Multifunctional electrochromic supercapacitor (ESC) materials, which enable real-time visual monitoring of energy storage levels through color variations, show great application potential in smart displays, wearable electronics, and energy recycling systems. However, developing materials that integrate high-performance electrochromic and energy storage capabilities remains challenging. Herein, two novel dibenzothiophene (DBT)-based organic monomers were designed and synthesized by incorporating DBT units at the 3,7-positions into conjugated backbones. The corresponding polymer films (pDBT-E and pDBT-P) were successfully obtained through electropolymerization of the thiophene units. Experimental and density functional theory calculations revealed that incorporating DBT at positions 3 and 7 into conjugated backbones obtains monomers with narrower bandgaps compared to incorporation at the 2,8-positions. The resulting polymers pDBT-E and pDBT-P exhibit reversible color switching between orange/yellow and blue with significant color differences (Delta E*ab = 52.4 and 47.4, respectively). Among them, pDBT-P exhibits good electrochromic performance, including a high optical contrast of 46.7 % at 465 nm, rapid switching speeds (1.2 s/0.4 s), a high coloration efficiency of 675 cm2/C, and outstanding cycling stability with 72.0 % retention after 8000 cycles, representing one of the highest performances among DBT-based EC materials. In addition, pDBT-P also exhibits a high volumetric capacitance of 64.6 F/cm3, exceptional rate capability, and good cycling stability. Furthermore, asymmetric ESCs fabricated using these DBT-based polymer films as active layers manifest reversible color variation during charge/discharge processes, coupled with exceptional EC performance and high capacitive properties. Overall, this work establishes the first incorporation of DBT into ESCs, demonstrating and elucidating the significant application potential of DBT-based CPs for integrated real-time visual energy-state monitoring, electrochromic, and energy storage.
Soot aerosol, a key global warming contributor, undergoes morphological and chemical transformations during atmospheric transport, particularly in humidified marine environments. This study investigates morphology, mixing state, and aging mechanisms of soot particles collected in the Bohai Sea and Yellow Sea. Transmission electron microscopy analyses reveal that coated soot particles dominate the marine atmosphere, accounting for over 98 % of soot-containing particles, with a mean mixing state index (χ) of 0.83. The fractal dimension (Df) of soot particles is 1.84 ± 0.05 in the Northern Yellow Sea, 1.90 ± 0.08 in the Bohai Sea, and 1.96 ± 0.07 in the Southern Yellow Sea, indicating structural compaction during long-range transport. Correspondingly, the average Dp/Dcore ratios (particle to core size ratio) are 5.3 in the Bohai Sea, 4.2 in the Northern Yellow Sea, and 3.9 in the Southern Yellow Sea. Notably, those ratios are higher in marine environments compared to those observed during continental regional transport from northern to southern China (3.54), suggesting enhanced coating growth in humid marine air. The results highlight the important role of marine atmospheres in accelerating soot aging, which in turn leads to significantly stronger light absorption compared to soot in continental air. Our results highlight the necessity of incorporating compact morphologies, uniform mixing states, and thick coatings into optical models for accurate radiative forcing simulations.
The impact of isomerism on electrochemical/electrochromic (EC) materials remains insufficiently explored. In this work, two electrochromic-supercapacitor (ECS) bifunctional materials pBQ based on pyrazine unit and pDQ based on pyridazine unit featuring diazine isomers are synthesized through direct (hetero)arylation polymerization. The impact of diazine isomeric units on backbone structure, EC properties, and supercapacitor performance of materials are investigated in detail. The pBQ base on pyrazine displays enhanced backbone planarity, higher color saturation of 51.82 in the neutral state and lower color chroma of 0.26 in the oxidized state, indicating reversible color-changing between a more vivid colored state and highly transparent state. Furthermore, the pBQ presents improved electrochemical and EC properties than those of pDQ, including more reversible electrochemical behavior, larger coloring efficiency (279.5 cm2 C-1), better cycle stability (retaining >90 % of initial performance after 1000 cycles), and higher area-specific capacitance of 2.61 mF cm-2. The prototype EC labels base on pBQ and pDQ are assembled, enabling updatable information capabilities and dynamic data management. This work introduces a novel approach to precisely enhance backbone planarity, facilitate color tunability, and develop electrochromic-supercapacitor bifunctional materials with highperformance.
Black carbon (BC) is an atmospheric pollutant that adversely affects air quality, global climate, and human health. As an important BC source region, China has achieved substantial emission reductions over the past decade through stringent clean air policies, offering a unique opportunity to study changes of BC sources and properties under rapid emission changes. Concurrently, BC research in China has progressed rapidly, shifting from studying emission sources toward atmospheric processes and health impacts. This review focuses on five key topics in BC research, including ambient concentrations, emission sources, atmospheric aging, mixing state, and health effects. Ground observation networks and gridded datasets have shown a significant decrease in BC concentrations due to clean air policies, particularly in Northern and Eastern China. Emission inventories and source apportionment studies consistently identified fossil fuel combustion as the dominant BC source in China. Laboratory, field, and modeling studies have advanced understanding of BC aging and mixing state. The health evidence from China has linked BC exposure to respiratory, cardiovascular, and neurological diseases. The rapid expansion and heterogeneity of datasets underscore the urgent need for measurement standardization and cross-regional dataset comparison. In addition, this review calls for stronger integration of measurement and modeling to better study BC sources, aging, and mixing states, and highlights the need for assessing source-specific health impacts and understanding how atmospheric aging modifies BC toxicity.
Urban metro systems represent a semi-enclosed underground microenvironment where fine particulate matter (PM2.5) frequently accumulates, posing significant inhalation risks to commuters. This study conducted systematic field monitoring of PM2.5 mass concentrations and particle number size distributions within carriages and on platforms across Hangzhou Metro from January to March 2025. Commuter exposure was quantified using Monte Carlo simulations and Sobol sensitivity analysis. The average PM2.5 concentrations were 46.3 μg/m3 in carriages and 65.3 μg/m3 on platforms, representing 1.2- and 1.7-fold increases over concurrent outdoor ambient levels (38.9 μg/m3), respectively. Both microenvironments exceeded the annual PM2.5 Grade II limit of the Chinese National Ambient Air Quality Standard (25 μg/m3). Platform concentrations were significantly higher than those in carriages for particles sized 0.3 μm and ≥ 1 μm (p < 0.05). Analysis of 115 discrete train-arrival and door-opening events revealed that door cycles induced significant instantaneous PM2.5 surges (∼+2.18 μg/m3). Peak concentrations were observed 20-30 s post-opening, with levels returning to baseline after about 75 s. The mean exposure dose was estimated at 11.9 μg per commute, with a unit-time exposure intensity (20.4 μg/h) 1.07 times that of outdoor activity. Monte Carlo simulations indicated a right-skewed distribution of total exposure (median: 11.6 μg; 95th percentile: 19.4 μg). Sobol sensitivity analysis identified carriage exposure duration and carriage PM2.5 concentrations as the two primary drivers of total exposure uncertainty. These findings underscore that optimizing carriage filtration, enhancing platform ventilation, and minimizing transit duration are critical interventions for mitigating particulate matter exposure among metro commuters.
In the context of the continuously increasing energy demand, the ongoing advancement of innovative energy storage technologies is regarded as an important strategy to alleviate the energy crisis. Among various energy storage technologies, supercapacitors (SCs) demonstrate significant potential in the future energy storage sector due to their exceptional high-power density and long cycle life. As the core component of SCs, the choice of electrode materials is crucial to their performance, with carbon materials being favored for their excellent electrical conductivity and large specific surface area. In particular, porous carbon materials derived from biomass-based polymers have become a research hotspot due to their unique advantages. Through chemical modification and high-temperature carbonization, these materials can form more stable and optimized porous structures, significantly enhancing their electrochemical performance while meeting environmental protection requirements, thereby highlighting their superiority as electrode materials. This article aims to review the sources, production, and applications of carbon materials derived from biomass-based polymers. We have deeply summarized the preparation and activation methods of carbon from different biomass-based polymer sources. In addition, a comprehensive analysis and systematic comparison of novel modification techniques, such as heteroatom doping, copolymerization, and the incorporation of nanomaterials, were performed to enhance the performance of SCs. Finally, according to the technical challenges to be solved, the goal of large-scale development of biomass-based polymer-derived porous carbon in the field of energy storage is proposed, which is crucial for coping with the global energy crisis and reducing environmental impact.
The design of suitable polymorphic thermally activated delayed fluorescence (TADF) emitters is crucial for advancing multifunctional organic luminescent materials. Herein, a unique multifunctional molecule, the benzoimido-benzamide derivative DMAC-PYZ, was synthesized through a green photo-oxidation reaction. This compound exhibited polymorphism (DG and DY), TADF, mechanochromic luminescence (MCL), and aggregation-induced emission (AIE) properties. The DG and DY crystals displayed green and yellow fluorescence, respectively, with delayed fluorescence lifetimes of 65.76 mu s (DG) and 0.29 mu s (DY). Furthermore, it demonstrated an aggregation-dependent TADF characteristic and MCL behavior in response to mechanical stimuli. Crystal structure and density functional theory (DFT) analysis revealed that the aggregation-dependent TADF originated from variations in the D-A molecular twist angle across different aggregation states. Upon thermal stimulation at 60 degrees C, amorphous powders of DG and DY reversibly revert to their original crystalline packing structures and emission. These characteristics stemmed from the high stability of crystalline enantiomers. This rare reversible polymorph-toamorphous phase transition has been successfully applied to information security and encryption. This study presented a novel MCL-active TADF material capable of reversible polymorph-to-amorphous phase transition, elucidating the conformation-property relationship in aggregated states.
P-Phenylenediamines (PPDs), widely used tire antioxidants, undergo oxidation to form toxic quinones (PPD-Qs). Despite their detection in diverse environmental media, the role of cloud water in environmental fate remains unknown. This study employed ultrahigh-performance liquid chromatography-Orbitrap mass spectrometry to investigate ten PPDs and PPD-Qs in cloud water collected from Tianmu Mountain in China─a remote background site with minimal industrial/human activity. The concentrations of PPDs (3.0-43.7 ng/L) are markedly exceeding their transformation products (PPD-Qs, 0.2-11.5 ng/L), with IPPD and 6PPD dominating. PPDs exhibited greater accumulation in water-insoluble organic matter (WISOM) than in water-soluble organic matter (WSOM), with enrichment factors (concentration of PPDs in WISOM/concentration of PPDs in WSOM) ranging from 1.13 to 1.88, indicating a stronger tendency for particle-phase partitioning. Significant positive correlations linked PM2.5 levels with the deposition fluxes of both PPDs and PPD-Qs in WSOM and WISOM, demonstrating cloud water's key role in their atmospheric transport and wet deposition. This study presents the first characterization of PPDs and their quinone derivatives' distribution and environmental behavior in cloud water, revealing clouds' significant role in the fate of rubber-derived pollutants. The findings reveal clouds as pivotal reactors for tire-derived pollutants, driving oxidation and multiphase portioning, previously overlooked in global contaminant cycling.
Delhi, one of the world's most densely populated megacities, experiences extreme haze during the Diwali Festival─a nationwide celebration marked by intense fireworks coinciding with postmonsoon biomass burning. Although bulk measurements routinely show sharp PM2.5 spikes during Diwali, direct microscopic evidence linking specific aerosol types to these concurrent sources remains limited. Here, we combined transmission electron microscopy (TEM) with bulk chemical analysis to identify particle types and track their physicochemical evolution throughout the Diwali period. Before Diwali, aerosols were dominated by potassium (K)-rich particles (25%), carbonaceous particles (primary organic aerosol (POA) and soot, 29%), and their internal mixtures (K-POA/soot, 37%), with frequent spherical POA (i.e., tar balls), indicating a strong biomass-burning influence. During Diwali, particle populations shifted abruptly to a pyrotechnic signature of fireworks, characterized by abundant Al2O3 monomers (30-300 nm) and their agglomerates, either as bare (36-40%) or uniformly coated by K2SO4 (Al2O3-K, 46-47%). After Diwali, ultrafine Al2O3 particles (<100 nm) persisted and underwent coagulation with aged biomass-burning particles, forming distinctive Al2O3-K-POA/soot internal mixtures. Therefore, Al2O3 nanoparticles can serve as a tracer of fireworks and were further internally mixed with carbonaceous particles derived from biomass burning during severe haze events of Diwali. These metal-containing particles warrant particular attention because of their potential toxicity and adverse respiratory health effects in the densely populated megacity.
With the rapid expansion of China’s civil aviation industry, airport aircraft emissions have raised growing environmental concerns, making it imperative to clarify their emission characteristics and driving mechanisms. In this study, 10 major civil aviation airports in Shandong Province, a highly representative airport cluster in China, were selected to investigate the characteristics of aviation emissions using actual flight activity data from 2023. Our results show that the total emissions of HC, CO, NOx, SO2, PM, and CO2 from the airport aircraft were 144.6, 1890.4, 2571.8, 358.7, 18.2, and 584,822 tons, respectively, with NOx and CO being the dominant air pollutants. The taxiing phase was identified as the largest contributor to total emissions, and the B737-800 emerged as the largest emission-contributing aircraft type. Moreover, our results reveal that airport aircraft emissions exhibited spatiotemporal heterogeneity. These emissions peaked in July and August, but displayed low levels during wintertime. Spatially, these aviation emissions were predominantly concentrated in eastern Shandong Province, and Qingdao and Jinan cities were the top two contributors, jointly contributing more than 66% of the total emissions. This study further indicates that this spatiotemporal heterogeneity was primarily attributed to air passenger throughput, aircraft movements, and GDP. Our findings can be extended to other provinces in China and provide a scientific basis for the future mitigation of aviation emissions at airports across China.
Household coal smoke was evidenced to cause the uniquely high lung cancer mortalities in Xuan Wei, China. Lung cancer screening in local villagers found concurrently high prevalence of interstitial pneumonia. What could be the shared hazard linking those pathologies? Could it be some coal-derived mineral deposit in lungs that causes both fibrotic and malignant changes? A case-control study was conducted by recruiting 50 lung cancer cases and 30 pseudotumor controls among non-smoking women from Xuan Wei, China. The severity of interstitial lung abnormalities (ILAs) was compared between cases and controls by high-resolution computed tomography (HRCT) and histopathological analysis; mineral deposits in lung tissues were examined by light microscopy and electron microscopy techniques. The lung cancer case group and the pseudotumor group share this characteristic of abundant ILAs while the fibrotic changes are more severe in lung cancer than pseudotumor cases. Fibrotic changes are more severe in peribronchial lymph nodes than in lung parenchyma. Mineral deposits embedded in the anthracotic pigments are visible under polarized light microscopy (PLM) due to their birefringence. The morphology of this birefringent mineral resembles that of acicular berthierine-chamosite identified in Late Permian coal from Xuan Wei, China. These preliminary findings underscore the need for further investigation into the mineralogical factors contributing to the high incidence of lung cancer in this region.
The size of aerosol particles is a key factor influencing the fractional solubility of iron (Fe) deposited to the surface ocean, as particle size reflects both aerosol sources and atmospheric processing. However, the relationship between aerosol particle size and fractional Fe solubility remains poorly constrained. In this study, sizesegregated aerosol samples were collected at three representative sites-urban, background, and coastal-in eastern China during the winter from December 2020 to January 2021. The size-dependent fractional solubility of Fe was examined, along with the influence of source characteristics and aerosol acidification. The average fractional Fe solubility in total suspended particles (TSP) was highest at the background site (5.4%), followed by the urban (4.6%) and coastal (3.4%) sites. At all sites, fractional Fe solubility was about three times or more higher in the fine mode than in the coarse mode during both haze and clean periods. Size distributions of fractional Fe solubility generally exhibited a unimodal pattern with peaks at 0.56-1.0 mu m at the urban and background sites, whereas a predominantly trimodal distribution with peaks at 0.56-1.0 mu m or smaller was observed at the coastal site. Vehicle emissions, biomass burning, and aerosol acidification associated with sulfate and nitrate formation played important roles in enhancing fractional Fe solubility in fine particles.
Intelligent energy storage devices, particularly electrochromic supercapacitors (EC-SCs), have garnered considerable interest owing to their rapid charge/discharge kinetics and excellent cycling durability. In this work, we designed and synthesized electrochromic conjugated polymers D1 and D2 featuring cyclopentadithiophene (CPDT) donor and anthraquinone (AQ) dye acceptor via direct arylation polymerization. Both polymers exhibit robust electrochromic performance, including high cycle stability (retaining around 80 % after 1000 cycles) and short response times (1.34 s/1.39 s for D1 and 0.59 s/2.46 s for D2). Under an influence of an applied voltage, their optical states are reversibly modulated, transitioning from warm colors (pink and orange) in the neutral state to purple and a nearly transparent hue in the oxidized state. In addition, the polymers show competitive specific capacitance (1.06 mF cm-2 and 1.23 mF cm-2 at a current density of 0.05 mA cm-2) and sustained charge-discharge cycling stability (retaining around 90 % after 100 cycles), corroborating their bifunctional roles in simultaneous color switching and energy storage. Electrochromic energy storage devices based on anthraquinone dye-based electrochromic conjugated polymer thin films were fabricated and showed obvious color change during the charge-discharge process. Furthermore, the area specific capacitance of each EC-SCs was calculated to be 1.25 mF cm-2 for EC-SC-1, 0.92 mF cm-2 for EC-SC-2 at a current density of 0.05 mA cm-2. This work establishes a viable strategy for achieving efficient electrochromic switching and enhanced energy conversion in EC-SCs, advancing material design principles for multifunctional optoelectrochemical devices.
Winter haze over the North China Plain (NCP) remains a major air quality challenge. Molecular-level characterization of water-soluble organic carbon (WSOC) is needed to clarify how contrasting urban and rural emission mixtures, together with subsequent atmospheric processing, shape organic aerosol composition. Here we characterized wintertime PM2.5 collected from paired urban and rural sites using Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS), complemented by measurements of bulk aerosol components (i.e., PM2.5, organic carbon, WSOC, and major inorganic ions). Among all assigned molecular formulas, urban WSOC showed a higher formula-count contribution of nitrogen-containing species, with CHON formulas accounting for 29.1% compared with 21.3% at the rural site. In contrast, rural WSOC exhibited a slightly higher contribution of CHOS formulas (27.1%). Analysis of site-unique formulas further amplified these divergences. Urban-unique WSOC formulas were dominated by CHON formulas (47.6%), while rural-unique WSOC formulas were strongly enriched in sulfur-containing species, with CHOS and CHONS formulas collectively accounting for 67.9%. Atom-number fingerprints revealed that urban-unique CHON formulas had a larger contribution from formulas containing two N atoms and higher oxygen contents, whereas rural-unique CHON formulas were dominated by formulas containing one N atom, indicating distinct nitrogen functionalities and atmospheric processing environments. This work provides robust molecular evidence for pronounced urban-rural divergence in wintertime organic aerosol composition in the NCP and offers a molecular basis for source- and processinformed haze mitigation strategies.
Electrochromic (EC) technology, particularly dye-based electrochromic systems, has attracted increasing attention owing to its numerous advantages and broad prospects. In this work, two isomeric diketopyrrolopyrrole (DPP) dyes were synthesized and copolymerized with cyclopentadithiophene derivatives (CPDT) to produce two electrochromic polymers pDPP1 and pDPP2 with different linking sites of DPP group. Under an applied electric field, the neutral state of pDPP1 is red, and it becomes transparent upon oxidation. Meanwhile, the neutral state of pDPP2 is orange, while its oxidized state is olive green. Measurements show pDPP1 has a short bleaching time and coloring time of 0.48 s and 0.62 s, while pDPP2 has longer ones of 1.83 s and 1.05 s. In addition, coloration efficiencies of pDPP1 and pDPP2 are estimated to be 231.75 cm2 C-1 and 275.43 cm2 C-1, respectively. The polymer pDPP1 retains 86% of its optical contrast after 800 cycles, significantly higher than that of pDPP2 (67%). Under current density of 0.05 mA cm-2, pDPP1 achieves an areal capacitance of 5.43 mF cm-2. The capacitance retention was about 60% and the Coulombic efficiency remains 95% after 500 cycles. Electrochromic-supercapacitor devices (EC-SC-A) based on pDPP1 films achieved an areal specific capacitance of 6.03 mF cm-2 under the current density of 0.05 mA cm-2, with charging and discharging accompanied by a marked color change from red to transparent. This work achieves efficient electrochromic switching coupled with energy storage based on DPP dyes and provides a new strategy of electrochromi supercapacitor devices from dye material.
Subway systems are vital for urban transit, yet their air contains iron-oxide nanoparticles that may threaten commuters' respiratory and cardiovascular health. Despite their prevalence, the microscopic properties, formation mechanisms and health effect of these particles remain poorly understood. Here we analyze subway-derived dust sampled at four sites along three metro lines in Hangzhou, China, revealing that magnetic nanoparticles constitute a substantial fraction of subway aerosols. These particles exist in two forms: alpha-Fe2O3 from surface dust and airborne Fe3O4 nanoparticles with a magnetic core encapsulated in an amorphous SiO2 shell, primarily originating from wheel-rail and brake-wheel friction. Notably, we detect nanoscale Fe3O4 particles in lung tissues of subway commuters, demonstrating their inhalation and pulmonary deposition in humans. Mouse inhalation exposure experiments further confirm that Fe3O4 nanoparticles can induce pronounced lung injury. Our findings highlight friction-derived magnetic nanoparticles as a potential public health risk and underscore the need for strategies to mitigate commuter exposure in urban subway systems.
Black carbon (BC) is an important short-lived climate forcer that contributes to Arctic warming, yet observations of BC in the Arctic marine boundary layer remain sparse. Here, we report shipborne measurements of refractory BC (rBC) mass and particle mixing state during a cruise from southeast to west Greenland in May-June 2022. Using a single-particle soot photometer (SP2XR) and transmission electron microscopy (TEM), we characterize both rBC concentrations and individual-particle morphology, representing one of the first ship-based SP2XR data sets in the Arctic marine boundary layer. rBC concentrations were highest in the Greenland coastal region (2.4 ng m-3), compared with the open ocean (1.7 ng m-3) and the marginal ice zone (0.6 ng m-3). Mixing-state analysis shows that 54% of soot particles in coastal air masses were externally mixed, consistent with relatively fresh emissions, whereas most soot particles over the open sea and sea-ice regions were internally mixed, indicative of aged, transported aerosol. FLEXPART modeling suggests BC enhancements along the Greenland coast. Our data indicate that Greenland acts as a regional source of BC to the Arctic marine boundary layer in late spring and early summer, when midlatitude transport is weak.
Microplastics (MPs) have emerged as a critical anthropogenic pollutant, increasingly recognized for their persistence and ubiquity in the environment. While extensive research has focused on MPs in aquatic and terrestrial systems, studies of inhalable airborne MPs (AMPs) remain limited. In this study, we investigated the diurnal variability and physicochemical characteristics of AMPs in PM10 aerosols using a novel single-particle analytical approach that integrates fluorescence microscopy, Raman microspectrometry, and SEM/EDX. AMP number concentrations averaged ∼1,300 particles/m3 during the sampling period and were approximately 60% higher at night than during the day, a trend linked to boundary layer dynamics and air mass trajectories. Most AMPs were smaller than 10 μm (95%), with about 40% below 2.5 μm, indicating high inhalation potential. Morphological and spectral evidence showed that many particles were aged, with transformations from angular to rounded or lumpy forms becoming more pronounced as particle size decreased. Overall, these results indicate that AMP abundance is governed largely by meteorological conditions. AMPs resuspended from contaminated environments likely contribute significantly, alongside direct anthropogenic emissions. This study provides new insights into the diurnal variability, sources, and characteristics of inhalable AMPs and underscores the need for further research on their implications for air quality, climate, and human health. ENVIRONMENTAL IMPLICATION: Our findings provide direct evidence that airborne microplastics are not only an urban pollutant but also part of a global transport cycle, with their abundance strongly modulated by meteorology and resuspension from contaminated environments. This highlights the need to consider AMPs in assessments of air quality, climate interactions, and the redistribution of plastic pollution across environmental compartments. By quantifying inhalable fractions and demonstrating their environmental aging, this study offers a foundation for future work linking airborne microplastics to health risks, climate forcing, and feedback with terrestrial and aquatic systems.