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New Insights into the Mechanism of the UV/Sulfite Process: Formation of SO2•– Radicals and Their Derivatives under Acidic Conditions 紫外线/亚硫酸盐过程机理的新见解:酸性条件下二氧化硫自由基及其衍生物的形成
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-26 DOI: 10.1021/acs.estlett.4c00251
Linghao Kong, Zhe Jin, Feng Zhu, Mengchang He, Feng Qian and Xianjia Peng*, 

The UV/sulfite process shows great potential for reductively degrading or eliminating pollutants. While its mechanism in neutral and alkaline environments has been well-elucidated, the reaction pathway under acidic conditions remains unclear. Herein, we report the novel findings of the formation of reductive SO2•– radicals and their derivatives in the UV/sulfite process at pH levels below 4. Mechanistic investigation revealed that H• radicals and SO3•– radicals formed by the photolysis of sulfite under acidic conditions, with the H• radicals being scavenged by sulfite to produce SO2•– radicals. Subsequently, these SO2•– radicals are transformed into dithionite, thiosulfate, hydrogen sulfide, and elemental sulfur through a series of intricate reactions. This study is expected to expand the potential application of the UV/sulfite process under acid conditions.

紫外线/亚硫酸盐工艺在还原降解或消除污染物方面显示出巨大的潜力。虽然其在中性和碱性环境中的机理已被充分阐明,但在酸性条件下的反应途径仍不清楚。在此,我们报告了在 pH 值低于 4 的紫外线/亚硫酸盐过程中形成还原性 SO2 自由基及其衍生物的新发现。机理研究发现,在酸性条件下亚硫酸盐光解形成 H- 自由基和 SO3--自由基,其中 H- 自由基被亚硫酸盐清除后生成 SO2--自由基。随后,这些 SO2--自由基通过一系列错综复杂的反应转化为二亚硫酸盐、硫代硫酸盐、硫化氢和元素硫。这项研究有望拓展紫外线/亚硫酸盐工艺在酸性条件下的潜在应用。
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引用次数: 0
Landfill Gas: A Major Pathway for Neutral Per- and Polyfluoroalkyl Substance (PFAS) Release 垃圾填埋气:中性全氟和多氟烷基物质 (PFAS) 释放的主要途径
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-26 DOI: 10.1021/acs.estlett.4c00364
Ashley M. Lin, Jake T. Thompson, Jeremy P. Koelmel, Yalan Liu, John A. Bowden and Timothy G. Townsend*, 

The undisclosed and ubiquitous use of perfluoroalkyl and polyfluoroalkyl substances (PFAS) in consumer products has led to a growing issue of environmental pollution, particularly within the solid waste community, where the fate of volatile (neutral) PFAS in landfilled refuse is not well understood. Here, three municipal solid waste landfills in Florida were assessed for neutral PFAS in landfill gas and ionic PFAS in landfill leachate to compare the relative mobility between the two pathways. Landfill gas was directly sampled using a high volume, XAD-2 resin based sampling approach developed for adsorption and analysis of 27 neutral PFAS. Across sites, 13 neutral PFAS were identified from fluorotelomer alcohol (FTOH), fluorotelomer olefin (FTO), secondary FTOH, fluorotelomer acetate (FTOAc), and fluorotelomer methyl acrylate (FTMAc) classes; however, FTOHs dominated concentrations (87–97% total neutral PFAS), with most detections surpassing utilized calibration levels. Even under conservative assumptions, the mass of fluorine leaving in landfill gas (32–76%) was comparable to or greater than the mass leaving in landfill leachate (24–68%). These findings suggest that landfill gas, a less scrutinized byproduct, serves as a major pathway for the mobility of PFAS from landfills.

全氟烷基和多氟烷基物质 (PFAS) 在消费品中的未公开和普遍使用导致环境污染问题日益严重,尤其是在固体废物领域,人们对垃圾填埋场中挥发性(中性)PFAS 的去向还不甚了解。在此,我们对佛罗里达州的三个城市固体废物填埋场进行了评估,检测填埋气体中的中性全氟辛烷磺酸和填埋沥滤液中的离子全氟辛烷磺酸,以比较这两种途径之间的相对流动性。垃圾填埋场气体采用大容量、基于 XAD-2 树脂的采样方法直接采样,该方法是为吸附和分析 27 种中性全氟辛烷磺酸而开发的。在各个地点,从氟醚醇 (FTOH)、氟醚烯烃 (FTO)、仲氟醚醇 (FTOH)、氟醚醋酸酯 (FTOAc) 和氟醚丙烯酸甲酯 (FTMAc) 类别中鉴定出 13 种中性全氟辛烷磺酸;不过,氟醚醇的浓度占主导地位(占中性全氟辛烷磺酸总量的 87-97%),大多数检测结果都超过了使用的校准水平。即使按照保守的假设,垃圾填埋气中的氟残留量(32-76%)与垃圾填埋场渗滤液中的氟残留量(24-68%)相当或更大。这些研究结果表明,垃圾填埋气这一不太受关注的副产品是 PFAS 从垃圾填埋场迁移的主要途径。
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引用次数: 0
Control of Micropollutants in Water by Far-UVC Photolysis of Peracetic Acid 通过远紫外光分解过乙酸控制水中的微污染物
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-25 DOI: 10.1021/acs.estlett.4c00384
Ran Yin*, Xinyi Ruan, Jiadong Peng, Jing Zhao, Yuliang Zhang, Arnaud Heuzard and Chii Shang, 

Increasing radical yields to reduce energy consumption for micropollutant degradation would make advanced oxidation processes more sustainable in the context of the United Nations’ Sustainable Development Goals and carbon neutrality. We herein demonstrate that switching the UV radiation source from conventional low-pressure UV (UV254) to far-UVC (UV222) increases the UV fluence-based concentration of hydroxyl radicals (HO) in the UV/peracetic acid (UV/PAA) process by 4.1-fold and 27.9-fold in deionized water and real surface water, respectively. Acetyloxyl radicals (CH3C(O)O) are generated in the UV222/PAA process at a steady-state concentration of 2.4 × 10–12 M in deionized water, while they are undetectable in the UV254/PAA process under the comparable conditions. The enhancement to radical production is mainly attributed to the 15.7-fold higher molar absorption coefficients of PAA0 at 222 nm than 254 nm (50 vs 3.5 M–1 cm–1), which suppresses the compromised 1.1-fold lower innate quantum yield at 222 nm than 254 nm (0.78 vs 0.86 mol einstein–1). The enhanced radical generation and direct photolysis promote the fluence-based degradation rate constants of bisphenol A, phenol, and nitrobenzene by 4.1-fold, 3.3-fold, and 2.9-fold in the UV222/PAA process than the UV254/PAA process.

在联合国可持续发展目标和碳中和的背景下,提高自由基产量以降低微污染物降解的能耗,将使高级氧化工艺更具可持续性。我们在本文中证明,将紫外线辐射源从传统的低压紫外线(UV254)切换到远紫外线(UV222)后,紫外线/过乙酸(UV/PAA)过程中基于紫外线通量的羟基自由基(HO-)浓度在去离子水和实际地表水中分别增加了 4.1 倍和 27.9 倍。UV222/PAA 过程中产生的乙酰氧基(CH3C(O)O-)在去离子水中的稳态浓度为 2.4 × 10-12 M,而在 UV254/PAA 过程中,在类似条件下检测不到乙酰氧基。自由基生成的增强主要归因于 PAA0 在 222 纳米波段的摩尔吸收系数比 254 纳米波段高 15.7 倍(50 对 3.5 M-1 cm-1),从而抑制了在 222 纳米波段比 254 纳米波段低 1.1 倍的先天量子产率(0.78 对 0.86 摩尔爱因斯坦-1)。与 UV254/PAA 工艺相比,UV222/PAA 工艺中增强的自由基生成和直接光解促进了双酚 A、苯酚和硝基苯的基于通量的降解速率常数,分别提高了 4.1 倍、3.3 倍和 2.9 倍。
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引用次数: 0
Response to Comment on “Size-Resolved Elemental Composition of Respiratory Particles in Three Healthy Subjects” 对 "三位健康受试者呼吸道粒子的尺寸分辨元素组成 "评论的回应
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-25 DOI: 10.1021/acs.estlett.4c00484
Linsey C. Marr*, Zezhen Cheng, Weinan Leng, Swarup China and Aaron J. Prussin II, 
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引用次数: 0
Comment on “Size-Resolved Elemental Composition of Respiratory Particles in Three Healthy Subjects” 关于 "三名健康受试者呼吸道颗粒的尺寸分辨元素组成 "的评论
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-25 DOI: 10.1021/acs.estlett.4c00243
Steven C. Hill*,  and , David C. Doughty*, 
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引用次数: 0
Response to Comment on “Drinking Boiled Tap Water Reduces Human Intake of Nanoplastics and Microplastics” 对 "饮用煮沸的自来水可减少人体对纳米塑料和微塑料的摄入 "评论的回应
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-21 DOI: 10.1021/acs.estlett.4c00475
Zimin Yu, Zhanjun Li* and Eddy Y. Zeng*, 
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引用次数: 0
Nanocluster Aerosols from Ozone–Human Chemistry Are Dominated by Squalene–Ozone Reactions 臭氧-人类化学作用产生的纳米团簇气溶胶主要由角鲨烯-臭氧反应产生
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-21 DOI: 10.1021/acs.estlett.4c00289
Shen Yang*,  and , Dusan Licina, 

Nanocluster aerosols (NCAs, <3 nm particles) are associated with climate feedbacks and potentially with human health. Our recent study revealed NCA formation owing to the reaction of ozone with human surfaces. However, the underlying mechanisms driving NCA emissions remain unexplored. Squalene is the most abundant compound in human skin lipids that reacts with ozone, followed by unsaturated fatty acids. This study aims to examine the contribution of the squalene–ozone reaction to NCA formation and the influence of ozone and ammonia (NH3) levels. In a climate-controlled chamber, we painted squalene and 6-hexadecenoic acid (C16:1n6) on glass plates to facilitate their reactions with ozone. The squalene–ozone reaction was further investigated at different ozone levels (15 and 90 ppb) and NH3 levels (0 and 375 ppb). The results demonstrate that the ozonolysis of human skin lipid compounds contributes to NCA formation. With a typical squalene-C16:1n6 ratio found in human skin lipids (4:1), squalene generated 40 times more NCAs than did C16:1n6 and, thus, dominated NCA formation. More NCAs were generated with increased ozone levels, whereas increased NH3 levels were associated with the stronger generation of larger NCAs but fewer of the smallest ones. This study experimentally confirms that NCAs are primarily formed from squalene–ozone reactions in ozone–human chemistry.

纳米团簇气溶胶(NCAs,3 纳米颗粒)与气候反馈有关,也可能与人类健康有关。我们最近的研究揭示了由于臭氧与人体表面发生反应而形成的 NCA。然而,驱动 NCA 排放的根本机制仍有待探索。角鲨烯是人体皮肤脂质中与臭氧反应最多的化合物,其次是不饱和脂肪酸。本研究旨在考察角鲨烯-臭氧反应对 NCA 形成的贡献以及臭氧和氨(NH3)水平的影响。在气候控制室中,我们将角鲨烯和 6-十六碳烯酸(C16:1n6)涂在玻璃板上,以促进它们与臭氧的反应。在不同的臭氧水平(15 和 90 ppb)和 NH3 水平(0 和 375 ppb)下,我们进一步研究了角鲨烯与臭氧的反应。结果表明,人体皮肤脂质化合物的臭氧分解有助于 NCA 的形成。在人类皮肤脂质中发现的典型角鲨烯-C16:1n6 比率(4:1)下,角鲨烯产生的 NCA 是 C16:1n6 的 40 倍,因此,角鲨烯主导了 NCA 的形成。臭氧浓度升高会产生更多的 NCA,而 NH3 浓度升高会产生更多较大的 NCA,但产生较少最小的 NCA。这项研究通过实验证实,在臭氧-人类化学反应中,NCA 主要由角鲨烯-臭氧反应生成。
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引用次数: 0
Secondary Organic Aerosol Formation from Ambient Air in Summer in Urban Beijing: Contribution of S/IVOCs and Impacts of Heat Waves 北京城市夏季环境空气中二次有机气溶胶的形成:S/IVOCs 的贡献与热浪的影响
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-21 DOI: 10.1021/acs.estlett.4c00415
Zijun Zhang, Weiqi Xu, Siqi Zeng, Yongchun Liu, Tengyu Liu, Yi Zhang, Aodong Du, Yan Li, Ning Zhang, Junfeng Wang, Eleonora Aruffo, Pengfei Han, Jie Li, Zifa Wang and Yele Sun*, 

Semivolatile and intermediate volatility organic compounds (S/IVOCs) are known as crucial precursors of secondary organic aerosols (SOA), yet their specific contributions to SOA in urban areas remain unclear. Here, we investigate the real-time SOA formation from urban ambient air in summer in Beijing utilizing an oxidation flow reactor (OFR), coupled with aerosol and proton-transfer-reaction mass spectrometers. Our results show that the maximum photochemical formation of SOA in the OFR reached 2.9 μg m–3 at ∼1.5 days of photochemical age. Primary OA and less oxidized oxygenated OA experience mass loss at high photochemical ages (>3 days) in the OFR, whereas more oxidized oxygenated OA continues to show mass enhancement, indicating the role of heterogeneous processes in the formation of highly aged SOA. Closure studies demonstrate that SOA estimated from the known precursors contribute 50.0 ± 17.3% of the measured SOA. The relatively low contribution (10.3 ± 5.2%) of IVOCs emphasizes the importance of unmeasured S/IVOCs in SOA formation. Furthermore, we illustrate the impact of heat waves on ambient SOA formation by enhancing photochemical oxidation and biogenic emissions in summer.

众所周知,半挥发性和中间挥发性有机化合物(S/IVOCs)是二次有机气溶胶(SOA)的重要前体,但它们对城市地区 SOA 的具体贡献仍不清楚。在此,我们利用氧化流动反应器(OFR),结合气溶胶和质子转移反应质谱仪,研究了北京夏季城市环境空气中 SOA 的实时形成情况。我们的研究结果表明,在光化学龄期为 1.5 天时,氧化流反应器中 SOA 的最大光化学形成量达到 2.9 μg m-3。原生 OA 和氧化程度较低的含氧 OA 在 OFR 的光化学年龄较高(3 天)时会出现质量损失,而氧化程度较高的含氧 OA 则会继续出现质量增加,这表明异质过程在形成高度老化的 SOA 中发挥了作用。闭合研究表明,根据已知前体估算的 SOA 占测量 SOA 的 50.0 ± 17.3%。IVOCs 的贡献率相对较低(10.3 ± 5.2%),这强调了未测量的 S/IVOCs 在 SOA 形成过程中的重要性。此外,我们还说明了热浪在夏季通过加强光化学氧化和生物排放对环境 SOA 形成的影响。
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引用次数: 0
Toward Enhancing Wastewater Treatment with Resource Recovery in Integrated Assessment and Computable General Equilibrium Models 在综合评估和可计算一般均衡模型中利用资源回收加强废水处理
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-18 DOI: 10.1021/acs.estlett.4c00280
Jennifer B. Dunn*, Kristen Greene, Eveline Vasquez-Arroyo, Muhammad Awais, Adriana Gomez-Sanabria, Page Kyle, Ruslana R. Palatnik, Roberto Schaeffer, Pengxiao Zhou, Baya Aissaoui and Enrica De Cian, 

Sustainable water management is essential to increasing water availability and decreasing water pollution. The wastewater sector is expanding globally and beginning to incorporate technologies that recover nutrients from wastewater. Nutrient recovery increases energy consumption but may reduce the demand for nutrients from virgin sources. We estimate the increase in annual global energy consumption (1,100 million GJ) and greenhouse gas emissions (84 million t CO2e) for wastewater treatment in the year 2030 compared to today’s levels to meet sustainable development goals. To capture these trends, integrated assessment and computable general equilibrium models that address the energy-water nexus must evolve. We reviewed 16 of these models to assess how well they capture wastewater treatment plant energy consumption and GHG emissions. Only three models include biogas production from the wastewater organic content. Four explicitly represent energy demand for wastewater treatment, and eight include explicit representation of wastewater treatment plant greenhouse gas emissions. Of those eight models, six models quantify methane emissions from treatment, five include representation of emissions of nitrous oxide, and two include representation of emissions of carbon dioxide. Our review concludes with proposals to improve these models to better capture the energy-water nexus associated with the evolving wastewater treatment sector.

可持续水资源管理对于增加水资源供应和减少水污染至关重要。废水处理行业正在全球范围内扩展,并开始采用从废水中回收养分的技术。养分回收会增加能源消耗,但可以减少对原始来源养分的需求。我们估计,为实现可持续发展目标,2030 年全球废水处理的年能耗(11 亿 GJ)和温室气体排放量(8400 万吨 CO2e)将比现在有所增加。为了捕捉这些趋势,必须发展解决能源与水关系的综合评估和可计算一般平衡模型。我们对其中的 16 个模型进行了审查,以评估它们对污水处理厂能源消耗和温室气体排放的捕捉程度。只有三个模型包括利用废水中的有机物生产沼气。四个模型明确表示了污水处理的能源需求,八个模型明确表示了污水处理厂的温室气体排放。在这 8 个模型中,6 个模型量化了处理过程中的甲烷排放,5 个模型包含了一氧化二氮的排放,2 个模型包含了二氧化碳的排放。最后,我们提出了改进这些模型的建议,以更好地捕捉与不断发展的污水处理行业相关的能源-水关系。
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引用次数: 0
Decomposition of Clusters of Oxygenated Compounds with NO3– by Applying Voltage Scanning to Chemical Ionization Mass Spectrometry in Steady-State Experiments 在稳态实验中将电压扫描应用于化学电离质谱法,用 NO3- 分解含氧化合物团簇
IF 8.9 2区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-18 DOI: 10.1021/acs.estlett.4c00276
Hui Wang, Yarê Baker, Hongru Shen, Rongrong Wu, Sungah Kang, Defeng Zhao, Andreas Wahner, Sören R. Zorn* and Thomas F. Mentel, 

Oxygenated volatile organic compounds (OVOCs) contribute to atmospheric secondary organic aerosols. To better constrain OVOC distributions, e.g., from the oxidation of phenolics, voltage scanning was applied for the targeted destruction of product nitrate (NO3) clusters in a chemical ionization mass spectrometer. Herein, the voltage difference at which half of the clusters remain (dV50) represents their bond strength. This study identified the type and relative bond strength of adducts for product distributions that can be observed for hours in our steady-state chamber (SAPHIR*). An unexpected increase was observed in voltage scanning curves of clusters containing nitrated phenols [e.g., C7H7NO3(NO3)], which was attributed to the declustering of double-analyte clusters [e.g., C14H14N2O6(NO3)] at small voltage differences. Double-analyte clusters were distinguished from accretion product clusters [e.g., C12H(10,12)Ox(NO3)] by their significantly lower intermolecular forces. Misidentifying C14H14N2O6 as accretion products could lead to an overestimation of its contribution to particle mass. In addition, the higher bonding strength in C6H(6,8)O4–9(NO3) compared to that in H2SO4(NO3) indicates maximum sensitivities of C6H(6,8)O4–9 at the collision limit. We could elucidate the relative acidity of the analytes to HNO3. This study highlights additional dimensions gained from voltage scanning and suggests performing it to clarify the product distribution in complex urban air in the presence of nitrated phenols.

含氧挥发性有机化合物(OVOC)是大气中二次有机气溶胶的组成部分。为了更好地确定 OVOC 的分布情况,例如酚类物质的氧化情况,在化学电离质谱仪中采用了电压扫描来有针对性地破坏硝酸盐(NO3-)产物簇。其中,保留一半簇的电压差(dV50)代表其键强度。这项研究确定了在我们的稳态室(SAPHIR*)中可观察数小时的产物分布的加合物类型和相对键强度。在含有硝化酚[如 C7H7NO3(NO3-)]的簇的电压扫描曲线上观察到了意想不到的增长,这归因于双分析物簇[如 C14H14N2O6(NO3-)]在小电压差下的解簇。双分析物簇与吸积产物簇[如 C12H(10,12)Ox(NO3-)]的区别在于它们的分子间作用力明显较低。将 C14H14N2O6 误认为是吸积产物可能会导致高估其对粒子质量的贡献。此外,与 H2SO4(NO3-) 相比,C6H(6,8)O4-9(NO3-) 的键合强度更高,这表明 C6H(6,8)O4-9 在碰撞极限时具有最大灵敏度。我们可以阐明分析物对 HNO3 的相对酸性。这项研究强调了电压扫描所获得的额外维度,并建议使用电压扫描来阐明硝化酚存在时城市复杂空气中的产物分布情况。
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引用次数: 0
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Environmental Science & Technology Letters Environ.
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