Search Results (564)

Aerosol scattering strongly influences the Earth’s atmosphere energy balance and actinic flux, yet its efficiency remains uncertain due to limited understanding of chemical effects. Scattering efficiency primarily depends on aerosol size, scattering refractive index, and hygroscopicity, which are determined by emissions and chemical processes; however, their covariation characteristics are rarely explored. Here, we use long-term measurements of submicron aerosol size distributions, chemical composition, scattering properties, and hygroscopicity in Guangzhou to investigate their covariations and links to secondary aerosol formation. The results indicate that dry-state volume scattering efficiency (VSE) was mainly driven by variations in aerosol size (R² = 0.74), despite substantial refractive index variability (1.4–1.6), which showed overall independent variations with size. Source apportionment and case analyses suggest distinct size ranges for secondary organic (SOA) and inorganic aerosols (SIA). Accordingly, a new lognormal fitting methodology is proposed to retrieve particle volume size distribution (PVSD)-associated aerosol components by combining PVSD and composition data. Retrieved geometric mean diameters of SOA (Dg,_SOA, 175–400 nm; 246 ± 44 nm) and SIA (Dg,_SIA, 200–600 nm; 382 ± 68 nm) are significantly correlated (R² = 0.43), indicating coupled formation of SOA and SIA and their interdependent roles in aerosol scattering. In addition, pronounced joint increases in dry-state VSE and aerosol hygroscopicity driven by the co-enhancement of aerosol size and hygroscopicity are further revealed. These results demonstrate the interconnected roles of secondary aerosol formation in controlling scattering efficiency and underscore the need to better represent SOA–SIA interactions in simulating aerosol radiative effects and address the covariations of aerosol hygroscopicity and dry-state scattering efficiency in aerosol remote sensing. Full article

Atmospheric sea spray aerosol (SSA) undergoes chemical aging during long-distance transport, leading to significant alterations in its climate effects. However, the aging mechanisms of SSA driven by oxygenated volatile organic compounds (OVOCs) remain unclear. Hence, the aging processes of NaCl particles driven by glyoxal (GL), a representative OVOC, are systematically investigated using molecular dynamics (MD) simulations and density functional theory (DFT) calculations. MD simulations with high GL coverage show that GL readily mixes with NaCl and preferentially orients its carbonyl groups toward the NaCl surface. The adsorption of GL on the NaCl surface is dominated by the interaction between the O atom of GL (O_GL) and the Na atom of the surface. DFT calculations with single GL coverage further reveal the formation of the O_GL–Na bond between GL and NaCl. The mixing process of GL and NaCl is regulated by both the number of aldehyde groups engaging in the interfacial coordination and the corresponding lengths of O_GL–Na bonds. The subsequent heterogeneous oxidation of GL by an OH radical proceeds mainly via a barrierless H-abstraction pathway to form HC(O)CO radicals, which may further react with methylamine/ammonia and contribute to brown carbon formation. Our results reveal the importance of incorporating such aging mechanisms into atmospheric models to improve climate predictions. Full article

This study presents a novel, satellite-based framework for quantifying the relative contribution of regional transport in biomass burning aerosol (BBA) formation over the South China Sea (SCS). We integrate the biomass burning emission (BBE) rates from potential source regions with a random forest regression model, which is driven by backward trajectory analysis. This approach isolates and evaluates the relative contribution from transported sources. The model demonstrates robust predictive skill for BBA concentrations (R² = 0.78 on an independent test set), using only transport-weighted BBE rates and meteorological data as inputs. Quantitative interpretation via SHAP (Shapley Additive exPlanations) analysis reveals nonlinear relationships and the distinct importance of transport-source features. A key finding is that BBE originating from northern Laos and Thailand contributes 21.23% to the predicted BBA concentrations over the SCS. Furthermore, there is a clear nonlinear positive correlation between the regional BBE rates and downwind BBA concentration, except for transport from Cambodia. Our results pinpoint that the impact of regional transport is paramount, governed by a combination of source emission intensity, transport duration, and trajectory pathway. This study establishes a satellite-driven methodology for attributing aerosol sources and clarifies the dominant controls on BBA concentration variability in a major maritime receptor region. Full article

Coordinated control of fine particulate matter (PM_2.5) and ozone (O₃) is an urgent national strategic priority for China’s air pollution governance. Biogenic volatile organic compounds (BVOCs) are important precursors of O₃ and secondary organic aerosol (SOA). To quantify the species-specific impacts of BVOCs, we used the Model of Emissions of Gases and Aerosols from Nature (MEGAN, v3.2) and the Community Multiscale Air Quality (CMAQ, v5.3.2) model to investigate BVOC emission characteristics and their modulating effects on summertime O₃ and PM_2.5 across China. In July 2020, total BVOC emissions were 6.50 × 10⁶ tons, showing a spatial pattern that decreased from southeast to northwest and a unimodal diurnal variation that peaked at 13:00–14:00. BVOC emissions significantly promoted O₃ formation, with a maximum concentration increment of 47.36 μg m⁻³ in VOC-limited regions such as the Sichuan Basin (SCB) and Yangtze River Delta (YRD). Their impact on PM_2.5 was limited, with most regional increments below 3 μg m⁻³. Isoprene dominated O₃ enhancement, while monoterpenes acted as the key BVOC for PM_2.5 via SOA formation. Anthropogenic emission reductions elevated the relative contribution of BVOC emissions to air pollution in most regions. These findings highlighted the importance of considering BVOC emissions and their species-specific effects in China’s coordinated PM_2.5-O₃ control strategies for more precise air quality management. Full article

Background/Objectives: The development of dry powder formulations for pulmonary delivery of therapeutic antibodies requires careful stabilization strategies to preserve protein integrity during spray-drying and long-term storage. This study investigates the impact of various sugar-derivatives, a polyol (D-mannitol), a disaccharide (D-sucrose) and a polysaccharide (dextran 10 kDa), used individually or in combination, on the physical stability of bovine polyclonal immunoglobulin G (pAb) in dry powders for inhalation (DPIs). Methods: A design of experiments (DoE) approach was employed to evaluate the effects of these excipients on residual moisture (RM), low-order aggregates (LOA) and high-order aggregates (HOA), immediately after spray-drying (T0) and after 10 months of storage at room temperature in a desiccator (T10). Results: All DPIs exhibited a high amorphous content and a favorable glass transition temperature, with RM decreasing over time. The combination of D-mannitol and dextran 10 kDA (DPI-MD) demonstrated the most effective stabilization, minimizing LOA and HOA formation at T0 and T10. Although the ternary mixture, including D-sucrose (DPI-MSD) exhibited higher process stability, it was less stable over time in comparison to the binary mixture. The aerodynamic performance of these carrier-free DPIs, assessed via laser diffraction (% ˂ 5 µm), were between 51 ± 3 (DPI-MD) and 67 ± 4 (DPI MSD) and a Next Generation Impactor, confirmed that formulation produced aerosol with suitable size distribution and fine particle fractions (FPFn upt to 71 ± 5% for DPI-MSD), for deep pulmonary deposition. Conclusions: These findings highlight the importance of combining excipients with complementary physical properties to achieve robust protein stabilization. The DPI-MD emerged as the most promising candidate for pAb lung delivery, balancing protein integrity, powder stability, and aerodynamic efficiency. Full article

Surface solar radiation at the ground is affected by aerosols, clouds, and atmospheric moisture, as well as by circulation-related conditions that influence cloud formation and pollutant transport. In daily observations, these influences are mixed, which makes pollution-related variability difficult to interpret. We analyzed data from Beijing station 54511 (2015–2019), including daily integrated radiation components and collocated meteorological and pollution variables. We used wavelet coherence, pollution-stratified association analysis, and gray relational analysis, and compared two meteorological normalization methods: multiple linear regression (MLR) and random forest (RF). The results show that meteorological–radiation relationships vary systematically across pollution levels, indicating substantial meteorological confounding in daily radiation analyses. Among the radiation components, DR shows the clearest pollution-dependent shift in its relationship with RH, while several direct components become less sensitive to cloud cover under heavier pollution. RF reproduced daily radiation components with strong predictive performance (R² = 0.83–0.88), and the meteorologically adjusted anomalies from RF were consistent with those from MLR (r = 0.63–0.78 across components). These findings suggest that both MLR and RF can be effectively used to normalize meteorological effects in daily station records. The analysis supports routine interpretation of day-to-day surface radiation variability and can be extended to multi-site studies and finer temporal resolution. Full article

The formation and size evolution of gas-phase nanoparticles (NPs) in laser ablation inductively coupled plasma mass spectrometry critically influence aerosol transport, plasma ionization efficiency, and ultimately analytical accuracy. Nevertheless, burst-mode laser ablation, as an efficient and versatile strategy for controlling gas-phase NP size, remains insufficiently explored. Here, we combine experimental investigations and theoretical analysis to elucidate the mechanisms of gas-phase nanoparticle formation and size control by tuning the interpulse interval in burst-mode femtosecond (fs) laser ablation. The mean nanoparticle size exhibits a non-monotonic dependence on interpulse spacing, decreasing with a narrowing size distribution as the interval increases from 0 to 300 ps, and then increasing with distribution broadening at longer delays up to 1000 ps, closely correlating with ablation-crater depth. A characteristic transition at ~300 ps is identified, where both nanoparticle size and crater depth reach a minimum, revealing a critical timescale in pulse–plume–surface interactions. Simulations show that the interpulse interval governs the redistribution of laser energy between the surface and plume, driving a transition from surface-dominated ablation to plume-dominated absorption and partial recovery of surface coupling. This delay-dependent framework provides a unified explanation for nanoparticle formation, where particle size is determined by the competition between plume-mediated fragmentation and surface-driven material supply, and offers a basis for tailoring NP size distributions via temporal pulse shaping. Full article

Non-exhaust particulate emissions are expected to remain a relevant source of traffic-related air pollution, including an increase in electrified vehicle fleets. Particle formation results from tribological interactions and is influenced by both operating conditions and friction material system. This study presents an extended measurement methodology under application-relevant tribological conditions for the reproducible quantification of PM₁₀ and PM_2.5 emissions from dry-running friction systems and applies it to a systematic investigation of operating parameter and friction pairing effects. A dry inertial brake test bench with an enclosed friction chamber and integrated aerosol measurement chain was used under controlled tribologically relevant conditions. Specific friction work and specific friction power were varied by adjusting sliding velocity, contact pressure, and inertial load. Six friction pairings, comprising four representative friction lining types combined with either C45 cast steel or GGG40 gray cast iron, were examined. In situ PM₁₀ and PM_2.5 measurements were complemented by gravimetric wear and microstructural analyses. The results show that specific friction work has a direct influence on PM₁₀ and PM_2.5 emissions, whereas the independent effect of contact pressure is secondary. Friction power exhibits material-dependent effects. Emissions also vary strongly with friction pairing, indicating that operating conditions and material system must be considered jointly when assessing low-emission brake systems. Full article

Air pollution remains a major global environmental risk, and exposure to fine particulate matter (PM_2.5) is associated with adverse health outcomes even at low concentrations. Meteorological conditions influence PM_2.5 variability, and precipitation is often expected to reduce particle loads through wet removal. However, humid and wet conditions may coincide with elevated PM_2.5 under specific atmospheric and compositional conditions. Here, we investigate long-term relationships between precipitation regimes and PM_2.5 concentrations in the Metropolitan Region of Belém (Eastern Amazonia) over the period 1980–2024. We combined PM_2.5 from the MERRA-2 reanalysis (including a bias-corrected product) with in situ precipitation records, and classified precipitation conditions using the Standardized Precipitation Index (SPI). We find statistically significant positive long-term tendencies in both precipitation and PM_2.5. Stratified analyses show that PM_2.5 concentrations are significantly higher under wet conditions, with a weak but significant positive relationship between SPI and PM_2.5 (r = 0.23 for the full period; r = 0.24 for the wet class, p-value < 0.01). These findings indicate that increased precipitation in a strong humid tropical urban environment does not necessarily lead to improved air quality. Instead, wet conditions may favor processes such as hygroscopic growth and secondary aerosol formation, contributing to higher PM_2.5 concentrations on a monthly scale. Overall, this study highlights the importance of considering precipitation regimes and associated atmospheric processes when assessing air quality in tropical urban environments. Full article

We report the synthesis of Fe/N/C ORR electrocatalysts by an original collinear CO₂ laser pyrolysis of liquid aerosol droplets in various configurations and compared them to a catalyst synthesized in the classical perpendicular one. While the precursors were always injected at the bottom side of the reactor, two collinear configurations of the laser entry into the reactor are considered: by the Top Side (T.S.) or by the Bottom Side (B.S.). The two corresponding catalysts sets show significant different ORR performances. An in-depth XPS analysis and fitting of the N1s spectra allowed for drawing the ORR performance as a function of FeN_x sites components. An original approach considering the energy delivered to a quantity of precursors in J.g⁻¹, linked to the flame temperature feature, evidenced very different conditions for perpendicular CO₂ laser pyrolysis and each of the two collinear configurations. This mass-weighted energy delivered in the classical perpendicular configuration is too low to allow for the formation of FeN_x sites and the resulting ORR performance is extremely poor, suggesting a marginal role of nitrogen species without interaction with iron atoms. In contrast, the delivered mass-weighted energies are sufficient in both collinear configurations to produce FeN_x sites. The ORR performance for catalysts produced in these both configurations is positively correlated with the amount of energy deposited on the precursors. The ORR performance in the T.S. laser configuration is positively correlated to the amount of FeN_x sites. The best performing catalysts obtained in the B.S. configuration show an opposite variation. These trends, and the ORR performance degradation of B.S. catalysts under prolonged chronoamperometry are discussed in light of the effect of temperature on the formation of the various kind of FeN_x sites. A tentative explanation is given, considering that N1s XPS fitting with a single FeN_x component may hinder the fact that Pyridinic sites components may contain a part of FeN_x sites, as suggested by theoretical calculation from the literature. The best catalysts obtained in this work by collinear configuration show similar performances to those obtained by double stage perpendicular pyrolysis previously reported with an ORR onset potential of ~860 mV. Full article

Ammonia (NH₃) emissions from concentrated animal feeding operations (CAFOs) are recognized contributors to secondary fine particulate matter (PM_2.5) formation, yet empirically derived secondary PM_2.5 emission factors applicable to livestock operations remain limited. This study investigated NH₃-derived secondary PM_2.5 formation under controlled laboratory conditions using a PTFE flow reactor in which NH₃ was reacted with sulfur dioxide (SO₂) across ammonia-rich NH₃:SO₂ ratios, with and without zero air. The resulting aerosols were characterized using gravimetric analysis, elemental analysis, Fourier-transform infrared spectroscopy (FTIR), scanning electron microscopy with energy-dispersive X-ray spectroscopy (SEM/EDS), and particle size distribution (PSD) measurements. The recovered particles were dominated by inorganic ammonium–sulfur species, with FTIR and elemental trends indicating sulfite-related intermediates under no-zero-air conditions and more oxidized ammonium–sulfur products under oxygenated conditions. Accounting for both filter-collected and wall-deposited particles, unit particulate emission factors normalized to ammonia input were derived. Size-based apportionment using PSD data indicated that approximately 76.6% of the recovered particulate mass was within the PM_2.5 size range. Scaling the experimentally derived unit emission factors using literature-based ammonia emission rates yielded an estimated secondary PM_2.5 emission factor of 0.351 ± 0.084 g PM_2.5 per animal head per day for cattle feedlots, corresponding to approximately 3–4% of reported total PM_2.5 emissions. Because the experimental system isolates NH₃–SO₂ interactions under idealized conditions and does not represent full atmospheric chemistry, the derived values should be interpreted as screening-level estimates of NH₃-derived secondary PM_2.5 formation potential intended to support comparative air quality assessments of CAFOs rather than direct predictions of ambient PM_2.5 concentrations. Full article

Volatile organic compounds (VOCs) are key precursors of ozone (O₃) and secondary organic aerosols (SOA), among which biogenic VOCs (BVOCs) constitute the dominant natural source. However, large uncertainties remain in the magnitude, spatial distribution, and seasonal variability of BVOC emissions in China under rapidly changing vegetation and climate conditions. In this study, a refined BVOC emission inventory for China in 2023 was developed using the Model of Emissions of Gases and Aerosols from Nature (MEGAN v3.2) driven by WRF meteorological simulations and MODIS vegetation data. The estimated annual BVOC emissions reached 41.70 Tg, including 26.90 Tg isoprene, 4.84 Tg monoterpenes, 0.55 Tg sesquiterpenes, and 9.41 Tg other VOCs. The corresponding ozone formation potential (OFP) and secondary organic aerosol formation potential (SOAFP) were 346.12 Tg yr⁻¹ and 2137.51 Gg yr⁻¹, respectively. Emissions exhibited a pronounced south–north gradient with hotspots in Guangxi, Guangdong, and Yunnan, and peaked in summer. Broadleaf forests were identified as the dominant emission sources, followed by savannas and shrublands. Isoprene contributed most to OFP, whereas monoterpenes dominated SOAFP. Compared with previous inventories, the updated vegetation data, meteorological inputs, and refined chemical speciation improve the representation of BVOC emissions and their spatial patterns in China. These results highlight the important role of BVOCs in regional O₃ and SOA formation and provide an improved emission basis for atmospheric chemistry modeling and air-quality management. Full article

The hydrocarbon composition of liquefied PM1 aerosol samples collected using the particle into liquid system (PILS) at the Atmospheric Radiation Measurement (ARM) site of the Southern Great Plains (SGP) of the USA was analyzed in terms of organic compound composition. The results indicate that anthropogenic aliphatic compounds contributed significantly to the organic pool of PM1 fine aerosols in the ambient air of the rural area of the Southern Great Plains, with a broad range of aliphatic hydrocarbons (HCs) being the dominant organic component. The molecular markers of hopanes and steranes were generally absent or present in trace amounts in most samples, but a significant number of low-abundance hopanes and steranes were detected in only two samples, while the aromatic compounds were generally insignificant and comprised mainly low molecular weight naphthalene and its methylated derivatives. The overall composition of organic compounds and the back trajectories analysis for the sampling days suggest that the local petroleum refinery and vehicular emissions are the two major sources of the aliphatic and aromatic compounds in the fine aerosols, while plant wax may occasionally contribute a minor portion of organic matter. Furthermore, it was found that the organic composition of PM1 fine aerosol was clearly related to the ambient air temperature and suggests that the temperature is a controlling factor of organic aerosol formation. Full article

The object of the study is a single heated carbonaceous particle of relatively small size, 0.003 to 0.01 m. Main hypothesis: The formation of soot particles and black carbon particles is caused by the thermochemical destruction of dry organic matter of forest fuel and the mechanical fragmentation of coke residue. The aim of the study is to conduct numerical simulations of heat and mass transfer in a single heated carbonaceous particle, taking into account the soot formation process and assessing its fragmentation with regard to heat exchange with the external environment in a 2D setting. As part of this study, a new model of heat and mass transfer in a pyrolyzed carbonaceous particle was developed, taking into account its step-by-step fragmentation (fragmentation tree model with four secondary particle formations from the initial particle). The calculations resulted in the distributions of temperature and volume fractions of phases in the carbonaceous particle across various scenarios. Scenarios of surface fires (initial temperatures of 900 K and 1000 K), crown fires (1100 K), and a firestorm (1200 K) for typical vegetation (pine, spruce, birch) are considered. Cubic carbonaceous particles are considered in the approximation of a 2D mathematical model. To describe heat and mass transfer in the structure of the carbonaceous particle, a differential equation of thermal conductivity with corresponding initial and boundary conditions of the third type is used, taking into account the gross reaction in the kinetic scheme of pyrolysis and soot formation. Differential analogues of partial differential equations are solved using the finite difference method of second-order approximation. Options for using the developed mathematical model and probabilistic fragmentation criterion for assessing aerosol emissions are proposed. Recommendations: The suggested mathematical model must be incorporated with mathematical models of forest fire plume and aerosol transport in the upper layers of the atmosphere. Moreover, probabilistic criteria for health assessment must be developed for the practical use of the suggested mathematical model. Full article

Naphthalene and methylnaphthalene (Nap and MN) are the most abundant polycyclic aromatic hydrocarbons (PAHs) and are important precursors of secondary organic aerosol (SOA) in the atmosphere. 1.2-Phthalic acid (1,2-PhA) and 4-methylphthalic acid (4-MPhA) are usually treated as tracers of SOA from Nap and MN. However, the two tracers also have primary sources, and directly using the tracers to estimate SOA would lead to an overestimation. In this study, we conducted a one-year synchronous observation of the two-ring PAH SOA (SOA_2-rings) tracers at nine sites in the Pearl River Delta (PRD) region. We measured and filtered the suitable emission characteristics of SOA_2-rings tracers for biomass burning, coal combustion, industrial processes and vehicle exhaust sources. Then, we developed a method to distinguish 1,2-PhA and 4-MPhA from primary emissions and secondary formation. The average proportions of 1,2-PhA_pri and 4-MPhA_pri in 1,2-PhA and 4-MPhA were 26.7% and 29.2%, respectively. The direct application of measured 1,2-PhA for estimating SOA_2-rings would lead to an overestimation exceeding 30% in the PRD. Furthermore, we estimated SOA_2-rings using the separated 1,2-PhA_sec and 4-MPhA_sec by the tracer-based method. The average contribution of MN to SOA was around three times that of Nap. In addition, when combined with monocyclic aromatic SOA (SOA_1-ring) and biogenic SOA, the contributions of SOA_1-ring (21%) and SOA_2-rings (25%) to total SOA were comparable. SOA_2-rings was even the largest contributor to total SOA (~44%) in winter. This study revealed that whether to separate the SOA_2-rings tracers for primary emissions and secondary formation is essential in SOA estimation and highlighted that two-ring PAHs make a significant contribution to SOA in the PRD. Full article