Surface wettability control and electron transport regulation in zerovalent iron for enhanced removal of emerging polystyrene microplastics-heavy metal contaminants.

Emerging microplastics-heavy metal (MPs-HM) contaminants in wastewaters pose an emerging health and environmental risk due to their persistence and increasing ecological risks (e.g., "Trojan horse" effect). Hence, removing MPs in solution and preventing secondary releases of HM has become a key challenge when tackling with MPs pollution. Leveraging the hydrophobic nature of MPs and the electron transfer efficiency from Fe0 to HM, we demonstrate an alkylated and sulfidated nanoscale zerovalent iron (AS-nZVI) featuring a delicate "core-shell-hydrophobic film" nanostructure. Exemplified by polystyrene (PS) MPs-Pb(II) removal, the three nanocomponents offer synergistic functions for the rapid separation of MPs, as well as the reduction and stabilization of Pb(II). The outmost hydrophobic film of AS-nZVI greatly improves the anticorrosion performance of nanoscale zerovalent iron and the enrichment abilities of hydrophobic MPs, achieving a maximum removal capacity of MPs to 2725.87 mgMPs·gFe-1. This MPs enrichment promotes the subsequent reductive removal of Pb(II) through the electron transfer from the iron core of AS-nZVI to Pb(II), a process further strengthened by the introduced sulfur. When considering the inevitable aging of MPs in wastewaters due to mechanical wear or microbial degradation, our study concurrently examines the efficiencies and behaviors of AS-nZVI in removing virgin-MPs-Pb(II) and aged-MPs-Pb(II). The batch results reveal that AS-nZVI has an exceptional ability to remove above 99.6 % Pb(II) for all reaction systems. Overall, this work marks a pioneering effort in highlighting the importance of MPs-toxin combinations in dealing with MPs contamination and in demonstrating the utility of nZVI techniques for MPs-contaminated water purification.

Evaluating the impacts of burning biomass on PM2.5 regional transport under various emission conditions.

The fine particulate matter (PM2.5) emitted by burning biomass has become the main source of pollution in cities; this pollution seriously threatens the ecosystem and inhabitants' health. A major challenge in dealing with this issue is the uncertainty regarding the influence of burning biomass on PM2.5 regional transport. In this study, Harbin-Changchun Megalopolis is the research area. Using the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model combined with satellite data and PM2.5 monitoring data, we quantitatively analyzed the regional transport of PM2.5 from burning biomass upwind of each city under different emission conditions. Conditions at burn sites, especially emission intensity and meteorological factors, as well as transport distance play significant roles in the regional transport of PM2.5. Higher emission intensity aggravated the concentration of downwind PM2.5, at most 19.7 µg ⋅ m-3. Shorter transport distance strengthened the impact of biomass burning on downstream PM2.5 by weakening elimination, which could be up to 96.8 µg ⋅ m-3. Moreover, meteorological factors at fire points were closely related to the transport of PM2.5. First, lower planetary boundary layer height could enhance the transport of PM2.5 from the burning biomass by inhibiting vertical diffusion, and the enhancement could be up to 46.1 µg ⋅ m-3. Second, compared to strong wind, light wind caused the weaker dilution, enhancing PM2.5 regional transport by as much as 32.5 µg ⋅ m-3. Third, relatively humidity at 30%-40% had the strongest effect in facilitating the transport of PM2.5 from burning biomass. We conclude that comprehensively considering these three factors, namely the emission intensity, transport distance and meteorological factors at burn sites can facilitate the cross-regional development of accurate prediction models and effective pollution control measures.

Probing the dynamic characteristics of aerosol originated from South Asia biomass burning using POLDER/GRASP satellite data with relevant accessory technique design.

The dynamic characteristics of biomass burning aerosol originated from South Asia are investigated in this research using nearly 9 years of POLDER/GRASP satellite aerosol dataset. The POLDER/GRASP remote sensing data can provide global, repeatable, various, and sufficient real-world aerosol information even in the remote ocean region, which can't be offered by the ground measurement, laboratory observation or model simulation. The MODIS thermal anomalies/fire dataset and HYSPLIT backward trajectory are applied to search the aerosol originated from South Asia biomass burning. The biomass burning aerosol originated from South Asia could transport to and influence the north part of Indian Ocean (including Bay of Bengal and Arabian Sea), the north part of Indo-China Peninsula, South China, and even far to the Pacific Ocean (including part of East China Sea and South China Sea). The chemical, physical and optical characteristics of biomass burning aerosol over land and over ocean show different features and evolution patterns. Such difference is caused by the different ambient environment and different mixed aerosol during the transport process (urban/industrial aerosol over land and sea salt over ocean). During the 48-hours aging process, the volume fraction of black carbon, AAOD and Angstrom Exponent decrease. Meanwhile, the aerosol sphere fraction and SSA increase. The biomass burning aerosol over land shows a more obvious evolution trend than that over ocean. The biomass burning aerosol over ocean generally have higher SSA and lower volume fraction of black carbon, aerosol sphere fraction, AAOD and Angstrom Exponent. The aerosol radiative forcing efficiency also varies between land and ocean, due to their different features of aerosol and surface properties. In general, a negative clear-sky aerosol radiative forcing efficiency (cooling effect) at the TOA is observed. The aerosol cooling effect at the TOA over ocean (-82 W/m2 on average) is much stronger than that over land (-36 W/m2 on average). During the 48-hours aging process, a significant enhancement of the negative radiative forcing efficiency at the TOA is found over land. Over ocean, the enhancement of the negative radiative forcing efficiency at the TOA is weaker.

The role of biomass burning states in light absorption enhancement of carbonaceous aerosols.

Carbonaceous aerosols, which are emitted from biomass burning, significantly contribute to the Earth's radiation balance. Radiative forcing caused by biomass burning has been poorly qualified, which is largely attributed to uncertain absorption enhancement values (Eabs) of black carbon (BC) aerosols. Laboratory measurements and theoretical modelling indicate a significant value of Eabs; but this enhancement is observed to be negligible in the ambient environment, implying that models may overestimate global warming due to BC. Here, we present an aggregate model integrating BC aerosol ensembles with different morphologies and mixing states and report a quantitative analysis of the BC Eabs from different combustion states during biomass burning. We show that the BC Eabs produced by flaming combustion may be up to two times more than those produced by smouldering combustion, suggesting that the particle morphology and mixing state of freshly emitted BC aerosols is an important source of the contrasting values of Eabs. The particle morphology of freshly emitted BC aerosols is widely assumed to be bare in models, which is rare in the ambient environment and leads to small estimates of Eabs by field observations. We conclude that the exact description of freshly emitted carbonaceous aerosols plays an important role in constraining aerosol radiative forcing.

Study on the characteristics of black carbon during atmospheric pollution conditions in Beijing.

Black carbon (BC), not only has a negative impact on human health, but also contributes to visibility degradation and the attenuation of solar radiation due to light absorption. In this paper, we investigated the variations of BC concentration, BC optical characteristics and its effects on the physical and optical properties of atmospheric aerosols based on AERONET data during atmospheric pollution conditions in Beijing from 2012 to 2017. The results indicated that the average annual ground-level BC concentration and BC/PM2.5 were 8.9 µg m-3 and 6.7%, respectively, from 2012 to 2017 during atmospheric pollution conditions in Beijing. The annual mean ground-level BC concentration showed weak variation, but the monthly variation was pronounced during atmospheric pollution conditions. Moreover, the BC column concentration had a higher correlation with absorptive aerosol optical thickness (AAOT) at 870 nm (R2 = 0.93) than 440 nm (R2 = 0.73). The difference in AAOT between 440 nm and 870 nm was more significant under high BC column concentration. The seasonal variation of the BC column concentration that contributed to the AAOT at 870 nm displayed a consistent monthly average variation tendency. The BC column concentrations were divided into three segments of low, moderate, and high according to the results of the approximately normal distribution of the BC column concentration. Compared with high BC concentration, the single scattering albedo (SSA) and asymmetry parameter were enhanced by 0.05 and 0.04 in low BC concentrations, respectively. On the contrary, the fine mode fraction (FMF) was dropped by 12.5% in low BC concentrations. A higher BC concentration contributed to the enhancement in the AAOT and the extinction ratio of the fine mode aerosol. Meanwhile, the atmospheric particles' forward scattering ability was also attenuated under a high BC concentration.

Spatial and temporal variations of air quality and six air pollutants in China during 2015-2017.

Air pollution has aroused significant public concern in China, therefore, long-term air-quality data with high temporal and spatial resolution are needed to understand the variations of air pollution in China. However, the yearly variations with high spatial resolution of air quality and six air pollutants are still unknown for China until now. Therefore, in this paper, we analyze the spatial and temporal variations of air quality and six air pollutants in 366 cities across mainland China during 2015-2017 for the first time to the best of our knowledge. The results indicate that the annual mean mass concentrations of PM2.5, PM10, SO2, and CO all decreased year by year during 2015-2017. However, the annual mean NO2 concentrations were almost unchanged, while the annual mean O3 concentrations increased year by year. Anthropogenic factors were mainly responsible for the variations of air quality. Further analysis suggested that PM2.5 and PM10 were the main factors influencing air quality, while NO2 played an important role in the formation of PM2.5 and O3. These findings can provide a theoretical basis for the formulation of future air-pollution control policy in China.

Biomass burning aerosol characteristics for different vegetation types in different aging periods.

Eighteen years of sun/sky photometer measurements at seven worldwide AErosol RObotic NETwork (AERONET) sites in typical biomass burning regions were used in this research. The AERONET measurements were analyzed with the help of Moderate-resolution Imaging Spectroradiometer (MODIS) fire products and the HYbrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model. The variation in the physicochemical and optical properties of biomass burning aerosols (BBAs), as well as their shortwave radiative forcing, was revealed for different vegetation types in different aging periods. The result indicated that, with aerosol aging, the BBA characteristics have a non-negligible evolution trend with obvious clustering features for different burning vegetation types. During the aging process, the volume fraction of black carbon (BC) declined (with a maximum drop of 38%) accompanied by particle size growth (with a maximum increment of 0.017 µm). Driven by the change in physicochemical properties, the Single Scattering Albedo (SSA) and the asymmetry factor increased as the aerosol aged (with maximum increments of 0.026 and 0.018 for the SSA and asymmetry factor respectively). The grass and shrub type had a higher volume fraction of BC (2.5 times higher than that in the forest and peat type) and a smaller fine mode volume median radius (with a difference of 0.037 µm from that of the forest and peat type). Such a phenomenon results in a lower SSA (with a difference of 0.103) and asymmetry factor (with a difference of 0.035) in the grass and shrub type when compared to the forest and peat type. Negative (-74 to -30 W/m2) clear-sky top of atmosphere (TOA) shortwave radiative forcing, strengthened during the aging process, was generally found for BBA. The BBA in the forest and peat region usually had stronger negative radiative forcing efficiency.

Contribution of meteorological factors to particulate pollution during winters in Beijing.

Associated with its modernization, Beijing has experienced significant fine particulate matter (PM2.5) pollution, especially in winter. In 2016, severe PM2.5 pollution (PM2.5 > 250 µg/m3) lasted over 6 days and affected over 23 million people. A major challenge in dealing with this issue is the uncertainty regarding the influence of individual meteorological factors to the overall PM2.5 concentration in Beijing. Thus, applying an empirical regression method to long-term ground-based PM2.5 data and meteorological sounding measurements, we attempted to analyze the influence of individual meteorological factors on PM2.5 pollution during winters in Beijing. We found that horizontal dilution and vertical aggregation plays a major role in PM2.5 pollution during the winter of 2016. The impact of horizontal wind on PM2.5 concentration in Beijing was mainly from its dilution, the dilution of northerly wind contributed 27.8% in 2016, far below its contribution in 2015 (32.2%). The contribution from the growing vertical aggregation observed in 2016 was mainly the result of both the lower height of the planetary boundary layer and the greater depth of the temperature inversion. The dilution of the planetary boundary layer height contributed 9.8% to PM2.5 pollution in 2016, 5.4% lower than that in 2017. Compared with the temperature difference of the inversion layer, the temperature inversion depth better reflects the aggregated impact of temperature inversions to PM2.5, which was 10.9% in 2015, and the ratio rose to 14.3% in 2016. Relative humidity is also an important impacting factor, which contributed 41.0%, far higher than the ratio in 2017 (26.7%). Such results imply that we should focus on not only local emission control, but also horizontal atmospheric transport and meteorological conditions in order to provide a more accurate analysis of pollution mechanisms, conductive to air pollution governance in Beijing.

Assessing Spatial and Temporal Patterns of Observed Ground-level Ozone in China.

Elevated ground-level ozone (O3), which is an important aspect of air quality related to public health, has been causing increasing concern. This study investigated the spatiotemporal distribution of ground-level O3 concentrations in China using a dataset from the Chinese national air quality monitoring network during 2013-2015. This research analyzed the diurnal, monthly and yearly variation of O3 concentrations in both sparsely and densely populated regions. In particular, 6 major Chinese cities were selected to allow a discussion of variations in O3 levels in detail, Beijing, Chengdu, Guangzhou, Lanzhou, Shanghai, and Urumchi, located on both sides of the Heihe-Tengchong line. Data showed that the nationwide 3-year MDA8 of ground-level O3 was 80.26 µg/m3. Ground-level O3 concentrations exhibited monthly variability peaking in summer and reaching the lowest levels in winter. The diurnal cycle reached a minimum in morning and peaked in the afternoon. Yearly average O3 MDA8 concentrations in Beijing, Chengdu, Lanzhou, and Shanghai in 2015 increased 12%, 25%, 34%, 22%, respectively, when compared with those in 2013. Compared with World Health Organization O3 guidelines, Beijing, Chengdu, Guangzhou, and Shanghai suffered O3 pollution in excess of the 8-hour O3 standard for more than 30% of the days in 2013 to 2015.

Assessment of PM2.5 concentrations and exposure throughout China using ground observations.

Exposure to PM2.5 results in negative effects on human health. However, PM2.5 exposure at the national scale is poorly known for China owing to limited spatial and temporal PM2.5 concentration data. In this study, we present analyses of PM2.5 exposure throughout China using high-resolution temporal and spatial ground-level PM2.5 data from 2015. Our results indicated that the annual mean PM2.5 concentration was 52.81µg/m3, and that the highest annual mean PM2.5 concentrations primarily appeared in the North China Plain. We also found the lowest and highest monthly mean PM2.5 concentrations appeared in August and January, respectively, while the lowest and highest diurnal mean PM2.5 concentrations occurred at 16:00 and 10:00, respectively. Moreover, comparisons to data from 2013 indicated that the annual mean PM2.5 concentrations decreased by 12.31% from 2013 to 2015, which was likely due to the implementation of environmental protection laws in early 2015. Our findings provide new insights, for not only studies of PM2.5 exposure and human health, but also to inform the implementation of national and regional air pollution reduction policies.