Aerosol Processes Research Articles

Advanced Carbon Sphere-Based Hybrid Materials Produced by Innovative Aerosol Process for High-Efficiency Rechargeable Batteries

Advanced Carbon Sphere-Based Hybrid Materials Produced by Innovative Aerosol Process for High-Efficiency Rechargeable Batteries

Efficient integration of calcium looping with methane Bi-reforming using Pd-enhanced Ni-CaO dual functional nanomaterials

Integration technology of methane bi-reforming (BRM; a combination of methane steam and dry reforming) with calcium looping (CaL-BRM) offered a novel solution to reduce CO2 emission, enabling direct capture and conversion of low-concentration CO2 from sources into value-added products (H2, syngas) within the same reactor. In this study, Ni-CaO-based dual-functional material (DFM), with a small quantity of palladium in the nanostructure, was developed via a continuous two-stage aerosol process and employed in the CaL-BRM. Experimental results demonstrate that Pd-Ni-CaO exhibited high activity and cyclic stability over multiple cycles, maintaining effective CO2 capture (12.0 mmolCO2/gCaO) and BRM performance (>98 % CO2 conversion; H2/CO = 2) at a relatively low temperature (600 °C). Density functional theory calculations reveal that the presence of Pd lowered the activation energy of CH* dissociation, the rate-determining step, from 1.14 to 0.67 eV. The higher adsorption energy (−0.87 eV) of H2O on the Ni-Pd surface and the lower energy barrier (0.62 eV) for subsequent dissociation contributed to the promising catalytic performance in the presence of steam. These findings underscore the significance of utilizing appropriate DFM and demonstrate the potential of CaL-BRM for efficient integrated carbon capture and utilization.

Dimethyl sulfide (DMS) climatologies, fluxes, and trends – Part 1: Differences between seawater DMS estimations

Abstract. Dimethyl sulfide (DMS) is a naturally emitted trace gas that can affect the Earth's radiative budget by changing cloud albedo. Most atmospheric models that represent aerosol processes depend on regional or global distributions of seawater DMS concentrations and sea–air flux parameterizations to estimate its emissions. In this study, we analyse the differences between three estimations of seawater DMS, one of which is an observation-based interpolation method following Hulswar et al. (2022) (hereafter referred to as H22) and two of which are proxy-based parameterization methods following Galí et al. (2018) (hereafter referred to as G18) and Wang et al. (2020a) (hereafter referred to as W20). The interpolation-based method depends on the distribution of observations and the methods used to fill data between observations, while the parameterization-based methods rely on establishing a relationship between DMS and environmental parameters such as chlorophyll a, mixed-layer depth, nutrients, sea surface temperature, etc., which can then be used to predict DMS concentrations. On average, the interpolation-based methods show higher DMS values compared to the parameterization-based methods. Even though the interpolation method shows higher values than the parameterization-based methods, it fails to capture mesoscale variability. The regression-based parameterization method (G18) shows the lowest values compared to other estimations, especially in the Southern Ocean, which is the high-DMS region in austral summer. The parameterization-based methods suggest positive long-term trends in seawater DMS (3.82±0.79 % per decade for G18 and 2.13±0.32 % per decade for W20). Since large differences, often more than 100 %, are observed between the different estimations of seawater DMS, the derived sea–air fluxes and, hence, the impact of DMS on the radiative budget are sensitive to the estimate used.

Global Influence of Organic Aerosol Volatility on Aerosol Microphysical Processes: Composition and Number

AbstractWe present MATRIX‐VBS, a new aerosol scheme that simulates organic partitioning in an aerosol microphysics model, as part of the NASA GISS ModelE Earth System Model. MATRIX‐VBS builds on its predecessor aerosol microphysics model MATRIX (Bauer et al., 2008, https://doi.org/10.5194/acp‐8‐6003‐2008) and was developed in the box model framework (Gao et al., 2017, https://doi.org/10.5194/gmd‐10‐751‐2017). The scheme features the inclusion of organic partitioning between the gas and particle phases and the photochemical aging process using the volatility‐basis set (Donahue et al., 2006, https://doi.org/10.1021/es052297c). To assess the performance of the new model, we compared its mass concentration, number concentration, and activated number concentration to the original scheme MATRIX, and evaluated its mass concentrations in four seasons against data from the NASA Atmospheric Tomography Mission (ATom) aircraft campaign. Results from MATRIX‐VBS show that organics are transported further away from their source, and their mass concentration increases aloft and decreases at the surface compared to those in MATRIX. The mass concentration of organics at the surface agrees well with measurements, and there are discrepancies for vertical profiles aloft. In the new scheme, the global mass load of organic aerosols increased by 50%, there is also an increased number of particles at the surface and fewer activated ones in most regions. The new scheme presents advanced and more comprehensive capability in simulating aerosol processes.

Synthesis of Titanium-Based Powders from Titanium Oxy-Sulfate Using Ultrasonic Spray Pyrolysis Method.

Submicron and nanosized powders have gained significant attention in recent decades due to their broad applicability in various fields. This work focuses on ultrasonic spray pyrolysis, an efficient and flexible method that employs an aerosol process to synthesize titanium-based nanoparticles by transforming titanium oxy-sulfate. Various parameters are monitored to better optimize the process and obtain better results. Taking that into account, the influence of temperature on the transformation of titanium oxy-sulfate was monitored between 700 and 1000 °C. In addition to the temperature, the concentration of the starting solution was also changed, and the flow of hydrogen and argon was studied. The obtained titanium-based powders had spherical morphology with different particle sizes, from nanometer to submicron, depending on the influence of reaction parameters. The control of the oxygen content during synthesis is significant in determining the structure of the final powder.

Recent improvements and maximum covariance analysis of aerosol and cloud properties in the EC-Earth3-AerChem model

Abstract. Given the importance of aerosols and clouds and their interactions in the climate system, it is imperative that the global Earth system models accurately represent processes associated with them. This is an important prerequisite if we are to narrow the uncertainties in future climate projections. In practice, this means that continuous model evaluations and improvements grounded in observations are necessary. Numerous studies in the past few decades have shown both the usability and the limitations of utilizing satellite-based observations in understanding and evaluating aerosol–cloud interactions, particularly under varying meteorological and satellite sensor sensitivity paradigms. Furthermore, the vast range of spatio-temporal scales at which aerosol and cloud processes occur adds another dimension to the challenges faced when evaluating climate models. In this context, the aim of this study is two-fold. (1) We evaluate the most recent, significant changes in the representation of aerosol and cloud processes implemented in the EC-Earth3-AerChem model in the framework of the EU project FORCeS compared with its previous CMIP6 version (Coupled Model Intercomparison Project Phase 6; https://pcmdi.llnl.gov/CMIP6/, last access: 13 February 2019). We focus particularly on evaluating cloud physical properties and radiative effects, wherever possible, using a satellite simulator. We report on the overall improvements in the EC-Earth3-AerChem model. In particular, the strong warm bias chronically seen over the Southern Ocean is reduced significantly. (2) A statistical, maximum covariance analysis is carried out between aerosol optical depth (AOD) and cloud droplet (CD) effective radius based on the recent EC-Earth3-AerChem/FORCeS simulation to understand to what extent the Twomey effect can manifest itself in the larger spatio-temporal scales. We focus on the three oceanic low-level cloud regimes that are important due to their strong net cooling effect and where pollution outflow from the nearby continent is simultaneously pervasive. We report that the statistical covariability between AOD and CD effective radius is indeed dominantly visible even at the climate scale when the aerosol amount and composition are favourably preconditioned to allow for aerosol–cloud interactions. Despite this strong covariability, our analysis shows a strong cooling/warming in shortwave cloud radiative effects at the top of the atmosphere in our study regions associated with an increase/decrease in CD effective radius. This cooling/warming can be attributed to the increase/decrease in low cloud fraction, in line with previous observational studies.

Optimizing indoor air models through k-means clustering of nanoparticle size distribution data

Sectional physics-based aerosol models imply a computational effort that hinders their use in building digital twins, real-time predictive control, and computer-based iterative optimization versus black-box approaches. The innovation of this paper lies in the proposal of a novel systematic methodology to optimize the number of size bins in sectional reduced-order models for particle concentration simulations. This allows its application in indoor air quality management and overcomes generalizability and data-dependency issues of black-box models. This method, based on k-means clustering, aims to ensure precision when tackling relatively fast fine and ultrafine particle simulations targeting the reduction of time and resource consumption from experimentally-determined aerosol size distribution time series. Consequently, three tests were carried out using combustion aerosols inside a custom-designed emission chamber to simulate emission hotspots in non-commercial and occupational settings. 2-, 3-, 4-, and 5-cluster classifications were evaluated for data coming from 13 particle size bins through silhouette analysis and the study of their temporal profiles. Results show that the 4-cluster classification summarizes the behavior of data in the 10–420 nm range, ensuing up to a 77 % improvement in the model's computational demand. Moreover, this method allows an accurate definition of the necessary size ranges to calculate nanoparticle concentrations inside the chamber and facilitates the interpretation of aerosol behavior and processes through the resulting clusters' temporal profiles.

PM2.5 episodes in northern Taiwan under southerly winds in late winter

When northern Taiwan is influenced locally, PM2.5 events occur in specific conditions. If it is also affected by long-range transport from mainland China in the northwest, the probability of these PM2.5 events increases. The current study applies WRF/CMAQ to study such case but focus on the local. From April 7 to 9, 2019, the Pacific high pressure extended westward, causing the prevailing weak southerly wind near Taiwan. The intensity of the Pacific high pressure weakened, and the wind speed near Taiwan also weakened. Therefore, the PM2.5 concentration in Taiwan increased. In northern Taiwan, the hourly PM2.5 concentration will inevitably increase to approximately 70 μg m−3. The ISAM of the CMAQ model demonstrates that local contributions to daily PM2.5 concentrations at the four representative monitoring stations in northern Taiwan are 3.5 to 16.2 μg m−3, greater than those from central, southern, and eastern Taiwan, from 1.8 to 6.7 μg m−3. We use the integrated process rate (IPR) and integrated reaction rate (IRR) of CMAQ to explore the formation mechanisms of PM2.5. The main causes of the increase in PM2.5 concentration are horizontal advection (HADV), aerosol processes (AERO), emissions (EMIS), and a small amount of cloud processes and aqueous chemistry (CLDS). The main source of NO3− is the reaction between OH and NO2 during the day and the reaction between N2O5 and water vapor at night. The gaseous HNO3 concentration reaches a peak near noon or soon after. The aerosol ANO3 concentration is high in the early morning. We also use the Sulfur Tracking Method (STM) of CMAQ to explore the sources of SO42−. Mainly it is from the local reaction of SO2 and H2O2. Finally, we apply AERO7 in CMAQ to explore the main sources of carbon components. The organic carbon (OC) concentration is much greater than the element carbon (EC) concentration, which indicates a strong local photochemical effect in northern Taiwan. OC mainly comes from low-volatility/semivolatile oxidized combustion OC, followed by low-volatility/semivolatile POA. Similar weather conditions occur in autumn, winter, and spring. When the weak southerly wind was around Taiwan, PM2.5 in northern Taiwan was noticed.

One‐Step Aerosol Synthesis of Thiocyanate Passivated Hybrid Perovskite Microcrystals: Impact of (Pseudo‐)Halide Additives on Crystallization and Access to a Novel Binary Model

AbstractHybrid Perovskite materials have gone through an astonishing development due to their unique optoelectronic behavior, leading to the creation of a wide range of synthetic strategies. As the materials’ surface is found to play a crucial role with respect to the properties, e.g. hydration, stability and carrier mobilities, considerable efforts have been made to optimize the surface through various approaches. Especially the passivation of the perovskite surface attracted a lot of attention in this field, often resulting in more complex, multi‐step synthetic processes. In this study, a simple one‐step aerosol‐assisted synthetic approach is presented to obtain thiocyanate (SCN) passivated single‐crystal MAPbBr3 microcrystals. To elucidate the role of the additive in the crystallization process, mixed (pseudo‐)halide precursors are systematically investigated. The as processed, passivated microcrystals exhibit enhanced stability and charge carrier lifetimes. Additionally, a decrease in surface photovoltage, attributed to the presence of the SCN additive, is observed. Furthermore, the aerosol process is further developed resulting in a novel binary system containing MAPbBr3‐SCN perovskite microcrystals and Au nanostructures. This system serves as a promising model for further investigations into potential interactions between plasmonic and semiconducting materials, with initial results indicating prolonged charge carrier lifetimes.

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

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

Aerosolized e-liquid base constituents induce cytotoxicity and genotoxicity in oral keratinocytes.

Electronic cigarette (e-cigarette) use among adults in the United States continues to rise. Particularly concerning is the impact of e-cigarette aerosol inhalation on the oral mucosa. Aerosols are derived from a heated e-liquid base of propylene glycol/glycerin (PG/G) often mixed with nicotine and chemical flavors. Of note, harmful and potentially harmful constituents (HPHCs), including metals and volatile organic compounds, have been detected in e-cigarette aerosols. It remains unknown, however, whether aerosols exclusively derived from e-liquid PG/G are detrimental to oral keratinocytes. The present study analyzed toxicological outcomes in normal oral keratinocytes exposed to model nicotine-free, unflavored PG/G e-liquid aerosols. Cell viability/cytotoxicity, genotoxicity, and immunoblotting assays were conducted in NOKSI, a gingiva-derived oral keratinocyte cell line, following exposure to model e-liquid aerosols or non-aerosolized controls. The HPHC acrolein, reported to form DNA adducts in the buccal mucosa from e-cigarette users, was also used in similar assays. PG/G e-liquid aerosol extracts significantly enhanced cytotoxic and DNA damaging responses in NOKSI cells when compared to non-aerosolized e-liquid treatment. Acrolein treatment led to similar results. The aerosolization process of PG/G e-liquid is a critical determinant of marked cytotoxic and genotoxic stimuli in oral keratinocytes.

Spectral Characteristics of Unsaturated and Supersaturated Inorganic Aerosols: Insights into Deliquescence Kinetics.

The deliquescence phase transition of atmospheric aerosols is crucial for radiative forcing and atmospheric chemistry. However, the deliquescence kinetics of micrometer-sized aerosols, especially the formation and evolution of surface solution films, remain poorly understood. In this study, IR spectral characteristics were employed for the first time to quantify the solute concentration evolution in surface solution films. At a constant relative humidity (RH) of ∼65%, solution films on NaCl crystals exhibited a very low solute concentration (3.06 ± 0.18 mol/L), comparable to aqueous NaCl droplets above 90% RH. These films reached saturation at ∼74% RH, i.e., the deliquescence RH of NaCl, maintaining a nearly constant saturation level during deliquescence. In contrast, amorphous NaNO3 solids showed supersaturated solution films before deliquescence. Following deliquescence, the saturation level of solution phases increased due to faster solid dissolution rates than liquid water condensation. These findings address knowledge gaps in the complex nonequilibrium dissolution processes of crystalline or amorphous atmospheric aerosols.

Prolonged Dark Chemical Processes in Secondary Organic Aerosols on Filters and in Aqueous Solution.

Secondary organic aerosol (SOA) represents a large fraction of atmospheric aerosol particles that significantly affect both the Earth's climate and human health. Laboratory-generated SOA or ambient particles are routinely collected on filters for a detailed chemical analysis. Such filter sampling is prone to artifactual changes in composition during collection, storage, sample workup, and analysis. In this study, we investigate the chemical composition differences in SOA generated in the laboratory, kept at room temperature as aqueous extracts or on filters, and analyzed in detail after a storage time of a day and up to 4 weeks using liquid chromatography coupled to high-resolution mass spectrometry. We observe significantly different temporal concentration changes for monomers and oligomers in both extracts and on filters. In SOA aqueous extracts, many monomers increase in concentration over time, while many dimers decay at the same time. In contrast, on filters, we observe a strong and persistent concentration increase of many dimers and a decrease of many monomers. This study highlights artifacts arising from SOA chemistry occurring during storage, which should be considered when detailed organic aerosol compositions are studied. The particle-phase reactions on filters can also serve as a model system for atmospheric particle aging processes.

Immunogenicity and Protective Efficacy of Aerosolized Live-Attenuated Yellow Fever 17D Vaccine in Mice.

Yellow fever (YF), caused by the yellow fever virus (YFV), continually spreads and causes epidemics worldwide, posing a great threat to human health. The live-attenuated YF 17D vaccine (YF-17D) has been licensed for preventing YFV infection and administrated via the intramuscular (i.m.) route. In this study, we sought to determine the immunogenicity and protective efficacy of aerosolized YF-17D via the intratracheal (i.t.) route in mice. YF-17D stocks in liquids were successfully aerosolized into particles of 6 μm. Further in vitro phenotype results showed the aerosolization process did not abolish the infectivity of YF-17D. Meanwhile, a single i.t. immunization with aerosolized YF-17D induced robust humoral and cellular immune responses in A129 mice, which is comparable to that received i.p. immunization. Notably, the aerosolized YF-17D also triggered specific secretory IgA (SIgA) production in bronchoalveolar lavage. Additionally, all immunized animals survived a lethal dose of YFV challenge in mice. In conclusion, our results support further development of aerosolized YF-17D in the future.

An oxidation flow reactor for simulating and accelerating secondary aerosol formation in aerosol liquid water and cloud droplets

Abstract. Liquid water in cloud droplets and aqueous aerosols serves as an important reaction medium for the formation of secondary aerosol through aqueous-phase reactions (aqSA). Large uncertainties remain in estimates of the production and chemical evolution of aqSA in the dilute solutions found in cloud droplets and the concentrated solutions found in aerosol liquid water, which is partly due to the lack of available measurement tools and techniques. A new oxidation flow reactor (OFR), the Accelerated Production and Processing of Aerosols (APPA) reactor, was developed to measure secondary aerosol formed through gas- and aqueous-phase reactions, both for laboratory gas mixtures containing one or more precursors and for ambient air. For simulating in-cloud processes, ∼ 3.3 µm diameter droplets formed on monodisperse seed particles are introduced into the top of the reactor, and the relative humidity (RH) inside it is controlled to 100 %. Similar measurements made with the RH in the reactor < 100 % provide contrasts for aerosol formation with no liquid water and with varying amounts of aerosol liquid water. The reactor was characterized through a series of experiments and used to form secondary aerosol from known concentrations of an organic precursor and from ambient air. The residence time distributions of both gases and particles are narrow relative to other OFRs and lack the tails at long residence time expected with laminar flow. Initial cloud processing experiments focused on the well-studied oxidation of dissolved SO2 by O3, with the observed growth of seed particles resulting from the added sulfuric acid agreeing well with estimates based on the relevant set of aqueous-phase reactions. The OH exposure (OHexp) for low RH, high RH, and in-cloud conditions was determined experimentally from the loss of SO2 and benzene and simulated from the KinSim chemical kinetics solver with inputs of the measured 254 nm UV intensity profile through the reactor and loss of O3 due to photolysis. The aerosol yield for toluene at high OHexp ranged from 21.4 % at low RH with dry seed particles present in the reactor to 78.1 % with cloud droplets present. Measurement of the composition of the secondary aerosol formed from ambient air using an aerosol mass spectrometer showed that the oxygen-to-carbon ratio (O : C) of the organic component increased with increasing RH (and liquid water content).

Stratospheric aerosol characteristics from SCIAMACHY limb observations: two-parameter retrieval

Abstract. Stratospheric aerosols play a key role in atmospheric chemistry and climate. Their particle size is a crucial factor controlling the microphysical, radiative, and chemical aerosol processes in the stratosphere. Despite its importance, available observations on aerosol particle size are rather sparse. This limits our understanding and knowledge about the mechanisms and importance of chemical and climate aerosol feedbacks. The retrieval described by Malinina et al. (2018) provides the stratospheric particle size distribution (PSD) from SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY) limb observations in the tropics. This algorithm has now been improved and extended to work on the entire globe. Two PSD parameters of a unimodal lognormal PSD, the median radius and the geometric standard deviation, are retrieved between 18 and 35 km altitude from SCIAMACHY limb observations by a multiwavelength nonlinear regularized inversion. The approach assumes an aerosol particle number density profile that does not change during the retrieval. The effective Lambertian surface albedo pre-retrieved from coinciding SCIAMACHY nadir observations is integrated into the retrieval algorithm to mitigate the influence of the surface albedo on the retrieval results. The extinction coefficient and the effective radius are calculated from the PSD parameters. The aerosol characteristics from SCIAMACHY are compared with in situ balloon-borne measurements from Laramie, Wyoming, and retrievals from the satellite instruments of the Stratospheric Aerosol and Gas Experiment series (SAGE II and SAGE III) and Optical Spectrograph and InfraRed Imager System (OSIRIS). In the Northern Hemisphere, the median radius differs by less than 27 % and the geometric standard deviation by less than 11 % from both balloon-borne and SAGE III data. Differences are mainly attributed to errors in the assumed a priori number density profile. Globally, the SCIAMACHY extinction coefficient at 750 nm deviates by less than 35 % from SAGE II, SAGE III, and OSIRIS data. The effective radii from SCIAMACHY, balloon-borne measurements, and SAGE III agree within about 18 %, while the effective radius based on SAGE II measurements is systematically larger. The novel data set containing the PSD parameters, the effective radius, and the aerosol extinction coefficients at 525, 750, and 1020 nm from SCIAMACHY observations is publicly available.

Modeling the evolution of aerosol particles from a radiological dispersal device

Radiological dispersal devices (RDDs) have a potential to disperse radioactive aerosols into the atmosphere through explosions. Accurately estimating the respirable fraction of these aerosols through experiments presents a considerable challenge. Also, the modeling of aerosol particle evolution stemming from an RDD explosion is inherently complex, involving the interplay of various physical processes operating at different time scales. In this study, we propose a comprehensive numerical model to estimate the respirable fraction of aerosols generated during RDD explosions, integrating the thermodynamic properties of detonation products with microphysical aerosol processes. The model assumes particles are spherical and ignores charge effects. It is also assumed that the thermodynamic properties of the cloud are uniform within its volume and that thermal equilibrium exists between particles and the surrounding medium. Numerical simulations are conducted for diverse experimental scenarios, and performance of the model is assessed by comparing its predictions with experimental data pertaining to Carbon and Cobalt particles. Notably, the model predicts the average particle diameter of Carbon particles within the detonation front of TNT at 13.8 nm, closely matching the experimental observation of 13 nm (Rubtsov et al., 2019). Additionally, the model captures the peak value of the cobalt particle mass fraction distribution, approximating it to be around 0.7μm, in agreement with experimental findings (Di Lemma et al., 2016). These findings indicate that the proposed model is capable of predicting the behavior of both radioactive and non-radioactive aerosols. Also, this study underscores the potential of modeling approaches in addressing existing knowledge gaps related to RDDs, thereby contributing to enhanced impact assessment and management strategies for incidents involving RDDs.

Bifunctional polyoxometalate clusters-modified single-walled carbon nanotubes for high-energy–density micro-supercapacitors

The rapid advancement of wearable electronics has pushed the urgent demand for flexible power sources with high energy density and fast integrations. Herein, we created high-energy–density micro-supercapacitors (MSCs) based on phosphomolybdic acid (PMo12) clusters anchored single-walled carbon nanotubes (SWCNTs) via the electrostatic assembly. The SWCNT microelectrodes for MSCs were directly fabricated by an aerosol process without any solvent-based treatment. The PMo12 clusters were found to not only increase the electrical conductivity of SWCNT thin-film electrodes, but also offer significant pseudo-capacitance of MSCs. The MSCs based on PMo12-modified SWCNTs demonstrated an areal capacitance of 10.2 mF cm−2 when scanned at 5 mV s−1, coupled with a notable energy density of 0.71 μWh cm−2 at a power density of 7 μW cm−2, being much higher than the one without PMo12 modification. The density functional theory simulation further reveals the enhancement of electrical conductivity and areal capacitance induced by PMo12 modifications. Moreover, our strategy is highly scalable for integrations via series or parallel connections, which could deliver higher voltage output or areal capacitance. This work demonstrates great potential for high-performance MSCs toward wearable electronics applications.

Intercomparison of aerosol optical depths from four reanalyses and their multi-reanalysis consensus

Abstract. The emergence of aerosol reanalyses in recent years has facilitated a comprehensive and systematic evaluation of aerosol optical depth (AOD) trends and attribution over multi-decadal timescales. Notable multi-year aerosol reanalyses currently available include NAAPS-RA from the US Naval Research Laboratory, the NASA MERRA-2, JRAero from the Japan Meteorological Agency (JMA), and CAMSRA from Copernicus/ECMWF. These aerosol reanalyses are based on differing underlying meteorology models, representations of aerosol processes, as well as data assimilation methods and treatment of AOD observations. This study presents the basic verification characteristics of these four reanalyses versus both AERONET and MODIS retrievals in monthly AOD properties and identifies the strength of each reanalysis and the regions where divergence and challenges are prominent. Regions with high pollution and often mixed fine-mode and coarse-mode aerosol environments, such as South Asia, East Asia, Southeast Asia, and the Maritime Continent, pose significant challenges, as indicated by higher monthly AOD root mean square error. Moreover, regions that are distant from major aerosol source areas, including the polar regions and remote oceans, exhibit large relative differences in speciated AODs and fine-mode versus coarse-mode AODs among the four reanalyses. To ensure consistency across the globe, a multi-reanalysis consensus (MRC, i.e., ensemble mean) approach was developed similarly to the International Cooperative for Aerosol Prediction Multi-Model Ensemble (ICAP-MME). Like the ICAP-MME, while the MRC does not consistently rank first among the reanalyses for individual regions, it performs well by ranking first or second globally in AOD correlation and RMSE, making it a suitable candidate for climate studies that require robust and consistent assessments.

Measurement report: Optical characterization, seasonality, and sources of brown carbon in fine aerosols from Tianjin, North China: year-round observations

Abstract. To investigate the optical characteristics and sources of brown carbon (BrC) in North China, where the atmospheric aerosol loadings are high and have severe impacts on Earth's climate system, we collected fine aerosols (PM2.5) at an urban site in Tianjin over a 1-year period. We measured the ultraviolet (UV) light absorption and excitation emission matrix (EEM) fluorescence of the water-soluble BrC (WSBrC) and the water-insoluble but methanol-soluble BrC (WI-MSBrC) in the PM2.5 using a three-dimensional fluorescence spectrometer. The average light absorption efficiency of both WSBrC (Abs365, WSBrC) and WI-MSBrC (Abs365, WI-MSBrC) at 365 nm was found to be highest in winter (10.4 ± 6.76 and 10.0 ± 5.13 Mm−1, respectively) and distinct from season to season. The averages of the fluorescence index (FI) and the biological index (BIX) of WSBrC were lower in summer than in the other seasons and opposite to that of the humification index (HIX), which implied that the secondary formation and further chemical processing of aerosols were more intensive during the summer period than in the other seasons. However, in winter, the higher HIX together with the higher FI and BIX of WI-MSBrC suggested that the BrC loading was mainly influenced by primary emissions from biomass burning and coal combustion. Based on the EEM, the types of fluorophores in WSBrC were divided into humic-like substances (HULIS), including low-oxygenated and high-oxygenated species and protein-like compounds (PLOM), though mostly PLOM in the WI-MSBrC. The direct radiation absorption by both WSBrC and WI-MSBrC in the range of 300–400 nm accounted for ∼ 40 % of that (SFEAbs, 4.97 ± 2.71 and 7.58 ± 5.75 W g−1, respectively) in the range 300–700 nm.