Secondary Organic Carbon Research Articles

Stark seasonal contrast of fine aerosol levels, composition, formation mechanism, and characteristics in a polluted megacity.

In this study, we investigated the temporal variation of organic and inorganic aerosol with its optical properties in Mumbai (India), an urban coastal region. Mean PM2.5concentrations during the sampling period were 175μg/m3 (winter) and 90μg/m3 (summer). During winter, the average concentrations of organic (OC), elemental (EC), and water-soluble organic carbon (WSOC) were three times higher than in summer. Secondary organic carbon (SOC) contribution in OC was higher in summer (78%) than in winter (53%), and strong solar radiation in summer likely caused this outcome. Aerosols were slightly acidic in both seasons, with an average pH of 5.7 (winter) and 6.0 (summer). A correlation was observed between SOC and the acidity of particles in summer (R2 = 0.6), indicating some amount of acid-catalysed SOC formation. In both seasons, the sulphate oxidation ratio (SOR) was higher than the nitrate oxidation ratio (NOR), which may reflect a preference for SO2 oxidation over NO2 or the difference in partitioning ammonium nitrate into ammonium sulphate under high RH. The dominant mechanism of SOC formation (gas vs aqueous phase oxidation) also showed seasonal variation. In winter, a relatively steep reduced major axis (RMA) slope of O3/CO suggests gas phase oxidation was the dominant mechanism of SOC production. Winter has more BrC fraction than summer, indicating higher absorbing aerosols, though the efficiency of absorbing the light was higher in summer. To assess the radiative forcing of PM2.5 on a local scale, an effective carbon ratio (ECR) was computed. The findings pointed to a local radiative heating impact caused by PM2.5. The spectral slope ratio and MAE at 250 to 300nm ratio (E2/E3) revealed a higher abundance of high molecular weight species in WSOC during summer than in winter.

Ratios of organic mass to organic carbon in fine particulate matter at urban sites in China and Korea during winter and summer.

This study evaluates the composition and seasonal characteristics of fine particulate matter (PM2.5) during winter and summer through simultaneous measurements conducted at the Gwangju Institute of Science and Technology in South Korea and the Changping campus of Peking University in China. PM2.5 samples were concurrently collected at both sites, and chemical analyses were conducted to quantify various components, including carbonaceous materials, ionic species, and metals. Although the average PM2.5 concentrations were comparable between the two sites, there were distinct differences in the concentrations of major components. Organic indicator compounds were analyzed to discern the contributions of primary and secondary pollution sources. Changping displayed a mix of primary and secondary pollution, characterized by higher concentrations of primary organic carbon (POC) such as polycyclic aromatic hydrocarbons and hopanes, compared to Gwangju. In contrast, Gwangju demonstrated a higher prevalence of secondary organic carbon (SOC), particularly water-soluble organic carbon not related to biomass burning (WSOCnbb) and various polar organic compounds. The organic mass to organic carbon (OM/OC) ratios estimated using the mass balance method revealed significant differences, with Gwangju showing a higher ratio of 2.3 compared to 1.9 at Changping, indicating a greater influence of secondary pollutants at Gwangju. Additionally, both Changping and Gwangju exhibited higher OM/OC ratios in summer (Changping: 2.0, Gwangju: 2.5) compared to winter (Changping: 1.8, Gwangju: 2.2), indicating seasonal differences in organic mass contributions to PM2.5. These findings underscore the importance of accounting for spatial and seasonal variations in air pollution studies and suggest that updating commonly used OM/OC ratios could enhance the reliability of research outcomes.

Assessment of Multiple Planetary Boundary Layer Height Retrieval Methods and Their Impact on PM2.5 and Its Chemical Compositions throughout a Year in Nanjing

In this study, we investigate the planetary boundary layer height (PBLH) using micro-pulse lidar (MPL) and microwave radiometer (MWR) methods, examining its relationship with the mass concentration of particles less than 2.5 µm in aerodynamic diameter (PM2.5) and its chemical compositions. Long-term PBLH retrieval results are presented derived from the MPL and the MWR, including its seasonal and diurnal variations, showing a superior performance regarding the MPL in terms of reliability and consistency with PM2.5. Also examined are the relationships between the two types of PBLHs and PM2.5. Unlike the PBLH derived from the MPL, the PBLH derived from the MWR does not have a negative correlation under severe pollution conditions. Furthermore, this study explores the effects of the PBLH on different aerosol chemical compositions, with the most pronounced impact observed on primary aerosols and relatively minimal influence on secondary aerosols, especially secondary organics during spring. This study underscores disparities in PBLH retrievals by different instruments during long-term observations and unveils distinct relationships between the PBLH and aerosol chemical compositions. Moreover, it highlights the greater influence of the PBLH on primary pollutants, laying the groundwork for future research in this field.

Stable isotope compositions, source apportionment and transformation processes of carbonaceous aerosols in PM10 in the urban city of Hyderabad, India

This study apportions sources of carbonaceous aerosols using isotopic characteristics of total carbon (TC) and elemental carbon (EC) in PM10 aerosols using filter-based CTO-375 method for pre-monsoon (summer), post-monsoon, and winter (2019–2021) over Hyderabad, India. Highest secondary organic carbon, SOC (primary organic carbon, POC) of 13.78 ± 10.25 (7.87 ± 2.48) μg/m3 was during post-monsoon 2020 (2019), while lowest was 8.90 ± 5.55 (4.18 ± 0.92) μg/m3 during pre-monsoon 2021 (post-monsoon 2020), respectively. Average effective carbon ratio (ECR) > 1 indicates dominance of light scattering aerosols during pre-monsoon and post-monsoon. δ13CTC and δ13CEC varied from – 28.1 to – 24.7 ‰ (avg. – 26.5 ± 0.7) and - 32.5 to – 24.6 ‰ (avg. – 27.4 ± 1.1), indicating contribution from C3 plant burning and liquid fuel combustion. Positive value of δ13COC – δ13CEC and heavier δ13CTC, along with gradual enrichment in δ13CTC and δ13CEC from December 2020 to March 2021, suggested photochemical aging of carbonaceous aerosols. Lighter δ13CTC and OC/EC > 4 for all seasons indicates dominance of biomass burning (wood and crop residue burning), photochemical oxidation and secondary organic aerosol (SOA) formation. The tropical study experiences dominance of lighter δ13CEC compared to subtropical, high latitude regions.

Seasonal variation of water-soluble inorganic ions and carbonaceous components of PM2.5 and PM1 in industrial and residential areas of Suizhou, China

Seasonal variations of fine particulate matter (PM) and its chemical components in Suizhou are investigated by collecting PM2.5 and PM1 samples from industrial and residential areas between March 2017 and February 2018. The findings reveal more severe PM pollution in industrial areas compared to residential areas. Concentrations and percentages of water-soluble inorganic ions (WSII) in PM are higher in spring and winter. Notably, the high levels of SO42− and NO3− in PM1-2.5 indicate that secondary transformation of SO2 and NOx significantly contribute to the rapid increase in PM1-2.5. The conversion of NO2 to NO3− is a key factor in the winter increase of mass concentrations of PM2.5 [ρ(PM2.5)], while photochemical reactions involving NO2 drive the summer increase of ρ(PM2.5). Organic carbon (OC) and elemental carbon (EC) are mainly distributed in PM1, with OC peaking in winter. Chemical fractionation of PM reveals that carbonaceous components have a greater impact on PM1 concentration than WSII, whereas WSII more significantly affects ρ(PM2.5) than carbonaceous components. The OC to EC ratio in industrial areas (2.5 ± 1.4) and residential areas (1.9 ± 0.8) suggests more prominent secondary aerosol pollution in industrial areas. Significant correlations between secondary organic carbon (SOC), SOC conversion rate (ηSOC), and concentrations of O3-8h and NO2 in Suizhou further indicate that O3 and NO2 levels in the atmosphere influence the generation of SOC and ηSOC.

Characterizing water solubility of fresh and aged secondary organic aerosol in PM2.5 with the stable carbon isotope technique

Abstract. The investigation of the water-soluble characteristics of secondary organic carbon (SOC) is essential for a more comprehensive understanding of its climate effects. However, due to the limitations of the existing source apportionment methods, the water solubility of different types of SOC remains uncertain. This study analyzed stable carbon isotope and mass spectral signatures of total carbon (TC) and water-soluble organic carbon (WSOC) in ambient PM2.5 samples for 1 year and established stable carbon isotope profiles of fresh and aged SOC. Furthermore, a Bayesian stable isotope mixing (BSIM) model was employed to reveal the water solubility characteristics of fresh and aged SOC in a coastal megacity of China. WSOC was dominated by secondary sources, with fresh and aged SOC contributing 28.1 % and 45.2 %, respectively. Water-insoluble organic carbon (WIOC) was dominated by primary sources, to which fresh and aged SOC contributed 23.2 % and 13.4 %. We also found that the aging degree of SOC has considerable impacts on its water solubility due to the much higher water-soluble fraction of aged SOC (76.5 %) compared to fresh SOC (54.2 %). Findings of this study may provide a new perspective for further investigation of the hygroscopicity effects of SOC with different aging degrees on light extinction and climate change.

PM2.5 and its components and respiratory disease healthcare encounters – Unanticipated increased exposure-response relationships in recent years after environmental policies

Prior studies reported excess rates (ERs) of cardiorespiratory events associated with short-term increases in PM2.5 concentrations, despite implementation of pollution-control policies. In 2017, Federal Tier 3 light-duty vehicle regulations began, and to-date there have been no assessments of population health effects of the policy. Using the NYS Statewide Planning and Research Cooperative System (SPARCS) database, we obtained hospitalizations and ED visits with a principal diagnosis of asthma or chronic obstructive pulmonary disease (COPD) for residents living within 15 miles of six urban PM2.5 monitoring sites in NYS (2014–2019). We used a time-stratified case-crossover design and conditional logistic regression (adjusting for ambient temperature, relative humidity, and weekday) to estimate associations between PM2.5, POC (primary organic carbon), SOC (secondary organic carbon), and rates of respiratory disease hospitalizations and emergency department (ED) visits from 2014 to 2019. We evaluated demographic disparities in these relative rates and compared changes in ERs before (2014–2016) and after Tier 3 implementation (2017–2019). Each interquartile range increase in PM2.5 was associated with increased ERs of asthma or COPD hospitalizations and ED visits in the previous 7 days (ERs ranged from 1.1%–3.1%). Interquartile range increases in POC were associated with increased rates of asthma ED visits (lag days 0–6: ER = 2.1%, 95% CI = 0.7%, 3.6%). Unexpectedly, the ERs of asthma admission and ED visits associated with PM2.5, POC, and SOC were higher during 2017–2019 (after Tier 3) than 2014–2016 (before Tier-3). Chronic obstructive pulmonary disease analyses showed similar patterns. Excess Rates were higher in children (<18 years; asthma) and seniors (≥65 years; COPD), and Black, Hispanic, and NYC residents. In summary, unanticipated increases in asthma and COPD ERs after Tier-3 implementation were observed, and demographic disparities in asthma/COPD and PM2.5, POC, and SOC associations were also observed. Future work should confirm findings and investigate triggering of respiratory events by source-specific PM.

UV light absorption at 370 nm by mineral dust, organic carbon, and elemental carbon in the Himalayas and Tibetan Plateau

The mass and light absorption contributions of organic carbon (OC), elemental carbon (EC), and mineral dust influence glacial melting and potentially contribute to climate change over the high Himalayas and Tibetan Plateau (HTP). Plateau-scale investigations of these components and their respective light absorption are limited due to the high altitude. In this study, we combined the analysis of major light-absorbing substances and their corresponding multiwavelength absorption to determine their specific contributions firstly. We investigated the spatial variations of total suspended particle (TSP) mass across the HTP, noting high contributions from dust, carbonaceous components, and secondary inorganic aerosols (SNA, including sulfate, nitrate, and ammonium). Enhanced levels of primary and secondary OC and SNA were observed in the marginal areas of the HTP, associated with high relative humidity (RH) and OX levels (O3+NO2). EC was the primary contributor to light absorption, accounting for approximately 68%, 46%, and 64% in Ngari, Qinghai Lake, and Beiluhe, respectively. We found higher light-absorbing contributions from carbonaceous aerosols in the marginal areas compared to the central HTP site, particularly during the heating seasons (∼90%). Fugitive dust significantly contributed to TSP mass but not to light absorption. The concurrent constraints on the mass and optical properties of OC, EC, and dust in this study can help reduce uncertainties in climate models specific to the HTP.

Distribution Characteristics and Source Analysis of Carbonaceous Aerosols Before and After the Spring Festival in the Guanzhong Plain

The spatio-temporal variation characteristics and potential sources of carbonaceous aerosols in the Guanzhong Plain during the Spring Festival in 2023 were analyzed using inverse distance weighting spatial interpolation （IDW）, secondary organic carbon （SOC） estimation, and potential source contribution factor analysis （PSCF）, with the OC and EC in the PM2.5 of five cities： Xi'an, Baoji, Xianyang, Weinan, and Tongchuan as the research objects. The results showed that in terms of time distribution, ρ（OC） was as follows： after the Spring Festival [（18.6 ±11.0） μg·m-3] &gt; during the Spring Festival [（16.2 ±15.1） μg·m-3] &gt; before the Spring Festival [（10.0 ±8.3） μg·m-3], and ρ（EC） was as follows： after the Spring Festival [（2.2 ±1.2） μg·m-3] &gt; during the Spring Festival [（1.7 ±1.5） μg·m-3] &gt; before the Spring Festival [（1.4 ±1.1） μg·m-3], which indicated that OC and EC concentrations were the most severe after the Spring Festival. In terms of spatial distribution, ρ（OC） was as follows： Xianyang [（21.4 ±17.3） μg·m-3] &gt; Baoji [（15.8 ±12.8） μg·m-3] &gt; Xi'an [（13.6 ±11.3） μg·m-3] &gt; Weinan [（11.6 ±9.1） μg·m-3] &gt; Tongchuan [（10.0 ±8.3） μg·m-3], and ρ（EC） was as follows： Xianyang [（2.1 ±1.4） μg·m-3] &gt; Weinan [（1.8 ±1.4） μg·m-3] &gt; Xi'an [（1.8 ±1.2） μg·m-3] &gt; Tongchuan [（1.6 ±1.4） μg·m-3] &gt; Baoji [（1.2 ±0.9） μg·m-3]. Overall, Xianyang had the most severe PM2.5 and carbon aerosol pollution, whereas Tongchuan had the least pollution. IDW results showed that the high-value center of OC and EC concentration [ρ（OC） &gt; 27.3 μg·m-3, ρ（EC） &gt; 2.9 μg·m-3] was in the middle of the plain, the low-value center of OC and EC concentration [ρ（OC） <7.0 μg·m-3, ρ（EC） < 1.0 μg·m-3] was in the northern plain, and the distribution of OC was higher in the west and lower in the east, whereas the distribution of EC was higher in the east and lower in the west. The proportion of SOC in OC was as follows： after the Spring Festival （51.7%） &gt; during the Spring Festival （41.1%） &gt; before the Spring Festival （36.8%）. The SOC/OC values of each city and the contribution rate of SOC of each city to the Guanzhong Plain indicated that Tongchuan, Baoji, and Xianyang were greatly affected by the secondary conversion of organic carbon. The correlation of OC and EC before, during, and after the Spring Festival （r = 0.85, r = 0.98, and r = 0.94, respectively） indicated a high degree of homology between them. Carbonaceous aerosols had a certain correlation with humidity and wind speed before and during the Spring Festival but had a weak correlation with meteorological factors after the Spring Festival. Carbonaceous aerosols generally were strongly correlated with CO and NO2, and the correlation was strongest after the Spring Festival, whereas the correlation with SO2 was strongest during the Spring Festival. The potential source areas of carbonaceous aerosols in the five cities were mainly concentrated in the local and surrounding areas of southern Gansu, northern Shaanxi, and southern Shaanxi. They were also affected by long-distance transportation from the northwest before the Spring Festival.

Effects of " Air Pollution Prevention and Control Action Plan " on PM2.5 and Chemical Compositions in Zhengzhou in Polluted Winters

The Air Pollution Prevention and Control Action Plan （APPCAP） was promulgated in China in 2013. To explore the effectiveness of APPCAP on PM2.5 in winter in Zhengzhou, PM2.5 samples were collected in Zhengzhou Monitoring Center during December 2013 and December 2018. The chemical composition of PM2.5 was analyzed, including EC, OC, water soluble ions, and metal elements. Pollution episodes under different stages were selected to investigate the changes in PM2.5 concentration and composition. The results showed that： ① The average concentration of PM2.5 in winter in Zhengzhou decreased from （215.38 ±107.28） μg·m-3 in 2013 to （77.45 ±49.81） μg·m-3 in 2018, with a decrease rate of 64%. ② The concentrations of EC, K+, SO42-, and Cl- decreased by 85%, 80%, 78%, and 72%, respectively, and the decrease rate in OC, NH4+, and NO3- was 50%, 41%, and 32%, respectively. ③ Compared with those in winter of 2013, the ratios of OC/EC in winter of 2018 increased by 2.6 times, and the proportion of secondary organic carbon in OC increased to 57%； meanwhile, values of sulfur oxidation rate and nitrogen oxidation rate increased by 1.5 and 1.0 times, respectively, indicating heavy secondary pollution in Zhengzhou. ④ The mass ratios of NO3-/SO42-increased from 0.8 ±0.2 in 2013 to 2.5 ±1.0 in 2018, indicating that the contribution of mobile sources increased and surpassed fixed sources as the main source in Zhengzhou. ⑤The comparison results of different stages of the heavy pollution process showed that ρ（PM2.5） decreased significantly in 2018 compared with that in 2013, with the peak concentration decreasing by 61%. The main chemical composition changed from OC, NO3-, SO42-, and NH4+ to OC, NO3-, and NH4+. The results indicated that the primary emission source control in Zhengzhou had achieved remarkable effects, but the contribution of secondary generation to PM2.5 showed an elevated trend； thus, the influence of secondary generation requires further attention in the future.

The role of naphthalene and its derivatives in the formation of secondary organic aerosol in the Yangtze River Delta region, China

Abstract. Naphthalene (Nap) and its derivatives, including 1-methylnaphthalene (1-MN) and 2-methylnaphthalene (2-MN), serve as prominent intermediate volatile organic compounds (IVOCs) and contribute to the formation of secondary organic aerosol (SOA). In this study, the Community Multiscale Air Quality (CMAQ) model coupled with detailed emissions and reactions of these compounds was utilized to examine their roles in the formation of SOA and other secondary pollutants in the Yangtze River Delta (YRD) region during summer. Significant underestimations of Nap and MN concentrations (by 79 % and 85 %) were observed at the Taizhou site based on the model results using the default emissions. Constrained by the observations, anthropogenic emissions of Nap and MN in the entire region were multiplied by 5 and 7, respectively, to better capture the evolution of pollutants. The average concentration of Nap reached 25 ppt (parts per trillion) in the YRD, with Nap contributing 4.1 % and 8.1 % (up to 12.6 %) of total aromatic emissions and aromatic-derived secondary organic carbon (SOC), respectively. The concentrations of 1-MN and 2-MN were relatively low, averaging 2 and 5 ppt, respectively. Together, they accounted for only 2.4 % of the aromatic-derived SOC. The impacts of Nap and MN oxidation on ozone and radicals were insignificant at regional scales but were not negligible when considering daily fluctuations in locations with high emissions of Nap and MN. This study highlights the significant roles of Nap and MN in the formation of SOA, which may pose environmental risks and result in adverse health effects.

Characterization of PM2.5 Carbonaceous Components in a Typical Industrial City in China under Continuous Mitigation Measures.

The goals of the "dual carbon" program in China are to implement a series of air pollution policies to reduce the emission of carbon-bearing particulate matter (PM). Following improvements in the reduction in carbon emissions in Handan City, China, fine particulate matter (PM2.5) was collected in the winters from 2016 to 2020 to characterize the concentrations and sources of carbonaceous components in PM2.5. Trend analysis revealed that both organic carbon (OC) and elemental carbon (EC) concentrations significantly decreased. The proportion of total carbon aerosol (TCA) in PM2.5 decreased by 47.0%, highlighting the effective reduction in carbon emissions. Secondary organic carbon (SOC) concentrations increased from 2016 (12.86 ± 14.10 μg·m-3) to 2018 (36.76 ± 21.59 μg·m-3) and then declined gradually. SOC/OC was larger than 67.0% from 2018 to 2020, implying that more effective synergistic emission reduction measures for carbonaceous aerosol and volatile organic compounds (VOCs) were needed. In the winters from 2016 to 2020, primary organic carbon (POC) concentrations reduced by 76.1% and 87.6% under a light/moderate pollution period (LP) and heavy/severe pollution periods (HPs), respectively. The TCA/PM2.5 showed a decreasing trend under LP and HP conditions, decreasing by 42.1% and 54.7%, respectively. Source analysis revealed that carbonaceous components were mainly from biomass burning, coal combustion and automotive exhaust emissions in the winters of 2016 and 2020. OC/EC and K+/EC analysis pointed out that air pollutant reduction measurements should focus on rectification biomass fuels in the next stage. Compared with 2016, the contributions of automotive exhaust emissions decreased in 2020. OC and EC concentrations decreased due to control measures on automotive exhaust emissions.

Non-negligible secondary contribution to brown carbon in autumn and winter: inspiration from particulate nitrated and oxygenated aromatic compounds in urban Beijing

Abstract. Nitrated aromatic compounds (NACs) and oxygenated derivatives of polycyclic aromatic hydrocarbons (OPAHs) play vital roles within brown carbon (BrC), influencing both climate dynamics and human health to a certain degree. The concentrations of these drug classes were analyzed in PM2.5 from an urban area in Beijing during the autumn and winter of 2017 and 2018. There were four heavy haze episodes during the campaign, two of which happened prior to heating and the other two during heating. During the entire course of sampling, the mean total concentrations of the nine NACs and the eight OPAHs were 1.2–263 and 2.1–234 ng m−3, respectively. The concentrations of both NACs and OPAHs were approximately 2–3 times higher in the heating period than before heating. For NACs, the relative molecular composition did not change significantly before and during heating, with 4-nitrocatechol and 4-nitrophenol demonstrating the highest abundance. For OPAHs, 1-naphthaldehyde was the most abundant species before and during heating, while the relative proportion of anthraquinone increased by more than twice, from 13 % before heating to 31 % during the heating. In Beijing's urban area during autumn and winter, significant sources of NACs and OPAHs have been traced back to automobile emissions and biomass burning activities. Interestingly, it was observed that the contribution from coal combustion increased notably during heating. It is worth noting that the secondary generation of BrC was important throughout the whole sampling period, which was manifested by the photochemical reaction before heating and the aqueous reaction during heating. It was further found that the haze in autumn and winter was nitrate-driven before heating and secondary organic carbon (SOC)-driven during heating, and the secondary formation of BrC increased significantly in pollution events, particularly during heating.

Bayesian inference-based estimation of hourly primary and secondary organic carbon in suburban Hong Kong: multi-temporal-scale variations and evolution characteristics during PM2.5 episodes

Abstract. Observation-based data of primary and secondary organic carbon in ambient particulate matter (PM) are essential for model evaluation, climate and air quality research, health effect assessments, and mitigation policy development. Since there are no direct measurement tools available to quantify primary organic (POC) and secondary organic carbon (SOC) as separate quantities, their estimation relies on inference approaches using relevant measurable PM constituents. In this study, we measured hourly carbonaceous components and major ions in PM2.5 for a year and a half in suburban Hong Kong from July 2020 to December 2021. We differentiated POC and SOC using a novel Bayesian inference approach. The hourly POC and SOC data allowed us to examine temporal characteristics varying from diurnal and weekly patterns to seasonal variations, as well as their evolution characteristics during individual PM2.5 episodes. A total of 65 city-wide PM2.5 episodes were identified throughout the entire study period, with SOC contributions during individual episodes varying from 10 % to 66 %. In summertime typhoon episodes, elevated SOC levels were observed during daytime hours, and high temperature and NOx levels were identified as significant factors contributing to episodic SOC formation. Winter haze episodes exhibited high SOC levels, likely due to persistent influences from regional transport originating from the northern region to the sampling site. Enhanced SOC formation was observed with increase in the nocturnal NO3 radical (indicated by the surrogate quantity of [NO2][O3]) and under conditions characterized by high water content and strong acidity. These results suggest that both NO3 chemistry and acid-catalyzed aqueous-phase reactions likely make notable contributions to SOC formation during winter haze episodes. The methodology employed in this study for estimating POC and SOC provides practical guidance for other locations with similar monitoring capabilities in place. The availability of hourly POC and SOC data is invaluable for evaluating and improving atmospheric models, as well as understanding the evolution processes of PM pollution episodes. This, in turn, leads to more accurate model predictions and a better understanding of the contributing sources and processes.

New insights into black carbon light absorption enhancement: A comprehensive analysis of two differential behaviors

High uncertainty in optical properties of black carbon (BC) involving heterogeneous chemistry has recently attracted increasing attention in the field of atmospheric climatology. To fill the gap in BC optical knowledge so as to estimate more accurate climate effects and serve the response to global warming, it is beneficial to conduct site-level studies on BC light absorption enhancement (Eabs) characteristics. Real-time surface gas and particulate pollutant observations during the summer and winter over Wuhan were utilized for the analysis of Eabs simulated by minimum R squared (MRS), considering two distinct atmospheric conditions (2015 and 2017). In general, differences in aerosol emissions led to Eabs differential behaviors. The summer average of Eabs (1.92 ± 0.55) in 2015 was higher than the winter average (1.27 ± 0.42), while the average (1.11 ± 0.20) in 2017 summer was lower than that (1.67 ± 0.69) in winter. Eabs and RBC (representing the mass ratio of non-refractory constituents to elemental carbon) constraints suggest that Eabs increased with the increase in RBC under the ambient condition enriched by secondary inorganic aerosol (SIA), with a maximum growth rate of 70.6% in 2015 summer. However, Eabs demonstrated a negative trend against RBC in 2017 winter due to the more complicated mixing state. The result arose from the opposite impact of hygroscopic SIA and absorbing OC/irregular distributed coatings on amplifying the light absorbency of BC. Furthermore, sensitivity analysis revealed a robust positive correlation (R > 0.9) between aerosol chemical compositions (including sulfate, nitrate, ammonium and secondary organic carbon), which could be significantly perturbed by only a small fraction of absorbing materials or restructuring BC through gaps filling. The above findings not only deepen the understanding of BC, but also provide useful information for the scientific decision-making in government to mitigate particulate pollution and obtain more precise BC radiative forcing.

Phenomenology of the Composition of PM2.5 at an Urban Site in Northern France

In this work, PM2.5 was sampled at Dunkerque, a medium-sized city located in northern France. The mean concentration of PM2.5 during the sampling period was 12.6 ± 9.5 μg·m−3. Samples were analyzed for elemental and organic carbon (EC/OC), water-soluble organic carbon (WSOC), humic-like substances (HULIS-C), water-soluble inorganic ions, and major and trace elements. The origin and the variations of species concentrations were examined using elemental enrichment factors, bivariate polar plot representations, and diagnostic concentration ratios. Secondary inorganic ions were the most abundant species (36% of PM2.5), followed by OC (12.5% of PM2.5). Secondary organic carbon (SOC) concentrations were estimated to account for 52% of OC. A good correlation between SOC and WSOC indicated that secondary formation processes significantly contribute to the WSOC concentrations. HULIS-C also represents almost 50% of WSOC. The determination of diagnostic ratios revealed the influence of anthropogenic emission sources such as integrated steelworks and fuel oil combustion. The clustering of 72 h air masses backward trajectories data evidenced that higher concentrations of PM2.5, OC, and secondary inorganic aerosols were recorded when air masses came from north-eastern Europe and the French continental sector, showing the considerable impact of long-range transport on the air quality in northern France.

Long-term evolution of carbonaceous aerosols in PM2.5 during over a decade of atmospheric pollution outbreaks and control in polluted central China

Against the backdrop of an uncertain evolution of carbonaceous aerosols in polluted areas over the long term amid air pollution control measures, this 11-year study (2011–2021) investigated fine particulate matter (PM2.5) and carbonaceous components in polluted central China. Organic carbon (OC) and elemental carbon (EC) averaged 16.5 and 3.4 μg/m3, constituting 16 and 3 % of PM2.5 mass. Carbonaceous aerosols dominated PM2.5 (35 and 27 %) during periods of excellent and good air quality, while polluted days witnessed other components as dominants, with a significant decrease in primary organic aerosols and increased secondary pollution. From 2011 to 2021, OC and EC decreased by 53 and 76 %, displaying a high-value oscillation phase (2011–2015) and a low-value fluctuation phase (post-2016). A substantial reduction in high OC and EC concentrations in 2016 marked a milestone in significant air quality improvement attributed to effective control measures, especially targeting OC and EC, evident from their decreased proportion in PM2.5. Primary OC (POC) in winter exhibited the most pronounced reduction (8 % per year), and the seasonal disparities in PM2.5 and carbonaceous components were reduced, showcasing the effectiveness of control measures. Contrary to the more pronounced reduction of EC, which decreased in proportion to PM2.5, secondary OC (SOC) in PM2.5 exhibited an increasing trend. Along with rising OC/EC, SOC/OC, and SOC/EC ratios, this indicates a growing prominence of secondary pollution compared to the decrease in primary pollution. SOC shows an increasing trend with NO2 rise (r = 0.53), without O3 promoting SOC. Positive correlations of SOC with SO2, CO (r = 0.41, 0.59), also highlight their influence on atmospheric conditions, oxidative capacity, and chemical reactions, indirectly impacting SOC formation. The implementation of precise precursor emission reduction measures holds the key to future efforts in mitigating SOC pollution and reducing PM2.5 concentrations, thereby contributing to improved air quality.

Modeling the molecular composition of secondary organic aerosol under highly polluted conditions: A case study in the Yangtze River Delta Region in China

A near-explicit mechanism, the master chemical mechanism (MCMv3.3.1), coupled with the Community Multiscale Air Quality (CMAQ) model (CMAQ-MCM-SOA), was applied to investigate the characteristics of secondary organic aerosol (SOA) during a pollution event in the Yangtze River Delta (YRD) region in summer 2018. Model performances in predicting explicit volatile organic compounds (VOCs), organic aerosol (OA), secondary organic carbon (SOC), and other related pollutants in Taizhou, as well as ozone (O3) and fine particulate matter (PM2.5) in multiple cities in this region, were evaluated against observations and model predictions by the CMAQ model coupled with a lumped photochemical mechanism (SAPRC07tic, S07). MCM and S07 exhibited similar performances in predicting gaseous species, while MCM better captured the observed PM2.5 and inorganic aerosols. Both models underpredicted OA concentrations. When excluding data during biomass burning events, SOC concentrations were underpredicted by the CMAQ-MCM-SOA model (−28.4 %) and overpredicted by the CMAQ-S07 model (134.4 %), with better agreement with observations in the trend captured by the CMAQ-MCM-SOA model. Dicarbonyl SOA accounted for a significant fraction of total SOA in the YRD, while organic nitrates originating from aromatics were the most abundant species contributing to the SOA formation from gas-particle partitioning. The oxygen-to‑carbon ratio (O/C) for SOA and OA were 0.68–0.75 and 0.20–0.65, respectively, indicating a higher oxidation state in the areas influenced by biogenic emissions. Finally, the phase state of SOA was examined by calculating the glass transition temperature (Tg) based on its molecular composition. It was found that semi-solid state characterized SOA in the YRD, which could potentially impact their chemical transformation and lifetimes along with those of their precursors.

Characteristics of PM2.5 bounded carbonaceous aerosols, carbon dioxide and its stable carbon isotopes (δ13C) in rural households in northwest China: Effect of different fuel combustion

In order to fully understand the carbon emission from different fuels in rural villages of China, especially in the typical atmospheric pollution areas. The characteristics of carbonaceous aerosols and carbon dioxide (CO2) with its stable carbon isotope (δ13C) were investigated in six households, which two households used coal, two households used wood as well as two households used biogas and liquefied petroleum gas (LPG), from two rural villages in Fenwei Plain from March to April 2021. It showed that the fine particulate matter (PM2.5) emitted from biogas and LPG couldn't be as lower as expected in this area. However, the clean fuels could relatively reduce the emissions of organic carbon (OC) and element carbon (EC) in PM2.5 compare to the solid fuels. The pyrolyzed carbon (OP) accounted more total carbon (TC) in coal than the other fuels use households, indicating that more water-soluble OC existed, and it still had the highest secondary organic carbon (SOC) than the other fuels. Meantime, the coal combustions in the two villages had the highest CO2 concentration of 527.6 ppm and 1120.6 ppm, respectively, while the clean fuels could effectively reduce it. The average δ13C values (−26.9‰) was much lighter than almost all the outdoor monitoring and similar to the δ13C values for coal combustion and vehicle emission, showing that they might be the main contributors of the regional atmospheric aerosol in this area. During the sandstorm, the indoor PM2.5 mass and CO2 were increasing obviously. The indoor cancer risk of PAHs for adults and children were greater than 1 × 10−6, exert a potential carcinogenic risk to human of solid fuels combustion in rural northern China. It is important to continue concern the solid fuel combustion and its health impact in rural areas.

Chemical characterization and source apportionment of PM2.5 in a Northeastern China city during the epidemic period.

To investigate the influence of COVID-19 lockdown measures on PM2.5 and its chemical components in Shenyang, PM2.5 samples were continuously collected from January 1 to May 31, 2020. The samples were then analyzed for water-soluble inorganic ions, metal elements, organic carbon, and elemental carbon. The findings indicated a significant decrease in PM2.5 and its various chemical components during the lockdown period, compared to pre-lockdown levels (p < 0.05), suggesting a substantial improvement in air quality. Water-soluble inorganic ions (WSIIs) were identified as the primary contributors to PM2.5, accounting for 47% before the lockdown, 46% during the lockdown, and 37% after the lockdown. Ionic balance analysis revealed that PM2.5 exhibited neutral, weakly alkaline, and alkaline characteristics before, during, and after the lockdown, respectively. NH4+ was identified as the main balancing cation and was predominantly present in the form of NH4NO3 in the absence of complete neutralization of SO42- and NO3-. Moreover, the higher sulfur oxidation ratio (SOR) and nitrogen oxidation ratio (NOR), along with the significant increase in PM2.5/EC, suggested intense secondary transformation during the lockdown period. The elevated OC/EC ratio during the lockdown period implied higher secondary organic carbon (SOC), and the notable increase in SOC/EC ratio indicated a significant secondary transformation of total carbon. The enrichment factor (EF) results revealed that during the lockdown, 9 metal elements (As, Sn, Pb, Zn, Cu, Sb, Ag, Cd, and Se) were substantially impacted by anthropogenic emissions. Source analysis of PMF was employed to identify the sources of PM2.5 in Shenyang during the study period, and the analysis identified six factors: secondary sulfate and vehicle emissions, catering fume sources, secondary nitrate and coal combustion emissions, dust sources, biomass combustion, and industrial emissions, with secondary sulfate and vehicle emissionsand catering fume sourcescontributing the most to PM2.5.