core data for wildfire history reconstruction in the Tibetan Plateau Glacier regions.


Asunto(s)
Contaminantes Atmosféricos , Biomasa , Monitoreo del Ambiente , Cubierta de Hielo , Tibet , Cubierta de Hielo/química , Monitoreo del Ambiente/métodos , Contaminantes Atmosféricos/análisis , Incendios Forestales , Cambio Climático , Incendios , Glucosa/análogos & derivados , Glucosa/análisis
3.
ChemistryOpen ; : e202300311, 2024 May 29.
Artículo en Inglés | MEDLINE | ID: mdl-38809079

RESUMEN

Pyrolysis-based saccharification consisting of fast pyrolysis followed by hydrolysis of the resulting anhydrosugars such as levoglucosan is a promising method for converting cellulosic biomass into glucose that can be used for producing biofuels and biochemicals. In the present study, hydrolysis of levoglucosan was evaluated in water with a polystyrene sulfonic acid resin (a solid acid catalyst) by heating under microwave irradiation or in an oil bath at 95 °C-120 °C. When the equilibrium temperature of the solution was the same, the conversion rate of levoglucosan was greater under microwave irradiation than in an oil bath. Model experiments indicate that the sulfonyl groups of the solid acid catalyst were selectively heated by microwave irradiation. The temperature of the reaction solution in the vicinity of the catalyst was locally higher than the equilibrium temperature of the solution, which enabled hydrolysis to proceed efficiently.

4.
Bioresour Technol ; 400: 130667, 2024 May.
Artículo en Inglés | MEDLINE | ID: mdl-38583674

RESUMEN

Due to the complexity of biomass structures, the conversion of raw biomass into value-added chemicals is challenging and often requires efficient pretreatment of the biomass. In this paper, a simple and green pre-oxidation method, which was conducted under the conditions of 2 wt% H2O2, 80 min, and 150 °C, was reported to significantly increase the production of levoglucosan (LG) from biomass pyrolysis. The result showed that the LG yield significantly increased from 2.3 wt% (without pre-oxidation) to 23.1 wt% when pine wood was employed as a sample for pyrolysis at 400 °C, resulting from the removal of hemicellulose fraction and the in-situ acid catalysis of lignin carboxyl groups formed during the pre-oxidation. When the conditions for pre-oxidation became harsher than the above, the LG yield reduced because the decomposition of cellulose fraction in biomass. The study supplies an effective method for utilization of biomass as chemicals.


Asunto(s)
Biomasa , Glucosa , Glucosa/análogos & derivados , Peróxido de Hidrógeno , Oxidación-Reducción , Pirólisis , Peróxido de Hidrógeno/química , Glucosa/química , Madera/química , Pinus/química , Lignina/química , Lignina/análogos & derivados
5.
Chemosphere ; 357: 142073, 2024 Jun.
Artículo en Inglés | MEDLINE | ID: mdl-38641289

RESUMEN

Open biomass burning (BB) events are a well-known primary aerosol source, resulting in the emission of significant amount of gaseous and particulate matter and affecting Earth's radiation budget. The 2019-2020 summer, known as "Australian Black Summer", showed exceptional duration and intensity of seasonal wildfires, triggered by high temperatures and severe droughts. Since increasing megafires are predicted due to expected climate changes, it is critical to study the impact of BB aerosol on a large scale and evaluate related transport processes. In this study, five aerosol samples (total suspended particles with a diameter >1 µm) were collected during the XXXV Italian Expedition in Antarctica on board of the R/V Laura Bassi from 6th of January to February 16, 2020, along the sailing route from Lyttelton harbor (New Zealand) to Terra Nova Bay (Antarctica). Levoglucosan and its isomers have been analyzed as markers of BB, together with polycyclic aromatic hydrocarbons (PAHs), sucrose and alcohol sugars. Ionic species and carboxylic acids have been analyzed to support the identification of aerosol sources and its aging. Results showed high levoglucosan concentrations (325-1266 pg m-3) during the campaign, suggesting the widespread presence of smoke in the region, because of huge wildfire releases. Backward trajectories indicated the presence of long-range atmospheric transport from South America, probably carrying wildfires plume, in agreement with literature. Regional sources have been suggested for PAHs, particularly for 3-4 rings' compounds; monosaccharides, sucrose, arabitol, and mannitol were related to marine and biogenic contributions. In a warming climate scenario, more frequent and extensive wildfire episodes are expected in Australia, potentially altering albedo, aerosol radiative properties, and cloud interactions. Therefore, it is crucial to strengthens the investigations on the regional climatic effects of these events in Antarctica.


Asunto(s)
Aerosoles , Contaminantes Atmosféricos , Monitoreo del Ambiente , Glucosa/análogos & derivados , Estaciones del Año , Humo , Incendios Forestales , Aerosoles/análisis , Regiones Antárticas , Contaminantes Atmosféricos/análisis , Humo/análisis , Nueva Zelanda , Hidrocarburos Policíclicos Aromáticos/análisis , Australia , Material Particulado/análisis , Biomasa , Cambio Climático
6.
Huan Jing Ke Xue ; 44(12): 6518-6528, 2023 Dec 08.
Artículo en Chino | MEDLINE | ID: mdl-38098380

RESUMEN

Carbonaceous aerosols are an important component of fine particulate matter (PM2.5) in the atmosphere, having great impacts on air quality, human health, and the climate. In this study, PM2.5 samples were collected from November 2017 to October 2018 in a background site of Guangxi Province to investigate the potential impacts of biomass burning, an essential source of carbonaceous aerosols, on carbonaceous aerosols. Further, the composition of carbonaceous aerosols, sugar compounds, and the light absorption coefficient (babs) of water-soluble brown carbon (BrC) were also conducted. Considering the effect of the degradation of atmospheric levoglucosan (LG), the concentration of the corrected LG was quantified using the aging of air masses (AAM) index. Then, the contribution of biomass burning (BB) to organic carbon (OC) [BB-OC] was quantified using the corrected LG-derived molecular tracer method combined with the Bayesian mixing model. Here, we further explored the potential sources of water-soluble BrC using correlation analysis. In this research, the mean AAM index was 0.40±0.28 during the study period, indicating that the atmospheric LG had undergone a photochemical degradation process. The characteristic ratio combined with the Bayesian mixing model indicated that the crop straw (i.e., corn, rice, and sugarcane straw) was the dominant biomass fuel type in the Guangxi Region, contributing 22%, 23%, and 18% of OC without the correction of LG and 16%, 21%, and 17% with the corrected LG concentration, respectively. The neglection of LG degradation led to the underestimation of BB-OC, in which the BB-OC values with and without correction were 49.0% and 21.1%, respectively. Here, the annual mean babs of water-soluble BrC was (8.7±10.7) Mm-1, and its main sources were BB, fossil fuel combustion, and vegetation emission.

7.
Environ Sci Technol ; 57(48): 19473-19486, 2023 Dec 05.
Artículo en Inglés | MEDLINE | ID: mdl-37976408

RESUMEN

Biomass burning is common in much of the world, and in some areas, residential wood-burning has increased. However, air pollution resulting from biomass burning is an important public health problem. A sampling campaign was carried out between May 2017 and July 2018 in over 64 sites in four sessions, to develop a spatio-temporal land use regression (LUR) model for fine particulate matter (PM) and wood-burning tracers levoglucosan and soluble potassium (Ksol) in a city heavily impacted by wood-burning. The mean (sd) was 46.5 (37.4) µg m-3 for PM2.5, 0.607 (0.538) µg m-3 for levoglucosan, and 0.635 (0.489) µg m-3 for Ksol. LUR models for PM2.5, levoglucosan, and Ksol had a satisfactory performance (LOSOCV R2), explaining 88.8%, 87.4%, and 87.3% of the total variance, respectively. All models included sociodemographic predictors consistent with the pattern of use of wood-burning in homes. The models were applied to predict concentrations surfaces and to estimate exposures for an epidemiological study.


Asunto(s)
Contaminantes Atmosféricos , Material Particulado , Material Particulado/análisis , Contaminantes Atmosféricos/análisis , Madera/química , Chile , Monitoreo del Ambiente/métodos
8.
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
9.
Talanta ; 265: 124799, 2023 Dec 01.
Artículo en Inglés | MEDLINE | ID: mdl-37327665

RESUMEN

A new Continuous Flow Analysis (CFA) system coupled with Fast Liquid Chromatography - tandem Mass Spectrometry (FLC-MS/MS) has been recently developed for determining organic markers in ice cores. In this work we present an upgrade of this innovative technique, optimized for the detection of levoglucosan in ice cores, a crucial tracer for reconstructing past fires. The upgrade involved a specific optimization of the chromatographic and mass spectrometric parameters, allowing for a higher sampling resolution (down to 1 cm) and the simultaneous collection of discrete samples, for off-line analysis of water stable isotopes and additional chemical markers. The robustness and repeatability of the method has been tested by the analysis of multiple sticks of ice cut from the same shallow alpine ice core, and running the system for several hours on different days. The results show similar and comparable trends between the ice sticks. With this upgraded system, a higher sensitivity and a lower limit of detection (LOD) was achieved compared to discrete analysis of alpine samples for levoglucosan measurements. The new LOD was as low as 66 ng L-1, a net improvement over the previous LOD of 600 ng L-1.

10.
Bioresour Technol ; 382: 129166, 2023 Aug.
Artículo en Inglés | MEDLINE | ID: mdl-37210033

RESUMEN

Saccharification is a pivotal step in the conversion of lignocellulose to biofuels and chemicals. In this study, crude glycerol derived from biodiesel production was used in pretreatment to facilitate efficient and clean pyrolytic saccharification of sugarcane bagasse. Delignification, demineralization, destruction of lignin-carbohydrate complex structure, and cellulose crystallinity improvement in crude glycerol pretreated biomass could enhance levoglucosan producing reactions against competitive reactions, and therefore facilitate a kinetically controlled pyrolysis with apparent activation energy increased by 2-fold. Accordingly, selective levoglucosan production (44.4%) was promoted by 6-fold whilst light oxygenates and lignin monomers were limited to <25% in bio-oil. Owing to the high-efficiency saccharification, life cycle assessment suggested that the environmental impacts of the integrated process were less than those of typical acid pretreatment and petroleum-based processes, especially on the acidification (8-fold less) and global warming potential. This study provides an environmentally benign approach to efficient biorefinery and waste management.


Asunto(s)
Celulosa , Saccharum , Animales , Celulosa/química , Lignina/química , Glicerol , Pirólisis , Cinética , Biomasa , Biocombustibles , Estadios del Ciclo de Vida , Hidrólisis
11.
Environ Sci Technol ; 57(14): 5532-5543, 2023 04 11.
Artículo en Inglés | MEDLINE | ID: mdl-36976662

RESUMEN

Residential heating with solid fuels is one of the major drivers for poor air quality in Central and Eastern Europe, and coal is still one of the major fuels in countries, such as Poland, the Czech Republic, and Hungary. In this work, emissions from a single-room heater fueled with brown coal briquettes (BCBs) and spruce logs (SLs) were analyzed for signatures of inorganic as well as semivolatile aromatic and low-volatile organic constituents. High variations in organic carbon (OC) emissions of BCB emissions, ranging from 5 to 22 mg MJ-1, were associated to variations in carbon monoxide (CO) emissions, ranging from 900 to 1900 mg MJ-1. Residential BCB combustion turned out to be an equally important source of levoglucosan, an established biomass burning marker, as spruce logwood combustion, but showed distinct higher ratios to manosan and galactosan. Signatures of polycyclic aromatic hydrocarbons emitted by BCB combustion exhibited defunctionalization and desubstitution with increasing combustion quality. Lastly, the concept of island and archipelago structural motifs adapted from petroleomics is used to describe the fraction low-volatile organic compounds in particulate emissions, where a transition from archipelago to island motifs in relation with decreasing CO emissions was observed in BCB emissions, while emissions from SL combustion exhibited the island motif.


Asunto(s)
Contaminantes Atmosféricos , Hidrocarburos Policíclicos Aromáticos , Material Particulado/análisis , Contaminantes Atmosféricos/análisis , Carbón Mineral/análisis , Calefacción , Aerosoles
12.
J Chromatogr A ; 1695: 463935, 2023 Apr 26.
Artículo en Inglés | MEDLINE | ID: mdl-36965285

RESUMEN

The analysis of trace quantities of monosaccharide anhydrides (MAs) in sediments is complicated by the lack of fast and reliable technologies to selectively extract these water-soluble non-ionic compounds from samples of complex composition. Here we describe a solid phase extraction method that takes advantage of the affinity between monosaccharide anhydrides (MAs) and immobilized Na+ ions related to ligand-exchange processes (LE-SPE). The capacity factor of LE-SPE columns was enhanced by using non-aqueous mobile phases such as DCM/MeOH mixtures. We have used the unique properties of LE-SPE columns to selectively extract MAs from lacustrine, coastal, and deep-sea oceanic sediment samples. The analytical procedure produces extracts with low ion suppression effects (0-20%), resulting in ideal conditions for MAs quantification with LC-ESI-MS/MS systems irrespective of the sedimentary matrix and MAs concentration. The analytical method yields repeatable concentration values (RSD of 9-23% for levoglucosan and 15-34% for mannosan and galactosan) and an IS recovery of 45-70%. The instrumental dynamic range is 10-10000 pg injected, but in practice, the methodological lower limit of quantification is constrained by sample contamination during processing. The combination of LE-SPE and LC-ESI-MS/MS has the potential to produce sensitive and reliable technologies to analyze saccharides and amino acids in environmental and biological samples.


Asunto(s)
Espectrometría de Masa por Ionización de Electrospray , Espectrometría de Masas en Tándem , Espectrometría de Masas en Tándem/métodos , Ligandos , Cromatografía Liquida , Monosacáridos/análisis , Anhídridos/análisis , Extracción en Fase Sólida/métodos , Cromatografía Líquida de Alta Presión/métodos
13.
Sci Total Environ ; 872: 162071, 2023 May 10.
Artículo en Inglés | MEDLINE | ID: mdl-36775179

RESUMEN

Biomass burning (BB) has significant impacts on air quality and climate change, especially during harvest seasons. In previous studies, levoglucosan was frequently used for the calculation of BB contribution to PM2.5, however, the degradation of levoglucosan (Lev) could lead to large uncertainties. To quantify the influence of the degradation of Lev on the contribution of BB to PM2.5, PM2.5-bound biomass burning-derived markers were measured in Changzhou from November 2020 to March 2021 using the thermal desorption aerosol gas chromatography-mass spectrometry (TAG-GC/MS) system. Temporal variations of three anhydro-sugar BB tracers (e.g., levoglucosan, mannosan (Man), and galactosan (Gal)) were obtained. During the sampling period, the degradation level of air mass (x) was 0.13, indicating that ~87 % of levoglucosan had degraded before sampling in Changzhou. Without considering the degradation of levoglucosan in the atmosphere, the contribution of BB to OC were 7.8 %, 10.2 %, and 9.3 % in the clean period, BB period, and whole period, respectively, which were 2.4-2.6 times lower than those (20.8 %-25.9 %) considered levoglucosan degradation. This illustrated that the relative contribution of BB to OC could be underestimated (~14.9 %) without considering degradation of levoglucosan. Compared to the traditional method (i.e., only using K+ as BB tracer), organic tracers (Lev, Man, Gal) were put into the Positive Matrix Factorization (PMF) model in this study. With the addition of BB organic tracers and replaced K+ with K+BB (the water-soluble potassium produced by biomass burning), the overall contribution of BB to PM2.5 was enhanced by 3.2 % after accounting for levoglucosan degradation based on the PMF analysis. This study provides useful information to better understand the effect of biomass burning on the air quality in the Yangtze River Delta region.


Asunto(s)
Contaminantes Atmosféricos , Humanos , Contaminantes Atmosféricos/análisis , Material Particulado/análisis , Biomasa , Monitoreo del Ambiente/métodos , China , Estaciones del Año , Aerosoles/análisis
14.
Sci Total Environ ; 874: 162365, 2023 May 20.
Artículo en Inglés | MEDLINE | ID: mdl-36822414

RESUMEN

Aerosol liquid water (ALW) can serve as an aqueous-phase medium for numerous chemical reactions and consequently enhance the formation of secondary aerosols in a highly humid atmosphere. However, the aqueous-phase formation of secondary organic aerosols (SOAs) is not well understood in the Indian regions, particularly in tropical peninsular India. In this study, we collected total suspended particulate samples (n = 30) at a semiarid station (Ballari; 15.15°N, 76.93°E; 495 m asl) in tropical peninsular India during the winter of 2016. Homologous series of dicarboxylic acids (C2-C12), oxoacids (ωC2-ωC9), pyruvic acid (Pyr), and glyoxal (Gly) were determined by employing a water-extraction of aerosol and analyzed using capillary gas chromatography (GC). Results show that oxalic acid (C2) was the most abundant organic acid, followed by succinic (C4), malonic (C3), azelaic (C9), and glyoxylic (ωC2) or phthalic (Ph) acids. Total diacids-C accounted for 1.7-5.8 % of water-soluble organic carbon (WSOC) and 0.6-3.6 % of total carbon (TC). ALW, estimated from the ISORROPIA 2.1 model, showed a strong linear relationship with sulfate (SO42-), C2, C3, C4, ωC2, Pyr, and Gly. Based on molecular distribution, specific mass ratios (C2/C3, C2/C4, C2/Gly, and Ph/C9), linear relationships among the measured organic acids, ALW, organic (levoglucosan and oleic acid), and inorganic (SO42-) marker compounds, we emphasize that diacids and related organic compounds, especially C2, majorly form via aqueous-phase oxidation of precursor compounds including aromatic hydrocarbons (HCs) and unsaturated fatty acids (FAs) originated from biomass burning and combustion-related sources. The present study demonstrates that sulfate driven ALW largely enhances the formation of SOAs via the aqueous-phase reactions over tropical peninsular India during winter.

15.
Sci Total Environ ; 867: 161460, 2023 Apr 01.
Artículo en Inglés | MEDLINE | ID: mdl-36626988

RESUMEN

The rapid warming of Arctic is causing increased fire activities in the boreal Northern Hemisphere (NH), leading to unprecedent changes in the global carbon cycling, human health and ecosystems. Understanding the interaction between fire and climate in this far north region is crucial for predicting future changes of wildfires. However, fire records over geological time scales are still scarce in the high latitudes of NH to provide comprehensive pictures of the fire history in this region. Here, we used the flux of levoglucosan (Lev) and its isomers in a sediment profile YN from Svalbard, high Arctic, as proxies for the changes in biomass burning from ∼9-2 kyr BP (thousand years before present). Backward trajectories and comparison with charcoal syntheses from various regions confirmed that the Lev transport to the profile site is sourced from the fire activities in the boreal NH, especially in northern Europe and northern Siberia. The Lev flux exhibited a slight overall decreasing trend at ∼3 %/kyr (p = 0.09) over the study period, as well as centennial maxima at ∼9, 8-7, 6, 5, and 4-3 kyr BP (p = 0.06). On sub-orbital scales, the long-term decrease in fire activities corresponded to trends of summer temperature in the extratropics of the NH (p = 0.01, r = 0.42), reflecting their regulation of fuel availability and flammability. On centennial to sub-millennial time scales, high levels of biomass burning were associated with periods of increased North Atlantic ice-rafted debris (p = 0.02, r = 0.38), which were indicative of cold and dry conditions over most of the source regions, reflecting the impacts of dryness on fuel flammability. The results suggested that enhanced Arctic amplification on centennial time scales may reduce biomass burning in most of the boreal NH, although fires in some mid-latitude regions may be facilitated.

16.
Environ Int ; 170: 107582, 2022 12.
Artículo en Inglés | MEDLINE | ID: mdl-36265357

RESUMEN

Field-based sampling can provide more accurate evaluation than MODIS in regional biomass burning (BB) emissions given the limitations of MODIS on unresolved fires. Polyurethane foam-based passive air samplers (PUF-PASs) are a promising tool for collecting atmospheric monosaccharides. Here, we deployed PUF-PASs to monitor monosaccharides and other BB-related biomarkers and presented a dataset of 31 atmospheric BB-related biomarkers in the Indo-China Peninsula (ICP) and Southwest China. The peak concentrations of monosaccharides in the ICP occurred before monsoon season. The highest concentrations were in the eastern Mekong plain, while the lowest were along the eastern coast. BB-related biomarkers displayed elevated concentrations after April, particularly in the monsoon season; however, fewer active fires were recorded by MODIS. This revealed the importance of MODIS unresolved fires (e.g., indoor biofuel combustion, small-scale BB incidents, and charcoal fires) to the regional atmosphere. The PAS derived levoglucosan concentrations indicated that, with the inclusion of MODIS unresolved fires, the estimated top-down emissions of PM (4194-4974 Gg/yr), OC (1234-1719 Gg/yr) and EC (52-384 Gg/yr) would be higher than previous bottom-up estimations in the ICP. Future studies on these MODIS unresolved fires and regional monitoring data of BB are vital for improving the modeling of regional BB emissions.


Asunto(s)
China
17.
Biotechnol Biofuels Bioprod ; 15(1): 94, 2022 Sep 14.
Artículo en Inglés | MEDLINE | ID: mdl-36104808

RESUMEN

Manufacturing fuels and chemicals from cellulose materials is a promising strategy to achieve carbon neutralization goals. In addition to the commonly used enzymatic hydrolysis by cellulase, rapid pyrolysis is another way to degrade cellulose. The sugar obtained by fast pyrolysis is not glucose, but rather its isomer, levoglucosan (LG). Here, we revealed that both levoglucosan kinase activity and the transportation of levoglucosan are bottlenecks for LG utilization in Saccharomyces cerevisiae, a widely used cell factory. We revealed that among six heterologous proteins that had levoglucosan kinase activity, the 1,6-anhydro-N-acetylmuramic acid kinase from Rhodotorula toruloides was the best choice to construct levoglucosan-utilizing S. cerevisiae strain. Furthermore, we revealed that the amino acid residue Q341 and W455, which were located in the middle of the transport channel closer to the exit, are the sterically hindered barrier to levoglucosan transportation in Gal2p, a hexose transporter. The engineered yeast strain expressing the genes encoding the 1,6-anhydro-N-acetylmuramic acid kinase from R. toruloides and transporter mutant Gal2pQ341A or Gal2pW455A consumed ~ 4.2 g L-1 LG in 48 h, which is the fastest LG-utilizing S. cerevisiae strain to date.

18.
J Sep Sci ; 45(18): 3422-3430, 2022 Sep.
Artículo en Inglés | MEDLINE | ID: mdl-35839084

RESUMEN

Saccharides, especially anhydro sugars present in atmospheric aerosols, can be used as tracers to track sources of atmospheric aerosols. High-performance anion-exchange chromatography with pulsed amperometric detection is a commonly used technique for determining these saccharides, but the reported methods suffer from three drawbacks. First, to achieve separation of the complete set of atmospheric saccharides, run times are very long, typically longer than 60 minutes. Second, some methods require two columns to achieve the desired separation. Finally, in an era when electrolytic eluent preparation allows for excellent precision and accuracy, these methods require manually prepared eluents, which can lead to separation inconsistency for closely eluting analytes. These drawbacks make existing methods difficult to automate. To address this issue, we developed a fast method that uses only a single column for separation and electrolytically generated eluent that resolves 12 key atmospheric aerosol saccharides in 20 minutes. The resolved saccharides include anhydro sugars (levoglucosan, galactosan, and mannosan), sugar alcohols (erythritol, xylitol, and mannitol), and mono-/disaccharides (arabinose, galactose, glucose, mannose, fructose, and sucrose). To our knowledge, this report is the first instance of achieving such a significant reduction in run time with good resolution for this set of saccharides.


Asunto(s)
Galactosa , Manosa , Aerosoles/análisis , Aniones , Arabinosa , Carbohidratos/análisis , Cromatografía/métodos , Disacáridos , Eritritol , Fructosa , Galactosa/análisis , Glucosa/análisis , Manitol , Manosa/análisis , Manosa/química , Sacarosa , Alcoholes del Azúcar , Azúcares , Xilitol
19.
Ann Work Expo Health ; 66(8): 985-997, 2022 10 11.
Artículo en Inglés | MEDLINE | ID: mdl-35652799

RESUMEN

Wildland firefighters (WLFFs) are exposed to a mixture of chemicals found in wildland fire smoke and emissions from nonwildland-fuel smoke sources such as diesel. We investigated compositional differences in exposure to particulate matter and explored differences in ventilation rate and potential inhaled dose relative to the work tasks of WLFFs. Repeated measures on ten professional and two volunteer firefighters were collected on prescribed burn and nonburn days. Personal monitoring consisted of real-time and gravimetric fine particulate matter (PM2.5), carbon monoxide (CO), and accelerometer measurements to estimate ventilation rate and potential dose of PM2.5. The fine particulate matter was analyzed for levoglucosan (LG) and light absorbing carbon as a surrogate for black carbon (BC). Breathing zone personal exposure concentrations of PM2.5, LG, BC, and CO were higher on burn days (P < 0.05). Differences in exposure concentrations were observed between burn day tasks (P < 0.05) with firefighters managing fire boundaries (holders) being exposed to higher CO and LG concentrations and less BC concentrations than those conducting lighting (lighters). While no statistical difference in PM2.5 exposure measures was observed between the two tasks, holders in the study tended to be exposed to higher PM2.5 concentrations (~1.4×), while lighters tended to have more inhaled amounts of PM2.5 (~1.3×). Our findings demonstrate possible diversity in the sources of particulate matter exposure at the fireline and suggest the potential importance of using dose as a metric of inhalation exposure in occupational or other settings.


Asunto(s)
Bomberos , Exposición Profesional , Monóxido de Carbono/análisis , Humanos , Exposición Profesional/análisis , Material Particulado , Ventilación Pulmonar , Humo
20.
Bioresour Technol ; 356: 127305, 2022 Jul.
Artículo en Inglés | MEDLINE | ID: mdl-35562026

RESUMEN

In order to identify the most environmental-friendly pretreatment for pyrolsis of wood residue to levoglucosan (LG), for the first time a comparative life cycle assessment (LCA) was carried out for hot water treatment (HWT), torrefaction, acid pretreatment (AP) and salt pretreatment (SP) pathways. Since LG production can facilitate both resource recovery (RR) and wood residue handling (WRH), two different functional units (FUs), i.e., 1 kg LG production and 1 kg wood residue handling were considered. AP was found to generate the least global warming potential of 134.60 kg CO2-eq and human carcinogenic toxicity of 0.59 kg 1,4-dichlorobenzene-eq. for RR perspective. However, for WRH perspective, HWT was found to be the best pretreatment (6.39 kg CO2-eq; 0.03 kg 1,4-dichlorobenzene-eq.). Sensitivity analysis revealed that a reduction in electricity consumption by 15% could reduce the overall impacts by 14.00-14.82 %. This study also highlights the impact of goal and FU selection on LCA.


Asunto(s)
Pirólisis , Madera , Animales , Biomasa , Dióxido de Carbono/análisis , Glucosa/análogos & derivados , Humanos , Estadios del Ciclo de Vida , Madera/química
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