Understanding the factors that affect spatial differences in PM2.5 composition is crucial for implementing emissions control and health policies. Although previous studies have explored modeling of spatial patterns as a tool to improve human exposure assessment, little work has employed a multivariate clustering approach to identify spatial patterns in particle composition. In this study, we used this approach to assess the spatial patterns of ambient PM2.5 elemental concentrations in Eastern Massachusetts in the United States. To distinguish one cluster of sites from another, we considered air pollution sources and geodemographic variables. We evaluated spatial patterns for 11 elemental components of ambient PM2.5, which included S, K, Ca, Fe, Zn, Cu, Ti, Al, Pb, V, and Ni. The analyses for S, Ca, Cu, Ti, Al, and Pb resulted in: 2 clusters for Fe, Zn, V, and Ni; 3 clusters; and for 12 clusters for K. Overall, our findings suggest substantial variation of clusters among PM2.5 components. In addition, land use, population density, and daily traffic were used as variables to more effectively characterize clusters of sites. We used R2 values to estimate the effectiveness of each variable in characterizing clusters. Larger R2 values indicate better the discrimination among the sites. For example, population density had the highest R2 value when the analysis was performed for S, Ca, Zn, Ti, Al, Pb, and V; land use presented the highest R2 value for Cu, V, and Ni; and, traffic showed the highest R2 value for PM2.5 mass concentration. This study improves the ability to model both the between- and within-area variability of source emissions and pollution regime, using concentrations of PM2.5 components.

In order to exhaustively investigate the physical and chemical mechanisms of heavy metal immobilization in sludge incineration residue (SIR)-based magnesium potassium phosphate cement (MKPC), this work investigated the influence of Pb²⁺ and Zn²⁺ on the compressive strength and microstructure of SIR-based MKPC, and the efficiency of Pb and Zn immobilization. Taking the difference of Ksp (solubility product) of different heavy metal compounds as the entry point, the physical and chemical mechanisms of Pb and Zn immobilization, and the competitive mechanism between coexisting ions, were comprehensively analyzed. It was discovered that Pb²⁺ is in the form Pb₃(PO₄)₂, and Zn²⁺ is immobilized in the form Zn₂(OH)PO₄ [Zn₃(PO₄)₂ is preferentially formed, when the pH > 7, Zn₃(PO₄)₂ is converted to Zn₂(OH)PO₄]. The low solubility of heavy metal phosphates is the main reason that Pb²⁺ and Zn²⁺ are well immobilized. The preferential formation of Pb₃(PO₄)₂ (Kₛₚ = 8 × 10⁻⁴³) and Zn₃(PO₄)₂ (Kₛₚ = 9.0 × 10⁻³³) reduced the amount of MgKPO₄·6H₂O (Kₛₚ = 2.4 × 10⁻¹¹), resulting in a decrease in compressive strength. Besides, coexisting Pb²⁺ and Zn²⁺ has a competitive effect: Pb²⁺ will weaken the immobilization efficiency of Zn²⁺. The new exploration of these mechanisms provide a theoretical basis for rationally adjusting the Magnesia/Phosphate ratio to enhance the compressive strength and improve the efficiency of heavy metals immobilization.

Current-use pesticides (CUPs) are widely applied in agriculture; however, little is known about their environmental behaviors, especially in the freshwater–seawater transitional zone. Water and sediment samples were collected in an intensively human impacted river (Xiaoqing River) from the headwaters to Laizhou Bay to investigate the distributions and environmental fates of four CUPs: trifluralin, chlorothalonil, chlorpyrifos, and dicofol. These CUPs were frequently detected in water and sediment samples. ∑CUPs in water and sediment samples ranged from 1.20 to 100.2 ng L⁻¹ and 6.6–2972.5 ng g⁻¹ dry weight (dw), respectively. Chlorpyrifos and chlorothalonil were the most abundant CUPs in water and sediment samples, respectively. Spatial distribution of CUPs in the Xiaoqing River aquatic ecosystem was mainly influenced by point sources, agricultural activities, the dilution effect by seawater, and environmental parameters. Field-based sediment water partitioning coefficients, normalized by organic carbon (log Koc), were calculated. Interestingly, temperature and salinity exhibited significant impacts on the distribution of log Koc of the four CUPs. The effect of temperature on the distribution of log Koc of the four CUPs varied between the CUPs. In most water samples, the levels of chlorpyrifos exceed the freshwater screening benchmarks. Hence, urgent control measures need to be devised and implemented.

Decabromodiphenyl ethane (DBDPE) is an alternative to the commercial decabromodiphenyl ether (deca-BDE) mixture but has potentially similar persistence, bioaccumulation potential and toxicity. While it is widely used as a flame retardant in electrical and electronic equipment (EEE) in China, DBDPE could be distributed globally on a large scale with the international trade of EEE emanating from China. Here, we performed a dynamic substance flow analysis to estimate the time-dependent mass flows, stocks and emissions of DBDPE in China, and the global spread of DBDPE originating in China through the international trade of EEE and e-waste. Our analysis indicates that, between 2006 and 2016, ∼230 thousand tonnes (kt) of DBDPE were produced in China; production, use and disposal activities led to the release of 196 tonnes of DBDPE to the environment. By the end of 2016, ∼152 kt of the DBDPE produced resided in in-use products across China. During the period 2000–2016, ∼39 kt of DBDPE were exported from China in EEE products, most of which (>50%) ended up in North America. Based on projected trends of China's DBDPE production, use and EEE exports, we predict that, by 2026, ∼74 and ∼14 kt of DBDPE originating in China will reside in in-use and waste stocks, respectively, in regions other than mainland China, which will act as long-term emission sources of DBDPE worldwide. This study discusses the considerable impact of DBDPE originating in China and distributed globally through the international trade of EEE; this is projected to occur on a large scale in the near future, which necessitates countermeasures.

Localised sites in Antarctica are contaminated with mixtures of metals, yet the risk this contamination poses to the marine ecosystem is not well characterised. Recent research showed that two Antarctic marine microalgae have antagonistic responses to a mixture of five common metals (Koppel et al., 2018a). However, the metal accumulating potential and risk to secondary consumers through dietary exposure are still unknown. This study investigates cellular accumulation following exposure to a mixture of cadmium, copper, nickel, lead, and zinc for the Antarctic marine microalgae, Phaeocystis antarctica and Cryothecomonas armigera. In both microalgae, cellular cadmium, copper, and lead concentrations increased with increasing exposures while cellular nickel and zinc did not. For both microalgae, copper in the metal mixture drives inhibition of growth rate with R2 values > -0.84 for all cellular fractions in both species and the observed antagonism was likely caused by zinc competition, having significantly positive partial regressions. Metal accumulation to P. antarctica and C. armigera is likely to be toxic to consumer organisms, with low exposure concentrations resulting in cellular concentrations of 500 and 1400 × 10−18 mol Zn cell−1 and 160 and 320 × 10−18 mol Cu cell−1, respectively.

Current air quality models usually underestimate the concentration of ambient air sulfate, but the cause of this underestimation remains unclear. One reason for the underestimation is that the sulfate formation mechanism in the models is incomplete, and does not adequately consider the impact of the synergistic effects of high concentrations of multiple pollutants on sulfate formation. In this work, the roles of gaseous NO₂, NH₃ and solution ionic strength in the formation of sulfate in the aqueous phase were quantitatively investigated using a glass reactor and a 30 m³ smog chamber, separately. The results showed that sulfate formation was enhanced to different degrees in the presence of gas-phase NO₂, NH₃ and their coexistence as solutes in both liquid solution and aerosol water. NH₃ enhances the aqueous oxidation of SO₂ by NO₂ mainly by accelerating the uptake of SO₂ through increased solubility. More importantly, we found that high ionic strength in aerosol water could significantly accelerate the aqueous oxidation of SO₂, resulting in unexpectedly high S(VI) formation rates. We estimate that under severe haze conditions, heterogeneous oxidation of SO₂ by NO₂ on aerosols may be much shorter than that through gas phase oxidation by OH, aided by high ionic strengths in aerosols. Considering the existence of complex air pollution conditions with high concentrations of NO₂, NH₃ and aerosol water, as expected in typical urban and suburban settings, the sulfate formation mechanisms revealed in the present work should be incorporated into air quality models to improve the prediction of sulfate concentrations.

The nanoscale size of plastic debris makes them potential efficient vectors of many pollutants and more especially of metals. In order to evaluate this ability, nanoplastics were produced from microplastics collected on a beach exposed to the North Atlantic Gyre. The nanoplastics were characterized using multi-dimensional methods: asymmetrical flow field flow fractionation and dynamic light scattering coupled to several detectors. Lead (II) adsorption kinetics, isotherm and pH-edge were then carried out. The sorption reached a steady state after around 200 min. The maximum sorption capacity varied between 97% and 78.5% for both tested Pb concentrations. Lead (II) adsorption kinetics is controlled by chemical reactions with the nanoplastics surface and to a lesser extent by intraparticle diffusion. Adsorption isotherm modeling using Freundlich model demonstrated that NPG are strong adsorbents equivalent to hydrous ferric oxides such as ferrihydrite (log Kadsfreundlich=8.36 against 11.76 for NPG and ferrihydrite, respectively). The adsorption is dependent upon pH, in response to the Pb(II) adsorption by the oxygenated binding sites developed on account of the surface UV oxidation under environmental conditions. They could be able to compete with Fe or humic colloids for Pb binding regards to their amount and specific areas. Nanoplastics could therefore be efficient vectors of Pb and probably of many other metals as well in the environment.

In this study, a series of BUC-21/titanate nanotube (BT-X) composites were facilely fabricated via ball-milling of 2-dimensional (2D) metal-organic framework (MOF) BUC-21 and titanate nanotubes (TNTs). The BT-X composites were characterized by powder X-ray diffraction (PXRD), Fourier transform infrared spectroscopy (FTIR), transmission electron microscopy (TEM), UV–visible diffuse-reflectance spectroscopy (UV–vis DRS), X-ray photoelectron spectrometer (XPS) and high resolution transmission electron microscopy (HRTEM). Both the photocatalytic reduction from Cr(VI) to Cr(III) and adsorptive removal of formed Cr(III) of BT-X composites were systematically investigated under different conditions including pH values and co-existing inorganic ions. It was found that BUC-21 (100 mg)/TNTs (100 mg) (BT-1) composites demonstrate remarkable ability of photocatalytic Cr(VI) reduction and adsorptive Cr(III) removal, as well as good reusability and stability. It is believed that the introduction of TNTs could capture the formed Cr(III) from the surface of BUC-21, which provided more active sites exposed to enhance the Cr(VI) reduction.

To mitigate severe wintertime pollution events in Western China, identifying the source of atmospheric fine particles with an aerodynamic diameter of ≤2.5 μm (PM2.5) is a crucial step. In this study, we first analyzed the meteorological and emission factors that caused a considerable increase in the PM2.5 concentration in December 2016. This severe pollution episode was found to be related with unfavorable meteorological conditions and increased residential emissions. The WRF-Chem simulations were used to calculate the residential contribution to PM2.5 through a hybrid source apportionment method. From the validation that used grid data and in situ observations in terms of meteorological elements, PM2.5 and its compounds, the simulated results indicated that the residential sector was the largest single contributor to the PM2.5 concentration (60.2%), because of its predominant contributions to black carbon (BC, 62.1%) and primary organic aerosol (POA, 86.5%), with these two primary components accounting for 70.7% of the PM2.5 mass. Compared with the remote background (RB) region covering the central part of the Tibetan Plateau, the residential sector contributed 11.3% more to PM2.5 in the highly populated mega-city (HM) region, including the Sichuan and Guanzhong Basins, due to greater contribution to the concentrations of primary PM2.5 components. As the main emission source of sulfur dioxide (SO2), nitrogen oxides (NOx), and secondary organic aerosol (SOA), the industrial sector was the second largest contributor to the PM2.5 concentration in the HM region. However, in the RB region, the dominating emissions of NOx, SOA, and BC were from the transport sector; thus, it was the next largest contributor to total PM2.5. An evaluation of the emission control experiment suggested that mitigation strategies that reduce emissions from residential sources can effectively reduce the PM2.5 concentration during heavy pollution periods.

Schwertmannite (SCH) has strong adsorption ability to As(III). However, there are few reports on the stability of SCH load with As(III) (SCH-As(III)). In this study, the effects of tartaric acid (TA), pH and coexisting ions including K+, Ca2+, Al3+ and CO32− on the photoreductive dissolution of SCH- As(III) and the release of the adsorbed As (III) were investigated. The results showed that under UV irradiation TA could greatly enhance the release of total Fe and total As from SCH-As(III). Nevertheless, the total Fe and total As in the solution decreased when TA was consumed up. Compared to SCH, the reductive dissolution of SCH-As(III) was obviously suppressed. In the dark, TA could slowly enhance the dissolution of SCH-As(III), but its effect on the release of adsorbed As(III) was weak. Low pH was conducive to the release of iron and arsenic. Ca2+, K+, and CO32− promoted the decrease of the dissolved total Fe in the later reaction. However, Al3+ inhibited the decrease of the dissolved total Fe and total As. The analyses of FTIR and XRD demonstrated that the mineralogical phase of SCH-As(III) after reaction changed. With light, the dissolved total Fe and total As existed mainly as Fe(II) and As(V), respectively. This is because Fe(II) was generated via ligand to metal charge transfer and As(III) was oxidized to As(V) by ·OH produced during the reaction. Thus, this study provides us with a comprehensive understanding of the stability of SCH-As(III) and the release of adsorbed As(III) in natural environments.