中国主要背景区域冬季大气PM2.5中非极性有机化合物组成及来源解析

本研究于2019年12月至2020年1月在5个区域大气本底站：临安、金沙、龙凤山、上甸子和瓦里关,同步采集了PM_2.5样品,分析了其中的非极性有机物：多环芳烃、正构烷烃和藿烷类化合物。结果表明,上甸子和龙凤山的多环芳烃平均浓度显著高于其他站点,分别为35.2±25.6 ng/m³和27.5±16.8 ng/m³;藿烷类物质的浓度在上甸子和临安出现高值,分别为2.72±1.78 ng/m³和2.47±0.990 ng/m³;正构烷烃浓度以临安最高,为86.7±40.6 ng/m³。对各站点多环芳烃和藿烷类化合物采用比值法,正构烷烃采用主峰碳数（C_max）、碳优势指数（carbon preference index,CPI）和植物蜡贡献率（% Wax C_n）,结合主成分分析-多元线性回归模型（PCA/MLR）综合进行源解析。结果显示采样期间除瓦里关外,其余站点燃烧源均以化石燃料源为主,贡献率分别为临安（94.9%） > 金沙（75.3%） > 龙凤山（74.7%） > 上甸子（62.5%） > 瓦里关（35.6%）。后向轨迹聚类分析（HYSPLIT）和潜在源贡献因子分析法（PSCF）表明各站点主要受到外来传输气团的影响,并查明了各站点的潜在污染源区。对背景站点的研究表明,东北地区和京津冀地区PM_2.5中非极性有机物来源相似,京津冀地区的生物质燃烧源贡献率高于东北地区;长江中下游地区化石燃料贡献率显著高于生物质燃烧;华中地区燃煤和交通排放源排放贡献率均低于长江三角洲地区;青藏高原地区生物质燃烧贡献率远高于其他地区。     

Cross-boundary transport and source apportionment for PM2.5 in a typical industrial city in the Hebei Province, China: A modeling study

Cross-boundary transport of air pollution is a difficult issue in pollution control for the North China Plain. In this study, an industrial district (Shahe City) with a large glass manufacturing sector was investigated to clarify the relative contribution of fine particulate matter (PM_2.5) to the city's high levels of pollution. The Nest Air Quality Prediction Model System (NAQPMS), paired with Weather Research and Forecasting (WRF), was adopted and applied with a spatial resolution of 5 km. During the study period, the mean mass concentrations of PM_2.5, SO₂, and NO₂ were observed to be 132.0, 76.1, and 55.5 μg/m³, respectively. The model reproduced the variations in pollutant concentrations in Shahe at an acceptable level. The simulation of online source-tagging revealed that pollutants emitted within a 50-km radius of downtown Shahe contributed 63.4% of the city's total PM_2.5 concentration. This contribution increased to 73.9±21.2% when unfavorable meteorological conditions (high relative humidity, weak wind, and low planetary boundary layer height) were present; such conditions are more frequently associated with severe pollution (PM_2.5 ≥ 250 μg/m³). The contribution from Shahe was 52.3±21.6%. The source apportionment results showed that industry (47%), transportation (10%), power (17%), and residential (26%) sectors were the most important sources of PM_2.5 in Shahe. The glass factories (where chimney stack heights were normally < 70 m) in Shahe contributed 32.1% of the total PM_2.5 concentration in Shahe. With an increase in PM_2.5 concentration, the emissions from glass factories accumulated vertically and narrowed horizontally. At times when pollution levels were severe, the horizontally influenced area mainly covered Shahe. Furthermore, sensitivity tests indicated that reducing emissions by 20%, 40%, and 60% could lead to a decrease in the mass concentration of PM_2.5 of of 12.0%, 23.8%, and 35.5%, respectively.     

Urinary concentrations of phenols, oxidative stress biomarkers and thyroid cancer: Exploring associations and mediation effects

Phenols have been shown to influence the cellular proliferation and function of thyroid in experimental models. However, few human studies have investigated the association between phenol exposure and thyroid cancer, and the underlying mechanisms are also poorly understood. We conducted a case-control study by age- and sex-matching 143 thyroid cancer and 224 controls to investigate the associations between phenol exposures and the risk of thyroid cancer, and further to explore the mediating role of oxidative stress. We found that elevated urinary triclosan (TCS), bisphenol A (BPA) and bisphenol S (BPS) levels were associated with increased risk of thyroid cancer (all P for trends < 0.05), and the adjusted odds ratios (ORs) comparing the extreme exposure groups were 3.52 (95% confidence interval (CI): 2.08, 5.95), 2.06 (95% CI: 1.06, 3.97) and 7.15 (95% CI: 3.12, 16.40), respectively. Positive associations were also observed between urinary TCS, BPA and BPS and three oxidative stress biomarkers measured by 8-hydroxy-2′-deoxyguanosine (8-OHdG), 8-iso-prostaglandin F_2α (8-isoPGF_2α) and 4-hydroxy-2-nonenal-mercapturic acid (HNE-MA), as well as between urinary 8-isoPGF_2α and HNE-MA and the risk of thyroid cancer. Mediation analysis showed that urinary 8-isoPGF_2α mediated 28.95%, 47.06% and 31.08% of the associations between TCS, BPA and BPS exposures and the risk of thyroid cancer, respectively (all P < 0.05). Our results suggest that exposure to TCS, BPA and BPS may be associated with increased risk of thyroid cancer and lipid peroxidation may be an intermediate mechanism. Further studies are warranted to confirm the findings.     

Destructing surfactant network in nanoemulsions by positively charged magnetic nanorods to enhance oil-water separation

The separation of ultrafine oil droplets from wasted nanoemulsions stabilized with high concentration of surfactants is precondition for oil reuse and the safe discharge of effluent. However, the double barriers of the interfacial film and network structures formed by surfactants in nanoemulsions significantly impede the oil-water separation. To destroy these surfactant protective layers, we proposed a newly-developed polyethyleneimine micelle template approach to achieve simultaneous surface charge manipulation and morphology transformation of magnetic nanospheres to magnetic nanorods. The results revealed that positively charged magnetic nanospheres exhibited limited separation performance of nanoemulsions, with a maximum chemical oxygen demand (COD) removal of 50%, whereas magnetic nanorods achieved more than 95% COD removal in less than 30 s. The magnetic nanorods were also applicable to wasted nanoemulsions from different sources and exhibited excellent resistance to wide pH changes. Owing to their unique one-dimensional structure, the interfacial dispersion of magnetic nanorods was significantly promoted, leading to the efficient capture of surfactants and widespread destruction of both the interfacial film and network structure, which facilitated droplet merging into the oil phase. The easy-to-prepare and easy-to-tune strategy in this study paves a feasible avenue to simultaneously tailor surface charge and morphology of magnetic nanoparticles, and reveals the huge potential of morphology manipulation for producing high-performance nanomaterials to be applied in complex interfacial interaction process. We believe that the newly-developed magnetic-nanorods significantly contribute to hazardous oily waste remediation and advances technology evolution toward problematic oil-pollution control.     

Fine particulate matter (PM2.5/PM1.0) in Beijing, China: Variations and chemical compositions as well as sources

Particulate matter (i.e., PM_1.0 and PM_2.5), considered as the key atmospheric pollutants, exerts negative effects on visibility, global climate, and human health by associated chemical compositions. However, our understanding of PM and its chemical compositions in Beijing under the current atmospheric environment is still not complete after witnessing marked alleviation during 2013–2017. Continuous measurements can be crucial for further air quality improvement by better characterizing PM pollution and chemical compositions in Beijing. Here, we conducted simultaneous measurements on PM in Beijing during 2018–2019. Results indicate that annual mean PM_1.0 and PM_2.5 concentrations were 35.49 ± 18.61 µg/m³ and 66.58 ± 60.17 µg/m³, showing a positive response to emission controls. The contribution of sulfate, nitrate, and ammonium (SNA) played an enhanced role with elevated PM loading and acted as the main contributors to pollution episodes. Discrepancies observed among chemical species between PM_1.0 and PM_2.5 in spring suggest that sand particles trend to accumulate in the range of 1–2.5 µm. Pollution episodes occurred accompanied with southerly clusters and high formation of SNA by heterogeneous reactions in summer and winter, respectively. Results from positive matrix factorization (PMF) combined with potential source contribution function (PSCF) models showed that potential areas were seasonal dependent, secondary and vehicular sources became much more important compared with previous studies in Beijing. Our study presented a continuous investigation on PM and sources origins in Beijing, which provides a better understanding for further emission control as well as a reference for other cities in developing countries.     

AP9/AE9/SPM辐射环境模型研究

对辐射环境模型AP9/AE9/SPM进行了系统研究,重点分析了AP9/AE9/SPM辐射环境模型的发展历程、建模数据、模型能力、模型使用方法、模型特点和局限性以及发展趋势。总结了AP9/AE9/SPM辐射环境模型“螺旋式上升”研发途径中所发布的11个版本的特点、数据覆盖时间范围和能量范围。指出AP9/AE9/SPM辐射环境模型在研发过程中是通过不断地将最新的观测数据和理论知识进行整合,达到扩展模型能量覆盖范围、增加空间粒子分布的目的。最新的AP9/AE9/SPM辐射环境模型具备了命令行和图形用户接口应用程序2种灵活便捷的使用方式,能覆盖完整的辐射带空间,基本实现了电子和质子能量范围的全覆盖。但目前最新版本的AP9/AE9/SPM仍然存在一些局限,这些局限会随着辐射带探测数据的积累和人类对辐射带机理的进一步认知而逐渐得到改善。该研究可帮助用户快速了解并正确使用AP9/AE9/SPM辐射环境模型,为我国自主辐射环境模型研发提供重要参考。     

Highly Oriented Thermoplastic Poly (vinyl alcohol) Films by Uniaxial Drawing: Effect of Stretching Temperature and Draw Ratio

Journal of Polymers and the Environment - With the advantages of excellent processability and biodegradability, polyvinyl alcohol (PVA) becomes an environmentally friendly and biocompatible...     

An antifouling catechol/chitosan-modified polyvinylidene fluoride membrane for sustainable oil-in-water emulsions separation

• Underwater superoleophobic membrane was fabricated by deposition of catechol/chitosan. • The membrane had ultrahigh pure water flux and was stable under harsh pH conditions. • The membrane exhibited remarkable antifouling property in O/W emulsion separation. • The hydration layer on the membrane surface prevented oil droplets adhesion. Low-pressure membrane filtrations are considered as effective technologies for sustainable oil/water separation. However, conventional membranes usually suffer from severe pore clogging and surface fouling, and thus, novel membranes with superior wettability and antifouling features are urgently required. Herein, we report a facile green approach for the development of an underwater superoleophobic microfiltration membrane via one-step oxidant-induced ultrafast co-deposition of naturally available catechol/chitosan on a porous polyvinylidene fluoride (PVDF) substrate. Membrane morphology and surface chemistry were studied using a series of characterization techniques. The as-prepared membrane retained the original pore structure due to the ultrathin and uniform catechol/chitosan coating. It exhibited ultrahigh pure water permeability and robust chemical stability under harsh pH conditions. Moreover, the catechol/chitosan hydrophilic coating on the membrane surface acting as an energetic barrier for oil droplets could minimize oil adhesion on the surface, which endowed the membrane with remarkable antifouling property and reusability in a cyclic oil-in-water (O/W) emulsion separation. The modified membrane exhibited a competitive flux of ~428 L/(m²·h·bar) after three filtration cycles, which was 70% higher than that of the pristine PVDF membrane. These results suggest that the novel underwater superoleophobic membrane can potentially be used for sustainable O/W emulsions separation, and the proposed green facile modification approach can also be applied to other water-remediation materials considering its low cost and simplicity.