Persistent Influence of Wildfire Emissions in the Western United States and Characteristics of Aged Biomass Burning Organic Aerosols under Clean Air Conditions.

Wildfire-influenced air masses under regional background conditions were characterized at the Mt. Bachelor Observatory (∼2800 m a.s.l.) in summer 2019 to provide a better understanding of the aging of biomass burning organic aerosols (BBOAs) and their impacts on the remote troposphere in the western United States. Submicron aerosol (PM1) concentrations were low (average ± 1σ = 2.2 ± 1.9 µg sm-3), but oxidized BBOAs (average O/C = 0.84) were constantly detected throughout the study. The BBOA correlated well with black carbon, furfural, and acetonitrile and comprised above 50% of PM1 during plume events when the peak PM1 concentration reached 18.0 µg sm-3. Wildfire plumes with estimated transport times varying from ∼10 h to >10 days were identified. The plumes showed ΔOA/ΔCO values ranging from 0.038 to 0.122 ppb ppb-1 with a significant negative relation to plume age, indicating BBOA loss relative to CO during long-range transport. Additionally, increases of average O/C and aerosol sizes were seen in more aged plumes. The mass-based size mode was approximately 700 nm (Dva) in the most oxidized plume that likely originated in Siberia, suggesting aqueous-phase processing during transport. This work highlights the widespread impacts that wildfire emissions have on aerosol concentration and properties, and thus climate, in the western United States.

Unexpected rise of atmospheric secondary aerosols from biomass burning during the COVID-19 lockdown period in Hangzhou, China.

After the global outbreak of COVID-19, the Chinese government took many measures to control the spread of the virus. The measures led to a reduction in anthropogenic emissions nationwide. Data from a single particle aerosol mass spectrometer in an eastern Chinese megacity (Hangzhou) before, during, and after the COVID-19 lockdown (5 January to February 29, 2020) was used to understand the effect lockdown had on atmospheric particles. The collected single particle mass spectra were clustered into eight categories. Before the lockdown, the proportions of particles ranked in order of: EC (57.9%) < K-SN (13.6%) < Fe-rich (10.2%) < ECOC (6.7%) < K-Na (6.6%) < OC (3.4%) < K-Pb (1.0%) < K-Al (0.7%). During the lockdown period, the EC and Fe-rich particles decreased by 42.8% and 93.2% compared to before lockdown due to reduced vehicle exhaust and industrial activity. By contrast, the K-SN and K-Na particles containing biomass burning tracers increased by 155.2% and 45.2% during the same time, respectively. During the lockdown, the proportions of particles ranked in order of: K-SN (39.7%) < EC (38.1%) < K-Na (11.0%) < ECOC (7.7%) < OC (1.2%) < K-Pb (0.9%) < Fe-rich (0.8%) < K-Al (0.6%). Back trajectory analysis indicated that both inland (Anhui and Shandong provinces) and marine transported air masses may have contributed to the increase in K-SN and K-Na particles during the lockdown, and that increased number of fugitive combustion points (i.e., household fuel, biomass combustion) was a contributing factor. Therefore, the results imply that regional synergistic control measures on fugitive combustion emissions are needed to ensure good air quality.

Direct Analysis of Soil Composition for Source Apportionment by Laser Ablation Single-Particle Aerosol Mass Spectrometry.

Soil has always been the most complex biomaterial on the planet. The rapid determination of the components in the soil and their original source is a prerequisite for soil quality, environmental, and human health risk assessments. In this study, the chemical compositions and source apportionment of surface soil samples collected from five sites in Shanghai, China, were successfully investigated using a laboratory-developed laser ablation single-particle aerosol mass spectrometry (LA-SPAMS) instrument combined with an adaptive resonance theory-based neural network algorithm (ART-2a) data-processing method for the first time. In total, more than 35,000 particles, ranging from 200 to 2000 nm, were sized, and around 15-20% of the particles were chemically analyzed by LA-SPAMS to generate both positive and negative mass spectra. The results show that there are significant differences in particle size distribution among the five samples, with peaks of various sizes and different profiles, while all five soil samples contain crustal elements, heavy metals, organic and inorganic components, and so forth. The chemical composition of each sample varied considerably, so different classes of SPAMS particle classes were identified, which were later grouped into seven general categories: EC-rich (containing elemental carbon), secondary components, organic nitrogen, crust, HM (containing heavy metal), PAH (containing polycyclic aromatic hydrocarbons), and NaK-rich particles, based on the dominant marked ions. The composition analysis and source apportionment showed that soil components in different areas have been affected by the local environment, such as local industrial emissions and automobile exhaust, which are usually characterized by varying degrees of mixing between the crust and environmental aerosols. In combination with the ART-2a method, LA-SPAMS enables rapid and direct analysis of soil samples based on real-time single-particle measurements, which will help in understanding the distribution, transport, and fate of the soil components, thus providing new insights into soil-quality assessment. Moreover, the established LA-SPAMS can also be practically applied to other daily inspection tasks, such as rocks, minerals, metals, ceramics, polymers, and other solid materials for ingredient analysis and quality evaluation.

"Mobile Health" for the Management of Spondyloarthritis and Its Application in China.

PURPOSE OF THE REVIEW: Spondyloarthritis (SpA) is a group of inflammatory diseases characterized by inflammation in the spine, peripheral joints, and entheses that usually start at the prime of one's life and lead to impaired physical function and reduced quality of life. Ankylosing spondylitis (AS) is prototype of SpA. This article reviews the opportunities and challenges of using mobile health (mHealth) in managing SpA, and report some of our experiences using a mHealth solution for management of SpA patients and performing related research in China. RECENT FINDINGS: The recent rapid development of mobile communications and the common use of intelligent electronic devices have led to the increasing application of mHealth for chronic disease management by healthcare providers and patients alike. This is a promising new technology that can help mitigate limitations in time and space for patient management, promote easier communication between patients and their healthcare providers, reduce medical expenses, and optimize medical services. We have developed a smartphone-based mHealth SpA management system (SpAMS) that also helps the patients to monitor, manage, and share information on their disease with their physician at regular intervals. There is a shift from a paternalistic model of healthcare to more personalized healthcare in which disease management is conducted by the patient together with their healthcare providers. The increasing utility of mHealth is expected to benefit disease management, promote patient-doctor communication, reduce medical expenses, and optimize medical services.

Effect of air masses motion on the rapid change of aerosols in marine atmosphere.

The impact of air masses motion on marine aerosol properties was investigated using an on-board single particle mass spectrometer (SPAMS) deployed for the determination of single particle size resolved chemical composition over Southeast China Sea. Two aerosol blooms (E1 and E2) were observed during the cruise. High average particle number count occurred in E1 (7320), followed by E2 (5850), which was more than 100-150 times of the average particle number count during normal periods. Particles were classified as four major sources, including continental source, shipping source, marine source, and transport source based on the mass spectral similarity. Transport source was identified as those particles with high particle number count occurred only during aerosol bloom period. Three sub-types of EC-Ca, OC-Ca, and Al-rich were classified as transport source. EC-Ca was the dominant particles of the transport source, accounting for more than 70% of the total particles in aerosol bloom events. A uni-modal size distribution in the size range of 0.1-2.0 µm was observed during normal period, while a bimodal distribution with a tiny mode (<0.3 µm) and a coarse mode between 0.4 and 0.6 µm was present during aerosol bloom. The variation of aerosol source is consistent with air masses back trajectories, for the reason that most of the long-range air trajectories are from the ocean, while short air trajectories originate in the continental regions, which means that air masses have a significant impact on the aerosol physical-chemical properties along their tracks.

Aicardi syndrome, an unsolved mystery: Review of diagnostic features, previous attempts, and future opportunities for genetic examination.

Aicardi syndrome is a rare, severe neurodevelopmental disorder classically characterized by the triad of infantile spasms, central chorioretinal lacunae, and agenesis of the corpus callosum. Aicardi syndrome only affects females, with the exception of a few males with a 47, XXY chromosome constitution. All cases are de novo and the only cases of definitive recurrence in families are in identical twins. It is now recognized that individuals with Aicardi syndrome commonly exhibit a variety of other neuronal migration defects, eye anomalies, and other somatic features, including skin, skeletal, and craniofacial systems. The etiology of Aicardi syndrome remains unknown despite an international effort exploring different genetic mechanisms. Although various technologies examining candidate genes, copy number variation, skewing of X-chromosome inactivation, and whole-exome sequences have been explored, no strong genetic candidates have been identified to date. New technologies that can detect low-level mosaicism and balanced rearrangements, as well as platforms examining changes at the DNA and chromatin level affecting regulatory regions are all potential avenues for future studies that may one day solve the mystery of the etiology of Aicardi syndrome.

Asphyxia due to laryngeal spasm as a severe complication of awake deep brain stimulation for Parkinson's disease: a case report.

BACKGROUND: In accordance with German neurosurgical and neurological consensus recommendations, lead placements for deep brain stimulation (DBS) in patients with Parkinson's disease (PD) are usually performed with the patient awake and in "medication off" state. This allows for optimal lead position adjustment according to the clinical response to intraoperative test stimulation. However, exacerbation of Parkinsonian symptoms after withdrawal of dopaminergic medication may endanger the patient by inducing severe "off" state motor phenomena. In particular, this can be a problem in awake craniotomies utilizing intraoperative airway management and resuscitation. CASE PRESENTATION: We report the case of a PD patient with progressive orofacial and neck muscle dystonia resulting in laryngeal spasm during DBS lead placement. This led to upper airway compromise and asphyxia, requiring resuscitation. CONCLUSIONS: Laryngeal spasms may occur as a rare "off" state motor complication in patients with PD. Other potential causes of intraoperative difficulties breathing include bilateral vocal cord palsy, positional asphyxia, and silent aspiration. In our practice, we have adjusted our medication regimen and now allow patients to receive their standard dopaminergic medication until the morning of surgery. Neurologists and neurosurgeons performing lead placement procedures for PD should be aware of this rare but unsafe condition to most optimized treatment.

Sources and characteristics of fine particles over the Yellow Sea and Bohai Sea using online single particle aerosol mass spectrometer.

Marine aerosols over the East China Seas are heavily polluted by continental sources. During the Chinese Comprehensive Ocean Experiment in November 2012, size and mass spectra of individual atmospheric particles in the size range from 0.2 to 2.0 µm were measured on board by a single particle aerosol mass spectrometer (SPAMS). The average hourly particle number (PN) was around 4560±3240 in the South Yellow Sea (SYS), 2900±3970 in the North Yellow Sea (NYS), and 1700±2220 in the Bohai Sea (BS). PN in NYS and BS varied greatly over 3 orders of magnitude, while that in SYS varied slightly. The size distributions were fitted with two log-normal modes. Accumulation mode dominated in NYS and BS, especially during episodic periods. Coarse mode particles played an important role in SYS. Particles were classified using an adaptive resonance theory based neural network algorithm (ART-2a). Six particle types were identified with secondary-containing, aged sea-salt, soot-like, biomass burning, fresh sea-salt, and lead-containing particles accounting for 32%, 21%, 18%, 16%, 4%, and 3% of total PN, respectively. Aerosols in BS were relatively enriched in particles from anthropogenic sources compared to SYS, probably due to emissions from more developed upwind regions and indicating stronger influence of continental outflow on marine environment. Variation of source types depended mainly on origins of transported air masses. This study examined rapid changes in PN, size distribution and source types of fine particles in marine atmospheres. It also demonstrated the effectiveness of high-time-resolution source apportionment by ART-2a.

Single particle mass spectral signatures from on-road and non-road vehicle exhaust particles and their application in refined source apportionment using deep learning.

With advances in vehicle emission control technology, updating source profiles to meet the current requirements of source apportionment has become increasingly crucial. In this study, on-road and non-road vehicle particles were collected, and then the chemical compositions of individual particles were analyzed using single particle aerosol mass spectrometry. The data were grouped using an adaptive resonance theory neural network to identify signatures and establish a mass spectral database of mobile sources. In addition, a deep learning-based model (DeepAerosolClassifier) for classifying aerosol particles was established. The objective of this model was to accomplish source apportionment. During the training process, the model achieved an accuracy of 98.49 % for the validation set and an accuracy of 93.36 % for the testing set. Regarding the model interpretation, ideal spectra were generated using the model, verifying its accurate recognition of the characteristic patterns in the mass spectra. In a practical application, the model performed hourly source apportionment at three specific field monitoring sites. The effectiveness of the model in field measurement was validated by combining traffic flow and spatial information with the model results. Compared with other machine learning methods, our model achieved highly automated source apportionment while eliminating the need for feature selection, and it enables end-to-end operation. Thus, in the future, it can be applied in refined and online source apportionment of particulate matter.

Impacts of the aerosol mixing state and new particle formation on CCN in summer at the summit of Mount Tai (1534m) in Central East China.

In this study, the aerosol size distributions, cloud condensation nuclei (CCN) number concentration (NCCN), single-particle chemical composition and meteorological data were collected from May 12 to June 8, 2017, at the summit of Mt. Tai. The effects of new particle formation (NPF) events and aerosol chemical components on CCN at Mt. Tai were analyzed in detail. The results showed that, NPF events significantly enhanced the CCN population, and the enhancement effect increased with increasing supersaturation (SS) value at Mt.Tai. NCCN at SS ranging from 0.1 to 0.9 % on NPF days was 10.9 %, 36.5 %, 44.6 %, 53.5 % and 51.5 % higher than that on non-NPF days from 10:00-13:00 as NPF events progressed. The effect of chemical components on CCN activation under the influence of NPF events was greater than that in the absence of NPF events. The correlation coefficients of EC-Nitrate particles (EC-Sulfate particles) and CCN at all SS levels on NPF days were 1.31-1.59 times (1.17-1.35 times) higher than those on non-NPF days. Nitrate particles promoted CCN activation but sulfate particles inhibited activation at Mt. Tai. There are differences or even opposite effects of the same group of particles on CCN activation under the influence of NPF events in different air masses. EC-Sulfate particles inhibited CCN activation at all SS levels for type I but weakly promoted activation at lower SS ranging from 0.1 to 0.3 % and weakly inhibited it at higher 0.9 % SS for type II. OCEC particles significantly inhibited CCN activation for type II, and this effect decreased with increasing SS. OCEC particles only weakly inhibited activation at SS ranging from 0.5 to 0.7 % for type I. OCEC particles only weakly inhibited this process at 0.1 % SS, while they very weakly promoted activation for SS > 0.1 %. This reveals that the CCN activity is not only related to the chemical composition of the particles, but the mixing state also has an important effect on the CCN activity.

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.

CDKL5-associated developmental and epileptic encephalopathy: A long-term, longitudinal electroclinical study of 22 cases.

OBJECTIVE: The study was conducted to analyze the possible diagnostic value of the electroclinical semiology of the epileptic seizures. METHODS: We evaluated the medical records of 17 females and 5 males with CDKL5 deficiency disorder (CDD) considering the long-term evolution, including the polygraphic video-EEG recordings. RESULTS: We recognized three disease phases. We found that the seizure semiology was already recognizable in the first phase of the syndrome. In the short-term evolution, all patients had focal motor and 12/21 hypermotor seizures. Both epileptic spasms and myoclonic seizures were already present in more than half of the cases in the first 2 months after onset. In the second phase, the intermediate period, the polymorphic pattern was maintained, but in eight patients the electroclinical pattern of epileptic encephalopathy with hypsarrhythmia appeared. In the long-term period, the seizure polymorphism continued but myoclonic and epileptic spasms diminished. Tonic seizures appeared in the last 2 phases. Progressively, with the aggravation of seizures and paroxysmal EEG abnormalities impairment of the neurocognitive status was observed. Severe behavioral disturbances were seen in eight and autistic-like features in 14. CONCLUSION: CDD is a true developmental and epileptic encephalopathy with a specific etiology characterized by the early appearance of epileptic seizures that quickly become polymorphic and drug resistant in infants that are most often female and already have neurological impairment. Polygraphic video-EEG recordings are important to recognize ictal events of the association of hypermotor seizures, epileptic spasms in clusters, and massive myoclonic jerks, already present at onset.

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.

Influence of regional emission controls on the chemical composition, sources, and size distributions of submicron aerosols: Insights from the 2014 Nanjing Youth Olympic Games.

High-intensity emission controls were implemented in Nanjing and in 8 surrounding cities to ensure good air quality during the 2014 summer Youth Olympic Games (YOG). An Aerodyne soot-particle aerosol mass spectrometer (SP-AMS) was deployed at a downwind site of downtown Nanjing to investigate the chemical composition, sources, and size distribution of submicron aerosols (PM1), in response to emission control policies. However, results show that emission controls played a negligible role in reducing PM1 concentration during the YOG period, yet primary precursors such as NOx and SO2 were decreased by 10-20%. Low wind speed, high relative humidity, and high ozone (O3) concentration likely play a significant role in the production and accumulation of the oxygenated organic aerosol (OOA) and the secondary inorganic aerosols (SIA) in summer Nanjing. We propose that long-term regional emission reduction could be a solution for future air pollution mitigation strategies in downwind cities of the YRD region, and that seasonal meteorological characteristics in a specific region should be considered before emission control policies are made.

Large contribution from worship activities to the atmospheric soot particles in northwest China.

Worship activities like burning joss paper during the Chinese Hanyi festival is a common, traditional custom in northwest China. However, the pollutants of e.g., soot particles, released from joss paper burning and the corresponding impacts on urban air quality were poorly investigated, which can be a particular concern since these activities are conducted in an uncontrolled manner. In this study, a long time-of-flight (LToF) soot particle aerosol mass spectrometry (SP-AMS) was deployed to characterize the refractory black carbon (rBC) emitted from the joss paper burning, as well as crop residue, coal combustion, and traffic during the Hanyi Festival in mid-November 2020 in the northwestern city of Xi'an in China. Large difference (from <5% to >100%) in the fragmentation patterns (Cn+) for the measured rBC from different source emissions were found when compared to the reference Regal Black. Using the receptor model of positive matrix factorization (PMF) with the multilinear engine (ME-2) algorithm, the obtained rBC mass spectra were used as the anchoring profiles to evaluate the emission strengths of different source types to the atmospheric rBC. Our results show that the burning of joss paper accounted for up to 42% of the atmospheric rBC mass, higher than traffic (14-17%), crop residue (10-17%), coal (18-20%) during the Hanyi festival in northwest China. Moreover, we show that the overall air quality can be worsened due to the practice of uncontrolled burning of joss paper during the festival, which is not just confined to the people who do the burning. Although worship activities occur mainly during festival periods, the pollution events contributed by joss paper burning may pose an acute exposure risk for public health. This is particularly important since burning joss paper during worship activities is common in China and most Asian countries with similar traditions.

Characterization of the spatial and temporal distribution of lead around a battery industrial park by LA-SPAMS.

A convenient technique for direct solids analysis, laser ablation single particle aerosol mass spectrometry (LA-SPAMS), was used to investigate lead and other components in soil and bark samples from around a battery industrial park. In total, over 50,000 particles ranging in size from 0.2 to 2 µm were sampled and approximately 15-35% of the particles were analyzed for chemical composition. The mean mass spectrum results showed that the intensity of lead varied widely among sampling points, reaching the highest intensity in the topsoil and bark at sampling point 4, located closest to the core factory. Based on the neural network algorithm of adaptive resonance theory (ART-2a), the topsoil and bark samples were classified into five categories: crustal composition (Ca+, silicates, aluminates, etc.), elemental carbon (C2-, C3-, C4-, etc.), organic carbon (CN-, levoglucosan, etc.), secondary inorganic sources (phosphates, nitrates, sulfates), and heavy metals (Pb+, Zn+, Cu+), with the proportion of Pb varying from 0.020 to 0.25% and 0.030-9.41% in topsoil and bark samples, respectively, while the proportion of Cu and Zn in topsoil and bark samples did not differ as greatly as Pb. In addition, the particle number concentrations of lead particles in topsoil and bark ranged from 0.14 to 3.48% and 0.36-37.93%, respectively. The concentrations of Pb in topsoil and bark samples measured by ICP-OES varied from 71 to 791 ppm and 172-2595 ppm, respectively. Overall, both the lead content in topsoil samples measured by LA-SPAMS and ICP-OES reached maximum values at sampling points 4 and 5, respectively, indicating moderate pollution with Pb at these two sites. This convenient LA-SPAMS method not only accurately detects the composition of solid samples, the mixing state of particulate matter, and the analytical component sources, but also omits tedious pretreatment steps, reduces the use of organic solvents, and shortens the detection time of solid samples, thereby providing an attractive method for soil environmental quality monitoring.

Deposition of ambient particles in the human respiratory system based on single particle analysis: A case study in the Pearl River Delta, China.

It is important to evaluate how ambient particles are deposited in the human respiratory system in view of the adverse effects they pose to human health. Traditional methods of investigating human exposure to ambient particles suffer from drawbacks related either to the lack of chemical information from particle number-based measurements or to the poor time resolution of mass-based measurements. To address these issues, in this study, human exposure to ambient particulate matter was investigated using single particle analysis, which provided chemical information with a high time resolution. Based on single particle measurements conducted in the Pearl River Delta, China, nine particle types were identified, and EC (elemental carbon) particles were determined to be the most dominant type of particle. In general, the submicron size mode was dominant in terms of the number concentration for all of the particle types, except for Na-rich and dust particles. On average, around 34% of particles were deposited in the human respiratory system with 13.9%, 7.9%, and 12.6% being distributed in the head, tracheobronchial, and pulmonary regions, respectively. The amount of Na-rich particles deposited was the highest, followed by EC. The overall deposition efficiencies of the Na-rich and dust particles were higher than those of the other particle types due to their higher efficiencies in the head region, which could be caused by the greater sedimentation and impaction rates of larger particles. In the head region, the Na-rich particles made the largest contribution (30.5%) due to their high deposition efficiency, whereas in the tracheobronchial and pulmonary regions, EC made the largest contribution due to its high concentration. In summary, the findings of this initial trial demonstrate the applicability of single particle analysis to the assessment of human exposure to ambient particles and its potential to support traditional methods of analysis.

The characteristics and mixing states of PM2.5 during a winter dust storm in Ningbo of the Yangtze River Delta, China.

Dust particulates play an essential role for the nucleation, hygroscopicity and also contribute to aerosol mass. We investigated the chemical composition, size distribution and mixing states of PM2.5 using a single-particle aerosol mass spectrometer (SPAMS), Monitor for AeRosols and Gases (MARGA), and off-line membrane sampling from 2018.1.24 to 2018.2.20 at a coastal supersite in Ningbo, a port city in Yangtze River Delta, China. During the study campaign, the eastern part of China had experienced a wide range of cooling, sandstorm, and snowfall processes. The entire sampling campaign was categorized into five sub-periods based on the levels of PM2.5 and the ratios of PM2.5/PM10, namely clean (T1), heavy pollution (T2), light pollution (T3), dust (sandstorm) (T4) and cleaning pollution (T5) period. After comparing the average mass spectrum for each period, it shows that the primary ions, such as Ca2+and SiO3-, rarely coexist with each other within a single particle, but secondary ions generally coexist with these primary ions. Furthermore, the coexistence of each two different ions within a particle does not show distinct variation for the whole study periods. All these suggest that the absorption and partitioning of gaseous contaminants into the surface of primary aerosol through heterogeneous reactions are the major pathways of aging and growth of aerosol; and the merging of particles through collisions usually is insignificant. Although the absolute concentrations of nitrate and sulfate all increased with the PM2.5 concentrations, the relative equivalent concentrations of NO3- and SO42- displayed opposite trends; the relative contribution of sulfate decreased and that of nitrate increased as the increase of pollution. During the dust period, the relative equivalent concentrations of calcium and/or potassium ions in PM2.5 are significantly higher. This study provided deep insights about the mixing states and characteristics of particulate after long-range transport and a visualization tool for aerosol study.

[Secondary Organic Aerosol Mass Yield and Characteristics from 4-ethylguaiacol Aqueous·OH Oxidation: Effects of Initial Concentration].

Aqueous-phase chemical processing, as an essential formation pathway of secondary organic aerosol (SOA), has attracted widespread attention from within atmospheric chemistry fields. Due to the complicated reaction nature, reaction mechanisms, and product characteristics of aqueous-phase chemical processing, its contribution to the SOA budget is still not fully understood. In this work, we investigate how the initial concentration (0.03-3 mmol·L-1) of 4-ethylguaiacol affects SOA formation of aqueous·OH photochemical oxidation. We use soot-particle aerosol mass spectrometry (SP-AMS) to monitor SOA mass yield and oxidation character, and gas chromatography-mass spectrometry (GC-MS) and ion chromatography (IC) to measure products and organic acids. Additionally, we use ultraviolet visible spectroscopy (UV-vis) and high-performance liquid spectrometry (HPLS) to track the formation of light-absorbing products such as humic-like substances (HULIS). Our research indicated that the range of the O/C ratio of EG-aqSOA measured by the SP-AMS exhibited increasing trends with increased reaction time 0.42-0.61 (0.03 mmol·L-1), 0.49-0.84 (0.3 mmol·L-1), and 0.49-0.63 (3 mmol·L-1). Dimers (C16H18 O2+, m/z 302) via SP-AMS were obviously higher under a higher initial concentration, thereby demonstrating that the oligomerization reaction proceeded more easily. The absorption at 250 nm recorded by UV-vis was distinctly enhanced, which might be attributed to new light-absorbing products with absorbance at 250 nm. Furthermore, the HULIS concentration increased with reaction time, in accordance with enhancement of absorbance in the 300-400 nm region, thus suggesting that aqueous-phase processing formed brown carbon. Small organic acids, including formic acid, malic acid, and oxalic acid, were detected by IC in all reaction solutions, with the highest concentration being for formic acid. GC/MS detected ketone, an OH monomer, and dimers in the aqSOA, which further indicates that functionalization and oligomerization took place.