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Activation of PAA at the Fe-Nx Sites by Boron Nitride Quantum Dots Enhanced Charge Transfer Generates High-Valent Metal-Oxo Species for Antibiotics Degradation. 氮化硼量子点增强电荷转移在 Fe-Nx 位激活 PAA,产生高价金属氧化物用于抗生素降解。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-28 DOI: 10.1021/acs.est.4c08224
Shuo Li, Yalun Yang, Junfeng Niu, Heshan Zheng, Wen Zhang, Yoong Kit Leong, Jo-Shu Chang, Bo Lai

Advanced oxidation processes (AOPs) based on peracetic acid (PAA) offer a promising strategy to address antibiotic wastewater pollution. In this study, Fe-doped graphitic carbon nitride (g-C3N4) nanomaterials were used to construct Fe-Nx sites, and the electronic structure was tuned by boron nitride quantum dots (BNQDs), thereby optimizing PAA activation for the degradation of antibiotics. The BNQDs-modified Fe-doped g-C3N4 catalyst (BNQDs-FCN) achieved an excellent reaction rate constant of 0.0843 min-1, marking a 21.6-fold improvement over the carbon nitride (CN)-based PAA system. DFT calculations further corroborate the superior adsorption capacity of the Fe-Nx sites for PAA, facilitating its activation. Charge transfer mechanisms, with PAA serving as an electron acceptor, were identified as the source of high-valent iron-oxo species. Moreover, the BNQDs-FCN system preferentially targets oxygen-containing functional groups in antibiotic structures, elucidating the selective attack patterns of these highly electrophilic species. This research not only elucidates the pivotal role of high-valent iron-oxo species in pollutant degradation within the PAA-AOPs framework but also pioneers a wastewater treatment system characterized by excellent degradation efficiency coupled with low ecological risk, thereby laying the groundwork for applications in wastewater management and beyond.

基于过乙酸(PAA)的高级氧化工艺(AOPs)为解决抗生素废水污染问题提供了一种前景广阔的策略。本研究利用掺杂铁的氮化石墨碳(g-C3N4)纳米材料构建铁-氮基点,并通过氮化硼量子点(BNQDs)调整其电子结构,从而优化了 PAA 对抗生素降解的活化作用。氮化硼量子点修饰的掺杂铁的 g-C3N4 催化剂(BNQDs-FCN)达到了 0.0843 min-1 的优异反应速率常数,比基于氮化碳(CN)的 PAA 系统提高了 21.6 倍。DFT 计算进一步证实,Fe-Nx 位点对 PAA 具有卓越的吸附能力,从而促进了 PAA 的活化。以 PAA 作为电子受体的电荷转移机制被确定为高价铁-氧物种的来源。此外,BNQDs-FCN 系统优先针对抗生素结构中的含氧官能团,阐明了这些高亲电性物种的选择性攻击模式。这项研究不仅在 PAA-AOPs 框架内阐明了高价铁氧物种在污染物降解中的关键作用,还开创了一种降解效率高、生态风险低的废水处理系统,从而为废水管理及其他领域的应用奠定了基础。
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引用次数: 0
High Viscosity and Two Phases Observed over a Range of Relative Humidities in Biomass Burning Organic Aerosol from Canadian Wildfires. 加拿大野火中生物质燃烧产生的有机气溶胶在一定相对湿度范围内观察到的高粘度和两相现象。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-28 DOI: 10.1021/acs.est.4c09148
Nealan G A Gerrebos, Julia Zaks, Florence K A Gregson, Max Walton-Raaby, Harrison Meeres, Ieva Zigg, Wesley F Zandberg, Allan K Bertram

Biomass burning organic aerosol (BBOA) is a major contributor to organic aerosol in the atmosphere. The impacts of BBOA on climate and health depend strongly upon their physicochemical properties, including viscosity and phase behavior (number and types of phases); these properties are not yet fully characterized. We collected BBOA field samples during the 2021 British Columbia wildfire season to constrain the viscosity and phase behavior at a range of relative humidities and compared them to previous studies on BBOA. Particles from all samples exhibited two-phased behavior with a polar hydrophilic phase and a nonpolar hydrophobic phase. We used the poke-flow viscosity technique to estimate the viscosity of the particles. Both phases of the BBOA had viscosities of >108 Pa s at relative humidities up to 50%. Such high viscosities correspond to mixing times within 200 nm BBOA particles of >5 h. Two phases and high viscosity have implications for how BBOA should be treated in atmospheric models.

生物质燃烧有机气溶胶(BBOA)是大气中有机气溶胶的主要来源。生物质燃烧有机气溶胶对气候和健康的影响在很大程度上取决于其物理化学特性,包括粘度和相态(相的数量和类型);这些特性尚未得到充分表征。我们在 2021 年不列颠哥伦比亚省野火季节期间采集了 BBOA 实地样本,以确定其在一系列相对湿度条件下的粘度和相行为,并将其与之前的 BBOA 研究进行比较。所有样本中的颗粒都表现出两相行为,即极性亲水相和非极性疏水相。我们使用戳流粘度技术来估算颗粒的粘度。当相对湿度达到 50%时,BBOA 的两相粘度都大于 108 Pa s。两相和高粘度对大气模型中如何处理 BBOA 产生了影响。
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引用次数: 0
Formation of Aromatic Halogenated Disinfection Byproducts in Swimming Pool Water during Chlorination: Organic Precursors and Mechanisms.
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-28 DOI: 10.1021/acs.est.4c08239
Junjie Wang, Hongyu Wu, Tao Ma, Haoran Chen, Chuze Chen, Yuting Wang, Qiming Xian, Tingting Gong

Disinfection byproducts (DBPs) in swimming pool water are a significant public health concern. The formation of aromatic halogenated DBPs in swimming pool water has not been clarified previously. In this study, the occurrence of aromatic halogenated DBPs in swimming pool water was examined, and it was found that halohydroxybenzoic acids (HBAs) and halobenzoquinones (HBQs) were the most dominant aromatic halogenated DBPs in swimming pool water that were continuously formed. Thus, the formation of HBAs and HBQs in swimming pool water from different organic precursors, including natural organic matter (NOM), pharmaceuticals and personal care products (PPCPs), during chlorination was examined. The results demonstrate that the formation of HBAs and HBQs from the PPCPs was relatively high compared with that from NOM, suggesting that the PPCPs from human inputs might be important organic precursors of aromatic halogenated DBPs in swimming pool water. The formation mechanisms of HBAs and HBQs from three typical PPCPs (benzophenone-3 (BP-3), methyl p-hydroxybenzoate (MeP) and carbamazepine) were further explored. The results show that the PPCPs containing phenolic groups with higher degradation rates (BP-3 and MeP) possessed higher formation of HBAs and HBQs. The three organic precursors underwent a series of substitution, hydrolysis, oxidation, rearrangement, and intramolecular cyclization reactions to form HBAs and HBQs, while the phenolic groups and ring structures may significantly affect the reactions. The chlorine dose, bromide/iodide concentration, and temperature significantly affected the formation of HBAs and HBQs from MeP during chlorination.

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引用次数: 0
Unraveling Potential Causative Components for the Deleterious Effect of Atmospheric Fine Particulate Matter on Red Blood Cells 揭示大气细颗粒物对红细胞产生有害影响的潜在致因成分
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-27 DOI: 10.1021/acs.est.4c06657
Yuzhu Zhang, Laijin Zhong, Jing Zhan, Zhipeng Yin, Yao Pei, Dong Cao, Qian S. Liu, Qunfang Zhou, Qian Liu, Guibin Jiang
Atmospheric fine particulate matter (PM2.5) poses threats to the cardiovascular system. Red blood cells (RBCs) are the most abundant cells in blood, which are actively involved in multiple hematological diseases, such as blood clot formation and thrombosis. Exploring how PM2.5 with spatiotemporal heterogeneity influences the hematological system by targeting RBCs would help gain insights into the deleterious effects of PM2.5 and provide clues for finding the causative components therein. Herein, the PM2.5 samples collected from 3 urban sites in Beijing (i.e., Chaoyang, Shunyi, and Yanqing districts) during 4 seasons of 2022 were studied for their toxicities to mouse RBCs, and the main contributing components were further explored through chemical analysis and correlation measure. The results showed that exposure to PM2.5 samples decreased adenosine triphosphate (ATP) levels and increased phosphatidylserine (PS) externalization of RBCs, causing cell morphological deformity. The Pearson correlation analysis showed that the aromaticity of the dissolved organic matter (DOM) in PM2.5 samples was positively correlated with PS exposure of RBCs, showing that the lignin-like compounds were the potential contributors. The negative correlation of zeta potentials of PM2.5 samples with PS exposure of RBCs showed the particle-derived bioactivities of this airborne pollutant. The simulative test based on artificial nanomaterials of carbon black (CB) and oxidized CB (OCB) confirmed the crucial role of particulate carbon in PM2.5-induced effects on RBCs, and soot with a certain oxidation degree was, thus, recognized as another contributor, given its ubiquitous existence in PM2.5 samples. This study, for the first time, revealed PM2.5-induced PS exposure of RBCs, and the causative components of DOM and soot were unraveled. Considering the inevitable contact of airborne PM2.5 with RBCs in the blood circulatory system, the findings obtained herein would help bridge the gap between PM2.5 exposure and the risk of cardiovascular diseases, like thrombogenesis.
大气中的细颗粒物(PM2.5)对心血管系统构成威胁。红细胞(RBC)是血液中含量最高的细胞,积极参与多种血液病的发生,如血凝块的形成和血栓的形成。探索具有时空异质性的 PM2.5 如何通过靶向红细胞影响血液系统,将有助于深入了解 PM2.5 的有害影响,并为找到其中的致病成分提供线索。本文研究了2022年4个季节在北京3个城市(朝阳区、顺义区和延庆区)采集的PM2.5样本对小鼠红细胞的毒性,并通过化学分析和相关测量进一步探讨了主要致病成分。结果表明,暴露于PM2.5样品会降低小鼠红细胞的三磷酸腺苷(ATP)水平,增加磷脂酰丝氨酸(PS)外化,导致细胞形态畸变。皮尔逊相关分析表明,PM2.5 样品中溶解有机物(DOM)的芳香度与 RBC 的 PS 暴露呈正相关,表明木质素类化合物是潜在的致病因素。PM2.5 样品的 zeta 电位与 RBC 的 PS 暴露呈负相关,这表明这种空气污染物的生物活性来源于颗粒。基于炭黑(CB)和氧化炭黑(OCB)人工纳米材料的模拟测试证实了颗粒碳在 PM2.5 诱导的对红细胞的影响中的关键作用,而具有一定氧化程度的烟尘由于在 PM2.5 样品中无处不在,因此被认为是另一个贡献者。这项研究首次揭示了 PM2.5 诱导的红细胞 PS 暴露,并揭示了 DOM 和烟尘的致病成分。考虑到空气中的PM2.5与血液循环系统中的红细胞不可避免地发生接触,本研究的发现将有助于弥合PM2.5暴露与心血管疾病(如血栓形成)风险之间的差距。
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引用次数: 0
Photothermal Upcycling of Waste Polyvinyl Chloride Plastics. 废聚氯乙烯塑料的光热再循环。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-27 DOI: 10.1021/acs.est.4c07350
Hao Han, Penglei Yan, Qingye Li, Shuyi Zhang, Binglei Jiao, Gaolei Wei, Zhao Wang, Muhan Cao, Panpan Xu, Qiao Zhang, Jinxing Chen

Upgrading the most difficult-to-recycle waste polyvinyl chloride remains a significant challenge due to the potential formation of highly toxic substances, such as polychlorinated biphenyls. Here, we introduce a paradigm shift with a mild photothermal dechlorination-carbonization process that converts waste polyvinyl chloride plastics into valuable carbon materials. Through detailed techno-economic assessment (TEA) process modeling, based on recycling 96,000 tons of plastics, we demonstrate that utilizing clean solar energy for photothermal conversion can save approximately 2.34 × 1012 kJ electricity and reduce the carbon footprint by 261,912.2 tons compared to traditional thermal-driven methods, offering clear environmental benefits. Notably, this photothermal recycling method can process more than 10 types of postconsumer and mixed waste polyvinyl chloride plastics, yielding carbon materials that exhibit excellent performance as components in sodium-ion energy storage batteries. Photothermal catalytic recycling of plastics thus emerges as a green and sustainable technology with promising applications.

由于可能形成多氯联苯等剧毒物质,如何升级最难回收的废弃聚氯乙烯仍是一项重大挑战。在这里,我们引入了一种温和的光热脱氯-碳化工艺,将废旧聚氯乙烯塑料转化为有价值的碳材料,从而实现了模式的转变。通过详细的技术经济评估(TEA)工艺建模,以回收 96,000 吨塑料为基础,我们证明了利用清洁太阳能进行光热转换与传统的热驱动方法相比,可节省约 2.34 × 1012 kJ 的电能,减少碳足迹 261,912.2 吨,具有明显的环境效益。值得注意的是,这种光热回收方法可以处理 10 多种消费后和混合废旧聚氯乙烯塑料,产生的碳材料作为钠离子储能电池的组件性能优异。因此,光热催化塑料回收是一种绿色可持续技术,具有广阔的应用前景。
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引用次数: 0
Mask Wearers at Risk of Inhaling Respirable Hazards from Leave-On Facial Cosmetics. 戴口罩者有可能吸入免洗面部化妆品的可吸入性危害。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-27 DOI: 10.1021/acs.est.4c07604
Han Dai, Shanshan He, Jie Han, Baoshan Xing

Previous research has widely overlooked the respiratory risks associated with cosmetic powder, a type of mixed particulate matter with intricate chemical compositions, especially in the context of wearing masks. This study investigated the inhalation risks posed by five face powders, focusing on both particulate matter (minerals and primary microplastics) and soluble components (preservatives and organic UV filters). Wearing masks significantly increased the inhalation risk of face powders, with exposure levels influenced by factors such as particle size, density, and composition. Additionally, different samples demonstrated irregular behavioral patterns when exposed to various human tissue environments. Soluble components analysis revealed that multiple additives dissolved in six body fluids, with a higher degree of release observed in the respiratory tract fluid compared to the digestive tract fluid. The alveoli may serve as a specific target for exposure to organic UV filters due to the solubilization effect of pulmonary surfactants. These findings revealed the importance of considering both particulate matter and soluble components when assessing respiratory and digestive exposure risks from cosmetic powders. Furthermore, understanding the interactions between cosmetic particles and body fluids, as well as potential synergistic toxic effects, is crucial for ensuring the safety of cosmetic products and safeguarding public health.

化妆品粉末是一种化学成分复杂的混合微粒物质,以往的研究普遍忽视了其对呼吸系统造成的风险,尤其是在佩戴口罩的情况下。本研究调查了五种粉饼的吸入风险,重点是颗粒物质(矿物质和初级微塑料)和可溶性成分(防腐剂和有机紫外线过滤剂)。戴口罩会大大增加吸入粉饼的风险,暴露水平受颗粒大小、密度和成分等因素的影响。此外,不同的样品在暴露于各种人体组织环境时会表现出不规则的行为模式。可溶性成分分析表明,多种添加剂溶解在六种体液中,与消化道体液相比,呼吸道体液中的释放程度更高。由于肺表面活性物质的溶解作用,肺泡可能是接触有机紫外线过滤剂的特定目标。这些研究结果表明,在评估呼吸道和消化道接触化妆品粉末的风险时,同时考虑颗粒物质和可溶性成分非常重要。此外,了解化妆品微粒与体液之间的相互作用以及潜在的协同毒性效应,对于确保化妆品的安全性和保障公众健康至关重要。
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引用次数: 0
Discerning Emittable from Extractable Chemicals Identified in Consumer Products by Suspect Screening GCxGC-TOFMS 通过疑似筛选 GCxGC-TOFMS 鉴别消费品中的可逸散和可提取化学品
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-27 DOI: 10.1021/acs.est.4c07903
William D. Watson, Jake A. Janssen, Michael J. Hartnett, Kristin K. Isaacs, Xiaoyu Liu, Alice Y. Yau, Kristin A. Favela, John F. Wambaugh
Characterization of chemicals in household products is important for understanding this potential source of chemical exposure. Increasingly, suspect screening and nontargeted analysis techniques are used to characterize as many chemical signatures as possible. Solids such as household products are most conveniently prepared using solvent extraction, revealing what chemicals are contained within the product matrix but providing no information about the potential of those chemicals to leave the matrix and cause actual exposure. In this work, the profile and relative abundances of “extractable” chemical signatures found after solvent extraction are compared to those “emittable” to the headspace for 81 household products analyzed by two-dimensional gas chromatography time-of-flight mass spectrometry. This study retrospectively fuses data collected in separate efforts over 3.8 years and 13 analytical batches. Management of the data is made possible by recent developments in processing systems for complex data such as Highlight. Compounds were generically classified as aromatic heteroatom, aromatic hydrocarbon, glycol, hydrocarbon, long chain heteroatom, nonaromatic heteroatom, and unknown/unclassified. Class-based retention time and abundance trends were observed. Liquid extraction resulted in the greatest number of features and the highest relative abundances, while low temperature emission conditions produced the smallest number of features and lowest relative abundances.
对家用产品中的化学物质进行定性,对于了解这一潜在的化学物质暴露源非常重要。为了描述尽可能多的化学特征,人们越来越多地使用可疑筛选和非目标分析技术。使用溶剂萃取法制备家用产品等固体最为方便,它可以揭示产品基质中含有哪些化学物质,但无法提供有关这些化学物质离开基质并导致实际暴露的可能性的信息。在这项研究中,通过二维气相色谱-飞行时间质谱法对 81 种家用产品进行了分析,将溶剂萃取后发现的 "可萃取 "化学特征的概况和相对丰度与顶空 "可释放 "的化学特征进行了比较。这项研究回顾性地融合了历时 3.8 年、分 13 个分析批次收集的数据。数据的管理得益于最近开发的复杂数据处理系统(如 Highlight)。化合物一般分为芳香杂原子、芳香烃、乙二醇、烃、长链杂原子、非芳香杂原子和未知/未分类。观察到了基于类别的保留时间和丰度趋势。液体萃取产生了最多的特征和最高的相对丰度,而低温排放条件下产生的特征最少,相对丰度最低。
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引用次数: 0
Secondary Organic Aerosol from Biomass Burning Phenolic Compounds and Nitrate Radicals can be Highly Viscous over a Wide Relative Humidity Range 生物质燃烧产生的二次有机气溶胶酚类化合物和硝酸根在较宽的相对湿度范围内具有高粘性
IF 9.028 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-27 DOI: 10.1021/acs.est.4c06235
Sepehr Nikkho, Bin Bai, Fabian Mahrt, Julia Zaks, Long Peng, Kristian J. Kiland, Pengfei Liu, Allan K. Bertram
Biomass burning events, including wildfires, can emit large amounts of phenolic compounds such as guaiacol. These phenolic compounds can undergo oxidation by nitrate radicals (NO3) to form secondary organic aerosol (SOA). Viscosity and hygroscopicity are key properties that affect SOA’s role in atmospheric chemistry, air quality, climate and public health. However, these properties have not been quantified for SOA formed from the reaction of phenolic compounds with NO3. We used the poke-flow technique and a quartz crystal microbalance (QCM) to measure the viscosity and hygroscopicity of SOA particles generated from the reaction of NO3 with guaiacol, termed guaiacol-NO3 SOA. The viscosity of this SOA is extremely high (≳5 × 107 Pa s) at RH ≲ 70% and drastically higher than other SOA types previously investigated with the poke-flow technique at RH ≳ 40%. The high viscosity for guaiacol-NO3 SOA can be attributed, at least in part, to the low hygroscopicity measured via the QCM. From the viscosity results, we calculated the mixing times of organic molecules within guaiacol-NO3 SOA. The results suggest that mixing times within this type of SOA exceed 1 h for most tropospheric conditions, with possible implications for predicting the size, mass, and long-range transport of pollutants in phenolic SOA.
包括野火在内的生物质燃烧事件会释放出大量的酚类化合物,如愈创木酚。这些酚类化合物会被硝酸根(NO3)氧化,形成二次有机气溶胶(SOA)。粘度和吸湿性是影响 SOA 在大气化学、空气质量、气候和公共健康中作用的关键特性。然而,我们尚未对酚类化合物与 NO3 反应形成的 SOA 的这些特性进行量化。我们使用戳流技术和石英晶体微天平(QCM)测量了由 NO3 与愈创木酚反应生成的 SOA 粒子(称为愈创木酚-NO3 SOA)的粘度和吸湿性。在相对湿度≲ 70% 时,这种 SOA 的粘度极高(≳5 × 107 Pa s),大大高于之前在相对湿度≲ 40% 时使用捅流技术研究的其他 SOA 类型。愈创木酚-NO3 SOA 的高粘度至少可部分归因于 QCM 测得的低吸湿性。根据粘度结果,我们计算了愈创木酚-NO3 SOA 中有机分子的混合时间。结果表明,在大多数对流层条件下,这类 SOA 内部的混合时间超过 1 小时,这可能对预测酚类 SOA 中污染物的大小、质量和长程飘移产生影响。
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引用次数: 0
Form-Specific Prospective Environmental Risk Assessment of Graphene-Based Materials in European Freshwater. 欧洲淡水中石墨烯基材料的特定形式前瞻性环境风险评估。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-27 DOI: 10.1021/acs.est.4c05153
Hyunjoo Hong, Bernd Nowack

As graphene-based materials (GBMs) such as pristine graphene, graphene oxide, and reduced graphene oxide show great potential to be integrated in various applications, the need for environmental risk assessments grows, aiming to navigate the environmental fate and potential risk of the different forms of GBM. This study used dynamic probabilistic material flow analysis (DPMFA) to ascertain the prospective production volumes and distribution of GBMs within European freshwaters. The hazard assessment leveraged 113 data sets from peer-reviewed studies, addressing aquatic ecotoxicity across 26 species, by performing probabilistic species sensitivity distributions (SSD). Our findings reveal distinct environmental distribution patterns for GBM forms with predicted environmental concentrations in European freshwaters by 2030 of approximately 0.67 ng/L (SD = 0.24 ng/L) for pristine graphene and 0.33 ng/L (SD = 0.10 ng/L) for both graphene oxide and reduced graphene oxide, suggesting not only similar but notably minimal exposure levels. The risk characterization ratios (RCRs) for all forms of GBM were significantly below 1, indicating a negligible environmental risk within the scenarios assessed. Through detailed analysis considering the forms of the material, this research can inform regulatory decisions, support sustainable material design, and provide a solid foundation for a further investigation considering the environmental fate of GBM.

由于原生石墨烯、氧化石墨烯和还原氧化石墨烯等石墨烯基材料(GBMs)在各种应用中显示出巨大的集成潜力,因此环境风险评估的需求日益增长,其目的是了解不同形式的 GBMs 的环境归宿和潜在风险。本研究采用动态概率物质流分析法(DPMFA)来确定 GBM 在欧洲淡水中的预期产量和分布情况。危害评估利用了来自同行评审研究的 113 个数据集,通过执行概率物种敏感性分布 (SSD) 解决了 26 个物种的水生生态毒性问题。我们的研究结果揭示了 GBM 形式的独特环境分布模式,预测到 2030 年欧洲淡水中原始石墨烯的环境浓度约为 0.67 纳克/升(标准差 = 0.24 纳克/升),氧化石墨烯和还原氧化石墨烯的环境浓度约为 0.33 纳克/升(标准差 = 0.10 纳克/升),这表明暴露水平不仅相似,而且明显极低。所有形式的 GBM 的风险表征比 (RCR) 都明显低于 1,表明在所评估的情景中,环境风险可以忽略不计。通过对各种形式的材料进行详细分析,这项研究可以为监管决策提供信息,支持可持续材料设计,并为进一步研究 GBM 的环境归宿奠定坚实的基础。
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引用次数: 0
Molecular Characterization of Organosulfur and Organonitrogen Compounds in Summer and Winter PM2.5 via UHPLC-Q-Orbitrap MS/MS. 通过超高效液相色谱-Q-轨道阱 MS/MS 对夏季和冬季 PM2.5 中的有机硫和有机氮化合物进行分子表征。
IF 10.8 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-27 DOI: 10.1021/acs.est.4c02727
Hui Li, Fengkui Duan, Tao Ma, Yongliang Ma, Yunzhi Xu, Shuxiao Wang, Qinqin Zhang, Jingkun Jiang, Lidan Zhu, Fan Li, Tao Huang, Takashi Kimoto, Kebin He

Organosulfur and organonitrogen compounds (OrgSs and OrgNs) notably influence haze formation, reflecting the intricacies of sulfur and nitrogen chemistry in the atmospheric process. Despite this, a comprehensive understanding of OrgSs and OrgNs remains elusive. Here, we conducted molecular analyses of OrgSs and OrgNs in PM2.5 concurrently during three haze episodes in winter and summer from 2016 to 2019. OrgSs and OrgNs collectively constituted 68.8-73.8% of identified organics, with CHON (35.8%) being the most prevalent followed by CHONS (13.6%), CHN (11.5%), CHOS (5.6%), CHNS (3.2%), and CHS (0.9%). Nitrogen within CHX (CH + CHN + CHS + CHNS) compounds were predominantly present as nitriles or amines, while sulfur existed as alkaline thioethers (ESI+) or acidic mercaptans and thiophenols (ESI-). Oxygen-containing OrgSs and OrgNs exhibited greater structural complexity. Specifically, most CHON were associated with nitric esters and nitro-compounds (ESI-), or basic amino acids (ESI+). CHONS primarily comprised nitrogen heterocyclic substances containing oxygen and sulfur, with some potentially containing organic sulfates (OSs) and organic nitrates if O ≥ 4S + 3N. CHOS with (O-3S)/C ≥ 0 were identified as sulfonic acids or sulfate esters. This comprehensive spectrum of OrgSs and OrgNs enhances the understanding of the physicochemical properties of aerosols, providing insights for future laboratory and air quality model studies.

有机硫和有机氮化合物(OrgSs 和 OrgNs)对灰霾的形成有显著影响,反映了大气过程中硫和氮化学的复杂性。尽管如此,全面了解 OrgSs 和 OrgNs 的工作仍然遥遥无期。在此,我们在2016年至2019年冬夏三次雾霾天气期间,同时对PM2.5中的OrgSs和OrgNs进行了分子分析。OrgSs和OrgNs共占已识别有机物的68.8-73.8%,其中CHON(35.8%)最普遍,其次是CHONS(13.6%)、CHN(11.5%)、CHOS(5.6%)、CHNS(3.2%)和CHS(0.9%)。CHX (CH + CHN + CHS + CHNS)化合物中的氮主要以腈类或胺的形式存在,而硫则以碱性硫醚(ESI+)或酸性硫醇和噻吩酚(ESI-)的形式存在。含氧的 OrgSs 和 OrgNs 具有更复杂的结构。具体来说,大多数 CHON 与硝酸酯和硝基化合物(ESI-)或碱性氨基酸(ESI+)有关。CHONS 主要由含氧和硫的氮杂环物质组成,如果 O ≥ 4S + 3N,则可能含有一些有机硫酸盐(OS)和有机硝酸盐。(O-3S)/C ≥ 0 的 CHOS 被鉴定为磺酸或硫酸酯。这一全面的 OrgSs 和 OrgNs 图谱加深了人们对气溶胶理化性质的了解,为未来的实验室和空气质量模型研究提供了启示。
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引用次数: 0
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环境科学与技术
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