Evaluation of laboratory and environmental exposure systems for protein modification upon gas pollutants and environmental factors

Chemical modifications of proteins induced by ambient ozone(O_(3))and nitrogen oxides(NOx)are of public health concerns due to their potential to trigger respiratory diseases.The laboratory and environmental exposure systems have been widely used to investigate their relevant mechanism in the atmosphere.Using bovine serum albumin(BSA)as a model protein,we evaluated the two systems and aimed to reduce the uncertainties of both the reactants and products in the corresponding kinetic study.In the laboratory simulation system,the generated gaseous pollutants showed negligible losses.Ten layers of BSA were coated on the flow tube with protein extraction recovery of 87.4%.For environmental exposure experiment,quartz fiber filter was selected as the upper filter with low gaseous O_(3)(8.0%)and NO_(2)(1.7%)losses,and cellulose acetate filter was appropriate for the lower filter with protein extraction efficiency of 95.2%.The protein degradation process was observed without the exposure to atmospheric oxidants and contributed to the loss of protein monomer mass fractions,while environmental factors(e.g.,molecular oxygen and ultraviolet)may cause greater protein monomer losses.Based on the evaluation,the study exemplarily applied the two systems to protein modification and both showed that O_(3) promotes the protein oligomerization and nitration,while increased temperature can accelerate the oligomerization and increased relative humidity can inhibit the nitration in the environmental exposure samples.The developed laboratory and environmental systems are suitable for studying protein modifications formed under different atmospheric conditions.A combination of the two will further reveal the actual mechanism of protein modifications.

One-year observation of the mixing states of oxygenated organics-containing single particles in Guangzhou,China

Oxygenated organic molecules(OOMs)play an important role in the formation of secondary organic aerosols(SOAs),but the mixing states of OOMs are still unclear.This study investigates the mixing states of OOM-containing single particles from the measurements taken using a single particle aerosol mass spectrometer in Guangzhou,China in 2022.Generally,the particle counts of OOM particles and the mass concentration of secondary organic carbon(SOC)exhibited similar temporal trends throughout the entire year.The OOM particles were consistently enriched in secondary ions,including 16O−,26CN−,46NO2−,62NO3−,and 97HSO4−.In contrast,the number fractions and diurnal patterns of OOM particles among the total detected particles showed similar distributions in August and October;however,the SOC ratios in fine particulate matter were quite different,suggesting that there were different mixing states of single-particle oxygenated organics.In addition,further classification results indicated that the OOM particles were more aged in October than August,even though the SOC ratios were higher in August.Furthermore,the distribution of hydrocarbon fragments exhibited a notable decrease from January to October,emphasizing the more aged state of the organics in October.In addition,the sharp increase in elemental carbon(EC)-OOM particles in the afternoon in October suggests the potential role of EC in the aging process of organics.Overall,in contrast to the bulk analysis of SOC mass concentration,the mixing states of the OOM particles provide insights into the formation process of SOAs in field studies.

Detection of polycyclic aromatic hydrocarbons using a high performance-single particle aerosol mass spectrometer

The real-time detection of the mixing states of polycyclic aromatic hydrocarbons(PAHs)and nitro-PAHs in ambient particles is of great significance for analyzing the source,aging process,and health effects of PAHs and nitro-PAHs;yet there is still few effective technology to achieve this type of detection.In this study,11 types of PAH and nitro-PAH standard sampleswere analyzed using a high performance-single particle aerosolmass spectrometer(HP-SPAMS)in lab studies.The identification principles‘parent ions’and‘mass-to-charge(m/z)=77’of each compound were obtained in this study.It was found that different laser energies did not affect the identification of the parent ions.The comparative experiments of ambient atmospheric particles,cooking and biomass burning emitted particles with and without the addition of PAHs were conducted and ruled out the interferences from primary and secondary organics on the identification of PAHs.Besides,the reliability of the characteristic ions extraction method was evaluated through the comparative study of similarity algorithm and deep learning algorithm.In addition,the real PAH-containing particles from vehicle exhaust emissions and ambient particles were also analyzed.This study improves the ability of single particle mass spectrometry technology to detect PAHs and nitro-PAHs,and HP-SPAMS was superior to SPAMS for detecting single particles containing PAHs and nitro-PAHs.This study provides support for subsequent ambient observations to identify the characteristic spectrum of single particles containing PAHs and nitro-PAHs.

Variations of aminiums in fine particles at a suburban site in Guangzhou, China: Importance of anthropogenic and natural emissions

Amines are important nitrogen-containing compounds in fine particles(PM2.5)in the atmosphere.Observations are necessary for in-depth understanding on the characteristics,sources and atmospheric processes of aminiums.In this study,the observation of ten C_(1)–C_(4) aminiums in PM_(2.5) was conducted in January and March of 2021 in suburban Guangzhou.The concentration and composition of aminiums showed significant differences between the pollution episodes and non-episode periods.Seasonal difference was also observed between winter and spring.The influence of meteorological factors(i.e.,wind speed,atmospheric pressure,temperature and relative humidity)was investigated.The variations of aminiums were also affected by different sources.Anthropogenic sources were suggested to be major contributor to aminiums in the pollution episodes,while biological sources were important sources to aminiums in the non-episode periods,especially in spring.Positive matrix factorization receptor model was applied to investigate the source contributions,and four major sources were identified.The results show that vehicular emission,industrial production,biological emission and soil/dust were the major sources of aminiums.This study emphasizes the importance of source contribution and meteorological conditions on the variations of aminiums,which provides further understanding of organic nitrogen in the atmosphere.

Seasonal variations of mass absorption efficiency of elemental carbon in PM_(2.5) in urban Guangzhou of South China

This study investigates seasonal variations of mass absorption efficiency of elemental carbon(MAE_(EC))and possible influencing factors in urban Guangzhou of South China.Mass concentrations of elemental carbon(EC)and organic carbon(OC)in PM_(2.5) and aerosol absorption coefficient(b_(ap))at multi-wavelengths were simultaneously measured in four seasons of 2018-2019 at hourly resolution by a semi-continuous carbon analyzer and an aethalometer.Seasonal average mass concentrations of EC were in the range of 1.36-1.70μgC/m^(3) with a lower value in summer than in the other seasons,while those of OC were in the range of 4.70–6.49μgC/m^(3) with the lowest value in summer and the highest in autumn.Vehicle exhaust from local traffic was identified to be the predominant source of carbonaceous aerosols.The average aerosol absorption Angstrom exponents(AAE)were lower than 1.2 in four seasons,indicating EC and b_(ap) were closely related with vehicle exhaust.Seasonal MAE EC at 550 nm was 11.0,8.5,10.4 and 11.3 m^(2)/g in spring,summer,autumn,and winter,respectively.High MAE EC was related with the high mass ratio of non-carbonaceous aerosols to EC and high ambient relative humidity.