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Coupling Electrochemical Alkalinization and Mineral Dissolution for Ambient Removal of Both Influent CO2 and Dissolved Nitrite in Seawater 将电化学碱化和矿物溶解耦合起来,在环境中同时去除海水中的二氧化碳和溶解亚硝酸盐
IF 10.9 2区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-05-20 DOI: 10.1021/acs.estlett.4c00313
Hong-Tao Cong, Xiao-Qiang Yan, Li-Kun Yang*, Yuan Jiang*, Chao Wang, Dongping Zhan, Yan Li and Minhan Dai, 

Marine carbon dioxide removal (mCDR) is increasingly recognized as a potential mitigation pathway to achieve the goals of the Paris Agreement. Among the scalable and cost-effective options for mCDR, ocean alkalinity enhancement (OAE) stands out as a potential eco-friendly option. Herein, a novel OAE strategy on the basis of coupled electrochemical alkalinization and CaCO3 dissolution is developed for the removal of influent CO2 in ambient conditions. The laboratory strategy also considers the additional benefit of converting dissolved nitrite, which can be toxic at high concentrations in seawater. The protons produced in the anodic sector are neutralized by timely dissolution of CaCO3 powders, which converts an equivalent mole of dissolved inorganic carbon. The alkalinity generated in the cathodic sector reacts with influent CO2 to form bicarbonate anions in seawater. As a result, the integrated OAE design produces increased total alkalinity and dissolved inorganic carbon in seawater with a relatively moderate energy consumption of 104.5 kJ/mol of CO2 and high electron efficiency. In addition, the anodic reaction converts nitrite to nitrate. The proof-of-concept module thus provides an eco-beneficial pathway for mCDR. A potential environmental scenario could be the integration of OAE and wastewater treatment in intensive and recirculating marine aquaculture.

海洋二氧化碳去除(mCDR)越来越被认为是实现《巴黎协定》目标的潜在减排途径。在可扩展且具有成本效益的海洋二氧化碳减排方案中,海洋碱度增强(OAE)作为一种潜在的生态友好型方案脱颖而出。本文在电化学碱化和 CaCO3 溶解耦合的基础上开发了一种新型 OAE 战略,用于在环境条件下去除进水二氧化碳。该实验室策略还考虑了转化溶解的亚硝酸盐的额外好处,亚硝酸盐在海水中浓度过高时可能具有毒性。阳极部门产生的质子通过 CaCO3 粉末的及时溶解得到中和,从而转化为等效摩尔的溶解无机碳。阴极区产生的碱度与流入的二氧化碳反应,在海水中形成碳酸氢根阴离子。因此,集成式 OAE 设计可增加海水中的总碱度和溶解无机碳,能耗相对较低,为 104.5 kJ/mol(二氧化碳),电子效率较高。此外,阳极反应还能将亚硝酸盐转化为硝酸盐。因此,概念验证模块为 mCDR 提供了一条有益于生态的途径。一个潜在的环境方案可能是将 OAE 与集约化循环海水养殖中的废水处理结合起来。
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引用次数: 0
Ultrahigh Salt Adsorption Capacity of Carbonaceous Electrode in a Rocking-Chair Capacitive Deionization through Surface Charge Modulation 通过表面电荷调制实现摇椅式电容去离子法中碳质电极的超高盐吸附能力
IF 10.9 2区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-05-17 DOI: 10.1021/acs.estlett.4c00219
Qifeng Wang, Mingyan Zhao, Qinghao Wu, Shujuan Meng, Xiaohu Li and Dawei Liang*, 

Addressing the challenges of ion adsorption capacity and electrode stability in capacitive deionization (CDI), this research introduces a pioneering anion exchange membrane (AEM)-based rocking chair CDI (RCDI) system equipped with activated carbon electrodes. Designed to counteract co-ion effects, this AEM-RCDI system significantly enhances ion-selective adsorption through improved electrode surface charge dynamics. This study also elucidates how these dynamics influence electrode potential distribution, the potential of zero charge, and the mechanism facilitating differential adsorption of ions, bridging fundamental electrochemical insight with practical improvement in desalination performance. Our investigation reveals that the oxidation of the carbon electrode, both during desalination and through targeted preoxidation, significantly boosts desalination efficacy and electrode stability. Especially, preoxidation increases cation adsorption, achieving an impressive desalination capacity of 87.3 mg g–1, rate of 12 mg g–1 min–1, and charge efficiency of 88.6%, with remarkable stability over 240 desalination cycles. This study not only unveils key insights into the deionization mechanisms and properties of carbonaceous electrodes in RCDI but also sets a new benchmark for commercial CDI development.

为了解决电容式去离子(CDI)中离子吸附容量和电极稳定性的难题,本研究率先推出了一种基于阴离子交换膜(AEM)的摇椅式电容式去离子(RCDI)系统,该系统配备了活性炭电极。这种 AEM-RCDI 系统旨在抵消共离子效应,通过改善电极表面电荷动态,显著提高离子选择性吸附能力。这项研究还阐明了这些动态如何影响电极电位分布、零电荷电位以及促进离子差异吸附的机制,从而将基本的电化学见解与海水淡化性能的实际改善结合起来。我们的研究发现,在海水淡化过程中以及通过有针对性的预氧化作用对碳电极进行氧化,可显著提高海水淡化效果和电极稳定性。特别是,预氧化增加了阳离子吸附,使脱盐能力达到惊人的 87.3 mg g-1,脱盐率达到 12 mg g-1 min-1,充电效率达到 88.6%,并且在 240 次脱盐循环中保持了出色的稳定性。这项研究不仅揭示了碳质电极在 RCDI 中的去离子机理和特性,还为商业 CDI 的开发树立了新的标杆。
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引用次数: 0
A Decade of Global Atmospheric Monitoring Delivers Mixed Report Card on the Stockholm Convention 全球大气监测十年为《斯德哥尔摩公约》交出喜忧参半的成绩单
IF 10.9 2区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-05-17 DOI: 10.1021/acs.estlett.4c00316
Chubashini Shunthirasingham, Michelle Hoang, Ying Duan Lei, Anya Gawor and Frank Wania*, 

Time trends in atmospheric concentrations serve to evaluate how effective the Stockholm Convention is in reducing or eliminating environmental releases of persistent organic pollutants (POPs). Twelve years (2005–2016) of continuous monitoring with a global network of 20 sampling sites reveals that concentrations of the pesticide endosulfan began to drop coincident with its listing as POP in 2011. Concentrations of other POPs started to decrease prior to listing and during the sampling period declined very slowly or not at all. Concentrations of some unintentionally produced POPs (hexachlorobenzene, hexachlorobutadiene) increased to become the most abundant and most widely dispersed POPs in the global atmosphere. Their formation processes and release locations need to be identified to facilitate the Convention’s goal of curbing releases from unintentional production.

大气浓度的时间趋势有助于评估《斯德哥尔摩公约》在减少或消除持久性有机污染物(POPs)环境排放方面的成效。通过对由 20 个采样点组成的全球网络进行 12 年(2005-2016 年)的连续监测发现,农药硫丹的浓度在 2011 年被列为持久性有机污染物后开始下降。其他持久性有机污染物的浓度在被列入之前就开始下降,而在采样期间,其下降速度非常缓慢,甚至根本没有下降。一些无意生产的持久性有机污染物(六氯苯、六氯丁二烯)的浓度上升,成为全球大气中含量最高、散布最广的持久性有机污染物。需要查明其形成过程和释放地点,以促进实现《公约》遏制无意生产释放的目标。
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引用次数: 0
Characterization of Chemical Additives in Daily Clothing Regarding Human Exposure and Environmental Emissions 从人体接触和环境排放的角度分析日常服装中的化学添加剂
IF 10.9 2区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-05-17 DOI: 10.1021/acs.estlett.4c00297
Xiaomeng Ji, Jiale Liu, Jie Shen, Pinjie Su, Jiefeng Liang, Xiaoxia Feng, Xiaoyun Liu and Runzeng Liu*, 

Despite the ubiquitous use of textiles, the chemical additives used in textile manufacturing, their human exposure, and their environmental release have been largely overlooked. Herein, we screened for numerous chemical additives, including synthetic antioxidants, organophosphate esters, and phthalate esters, detecting 93 of 98 chemicals in 78 items of clothing (sum concentration: 328 to 2.51 × 105 ng/g, median: 2.77 × 104 ng/g). Compared with organophosphate esters and phthalate esters, significantly high concentrations of synthetic antioxidants (median: 2.51 × 104 ng/g) were found in clothes for both children and adults. Different chemical compositions were observed between cotton and artificial fabrics, with 3 times higher concentrations observed in clothing for children than for adults. Dermal contact via sweaty clothes may be a major exposure pathway for 2,4-di-tert-butyl-phenol (contributing 39.1% to total exposure); thus, it is recommended to avoid rewearing sweaty clothes to minimize human exposure. Additionally, environmental emissions of chemicals through laundry wastewater were estimated at 11.2 tons/year in China. The discharge of 2,6-di-tert-butyl-p-benzoquinone via laundry wastewater contributed 20.4% of the total input into wastewater treatment plants in China, indicating a non-negligible source of this chemical. This work provides comprehensive evidence of unwanted chemical additives in clothes and underscores the necessity for continuous monitoring of environmental and human risks associated with textile products.

尽管纺织品的使用无处不在,但纺织品生产过程中使用的化学添加剂、人体接触情况及其环境释放情况却在很大程度上被忽视了。在本文中,我们对包括合成抗氧化剂、有机磷酸酯和邻苯二甲酸酯在内的多种化学添加剂进行了筛查,在 78 件衣物中检测出 98 种化学物质中的 93 种(总浓度:328 至 2.51 × 105 ng/g,中位数:2.77 × 104 ng/g)。与有机磷酸酯和邻苯二甲酸酯相比,儿童和成人衣物中合成抗氧化剂的浓度明显更高(中位数:2.51 × 104 纳克/克)。棉织物和人造织物的化学成分不同,儿童服装中的浓度是成人的 3 倍。通过汗湿衣服的皮肤接触可能是人体摄入 2,4- 二叔丁基苯酚的主要途径(占总摄入量的 39.1%);因此,建议避免重穿汗湿衣服,以尽量减少人体摄入量。此外,中国每年通过洗衣废水排放的化学物质估计为 11.2 吨。通过洗衣废水排放的 2,6-二叔丁基对苯醌占中国污水处理厂总输入量的 20.4%,表明这种化学物质的来源不可忽视。这项工作提供了衣服中不需要的化学添加剂的全面证据,并强调了持续监测与纺织产品相关的环境和人类风险的必要性。
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引用次数: 0
Primary and Secondary Emissions of Carboxylic Acids from Solid Fuel Combustion: Insight into the Source Markers and Secondary Formation Mechanism 固体燃料燃烧产生的羧酸的一次和二次排放:洞察源标记和二次形成机制
IF 10.9 2区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-05-17 DOI: 10.1021/acs.estlett.4c00339
Bin Zhang, Zhenxing Shen*, Xueting Yang, Kun He, Shasha Huang, Weidong Wu, Jian Sun, Hongmei Xu, Liu Yang and Jun-ji Cao, 

Carboxylic acids play an important role in atmospheric photochemical reactions, aerosol nuclei, and climate change. Primary and secondary carboxylic acid emissions from various combustion scenarios were quantified. Coal combustion emitted more low-molecular weight (MW) monocarboxylic acids (<C9) (12.7–16.4%), while biomass burning released more ultrahigh-MW monocarboxylic acids (>C29) (15.5–32.3%). Ultrahigh-MW monocarboxylic acid abundance and hexadecanoic acid (C16) versus nonadecanoic acid (C19) remained stable between the primary emission and aging processes, suggesting that they could be ideal markers for source characterization. Significant correlations were observed between the decreasing of toluene and benzene and the increasing of oxalic acid (C2), malonic acid (C3), fumaric acid (C4), suberic acid (C8), azelaic acid (C9), and sebacic acid (C10) (p < 0.05) during coal combustion, suggesting that oxidation of toluene and benzene lead to the formation of dicarboxylic acids during photochemical aging. On the other hand, the oxidation of monocarboxylic acids occurs on carbons farther away from the −COOH group, leading to the formation of dicarboxylic acids. The secondary formation mechanism of dicarboxylic acids from biomass burning differed from that of coal because of the abundance of low-chemical reactivity, ultrahigh-MW monocarboxylic acids; further study is required.

羧酸在大气光化学反应、气溶胶核和气候变化中发挥着重要作用。我们对各种燃烧方案产生的一次和二次羧酸排放进行了量化。煤炭燃烧排放了更多的低分子量(MW)单羧酸(C9)(12.7-16.4%),而生物质燃烧释放了更多的超高分子量单羧酸(C29)(15.5-32.3%)。超高分子量一元羧酸的丰度以及十六烷酸(C16)与非十六烷酸(C19)的对比在一次排放和老化过程之间保持稳定,这表明它们可以作为源特征描述的理想标记。在煤燃烧过程中,甲苯和苯的减少与草酸(C2)、丙二酸(C3)、富马酸(C4)、辛二酸(C8)、壬二酸(C9)和癸二酸(C10)的增加之间存在显著相关性(p <0.05),表明在光化学老化过程中甲苯和苯的氧化导致二羧酸的形成。另一方面,单羧酸的氧化发生在距离 -COOH 基团较远的碳上,导致二羧酸的形成。生物质燃烧产生的二羧酸的二次形成机制不同于煤炭,因为生物质燃烧产生的二羧酸中含有大量低化学反应活性、超高分子量的一元羧酸;还需要进一步研究。
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引用次数: 0
Removing Our Brief(s) 删除我们的 Brief
IF 10.9 2区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-05-14 DOI: 10.1021/acs.estlett.4c00259
William A. Arnold*, Alexandria B. Boehm*, Bryan W. Brooks, Jonathan W. Martin, James R. Mihelcic, Zhiyong Jason Ren, Daniel Schlenk and Shuxiao Wang, 
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引用次数: 0
Impact of Secondary Organic Aerosol on the Respiratory Viral Infection in Vitro 二次有机气溶胶对体外呼吸道病毒感染的影响
IF 10.9 2区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-05-14 DOI: 10.1021/acs.estlett.4c00217
Shunyao Wang*, Xi Zhang, Kaisen Lin, Guanwen HUANG, Yue Zhao, Hin Chu* and Arthur W.H. Chan, 

Inhalation of viable airborne pathogens often leads to respiratory infections. Among the different factors that affect the survival of airborne pathogens, specific aerosol composition, such as secondary organic aerosol (SOA), may impact the severity of respiratory infection by stimulating host cell apoptotic responses. Here, we studied the in vitro effects of SOA (biogenic and anthropogenic) on respiratory infection of the human influenza A virus (H1N1). Viral gene copies in the human bronchial epithelial cell line (BEAS-2B) and human fetal lung fibroflast cell line (MRC-5) treated with SOA were measured to be significantly different from the control group. A maximum enhancement of 56%, 77%, and 45% in H1N1 replication was observed for BEAS-2B cells exposed to different doses of α-pinene SOA, toluene SOA, and naphthalene SOA, respectively. SOA from various precursors impacted viral replication differently, indicating the importance of emission source and composition. For BEAS-2B cells, anthropogenic SOA (toluene and naphthalene) significantly suppressed viral replication at low doses (1 μg mL–1 and 5 μg mL–1) and enhanced viral replication at higher doses. Interplay among the source, composition, oxidative stress, host cell apoptosis, and respiratory viral infection highlights the importance of having air pollution mitigation strategies out of a public health perspective.

吸入空气中可存活的病原体往往会导致呼吸道感染。在影响空气传播病原体存活的不同因素中,特定的气溶胶成分,如二次有机气溶胶(SOA),可能会通过刺激宿主细胞凋亡反应来影响呼吸道感染的严重程度。在此,我们研究了二次有机气溶胶(生物源和人为)对人类甲型 H1N1 流感病毒呼吸道感染的体外影响。经测定,经 SOA 处理的人支气管上皮细胞系(BEAS-2B)和人胎儿肺纤维细胞系(MRC-5)中的病毒基因拷贝与对照组相比有显著差异。在暴露于不同剂量的α-蒎烯 SOA、甲苯 SOA 和萘 SOA 的 BEAS-2B 细胞中,观察到 H1N1 复制的最大增强率分别为 56%、77% 和 45%。来自不同前体的 SOA 对病毒复制的影响各不相同,这表明了排放源和成分的重要性。对于 BEAS-2B 细胞,人为 SOA(甲苯和萘)在低剂量(1 μg mL-1 和 5 μg mL-1)时明显抑制病毒复制,而在高剂量时则增强病毒复制。空气污染的来源、成分、氧化应激、宿主细胞凋亡和呼吸道病毒感染之间的相互作用凸显了从公共卫生角度制定空气污染缓解策略的重要性。
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引用次数: 0
Maximizing the Impact of Research Featuring Nucleic-Acid Sequencing Methods in Environmental Science & Technology and Environmental Science & Technology Letters 最大限度地发挥《环境科学与技术》和《环境科学与技术通讯》中采用核酸测序方法的研究的影响
IF 10.9 2区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-05-14 DOI: 10.1021/acs.estlett.4c00295
Alexandria B. Boehm*, Lutgarde Raskin, Pedro Alvarez and Pei-Ying Hong, 
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引用次数: 0
Flow and Transport of Methane from Leaking Underground Pipelines: Effects of Soil Surface Conditions and Implications for Natural Gas Leak Classification 地下管道泄漏甲烷的流动和迁移:土壤表面条件的影响及对天然气泄漏分类的意义
IF 10.9 2区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-05-09 DOI: 10.1021/acs.estlett.4c00039
J R R Navodi Jayarathne*, Daniel Zimmerle, Richard S Kolodziej, Stuart Riddick and Kathleen M Smits, 

Reducing methane (CH4) emissions from natural gas (NG) pipeline leaks is crucial to minimize global warming while also providing key safety benefits to communities. What is not well understood about pipeline leak scenarios is the impact of different soil surface conditions on the belowground leak transport behavior and subsequently the NG leak classification. In this study, we conducted a series of controlled leak experiments, varying based on the surface conditions including snow, moist soil layers, asphalt, and grass. Data indicated that temporary rain and snow surface cover conditions result in CH4 concentrations extending 3 times further than the equivalent leak scenario under dry soil conditions, resulting in levels that pose heightened environmental and safety risks. Furthermore, after leak termination, CH4 trapped under snow, moist soil, and asphalt surface conditions persisted for up to ∼12 days, with 5–15% CH4 (v/v) conditions persisting underground for 7.5 days. Even after leak termination, NG continued to migrate laterally away from the leak source, extending the plume boundary by 2–4%. While efforts to study a wider range of environmental conditions are underway, the findings of this study provide crucial insight into identifying and prioritizing leaks from the perspectives of both safety and the environment.

减少天然气(NG)管道泄漏造成的甲烷(CH4)排放对于最大限度地减少全球变暖至关重要,同时还能为社区带来重要的安全效益。人们对管道泄漏情况了解不多的是不同土壤表面条件对地下泄漏传输行为的影响,以及随后对 NG 泄漏分类的影响。在本研究中,我们进行了一系列受控泄漏实验,根据雪、潮湿土层、沥青和草地等地表条件的不同而变化。数据表明,暂时的雨雪表面覆盖条件会导致 CH4 浓度比干燥土壤条件下的同等泄漏情况高出 3 倍,从而增加环境和安全风险。此外,泄漏终止后,在积雪、潮湿土壤和沥青表面条件下残留的 CH4 可持续长达 12 天,地下 5-15% CH4 (v/v) 的条件可持续 7.5 天。即使在泄漏终止后,NG 仍继续从泄漏源横向迁移,将羽流边界扩大了 2-4%。虽然目前正在努力研究更广泛的环境条件,但这项研究的结果为从安全和环境角度识别泄漏并确定其优先次序提供了重要的启示。
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引用次数: 0
Tracing the Environmental Effects of Mineral Fertilizer Application with Trace Elements and Strontium Isotope Variations 利用痕量元素和锶同位素变化追踪矿物肥料施用对环境的影响
IF 10.9 2区 环境科学与生态学 Q1 Environmental Science Pub Date : 2024-05-09 DOI: 10.1021/acs.estlett.4c00170
Robert C. Hill, Gordon D. Z. Williams, Zhen Wang, Jun Hu, Tayel El-Hasan, Owen W. Duckworth, Ewald Schnug, Roland Bol, Anjali Singh and Avner Vengosh*, 

Fertilizer utilization is critical for food security. This study examines the occurrence of trace elements (TEs) and Sr isotope (87Sr/86Sr) variations in phosphate rocks and mineral fertilizers from a sample collection representative of major phosphate producing countries. We show high concentrations of several TEs in phosphate rocks (n = 76) and their selective enrichment in phosphate fertilizers (n = 40) of specific origin. Consistent with the concentrations in parent phosphate rocks, phosphate fertilizers from the U.S. and Middle East have substantially higher concentrations of U, Cd, Cr, V, and Mo than those in fertilizers from China and India. Yet, fertilizers from China and India generally have higher concentrations of As. The 87Sr/86Sr in phosphate fertilizers directly mimic the composition of their source phosphate rocks, with distinctive higher ratios in fertilizers from China and India (0.70955–0.71939) relative to phosphate fertilizers from U.S. and Middle East (0.70748–0.70888). Potash fertilizers have less Sr and TEs and higher 87Sr/86Sr (0.72017–0.79016), causing higher 87Sr/86Sr in mixed NPK-fertilizers. Selective extraction (Mehlich III) of soils from an experimental agricultural site shows relative enrichment of potentially plant-available P, Sr, and TEs in topsoil, which is associated with Sr isotope variation toward the 87Sr/86Sr of the local utilized phosphate fertilizer.

化肥的利用对粮食安全至关重要。本研究考察了磷酸盐岩和矿物肥料中微量元素(TEs)的含量和 Sr 同位素(87Sr/86Sr)的变化,样本收集来自主要磷酸盐生产国。我们在磷酸盐岩(n = 76)中发现了多种微量元素的高浓度,并在特定来源的磷肥(n = 40)中发现了这些微量元素的选择性富集。与母磷酸盐岩中的浓度一致,美国和中东磷肥中的铀、镉、铬、钒和钼的浓度远远高于中国和印度磷肥中的浓度。然而,中国和印度化肥中的砷浓度通常更高。磷肥中的 87Sr/86Sr 直接反映了磷矿石的成分,中国和印度肥料中的 87Sr/86Sr 比率(0.70955-0.71939)明显高于美国和中东地区的磷肥(0.70748-0.70888)。钾肥中的 Sr 和 TE 较少,而 87Sr/86Sr 较高(0.72017-0.79016),导致氮磷钾混合肥料中的 87Sr/86Sr 较高。对农业实验区土壤的选择性萃取(Mehlich III)表明,表层土壤中植物可能利用的磷、锶和毒性元素相对富集,这与当地使用的磷肥中锶同位素的 87Sr/86Sr 变化有关。
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引用次数: 0
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Environmental Science & Technology Letters Environ.
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