Single Particle Aerosol Mass Spectrometer Research Articles

Exploring secondary aerosol formation associated with elemental carbon in the lower free troposphere

The variability of element carbon (EC) mixed with secondary species significantly complicates the assessment of its environmental impact, reflecting the complexity and diversity of EC-containing particles' composition and morphology during their ascent and regional transport. While the catalytic role of EC in secondary aerosol formation is recognized, the effects of heterogeneous chemistry on secondary species formation within diverse EC particle types are not thoroughly understood, particularly in the troposphere. Alpine sites offer a prime environment to explore EC properties post-transport from the ground to the free troposphere. Consequently, we conducted a comprehensive study on the genesis of secondary aerosols in EC-containing particles at Mt. Hua (altitude: 2069 m) from 1 May to 10 July, using a single particle aerosol mass spectrometer (SPAMS). Our analysis identified six major EC particle types, with EC-K, EC-SN, and EC-NaK particles accounting for 27.6 %, 27.0 %, and 19.6 % of the EC particle population, respectively. The concentration-weighted trajectory (CWT) indicated that the lower free troposphere over Mt. Hua is significantly affected by anthropogenic emissions at ground-level, predominantly from northwestern and eastern China. Atmospheric interactions are crucial in generating high sulfate levels in EC-SN and EC-OC particles (> 70 %) and notable nitrate levels in EC-K, EC-BB, and EC-Fe particles (> 80 %). The observed high chloride content in EC-OC particles (56 ± 32 %) might enhance chlorine's reactivity with organic compounds via heterogeneous reactions within the troposphere. Distinct diurnal cycles for sulfate and nitrate are mainly driven by varying transport dynamics and formation processes, showing minimal dependency on EC particle types. Enhanced nocturnal oxalate conversion in EC-Fe particles is likely due to the aqueous oxidation of precursors, with Fe-catalyzed Fenton reactions enhancing OH radical production. This investigation provides critical insights into EC's role in secondary aerosol development during its transport in the lower free troposphere.

Characterizing leaf-deposited particles: Single-particle mass spectral analysis and comparison with naturally fallen particles

The size and composition of particulate matter (PM) are pivotal in determining its adverse health effects. It is important to understand PM’s retention by plants to facilitate its atmospheric removal. However, the distinctions between the size and composition of naturally fallen PM (NFPM) and leaf-deposited PM (LDPM) are not well-documented. Here we utilize a single-particle aerosol mass spectrometer, coupled with a PM resuspension chamber, to analyze these differences. We find that LDPM particles are 6.8–97.3% larger than NFPM. Employing a neural network algorithm based on adaptive resonance theory, we have identified distinct compositional profiles: NFPM predominantly consists of organic carbon (OC; 31.2%) and potassium-rich components (19.1%), whereas LDPM are largely composed of crustal species (53.9–60.6%). Interestingly, coniferous species retain higher OC content (11.5–13.7%) compared to broad-leaved species (0.5–1.2%), while the levoglucosan content exhibit an opposite trend. Our study highlights the active role of tree leaves in modifying PM composition beyond mere passive capture, advocating for a strategic approach to species selection in urban greening initiatives to enhance PM mitigation. These insights provide guidance for urban planners and environmentalists in implementing nature-based solutions to improve urban air quality.

Development and characterization of a high-performance single-particle aerosol mass spectrometer (HP-SPAMS)

Abstract. This study describes a high-performance single-particle mass spectrometry (HP-SPAMS) design in detail. The comprehensive improvements in the injection system, optical sizing system, mass spectrometry, and data acquisition system have improved particle detection efficiency and chemical analysis. The combination of an aerodynamic particle concentrator (APC) system and a wide range of aerodynamic lenses (ADLs) enables the concentration of particles in the 100–5000 nm range. Using an APC increases the instrument inlet flow by a factor of 3–5. The ion delayed-exaction technology of bipolar time-of-flight mass spectrometry improves the mass resolution by 2–3 times, allowing the differentiation of isobaric ions of different substances. Moreover, the four-channel data acquisition technology greatly enhances the dynamic range of mass spectrometry. The improved HP-SPAMS enhances the overall capability of the instrument in terms of particle detection number and scattering efficiency. Moreover, it improves accuracy and sensitivity for component identification of individual particles. The experimental performance of HP-SPAMS shows that the scattering efficiency of polystyrene latex microspheres is almost 70 %–100 % in the range of 300–3000 nm. Compared to the previous SPAMS, HP-SPAMS has a larger inlet flow rate and scattering efficiency and a higher laser frequency, which makes HP-SPAMS increase the effective number of particles detected and improve the temporal resolution of detection. For the analysis of individual particles, HP-SPAMS achieves an average mass spectral resolution of 2500 at m/z 208, which helps distinguish between most organic fragment ions and metal ions and facilitates the analysis of complex aerosol particles. For the analysis of individual particles, the increased resolution of the HP-SPAMS contributes to the differentiation of most organic fragment ions and metal ions and facilitates the evaluation of complex aerosol particles, in the case of atmospheric lead-containing particles. The improved detection efficiency and chemical analysis capability of HP-SPAMS will be of great importance for low-concentration aerosol detection and complex aerosol component analysis.

Mixing state and influence factors controlling diurnal variation of particulate nitrophenol compounds at a suburban area in northern China

Nitrophenols have received extensive attention due to their strong light-absorbing ability in the near-ultraviolet-visible region, which could be influenced by the atmospheric processes of nitrophenols. However, our knowledge and understanding of the formation and evolution of nitrophenols are still in the nascent stages. In the present study, the mixing states of four mononitrophenol particles (i.e., nitrophenol, methynitrophenol, nitrocatechol, and methoxynitrophenol), and one nitropolycyclic aromatic hydrocarbon particles (i.e., nitronaphthol (NN)) were investigated using a single-particle aerosol mass spectrometer (SPAMS) in November 2019 in Qingdao, China. The results showed, for the first time, that mononitrophenols and NN exhibit different mixing states and diurnal variations. Four mononitrophenols were internally mixed well with each other, and with organic acids, nitrates, potassium, and naphthalene. The diurnal variation in the number fraction of mononitrophenols presented two peaks at 07:00 to 09:00 and 18:00 to 20:00, and a valley at noon. Atmospheric environmental conditions, including NO2, O3, relative humidity, and temperature, can significantly influence the diurnal variation of mononitrophenols. Multiple linear regression and random forest regression models revealed that the main factors controlling the diurnal variation of mononitrophenols were photochemical reactions during the day and aqueous-phase reactions during the night. Unlike mononitrophenols, about 62–83% of NN were internally mixed with [NH4]+ and [H(NO3)2]-, but not with organic acids and potassium. The diurnal variation of NN was also different from that of mononitrophenols, generally increased from 17:00 to 10:00 and then rapidly decreaed from 11:00 to 16:00. These results imply that NN may have sources and atmospheric processes that are different from mononitrophenols. We speculate that this is mostly controlled by photochemical reactions and mixing with [NH4]+, which may influence the diurnal variation of NN in the ambient particles; however, this requires further confirmation. These findings extend our current understanding of the atmospheric formation and evolution of nitrophenols.

Characterization of carbonaceous particles by single particle aerosol mass spectrometer in the urban area of Chengdu, China.

Carbonaceous particles are an important chemical component of atmospheric fine particles. In this study, a single particle aerosol mass spectrometer was used to continuously measure the carbonaceous particles in Chengdu, one of the megacities most affected by haze in China, from January 22 to March 3, 2021. During the observation period, the average mass concentration of PM2.5 was 62.3 ± 37.2 μg m-3, and the emissions from mobile sources were more prominent. Carbonaceous particles accounted for 68.6% of the total particles and could be classified into 10 categories, with elemental carbon (EC) mixed with sulfate (EC-S) particles making the highest contribution (33.1%). EC particles rich in secondary components and organic carbon (OC) particles rich in secondary component exhibited different diurnal variations, suggesting different sources and mixing mechanisms. From "excellent" to "polluted" days, the contributions of EC-S, EC mixed with sulfate and nitrate (EC-SN) and OC mixed with EC (OC-EC) particles increased by 9.8%, 4.5% and 6.6%, respectively, and thus these particles are key targets for future pollution control. The potential source contribution of the southwest area was stronger than that of other areas, and the potential contribution of regional transport to EC-related particles was stronger than to OC-related particles. Most particles were highly mixed with sulfate or nitrate, and the level of secondary mixing further enhanced as pollution worsened.

Mixing state and effective density of aerosol particles during the Beijing 2022 Olympic Winter Games

Abstract. Mixing state and density are two key parameters of aerosol particles affecting their impacts on radiative forcing and human health. Here a single-particle aerosol mass spectrometer in tandem with a differential mobility analyzer and an aerodynamic aerosol classifier was deployed during the Beijing 2022 Olympic Winter Games (OWG) to investigate the impacts of emission controls on particle mixing state and density. Our results show the dominance of carbonaceous particles comprising mainly total elemental carbon (Total-EC, 13.4 %), total organic carbon (Total-OC, 10.5 %) and Total-ECOC (47.1 %). Particularly, the particles containing organic carbon and sulfate were enhanced significantly during OWG, although those from primary emissions decreased. The composition of carbonaceous particles also changed significantly which was characterized by the decreases in EC mixed with nitrate and sulfate (EC-NS), EC mixed with potassium nitrate (KEC-N), and amine-containing particles and increase in ECOC mixed with nitrate and sulfate (ECOC-NS). This result indicates that emission controls during OWG reduced the mixing of EC with inorganic aerosol species and amines yet increased the mixing of EC with organic aerosol. The average effective density (ρeff) of aerosol particles (150–300 nm) was 1.15 g cm−3 during the non-Olympic Winter Games (nOWG), with higher values during OWG (1.26 g cm−3) due to the increase in secondary particle contribution. In addition, the ρeff of most particles increased with the increases in pollution levels and relative humidity, yet they varied differently for different types of particles, highlighting the impacts of aging and formation processes on the changes of particle density and mixing state.

In-depth study of the formation processes of single atmospheric particles in the south-eastern margin of the Tibetan Plateau

Abstract. The unique geographical location of the Tibetan Plateau (TP) plays an important role in regulating global climate change, but the impacts of the chemical components and atmospheric processing on the size distribution and mixing state of individual particles are rarely explored in the south-eastern margin of the TP, which is a transport channel for pollutants from Southeast Asia to the TP during the pre-monsoon season. Thus a single-particle aerosol mass spectrometer (SPAMS) was deployed to investigate how the local emissions of chemical composition interact with the transporting particles and assess the mixing state of different particle types and secondary formation in this study. The TP particles were classified into six distinct types, mainly including the largest fraction of the potassium-rich (K-rich) type in the total particles (30.9 %), followed by the biomass burning (BB) type (18.7 %). Most particle types were mainly transported from the sampling site's surroundings and along the Sino-Myanmar border, but the air mass trajectories from north-eastern India and Myanmar show a greater impact on the number fraction of the BB (31.7 %) and dust (18.2 %) types, respectively. Then, the two episodes with high particle concentrations showed that the differences in the meteorological conditions in the same trajectory clusters could cause significant changes in chemical components, especially the dust and aged elemental carbon (aged EC) types, which changed by a total of 93.6 % and 72.0 %, respectively. Ammonium and dust particles distribute at a relatively larger size (∼600 nm), but the size peak of other types is present at ∼440 nm. Compared with the abundant sulfate (97HSO4-), the low nitrate (62NO3-) internally mixed in TP particles is mainly due to the fact that nitrate is more volatilized during the transport process. The formation mechanism of secondary speciation demonstrates that the formation capacity of atmospheric oxidation is presumably affected by the convective transmission and the regional transport in the TP. However, the relative humidity (RH) could significantly promote the formation of secondary species, especially 97HSO4- and 18NH4+. This study provides new insights into the particle composition and size, mixing state, and ageing mechanism in high time resolution over the TP region.

Secondary aerosol formation in incense burning particles by O3 and OH oxidation via single particle mixing state analysis

Incense burning is a common religious activity that emits abundant gaseous and particulate pollutants into the atmosphere. During their atmospheric lifetime, these gases and particles are subjected to oxidation, leading to the formation of secondary pollutants. We examined the oxidation of incense burning plumes under O3 exposure and dark condition using an oxidation flow reactor connected to a single particle aerosol mass spectrometer (SPAMS). Nitrate formation was observed in incense burning particles, mainly attributable to the ozonolysis of nitrogen-containing organic compounds. With UV on, nitrate formation was significantly enhanced, likely due to HNO3/HNO2/NOx uptake triggered by OH chemistry, which is more effective than ozone oxidation. The extent of nitrate formation is insensitive to O3 and OH exposure, possibly due to the diffusion limitation on interfacial uptake. The O3-UV-aged particles are more oxygenated and functionalized than O3-Dark-aged particles. Oxalate and malonate, two typical secondary organic aerosol (SOA) components, were found in O3-UV-aged particles. Our work reveals that nitrate, accompanied by SOA, can rapidly form in incense-burning particles upon photochemical oxidation in the atmosphere, which could deepen our understanding of air pollution caused by religious activities.

Bioaerosol Identification by Wide Particle Size Range Single Particle Mass Spectrometry

The properties of bioaerosols are complex and diverse, and have a direct impact on the environment, climate, and human health. The effective identification of bioaerosols in the atmosphere is very significant with regard to accurately obtaining the atmospheric chemical characteristics of bioaerosols and making biological early warnings and predictions. To improve the detection of large particle bioaerosol and non-bioaerosol interference in the process of bioaerosol recognition this study detected a variety of bioaerosols and abiotic aerosols based on a single particle aerosol mass spectrometer (SPAMS). Furthermore, the bioaerosol particle identification and classification algorithm based on Zawadowicz the ratio of phosphate to organic nitrogen is optimized to distinguish bioaerosols from abiotic aerosols. The influence of ionized laser energy on classification methods is thoroughly explored here. The results show that 15 kinds of pure fungal aerosols were detected by SPAMS based on a wide size range sampling system, and that fungal aerosols with a particle size of up to 10 μm can be detected. Through the mass spectra peak ratio method of PO3−/PO2− and CNO−/CN−, when discriminating abiotic aerosols such as disruptive biomass combustion particles, automobile exhaust, and dust from pure bacterial aerosols, the discrimination degree is up to 97.7%. The optimized ratio detection method of phosphate to organic nitrogen has strong specificity, which can serve as the discriminant basis for identifying bioaerosols in SPAMS analytical processes.

In-cloud scavenging of chemically segregated particle types by individual particle observation

While aerosol plays a significant role in the formation of cloud, the in-cloud scavenging of chemically segregated particle types were still insufficiently investigated and the controlling factors remain ambiguous. Several field observations were carried out during 2018–2021 at Mt. Tianjing (1690 m a.s.l.) in southern China, based on ground-based counterflow virtual impactor (GCVI)-single particle aerosol mass spectrometer (SPAMS), to investigate the in-cloud scavenging (activation) of various particle types, including black carbon (BC), organic-containing particles (OC), mineral dust (Dust), metal-containing particles (Metal), potassium-rich particles (K-rich) and sea salt (SS). GCVI was used to sample cloud droplet residual particles (Res) while PM2.5 inlet sampled interstitial particles (Inter) during cloud events and ambient particles (Amb) on sunny days, respectively. Different types of particles were recognized based on spectral characteristics obtained by the SPAMS. Based on the coupled GCVI-SPAMS measurements, the number-based scavenging efficiencies (NSEs) of various particle types could be quantified. Besides, the influence of liquid water content (LWC), PM2.5, particle size, and mixing state on the NSEs were discussed. The NSE of SS was the highest (32.4%) while OC showed the lowest NSE (9.1%). Other particle types shared similar NSEs with all the detected particles, with an average of ∼20–25%. Apart from OC, NSEs of other types of particles increased with the increase of LWC and decreased with the increase of the concentration of PM2.5, suggesting that numerous PM2.5 suppressed particles entering cloud droplets via competing for water vapor. The annual variations of NSEs were generally in accordance with LWC and PM2.5, reflecting the certain role of these environment conditions. The NSEs typically increased with particle size in a range of 0.2–2.0 μm, reflecting the dominant nucleation mechanism during in-cloud scavenging. Particles mixed with sulfate and nitrate were easier to be scavenged than those coated with organic compounds, e.g., the discrepancy reached 11.8% for the K-rich particles.

Analytical performance of single particle aerosol mass spectrometer for accurate sizing and isotopic analysis of individual particles

The commercial Hexin Single particle aerosol mass spectrometer (SPAMS) has been widely used for environmental aerosol monitoring and source apportionment. However, particle size measurement is easily affected by environment pressure fluctuation and sampling orifice clogging. The capability for quantitative analysis is poor, and few isotope measurement has been reported. This paper aims to evaluate the analytical performance of SPAMS and extend its application. First, the flight time of standard particles having different densities and sizes was measured under various conditions (aerodynamic lens upstream pressure and carrier gas). We proposed a universal method for particle size calibration, measurement and correction, taking into account the effects of lens geometry (acceleration nozzle diameter), particle parameters (density, diameter, and shape factor), and operating conditions (lens upstream pressure and carrier gas). Then, isotope measurement was performed when introducing a solution droplet containing a single element. Metal oxide and metal cluster ions were observed in the mass spectrum, indicating incomplete ionization of the sample droplet. The mass discrimination effect was carefully evaluated to correct the measured isotope ratio. Results show that the achievable accuracy of the corrected isotope ratio for elements investigated was 5%. The instrumental performance was relatively poor for elements having great ionization potential or bond energy. Finally, Ag/Eu2O3 suspension and yellow cake/ethanol suspension were analyzed for size, elemental and isotopic analysis. We confirmed that the mass discrimination effect during suspension introduction could be corrected using the mass discrimination correction factor obtained during solution introduction. The Ag, Eu and U in these suspension particles were all found to be at natural abundance. The uranium in the yellow cake was identified as sodium duranyate (Na2U2O7) with volumetric equivalent diameter of approximately 65 nm. The work presented here is beneficial for instrument improvement and wide application.

Long-Term Observation of Mixing States and Sources of Vanadium-Containing Single Particles from 2020 to 2021 in Guangzhou, China.

The distribution of vanadium (V) in aerosols is commonly used to track ship exhaust emissions, yet the atmospheric abundance of V has been greatly reduced due to the implementation of a clean fuel policy. Recent research mainly discussed the chemical compositions of ship-related particles during specific events, yet few studies focus on the long-term changes of V in the atmosphere. In this study, a single-particle aerosol mass spectrometer was used to measure V-containing particles from 2020 to 2021 in Huangpu Port in Guangzhou, China. The long-term trend of the particle counts of V-containing particles declined annually, but the relative abundance of V-containing particles in the total single particles increased in summer due to the influence of ship emissions. Positive matrix factorization revealed that in June and July 2020, 35.7% of the V-containing particles were from ship emissions, followed by dust and industrial emissions. Furthermore, more than 80% of the V-containing particles were found mixing with sulfate and 60% of the V-containing particles were found mixing with nitrate, suggesting that the majority of the V-containing particles were secondary particles processed during the transport of ship emissions to urban areas. Compared with the small changes in the relative abundance of sulfate in the V-containing particles, the relative abundance of nitrate exhibited clear seasonal variations, with a high abundance in winter. This may have been due to the increased production of nitrate from high concentrations of precursors and a suitable chemical environment. For the first time, the long-term trends of V-containing particles in two years are investigated to demonstrate changes in their mixing states and sources after the clean fuel policy, and to suggest the cautious application of V as an indicator of ship emissions.

Design and Simulation of Aerosol Inlet System for Particulate Matter with a Wide Size Range

A novel aerodynamic lens-based inlet system was developed for a wide particle size range, and it could extend the size range of transmitted particulate matter (PM) to 50 nm–10 μm. The lens system adopted a seven-stage aerodynamic focusing orifice to extend the range of transmitted PM, and a relaxation system with a virtual impact function was introduced at the front of the aerodynamic lens. Through the innovative design, the system could concentrate the input samples as well as effectively enhance the focusing effect on large PM. Furthermore, an additional aerodynamic pre-focusing inlet system was innovatively added to the front of the sampling orifice of the traditional aerodynamic lens, and it could pre-focus large PM into the axis region before it entered the small orifice and then solve the previous problem with loss of large PM. Fluid simulations indicated that the inlet system could achieve 100% effective transmission and focusing for PM in the range of 0.18–10 μm. The characterization and verification results obtained from the improved single-particle aerosol mass spectrometer (SPAMS) were remarkably consistent with the theoretical values. The practical tests indicated that bioaerosol particles up to 10 μm could be detected. Compared with the observation for the same type of lens, the focusing performance of this novel lens system has better advantages in particle size range and transmission efficiency and therefore, it has broad application prospects in bioaerosol research, single-cell analysis, etc.

Mixing states and secondary formation processes of organic nitrogen-containing single particles in Guangzhou, China

Organic nitrogen (ON) compounds play a significant role in the light absorption of brown carbon and the formation of organic aerosols, however, the mixing state, secondary formation processes, and influencing factors of ON compounds are still unclear. This paper reports on the mixing state of ON-containing particles based on measurements obtained using a high-performance single particle aerosol mass spectrometer in January 2020 in Guangzhou. The ON-containing particles accounted for 21% of the total detected single particles, and the particle count and number fraction of the ON-containing particles were two times higher at night than during the day. The prominent increase in the content of ON-containing particles with the enhancement of NOx mainly occurred at night, and accompanied by high relative humidity and nitrate, which were associated with heterogeneous reactions between organics and gaseous NOx and/or NO3 radical. The synchronous decreases in ON-containing particles and the mass absorption coefficient of water-soluble extracts at 365 nm in the afternoon may be associated with photo-bleaching of the ON species in the particles. In addition, the positive matrix factorization analysis found five factors dominated the formation processes of ON particles, and the nitrate factor (33%) mainly contributed to the production of ON particles at night. The results of this study provide unique insights into the mixing states and secondary formation processes of the ON-containing particles.

Brake wear-derived particles: Single-particle mass spectral signatures and real-world emissions

Brake wear is an important but unregulated vehicle-related source of atmospheric particulate matter (PM). The single-particle spectral fingerprints of brake wear particles (BWPs) provide essential information for understanding their formation mechanism and atmospheric contributions. Herein, we obtained the single-particle mass spectra of BWPs by combining a brake dynamometer with an online single particle aerosol mass spectrometer and quantified real-world BWP emissions through a tunnel observation in Tianjin, China. The pure BWPs mainly include three distinct types of particles, namely, Ba-containing particles, mineral particles, and carbon-containing particles, accounting for 44.2%, 43.4%, and 10.3% of the total BWP number concentration, respectively. The diversified mass spectra indicate complex BWP formation pathways, such as mechanical, phase transition, and chemical processes. Notably, the mass spectra of Ba-containing particles are unique, which allows them to serve as an excellent indicator for estimating ambient BWP concentrations. By evaluating this indicator, we find that approximately 4.0% of the PM in the tunnel could be attributable to brake wear; the real-world fleet-average emission factor of 0.28 mg km−1 veh−1 is consistent with the estimation obtained using the receptor model. The results presented herein can be used to inform assessments of the environmental and health impacts of BWPs to formulate effective emissions control policies.

Identify the contribution of vehicle non-exhaust emissions: a single particle aerosol mass spectrometer test case at typical road environment

Identify the contribution of vehicle non-exhaust emissions: a single particle aerosol mass spectrometer test case at typical road environment

Real-time, single-particle chemical composition, volatility and mixing state measurements of urban aerosol particles in southwest China

To investigate the volatility of atmospheric particulates and the evolution of other particulate properties (chemical composition, particle size distribution and mixing state) with temperature, a thermodenuder coupled with a single particle aerosol mass spectrometer was used to conduct continuous observations of atmospheric fine particles in Chengdu, southwest China. Because of their complex sources and secondary reaction processes, the average mass spectra of single particles contained a variety of chemical components (including organic, inorganic and metal species). When the temperature rose from room temperature to 280°C, the relative areas of volatile and semi-volatile components decreased, while the relative areas of less or non-volatile components increased. Most (> 80%) nitrate and sulfate existed in the form of NH4NO3 and (NH4)2SO4, and their volatilization temperatures were 50–100°C and 150–280°C, respectively. The contribution of biomass burning (BB) and vehicle emission (VE) particles increased significantly at 280°C, which emphasized the important role of regional biomass burning and local motor vehicle emissions to the core of particles. With the increase in temperature, the particle size of the particles coated with volatile or semi-volatile components was reduced, and their mixing with secondary inorganic components was significantly weakened. The formation of K-nitrate (KNO3) and K-sulfate (KSO4) particles was dominated by liquid-phase processes and photochemical reactions, respectively. Reducing KNO3 and BB particles is the key to improving visibility. These new results are helpful towards better understanding the initial sources, pollution formation mechanisms and climatic effects of fine particulate matter in this megacity in southwest China.

Characteristics of volatile organic compounds and secondary organic aerosol pollution in different functional areas of petrochemical industrial cities in Northwest China

The aim of this study was to better understand the characteristics of volatile organic compounds (VOCs) and secondary organic aerosol (SOA) pollution in different functional areas of petrochemical industrial cities. In Lanzhou, a typical petrochemical industrial city in Northwest China, with the use of an Integrated Atmospheric Mobile Monitoring Vehicle (IAMMV), various real-time online monitoring instruments, including a VOC monitoring instrument (TH-300B) and single-particle aerosol mass spectrometer (SPAMS), were used in combination. These instruments were employed to determine PM2.5, VOCs and other factors at monitoring sites in Xigu (XG) and Chengguan (CG) districts in September 2020 and 2021, respectively. The results revealed that during the monitoring period, the average VOC concentrations at the XG and CG monitoring sites were 102.3 and 35.8 ppb, respectively. Benzene (45.58 %) and toluene (24.47 %) significantly contributed to the SOA formation potential at the XG site. M/P-xylene (27.88 %) and toluene (23.64 %) more notably contributed to the SOA formation potential at the CG site. The PM2.5 mass concentration at the XG site (24.1 μg·m−3) was similar to that at the CG site (21.2 μg·m−3), but the proportion of particulate matter components greatly differed. The proportion of organic carbon (OC) at the XG site (19.00 %) was higher than that at the CG site (9.97 %). The number of particles containing C2H3O+ (m/z = 43) accounted for 36.96 % and 15.41 % of the total particles at the XG and CG sites, respectively. The mixing ratios of OC and hybrid carbon (OCEC) with C2H3O+ (m/z = 43) were 0.81 and 0.53, respectively, at the XG site and reached only 0.48 and 0.25, respectively, at the CG site. The secondary ageing degree of particles in XG district was high. These results could provide a reference for ambient air quality improvement and the formulation of governance measures in different functional areas of petrochemical industrial cities.

Ambient particle characteristics by single particle aerosol mass spectrometry at a coastal site in Hong Kong: a case study affected by the sea-land breeze.

The sea-land breeze (SLB) circulation plays a vital role in the transport of atmospheric pollutants in coastal cities. In this study, a single particle aerosol mass spectrometer (SPAMS) and combined bulk aerosol instruments were deployed to investigate the ambient particle characteristic at a suburban coastal site in Hong Kong from February 22 to March 10, 2013. Significant SLB circulations were captured from March 6-10, 2013, during the campaign. During the SLB periods, air quality worsened, with PM2.5 concentrations reaching a peak of 55.6 μg m-3 and an average value of 42.8 ± 4.5 μg m-3. A total of 235,894 particles were measured during the SLB stage. Eight major sources were identified by investigating the mixing states of the total particles, including the coal-burning related particles (48.1%), biomass burning particles (6.7%), vehicle emission-related particles (16.4%), sea salt (9.2%), ship emission particles (2.7%), dust/steeling industries (3.7%), waste incineration (6.3%), and road dust (3.9%). It was noteworthy that the PM2.5 concentrations and particle numbers increased sharply during the transition of land wind to the sea breeze. Meanwhile, the continental sourced pollutants recirculated back to land resulting in a cumulative increase in pollutants. Both individual and bulk measurements support the above results, with high contributions from coal burning, biomass burning, bulk K+, and NO3 -, which were probably from the regional transportation from the nearby area. In contrast, the ship and vehicle emissions increased during the SLB period, with a high sulfate concentration partially originating from the ship emission. In this study, field evidence of continental-source pollutants backflow to land with the evolution of sea breeze was observed and helped our current understanding of the effect of SLB on air quality in the coastal city.

Single-particle volatility and implications for brown carbon absorption in Beijing, China

Aerosol volatility has a substantial impact on gas-particle partitioning, aging process and hence brown carbon (BrC) absorption. Here we analyzed single-particle volatility in winter in Beijing using a thermodenuder coupled with a single particle aerosol mass spectrometer along with a suite of collocated measurements. Our results showed that elemental carbon, metals, organic nitrogen (ON) were the dominant low-volatility components. The ON-containing particles accounting for 50 % of the total low-volatility particles comprised mainly ON-organic carbon (ON-OC) particles which were associated with biomass burning and significantly enhanced during polluted periods with high relative humidity and nitrogen oxides (NOx) levels. By analyzing the relationship between single-particle volatility and BrC, we found that semi-volatile particles related to fossil fuel combustion contributed dominantly to the light absorption of BrC (~50 %). Comparatively, the low-volatility and semi-volatile particles related to biomass burning contributed 21–35 % and 10–15 %, respectively to the BrC light absorption. Our results demonstrated that single particles from different sources with different volatility showed different impacts on BrC absorption. Although low-volatility organic aerosol accounted only for ~16 % of the total ambient organics, they can contribute as much as ~30–40 % to BrC light absorption in winter in Beijing.