Sources of water-soluble organic carbon in fine particles at a southern European urban background site

In this study, the temporal evolution and sources of water-soluble organic carbon (WSOC) in submicron particles at an urban background site in Elche (Spain) were investigated. Measurements of PM1 (N = 200) were carried out over one year (2021). Samples were analysed for organic carbon (OC), elemental carbon (EC), WSOC, levoglucosan, elements and major ions. A positive matrix factorization (PMF) analysis was performed in order to identify the sources of WSOC on an annual and a monthly basis. During the study period, traffic restrictions due to COVID-19 led to lower concentrations of PM1 and carbonaceous compounds than expected. The WSOC annual average mass concentration was 0.95 mugm-3, with maximum values during the colder months. The apportionment results indicate that the biomass burning (BB) source contributed 30.63% to WSOC levels, road traffic (RT) accounted for 23.90% of the WSOC, while the contribution of a source related to secondary organic aerosol formation (ammonium sulfate-AS) was 33.80%. Minor sources of WSOC were: soil dust (SD) and secondary nitrate (SN), which contributed 7.44% and 4.22%, respectively, to WSOC concentrations. The WSOC/OC ratio did not exhibit significant variations during the study period, since source contributions were similar for WSOC and OC. The highest values of this ratio were recorded in summer, due to the higher contribution from the AS source to WSOC concentrations.Copyright © 2023 The Authors

Response of organic aerosol characteristics to emission reduction in Yangtze River Delta region.

Organic aerosol (OA) is a major component of atmospheric particulate matter (PM) with complex composition and formation processes influenced by various factors. Emission reduction can alter both precursors and oxidants which further affects secondary OA formation. Here we provide an observational analysis of secondary OA (SOA) variation properties in Yangtze River Delta (YRD) of eastern China in response to large scale of emission reduction during Chinese New Year (CNY) holidays from 2015 to 2020, and the COVID-19 pandemic period from January to March, 2020. We found a 17% increase of SOA proportion during the COVID lockdown. The relative enrichment of SOA is also found during multi-year CNY holidays with dramatic reduction of anthropogenic emissions. Two types of oxygenated OA (OOA) influenced by mixed emissions and SOA formation were found to be the dominant components during the lockdown in YRD region. Our results highlight that these emission-reduction-induced changes in organic aerosol need to be considered in the future to optimize air pollution control measures. Electronic Supplementary Material: Supplementary material is available in the online version of this article at 10.1007/s11783-023-1714-0 and is accessible for authorized users.

CCN activation of ultrafine biogenic-WSOC under restricted anthropogenic emissions: A study over eastern Himalaya in India

The present study was conducted to investigate the potential of water soluble organic carbon (WSOC) in CCN activation under restricted anthropogenic emissions over a high altitude station, Darjeeling (27.01° N and 88.15° E,∼2200 amsl and covered with huge coniferous forests) in the eastern parts of Himalaya in India. We measured CN, CCN, and ultrafine WSOC (WSOC0.1) during April–May 2020 (COVID-19 lockdown) and compared with the normal period (April–May 2019) to investigate the relative dominance of biogenic over anthropogenic emissions to the aerosol-CCN activation. Though an expected significant decline (53%) in CN concentration was observed, CCN exhibited ∼17% increase during the lockdown period. The activation ratio (AR: CCN/CN) jumped from 0.30 during normal to 0.72 during the lockdown period. The aerosol solubility was also found to be increased during the lockdown period (∼27% decrease in the k- parameter (k)). Lockdown-WSOC was higher (1.62 μg m−3) than the normal-WSOC (1.13 μg m−3) and exhibited better regression with CCN in absence of anthropogenic emissions (Lockdown: R2 = 0.83, p < 0.05;Normal: R2 = 0.40, p < 0.05). Here we hypothesize that under restricted fossil fuel emissions during lockdown (57% decline in NOx), surface ozone was increased by 31%, that in turn favored the photochemical oxidation of biogenic VOCs emitted only from coniferous forest cover to produce huge amount of SOC. The ultrafine "biogenic-only” WSOC (under restricted anthropogenic WSOC during lockdown) participated in CCN activation actively and with higher proficiency compared to the normal period. The study bears immense importance of the role of biogenic emissions in cloud droplet formation over this part of the Himalaya under restricted anthropogenic emissions. The present hypothesis could open a new route of aerosol formation and their CCN activation under high deficiency of anthropogenic emissions. © 2023 Elsevier B.V.

Drivers of High Concentrations of Secondary Organic Aerosols in Northern China during the COVID-19 Lockdowns.

During the COVID-19 lockdown in early 2020, observations in Beijing indicate that secondary organic aerosol (SOA) concentrations increased despite substantial emission reduction, but the reasons are not fully explained. Here, we integrate the two-dimensional volatility basis set into a state-of-the-art chemical transport model, which unprecedentedly reproduces organic aerosol (OA) components resolved by the positive matrix factorization based on aerosol mass spectrometer observations. The model shows that, for Beijing, the emission reduction during the lockdown lowered primary organic aerosol (POA)/SOA concentrations by 50%/18%, while deteriorated meteorological conditions increased them by 30%/119%, resulting in a net decrease in the POA concentration and a net increase in the SOA concentration. Emission reduction and meteorological changes both led to an increased OH concentration, which accounts for their distinct effects on POA and SOA. SOA from anthropogenic volatile organic compounds and organics with lower volatility contributed 28 and 62%, respectively, to the net SOA increase. Different from Beijing, the SOA concentration decreased in southern Hebei during the lockdown because of more favorable meteorology. Our findings confirm the effectiveness of organic emission reductions and meanwhile reveal the challenge in controlling SOA pollution that calls for large organic precursor emission reductions to rival the adverse impact of OH increase.

Effect of COVID-19 lockdown on the characterization and mixing state of carbonaceous particles in the urban atmosphere of Liaocheng, the North China Plain

To investigate the effect of COVID-19 control measures on aerosol chemistry, the chemical compositions, mixing states, and formation mechanisms of carbonaceous particles in the urban atmosphere of Liaocheng in the North China Plain (NCP) were compared before and during the pandemic using a single particle aerosol mass spectrometry (SPAMS). The results showed that the concentrations of five air pollutants including PM2.5, PM10, SO2, NO2, and CO decreased by 41.2%-71.5% during the pandemic compared to those before the pandemic, whereas O3 increased by 1.3 times during the pandemic because of the depressed titration of O3 and more favorable meteorological conditions. The count and percentage contribution of carbonaceous particles in the total detected particles were lower during the pandemic than those before the pandemic. The carbonaceous particles were dominated by elemental and organic carbon (ECOC, 35.9%), followed by elemental carbon-aged (EC-aged, 19.6%) and organic carbon-fresh (OCfresh, 13.5%) before the pandemic, while EC-aged (25.3%), ECOC (17.9%), and secondary ions-rich (SEC, 17.8%) became the predominant species during the pandemic. The carbonaceous particle sizes during the pandemic showed a broader distribution than that before the pandemic, due to the condensation and coagulation of carbonaceous particles in the aging processes. The relative aerosol acidity (Rra) was smaller before the pandemic than that during the pandemic, indicating the more acidic particle aerosol during the pandemic closely related to the secondary species and relative humidity (RH). More than 95.0% and 86.0% of carbonaceous particles in the whole period were internally mixed with nitrate and sulfate, implying that most of the carbonaceous particles were associated with secondary oxidation during their formation processes. The diurnal variations of oxalate particles and correlation analyses suggested that oxalate particles before the pandemic were derived from aqueous oxidation driven by RH and liquid water content (LWC), while oxalate particles during the pandemic were originated from O3dominated photochemical oxidation.(c) 2022 Chinese Society of Particuology and Institute of Process Engineering, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.

Molecular characteristics of ambient organic aerosols in Shanghai winter before and after the COVID-19 outbreak.

During the global pandemic of COVID-19, the world adopted different strategies to avoid the human and economic loss, and so does China. The reduction of human activities during this time period caused reduction in PM emissions. This study adopted a HPLC-Q-TOF-MS to compare the chemical compositions of ambient aerosol samples collected in Shanghai winter before (2018, 2019) and after (2021) the COVID-19 outbreak. The identified compositions were classified into subgroups of CHO, CHN, CHON, CHONS, CHOS and CHN compounds. Results showed that CHO compounds and CHON compounds were dominating the organic compounds in ESI- and ESI+, respectively. The average percentages of CHO- compounds were 57.97 % in 2018, 58.98 % in 2019, and 43.93 % in 2021, respectively. The average percentages of CHON+ compounds were 52.74 % in 2018, 50.34 % in 2019, and 52.02 % in 2021, respectively. The proportion of aliphatic compounds increased gradually during the three years, especially in 2021, indicating that CHO compounds were less affected by aromatic precursors after the COVID-19 outbreak. The contribution of anthropogenic emissions in Shanghai was weakened compared with the previous years. In addition, there was an enhanced emission source containing hydroxyl for CHOS compound formation in 2021. The variations of atmospheric oxidation degree among the three years were not significant.

Application of machine learning and statistical modeling to identify sources of air pollutant levels in Kitchener, Ontario, Canada

Machine learning is used across many disciplines to identify complex relations between outcomes and numerous potential predictors. In the case of air quality research in heavily populated urban centers, such techniques were used to correlate the impacts of Traffic-Related Air Pollutants (TRAP) on vulnerable members of communities, future pollutant levels, and potential solutions that mitigate adverse effects of poor air quality. However, machine learning tools have not been used to assess the variables that influence measured pollutant levels in a suburban environment. The objective of this study is to apply a novel combination of Random Forest (RF) modeling, a machine learning algorithm, and statistical significance analysis to assess the impacts of anthropogenic and meteorological variables on observed pollutant levels in two separate datasets collected during and after the COVID-19 lockdowns in Kitchener, Ontario, Canada. The results highlight that TRAP levels studied here are linked to meteorology and traffic count/type, with relatively higher sensitivity to the former. Upon taking statistical significance into account when assessing relative importance of variables affecting pollutant levels, our study found that traffic variables had a more discernible influence than many meteorological variables. Additional studies with a larger dataset and spread throughout the year are needed to expand upon these initial findings. The proposed approach outlines a "blueprint" method of quantifying the importance of traffic in mid-size cities experiencing fast population growth and development.

Changes in primary and secondary aerosols during a controlled Chinese New Year.

Large reductions in anthropogenic emissions during the Chinese New Year (CNY) holiday in Beijing have been well reported. However, the changes during the CNY of 2021 are different because most people stayed in Beijing to control the spread of coronavirus disease (COVID-19). Here a high-resolution aerosol mass spectrometer (HR-AMS) was deployed for characterization of the changes in size-resolved aerosol composition and sources during the CNY. We found that the reductions in traffic-related NOx and fossil fuel-related organic aerosol (OA), and cooking OA (1.3-12.7%) during the CNY of 2021 were much smaller than those in previous CNY holidays of 2013, 2015, and 2020. In contrast, the mass concentrations of secondary aerosol species except nitrate showed ubiquitous increases (17.6-30.4%) during the CNY of 2021 mainly due to a 4-day severe haze episode. OA composition also changed substantially during the CNY of 2021. In particular, we observed a large increase by nearly a factor of 2 in oxidized primary OA likely from biomass burning, and a decrease of 50.1% in aqueous-phase secondary OA. A further analysis of the severe haze episode during the CNY illustrated a rapid transition of secondary formation from photochemical to aqueous-phase processing followed by a scavenging process, leading to significant changes in aerosol composition, size distributions, and oxidation degree of OA. A parameterization relationship between oxygen-to-carbon (O/C) and f44 (fraction of m/z 44 in OA) from a collocated capture vaporizer aerosol chemical speciation monitor (CV-ACSM) was developed, which has a significant implication for characterization of OA evolution and the impacts on hygroscopicity due to the rapidly increased deployments of CV-ACSM worldwide.

Chemical Compositions in Winter PM2.5 in Changzhou of the Yangtze River Delta Region, China: Characteristics and Atmospheric Responses Along With the Different Pollution Levels

Changzhou, a typical industrial city located in the center of the Yangtze River Delta (YRD) region, has experienced serious air pollution in winter. However, Changzhou still receives less attention compared with other big cities in YRD. In this study, a four-month PM2.5 sampling campaign was conducted in Changzhou, China from 1 November 2019, to 1 February 2020. The period covers the entire wintertime and includes first week of the Level 1 response stage of the lockdown period due to the outbreak of COVID-19. The mean PM2.5 concentrations were 67.9 +/- 29.0 mu gm(-3), ranging from 17.4 to 157.4 mu gm(-3). Secondary inorganic ions were the most abundant species, accounting for 37 and 50% during the low and high PM2.5 pollution periods, respectively. Nitrogen oxidation ratio (NOR) during the high PM concentration level period was twice the low PM concentration period whereas sulfur oxidation ratio (SOR) showed a less significant increase. This represents that nitrate formation is potentially the predominant factor controlling the occurrence of PM pollution. The analysis of NOR, SOR as functions of relative humidity (RH) and ozone (O-3) concentrations suggest that the sulfate formation was mainly through aqueous-phase reaction, while nitrate formation was driven by both photochemistry and heterogeneous reaction. And, excess ammonium could promote the formation of nitrate during the high PM period, indicating that ammonia gas played a critical role in regulating nitrate. Furthermore, a special period-Chinese New Year overlapping first week of COVID-19 lockdown period, offered a precious window to study the impact of human activity pattern changes on air pollution variation. During the special period, the average PM2.5 mean concentration was 60.4 mu gm(-3), which did not show in a low value as expected. The declines in nitrogen oxide (NOx) emissions led to rapid increases in O-3 and atmospheric oxidizing capacity, as well as sulfate formation. The chemical profiles and compositions obtained during different periods provide a scientific basis for establishing efficient atmospheric governance policies in the future.

Exploring chemical changes of the haze pollution during a recent round of COVID-19 lockdown in a megacity in Northeast China.

COVID-19 rebounded in China in January 2021, with Heilongjiang as one of the worst-affected provinces. This resulted in a new round of lockdown in Harbin, the capital city of Heilongjiang, from 20 January to 22 February of 2021. A field campaign was conducted to explore the responses of haze pollution in Harbin to the lockdown. Levoglucosan was used to reflect biomass burning emissions, while the molar ratio of sulfur (the sum of sulfur dioxide and sulfate) to nitrogen (the sum of nitrogen dioxide and nitrate), i.e., RS/N, was used as an indicator for the relative importance of coal combustion and vehicle emissions. Based on a synthesis of the levoglucosan and RS/N results, reference period was selected with minimal influences of non-lockdown-related emission variations. As indicated by the almost unchanged sulfur dioxide concentrations, coal combustion emissions were relatively stable throughout the lockdown and reference periods, presumably because the associated activities, e.g., heating supply, power generation, etc., were usually uninterruptible. On the other hand, as suggested by the increase of RS/N, vehicle emissions were considerably reduced during lockdown, likely due to the stay-at-home orders. Compared to results from the reference samples, the lockdown period exhibited higher levels of ozone and various indicators for secondary aerosol formation, pointing to an enhancement of secondary pollution. In addition, photochemistry-related reactions in aqueous phase appeared to be present during the lockdown period, which have not been reported in the frigid atmosphere over Northeast China.

Variations and Sources of Organic Aerosol in Winter Beijing under Markedly Reduced Anthropogenic Activities During COVID-2019.

The COVID-19 outbreak provides a "controlled experiment" to investigate the response of aerosol pollution to the reduction of anthropogenic activities. Here we explore the chemical characteristics, variations, and emission sources of organic aerosol (OA) based on the observation of air pollutants and combination of aerosol mass spectrometer (AMS) and positive matrix factorization (PMF) analysis in Beijing in early 2020. By eliminating the impacts of atmospheric boundary layer and the Spring Festival, we found that the lockdown effectively reduced cooking-related OA (COA) but influenced fossil fuel combustion OA (FFOA) very little. In contrast, both secondary OA (SOA) and O3 formation was enhanced significantly after lockdown: less-oxidized oxygenated OA (LO-OOA, 37% in OA) was probably an aged product from fossil fuel and biomass burning emission with aqueous chemistry being an important formation pathway, while more-oxidized oxygenated OA (MO-OOA, 41% in OA) was affected by regional transport of air pollutants and related with both aqueous and photochemical processes. Combining FFOA and LO-OOA, more than 50% of OA pollution was attributed to combustion activities during the whole observation period. Our findings highlight that fossil fuel/biomass combustion are still the largest sources of OA pollution, and only controlling traffic and cooking emissions cannot efficiently eliminate the heavy air pollution in winter Beijing.