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Solid-Phase Reactivity-Directed Extraction (SPREx): An Alternative Approach for Simultaneous Extraction, Identification, and Prioritization of Toxic Electrophiles Produced in Water Treatment Applications 固相反应定向萃取(SPREx):同时萃取、鉴定和优先处理水处理应用中产生的有毒电致发光物的替代方法
Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-09-20 DOI: 10.1021/acsenvironau.4c00025
Daisy N. Grace, Matthew N. Newmeyer, Carsten Prasse
Current strategies to assess water quality are ineffective at prioritizing the most toxic chemicals within a treated water sample. Although it is well known that oxidation byproducts (OBPs) from water treatment processes (e.g., chlorination and ozonation) are linked to adverse health outcomes such as skin diseases, reproductive toxicity, and various cancers, we are still unable to account for a large fraction of the toxicity drivers. Previous approaches utilize in vitro or in vivo assays to assess OBPs on an individual basis, which is too time- and resource-intensive considering the countless number of transformation byproducts of unknown toxicities that exist in treated waters. In vitro assays have also been developed to analyze the toxicity of OBPs in environmental mixtures, but these approaches do not provide identification information about the responsible toxicants. Furthermore, an additional challenge for OBP detection arises during the extraction and detection stages of analysis, as certain OBPs are typically lost using traditional extraction methods or are not detectable via liquid-chromatography–high-resolution mass spectrometry (LC-HRMS) without derivatization. To address these issues, we have developed the analytical assay Solid-Phase Reactivity-directed Extraction (SPREx), which aims to provide an all-in-one evaluation for (i) in chemico toxicity screening, (ii) extraction, (iii) detection, and (iv) identification via LC-HRMS. The performance of SPREx was evaluated by testing different nucleophile probes for the capture and detection of 24 different carbonyl compounds, which serve as model electrophiles and are known OBPs that provide unique extraction and detection challenges. SPREx provided distinct advantages for extraction recoveries and was an effective screening tool for carbonyl detection and quantification in complex water matrices such as drinking water and wastewater.
目前的水质评估策略无法有效地对处理过的水样中毒性最强的化学物质进行优先排序。尽管众所周知,水处理过程(如氯化和臭氧处理)产生的氧化副产物(OBPs)与皮肤病、生殖毒性和各种癌症等不良健康后果有关,但我们仍然无法解释大部分毒性驱动因素。以往的方法是利用体外或体内检测法来单独评估 OBPs,考虑到处理过的水体中存在无数毒性未知的转化副产物,这种方法过于耗费时间和资源。此外,还开发了体外检测方法来分析环境混合物中的 OBPs 的毒性,但这些方法无法提供相关毒性物质的鉴定信息。此外,在萃取和检测分析阶段,OBP 的检测还面临着额外的挑战,因为使用传统的萃取方法通常会损失某些 OBP,或者在没有衍生化的情况下无法通过液相色谱-高分辨质谱(LC-HRMS)检测到 OBP。为了解决这些问题,我们开发了固相反应定向萃取(Solid-Phase Reactivity-directed Extraction,SPREx)分析检测方法,旨在为(i) 化学毒性筛选、(ii) 萃取、(iii) 检测和(iv) 通过液相色谱-高分辨质谱(LC-HRMS)鉴定提供一体化的评估。通过测试不同亲核探针对 24 种不同羰基化合物的捕获和检测,对 SPREx 的性能进行了评估。SPREx 在萃取回收率方面具有明显优势,是饮用水和废水等复杂水基质中羰基检测和定量的有效筛选工具。
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引用次数: 0
Recent Advances in Technologies for Phosphate Removal and Recovery: A Review 磷酸盐去除和回收技术的最新进展:综述
Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-09-11 DOI: 10.1021/acsenvironau.3c00069
Mallikarjuna N. Nadagouda, Gaiven Varshney, Vikas Varshney, Charifa A. Hejase
Phosphorus is a nonrenewable resource, yet an essential nutrient in crop fertilizers that helps meet growing agricultural and food demands. As a limiting nutrient for primary producers, an excess amount of phosphorus entering water sources through agricultural runoff can lead to eutrophication events downstream. Therefore, to address global issues associated with the depletion of phosphate rock reserves and minimize the eutrophication of water bodies, numerous studies have investigated the removal and recovery of phosphates in usable forms using various chemical, physical, and biological methods. This review provides a comprehensive and critical evaluation of the literature, focusing on the widely employed adsorption and chemical precipitation for phosphate recovery from various wastewaters. Several experimental performance parameters including temperature, pH, coexisting ions (e.g., NO3, HCO3, Cl, SO42–), surface area, porosity, and calcination are highlighted for their importance in optimizing adsorption capacity and struvite crystallization/precipitation. Furthermore, the morphological and structural characterization of various selected adsorbents and precipitated struvite crystals is discussed.
磷是一种不可再生资源,但却是作物肥料中不可或缺的养分,有助于满足日益增长的农业和粮食需求。作为初级生产者的一种限制性养分,过量的磷通过农业径流进入水源会导致下游水体富营养化。因此,为了解决与磷矿石储量枯竭相关的全球性问题,并最大限度地减少水体富营养化,许多研究都采用了各种化学、物理和生物方法来研究如何去除和回收可用形式的磷酸盐。本综述对相关文献进行了全面而严谨的评估,重点介绍了从各种废水中回收磷酸盐时广泛采用的吸附法和化学沉淀法。重点介绍了一些实验性能参数,包括温度、pH 值、共存离子(如 NO3-、HCO3-、Cl-、SO42-)、表面积、孔隙率和煅烧,因为这些参数对优化吸附能力和硬石膏结晶/沉淀非常重要。此外,还讨论了各种选定吸附剂和沉淀的闪石晶体的形态和结构特征。
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引用次数: 0
Microbial Community Changes across Time and Space in a Constructed Wetland 人工湿地微生物群落的时空变化
Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-26 DOI: 10.1021/acsenvironau.4c00021
Zeinah Elhaj Baddar, Raven Bier, Breann Spencer, Xiaoyu Xu
Constructed wetlands are artificial ecosystems designed to replicate natural wetland processes. Microbial communities play a pivotal role in cycling essential elements, particularly sulfur, which is crucial for trace metal fixation and remobilization in these ecosystems. By their response to their environment, microbial communities act as biological indicators of the wetland performance. To address knowledge gaps pertinent to the changes in trace metal bioavailability in relation to microbial activities in the H-02 constructed wetland, we performed this study to investigate temporal and spatial variations in microbial communities by using molecular biology tools. Quantitative polymerase chain reaction and next generation sequencing techniques were employed to analyze archaeal and bacterial groups associated with sulfur and methane cycling. Alpha diversity indices were used to assess species richness, evenness, and dominance. Results indicated high gene abundance of Desulfuromonas (5.37 × 106 g.cell–1), methane oxidizing bacteria (6.92 × 106 g.cell–1), and methanogenic microorganisms (3.02 × 105 g.cell–1) during cool months. Warm months were marked by sulfate reducing bacteria dominance (3.31 × 106 g.cell–1), potentially due to competitive interactions and environmental conditions, higher temperatures, and lower redox potential. Spatial variability among microbial groups was insignificant, but trends in gene abundance indicated complex factors influencing these groups. Next generation sequencing data demonstrated Firmicutes as the most abundant phylum with over 50% regardless of the season or sampling location. Cool months exhibited higher alpha diversity than warm months. Overall, this study showed that seasonal changes significantly impacted the microbial communities in the H-02 constructed wetland that are associated with the sulfur cycle and eventually trace metal biogeochemistry, revealing two distinct mechanisms of the sulfur cycle between the two main seasons, whereas spatial variability effects were not conclusive.
人工湿地是旨在复制自然湿地过程的人工生态系统。在这些生态系统中,微生物群落在重要元素(尤其是对痕量金属固定和再移动至关重要的硫)的循环中发挥着关键作用。微生物群落对环境的反应是湿地性能的生物指标。为了填补与 H-02 人工湿地微生物活动相关的痕量金属生物利用率变化方面的知识空白,我们利用分子生物学工具对微生物群落的时空变化进行了研究。定量聚合酶链反应和新一代测序技术被用来分析与硫和甲烷循环相关的古细菌和细菌群。阿尔法多样性指数用于评估物种丰富度、均匀度和优势度。结果表明,在凉爽月份,脱硫单胞菌(5.37 × 106 g.cell-1)、甲烷氧化细菌(6.92 × 106 g.cell-1)和产甲烷微生物(3.02 × 105 g.cell-1)的基因丰度较高。暖月则以硫酸盐还原菌(3.31 × 106 g.cell-1)为主,这可能是由于竞争性相互作用和环境条件、较高的温度和较低的氧化还原电位造成的。微生物群之间的空间变异并不显著,但基因丰度的变化趋势表明影响这些微生物群的因素很复杂。下一代测序数据表明,无论季节或取样地点如何,固着菌门都是数量最多的门类,占 50%以上。凉爽月份的α多样性高于温暖月份。总之,这项研究表明,季节变化对 H-02 人工湿地中与硫循环和最终痕量金属生物地球化学有关的微生物群落产生了重大影响,揭示了硫循环在两个主要季节之间的两种不同机制,而空间变化的影响并不确定。
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引用次数: 0
Simultaneous Oxidation of Trace Organics and Sorption of Trace Metals by Ferrate (Fe(VI))-Coated Sand in Synthetic Wastewater Effluent 合成洗涤剂废水中铁酸铜(Fe(VI))包覆砂对痕量有机物的同时氧化作用和对痕量金属的吸附作用
IF 6.7 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-10 DOI: 10.1021/acsenvironau.4c0002410.1021/acsenvironau.4c00024
Fanny E. K. Okaikue-Woodi, Reyna Morales Lumagui and Jessica R. Ray*, 

The increased presence of toxic chemicals in aquatic matrices and their associated health effects raise the need for more effective treatment technologies. The application of Fe(VI), an advanced oxidation treatment agent with disinfecting and coagulating capabilities, is limited by Fe(VI) aqueous instability. Our previous study proposed an Fe(VI)-coated sand media to overcome this constraint and demonstrated that Fe(VI)-coated sand was an effective medium for the treatment of phenolic compounds. In this study, we assessed the potential of the media for treatment of acetaminophen (ACM), benzotriazole (BZT), sulfamethoxazole (SMX), copper (Cu), lead (Pb), and zinc (Zn)─common contaminants found in wastewater effluents─in ultrapure and synthetic wastewater effluent. Fe(VI)-coated sand reactivity was influenced by the solution pH and aqueous chemistry. For example, the removal of Pb improved by 39% in the presence of trace organics, indicating that trace metal removal was enhanced by Fe(III) phases formed during Fe(VI) reactions with trace organics. While oxidation of trace organic compounds increased as pH decreased, trace metal sorption was more favorable at higher pH (i.e., pH 8 and 9). The oxidation efficiency of trace organics by the media was the highest for ACM and SMX while BZT degradation was limited due to formation of Cu–BZT complexes. Batch tests in synthetic wastewater effluent revealed that the presence of divalent cations (i.e., Ca2+ and Mg2+) can catalyze Fe(VI) self-decay and promote Fe(III) production and subsequent trace metal removal; however, oxidation of trace organics was hindered in this matrix. This study highlights the potential for Fe(VI)-coated sand application for the treatment of complex matrices more representative of natural and engineered aquatic systems.

水生基质中有毒化学物质的增加及其对健康的影响,提出了对更有效处理技术的需求。Fe(VI)是一种具有消毒和混凝功能的高级氧化处理剂,但其应用受到Fe(VI)水不稳定性的限制。我们之前的研究提出了一种铁(六价铬)涂层砂介质来克服这一限制,并证明铁(六价铬)涂层砂是处理酚类化合物的有效介质。在本研究中,我们评估了该介质处理超纯废水和合成废水中对乙酰氨基酚 (ACM)、苯并三唑 (BZT)、磺胺甲噁唑 (SMX)、铜 (Cu)、铅 (Pb) 和锌 (Zn) -- 废水中常见污染物 -- 的潜力。铁(VI)包覆砂的反应活性受溶液 pH 值和水化学的影响。例如,在有痕量有机物存在的情况下,铅的去除率提高了 39%,这表明在铁(VI)与痕量有机物反应过程中形成的铁(III)相提高了痕量金属的去除率。虽然痕量有机化合物的氧化作用随着 pH 值的降低而增强,但在 pH 值较高时(即 pH 值为 8 和 9 时)更有利于痕量金属的吸附。介质对痕量有机物的氧化效率最高的是 ACM 和 SMX,而 BZT 的降解则因 Cu-BZT 复合物的形成而受到限制。在合成废水中进行的批量试验表明,二价阳离子(即 Ca2+ 和 Mg2+)的存在可催化铁(VI)自衰变,促进铁(III)的生成和随后的痕量金属去除;然而,在这种基质中,痕量有机物的氧化受到阻碍。这项研究突出表明,Fe(VI)涂层砂有可能被用于处理更能代表自然和工程水生系统的复杂基质。
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引用次数: 0
Simultaneous Oxidation of Trace Organics and Sorption of Trace Metals by Ferrate (Fe(VI))-Coated Sand in Synthetic Wastewater Effluent 合成洗涤剂废水中铁酸铜(Fe(VI))包覆砂对痕量有机物的同时氧化作用和对痕量金属的吸附作用
IF 6.7 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-10 DOI: 10.1021/acsenvironau.4c00024
Fanny E. K. Okaikue-Woodi, Reyna Morales Lumagui, Jessica R. Ray
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引用次数: 0
Assessing the Relative Sustainability of Point-of-Use Water Disinfection Technologies for Off-Grid Communities 评估离网社区用水点消毒技术的相对可持续性
Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-09 DOI: 10.1021/acsenvironau.4c00017
Bright C. Elijah, Ali Ahmad, Yalin Li, Jaime Plazas-Tuttle, Lewis S. Rowles
Point-of-use (POU) water disinfection technologies can be adopted to provide access to safe drinking water by treating water at the household level; however, navigating various POU disinfection technologies can be difficult. While numerous conventional POU devices exist, emerging technologies using novel materials or advanced processes have been under development and claim to be of lower cost with higher treatment capacity. However, it is unclear if these claims are substantiated and how novel technologies compare to conventional ones in terms of cost and environmental impacts when providing the same service (i.e., achieving a necessary level of disinfection for safe drinking water). This research assessed the sustainability of four different POU technologies (chlorination using sodium hypochlorite, a silver-nanoparticle-enabled ceramic water filter, ultraviolet mercury lamps, and ultraviolet light-emitting diodes). Leveraging open-source Python packages (QSDsan and EXPOsan), the cost and environmental impacts of these POU technologies were assessed using techno-economic analysis and life cycle assessment as per capita cost (USD·cap–1·yr–1) and global warming potential (kg CO2 eq·cap–1·yr–1). Impacts of water quality parameters (e.g., turbidity, hardness) were quantified for both surface water and groundwater, and uncertainty and sensitivity analyses were used to identify which assumptions influence outcomes. All technologies were further evaluated across ranges of adoption times, and contextual analysis was performed to evaluate the implications of technology deployment across the world. Results of this study can potentially provide valuable insights for decision-makers, nonprofit organizations, and future researchers in developing sustainable approaches for ensuring access to safe drinking water through POU technologies.
使用点(POU)水消毒技术可通过在家庭层面处理水,为人们提供安全的饮用水;然而,驾驭各种 POU 消毒技术可能很困难。虽然有许多传统的 POU 设备,但使用新型材料或先进工艺的新兴技术也在开发之中,并声称成本更低,处理能力更强。然而,目前还不清楚这些说法是否属实,也不清楚在提供相同服务(即达到安全饮用水所需的消毒水平)时,新型技术与传统技术在成本和环境影响方面的比较。这项研究评估了四种不同的 POU 技术(使用次氯酸钠进行氯化、银纳米粒子陶瓷滤水器、紫外线汞灯和紫外线发光二极管)的可持续性。利用开源 Python 软件包(QSDsan 和 EXPOsan),通过技术经济分析和生命周期评估,以人均成本(美元-cap-1-yr-1)和全球升温潜能值(千克二氧化碳当量-cap-1-yr-1)评估了这些 POU 技术的成本和环境影响。对地表水和地下水的水质参数(如浊度、硬度)的影响进行了量化,并使用不确定性和敏感性分析来确定哪些假设会影响结果。在采用时间范围内对所有技术进行了进一步评估,并进行了背景分析,以评估技术在全球范围内部署的影响。这项研究的结果有可能为决策者、非营利组织和未来的研究人员提供有价值的见解,帮助他们制定可持续的方法,确保通过 POU 技术获得安全饮用水。
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引用次数: 0
Assessing the Relative Sustainability of Point-of-Use Water Disinfection Technologies for Off-Grid Communities 评估离网社区用水点消毒技术的相对可持续性
IF 6.7 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-07-09 DOI: 10.1021/acsenvironau.4c0001710.1021/acsenvironau.4c00017
Bright C. Elijah, Ali Ahmad, Yalin Li, Jaime Plazas-Tuttle and Lewis S. Rowles*, 

Point-of-use (POU) water disinfection technologies can be adopted to provide access to safe drinking water by treating water at the household level; however, navigating various POU disinfection technologies can be difficult. While numerous conventional POU devices exist, emerging technologies using novel materials or advanced processes have been under development and claim to be of lower cost with higher treatment capacity. However, it is unclear if these claims are substantiated and how novel technologies compare to conventional ones in terms of cost and environmental impacts when providing the same service (i.e., achieving a necessary level of disinfection for safe drinking water). This research assessed the sustainability of four different POU technologies (chlorination using sodium hypochlorite, a silver-nanoparticle-enabled ceramic water filter, ultraviolet mercury lamps, and ultraviolet light-emitting diodes). Leveraging open-source Python packages (QSDsan and EXPOsan), the cost and environmental impacts of these POU technologies were assessed using techno-economic analysis and life cycle assessment as per capita cost (USD·cap–1·yr–1) and global warming potential (kg CO2 eq·cap–1·yr–1). Impacts of water quality parameters (e.g., turbidity, hardness) were quantified for both surface water and groundwater, and uncertainty and sensitivity analyses were used to identify which assumptions influence outcomes. All technologies were further evaluated across ranges of adoption times, and contextual analysis was performed to evaluate the implications of technology deployment across the world. Results of this study can potentially provide valuable insights for decision-makers, nonprofit organizations, and future researchers in developing sustainable approaches for ensuring access to safe drinking water through POU technologies.

使用点(POU)水消毒技术可通过在家庭层面处理水,为人们提供安全的饮用水;然而,驾驭各种 POU 消毒技术可能很困难。虽然有许多传统的 POU 设备,但使用新型材料或先进工艺的新兴技术也在开发之中,并声称成本更低,处理能力更强。然而,目前还不清楚这些说法是否属实,也不清楚在提供相同服务(即达到安全饮用水所需的消毒水平)时,新型技术与传统技术在成本和环境影响方面的比较。这项研究评估了四种不同的 POU 技术(使用次氯酸钠进行氯化、银纳米粒子陶瓷滤水器、紫外线汞灯和紫外线发光二极管)的可持续性。利用开源 Python 软件包(QSDsan 和 EXPOsan),通过技术经济分析和生命周期评估,以人均成本(美元-cap-1-yr-1)和全球升温潜能值(千克二氧化碳当量-cap-1-yr-1)评估了这些 POU 技术的成本和环境影响。对地表水和地下水的水质参数(如浊度、硬度)的影响进行了量化,并使用不确定性和敏感性分析来确定哪些假设会影响结果。在采用时间范围内对所有技术进行了进一步评估,并进行了背景分析,以评估技术在全球范围内部署的影响。这项研究的结果有可能为决策者、非营利组织和未来的研究人员提供有价值的见解,帮助他们制定可持续的方法,确保通过 POU 技术获得安全饮用水。
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引用次数: 0
Safer Solvents for Active Pharmaceutical Ingredient Purification Using Column Chromatography 使用柱色谱法纯化活性药物成分的更安全溶剂
Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-24 DOI: 10.1021/acsenvironau.4c00015
Christian Ayafor, Toren Burton, Nathaniel George, Gregory Morose, Hsi-Wu Wong
Column chromatography is a technique widely used for the purification of active pharmaceutical ingredients (APIs). One of the common solvent systems used by this technique is blends of dichloromethane (DCM) and methanol (MeOH), thereby exposing workers to health and safety risks and making the pharmaceutical sector one of the major contributors to chlorinated solvent waste. In this work, API separation and purification using several alternative safer solvent blends in column chromatography were evaluated and compared to DCM/MeOH. Ibuprofen and acetaminophen were used as model APIs, and caffeine was used as a model additive. Overall, some of the safer solvent blends tested provided better performance, with higher API recovery and purity compared to DCM/MeOH, in addition to potential health, safety, and environmental benefits. Specifically, blends of heptane/ethyl acetate and heptane/methyl acetate showed the most promise. Our work demonstrates the potential of these safer solvent blends as possible replacements for DCM/MeOH in API purification, thereby addressing a critical safety concern in the pharmaceutical industry.
柱层析是一种广泛用于纯化活性药物成分 (API) 的技术。这种技术常用的溶剂系统之一是二氯甲烷(DCM)和甲醇(MeOH)的混合物,从而使工人面临健康和安全风险,并使制药行业成为产生含氯溶剂废物的主要行业之一。在这项工作中,对柱层析中使用几种更安全的混合溶剂进行原料药分离和纯化进行了评估,并与 DCM/MeOH 进行了比较。布洛芬和对乙酰氨基酚被用作示范原料药,咖啡因被用作示范添加剂。总体而言,与 DCM/MeOH 相比,一些经测试的更安全溶剂混合物性能更好,原料药回收率和纯度更高,此外还具有潜在的健康、安全和环境效益。具体来说,庚烷/醋酸乙酯和庚烷/醋酸甲酯的混合物最有前景。我们的研究表明,这些更安全的混合溶剂有可能在原料药提纯过程中替代 DCM/MeOH,从而解决制药行业的一个关键安全问题。
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引用次数: 0
Safer Solvents for Active Pharmaceutical Ingredient Purification Using Column Chromatography 使用柱色谱法纯化活性药物成分的更安全溶剂
IF 6.7 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-24 DOI: 10.1021/acsenvironau.4c0001510.1021/acsenvironau.4c00015
Christian Ayafor, Toren Burton, Nathaniel George, Gregory Morose and Hsi-Wu Wong*, 

Column chromatography is a technique widely used for the purification of active pharmaceutical ingredients (APIs). One of the common solvent systems used by this technique is blends of dichloromethane (DCM) and methanol (MeOH), thereby exposing workers to health and safety risks and making the pharmaceutical sector one of the major contributors to chlorinated solvent waste. In this work, API separation and purification using several alternative safer solvent blends in column chromatography were evaluated and compared to DCM/MeOH. Ibuprofen and acetaminophen were used as model APIs, and caffeine was used as a model additive. Overall, some of the safer solvent blends tested provided better performance, with higher API recovery and purity compared to DCM/MeOH, in addition to potential health, safety, and environmental benefits. Specifically, blends of heptane/ethyl acetate and heptane/methyl acetate showed the most promise. Our work demonstrates the potential of these safer solvent blends as possible replacements for DCM/MeOH in API purification, thereby addressing a critical safety concern in the pharmaceutical industry.

柱层析是一种广泛用于纯化活性药物成分 (API) 的技术。这种技术常用的溶剂系统之一是二氯甲烷(DCM)和甲醇(MeOH)的混合物,从而使工人面临健康和安全风险,并使制药行业成为产生含氯溶剂废物的主要行业之一。在这项工作中,对柱层析中使用几种更安全的混合溶剂进行原料药分离和纯化进行了评估,并与 DCM/MeOH 进行了比较。布洛芬和对乙酰氨基酚被用作示范原料药,咖啡因被用作示范添加剂。总体而言,与 DCM/MeOH 相比,一些经测试的更安全溶剂混合物性能更好,原料药回收率和纯度更高,此外还具有潜在的健康、安全和环境效益。具体来说,庚烷/醋酸乙酯和庚烷/醋酸甲酯的混合物最有前景。我们的研究表明,这些更安全的混合溶剂有可能在原料药提纯过程中替代 DCM/MeOH,从而解决制药行业的一个关键安全问题。
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引用次数: 0
Exploring Drivers of Historic Mercury Trends in Beluga Whales Using an Ecosystem Modeling Approach 利用生态系统建模方法探索白鲸汞历史趋势的驱动因素
IF 6.7 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-04 DOI: 10.1021/acsenvironau.3c0007210.1021/acsenvironau.3c00072
Emma J. Gillies*, Mi-Ling Li, Villy Christensen, Carie Hoover, Kristen J. Sora, Lisa L. Loseto, William W. L. Cheung, Hélène Angot and Amanda Giang*, 

While mercury occurs naturally in the environment, human activity has significantly disturbed its biogeochemical cycle. Inorganic mercury entering aquatic systems can be transformed into methylmercury, a strong neurotoxicant that builds up in organisms and affects ecosystem and public health. In the Arctic, top predators such as beluga whales, an ecologically and culturally significant species for many Inuit communities, can contain high concentrations of methylmercury. Historical mercury concentrations in beluga in the western Canadian Arctic’s Beaufort Sea cannot be explained by mercury emission trends alone; in addition, they could potentially be driven by climate change impacts, such as rising temperatures and sea ice melt. These changes can affect mercury bioaccumulation through different pathways, including ecological and mercury transport processes. In this study, we explore key drivers of mercury bioaccumulation in the Beaufort Sea beluga population using Ecopath with Ecosim, an ecosystem modeling approach, and scenarios of environmental change informed by Western Science and Inuvialuit Knowledge. Comparing the effect of historical sea ice cover, sea surface temperature, and freshwater discharge time series, modeling suggests that the timing of historical increases and decreases in beluga methylmercury concentrations can be better explained by the resulting changes to ecosystem productivity rather than by those to mercury inputs and that all three environmental drivers could partially explain the decrease in mercury concentrations in beluga after the mid-1990s. This work highlights the value of multiple knowledge systems and exploratory modeling methods in understanding environmental change and contaminant cycling. Future work building on this research could inform climate change adaptation efforts and inform management decisions in the region.

虽然汞天然存在于环境中,但人类活动极大地干扰了汞的生物地球化学循环。进入水生系统的无机汞可转化为甲基汞,这是一种强烈的神经毒剂,会在生物体内积聚,影响生态系统和公众健康。在北极地区,白鲸等顶级食肉动物可能含有高浓度的甲基汞,而白鲸对许多因纽特社区来说是一种具有重要生态和文化意义的物种。加拿大西部北极波弗特海白鲸体内的历史汞浓度不能仅用汞排放趋势来解释;此外,它们还可能受到气候变化的影响,如气温上升和海冰融化。这些变化会通过不同途径影响汞的生物累积,包括生态和汞迁移过程。在这项研究中,我们利用生态系统建模方法 Ecosim 中的 Ecopath 以及西方科学和因纽维阿鲁特知识(Inuvialuit Knowledge)提供的环境变化情景,探讨了波弗特海白鲸种群汞生物累积的关键驱动因素。通过比较历史上海冰覆盖率、海面温度和淡水排放时间序列的影响,建模表明,历史上白鲸甲基汞浓度增加和减少的时间可以更好地用生态系统生产力的变化而不是汞输入的变化来解释,而且所有三个环境驱动因素都可以部分解释 20 世纪 90 年代中期以后白鲸体内汞浓度的下降。这项工作凸显了多种知识体系和探索性建模方法在理解环境变化和污染物循环方面的价值。在此研究基础上开展的未来工作可为该地区适应气候变化的努力和管理决策提供信息。
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