首页 > 最新文献

Journal of environmental sciences最新文献

英文 中文
Evaluating the performance and influencing factors of three portable black carbon monitors for field measurement 评价三种便携式野外测量黑碳监测仪的性能及影响因素
IF 6.9 Q1 Environmental Science Pub Date : 2024-05-01 Epub Date: 2023-06-07 DOI: 10.1016/j.jes.2023.05.044
Liqing Wu , Yicheng Shen , Fei Che , Yuzhe Zhang , Jian Gao , Chong Wang

Black carbon (BC) is associated with adverse human health and climate change. Mapping BC spatial distribution imperatively requires low-cost and portable devices. Several portable BC monitors are commercially available, but their accuracy and reliability are not always satisfactory during continuous field observation. This study evaluated three models of portable black carbon monitors, C12, MA350 and DST, and investigates the factors that affect their performance. The monitors were tested in urban Beijing, where portable devices running for one month alongside a regular-size reference aethalometer AE33. The study considers several factors that could influence the monitors' performance, including ambient weather, aerosol composition, loading artifacts, and built-in algorithms. The results show that MA350 and DST present considerable discrepancies to the reference instrument, mainly occurring at lower concentrations (0–500 ng/m3) and higher concentrations (2500–8000 ng/m3), respectively. These discrepancies were likely caused by the anomalous noise of MA350 and the loading artifacts of DST. The study also suggests that the ambient environment has limited influence on the monitors' performance, but loading artifacts and accompanying compensation algorithms can result in unrealistic data. Based on the evaluation, the study suggests that C12 is the best choice for unsupervised field measurement, DST should be used in scenarios where frequent maintenance is available, and MA350 is suitable for research purposes with post-processing applicable. The study highlights the importance of assigning portable BC monitors to appropriate applications and the need for optimized real-time compensation algorithms.

黑碳(BC)与不利的人类健康和气候变化有关。绘制BC空间分布迫切需要低成本和便携式设备。市面上有几种便携式BC监测仪,但在连续现场观测过程中,它们的准确性和可靠性并不总是令人满意。本研究评估了C12、MA350和DST三种型号的便携式炭黑监测仪,并调查了影响其性能的因素。这些监测仪在北京进行了测试,便携式设备与常规尺寸的参考以太温度计AE33一起运行一个月。该研究考虑了可能影响监测器性能的几个因素,包括环境天气、气溶胶成分、加载伪影和内置算法。结果表明,MA350和DST与参考仪器存在相当大的差异,主要发生在较低浓度(0–500 ng/m3)和较高浓度(2500–8000 ng/m3)下。这些差异可能是由MA350的异常噪声和DST的加载伪影引起的。该研究还表明,周围环境对监视器性能的影响有限,但加载伪影和伴随的补偿算法可能会导致不切实际的数据。基于评估,该研究表明C12是无监督现场测量的最佳选择,DST应用于可进行频繁维护的场景,MA350适用于后处理的研究目的。该研究强调了将便携式BC监视器分配给适当应用的重要性,以及优化实时补偿算法的必要性。
{"title":"Evaluating the performance and influencing factors of three portable black carbon monitors for field measurement","authors":"Liqing Wu ,&nbsp;Yicheng Shen ,&nbsp;Fei Che ,&nbsp;Yuzhe Zhang ,&nbsp;Jian Gao ,&nbsp;Chong Wang","doi":"10.1016/j.jes.2023.05.044","DOIUrl":"https://doi.org/10.1016/j.jes.2023.05.044","url":null,"abstract":"<div><p><span><span>Black carbon (BC) is associated with adverse human health and climate change. Mapping BC spatial distribution imperatively requires low-cost and portable devices. Several portable BC monitors are commercially available, but their accuracy and reliability are not always satisfactory during continuous field observation. This study evaluated three models of portable black carbon monitors, C12, MA350 and DST, and investigates the factors that affect their performance. The monitors were tested in urban Beijing, where portable devices running for one month alongside a regular-size reference aethalometer AE33. The study considers several factors that could influence the monitors' performance, including ambient weather, </span>aerosol composition, loading artifacts, and built-in algorithms. The results show that MA350 and DST present considerable discrepancies to the reference instrument, mainly occurring at lower concentrations (0–500 ng/m</span><sup>3</sup>) and higher concentrations (2500–8000 ng/m<sup>3</sup>), respectively. These discrepancies were likely caused by the anomalous noise of MA350 and the loading artifacts of DST. The study also suggests that the ambient environment has limited influence on the monitors' performance, but loading artifacts and accompanying compensation algorithms can result in unrealistic data. Based on the evaluation, the study suggests that C12 is the best choice for unsupervised field measurement, DST should be used in scenarios where frequent maintenance is available, and MA350 is suitable for research purposes with post-processing applicable. The study highlights the importance of assigning portable BC monitors to appropriate applications and the need for optimized real-time compensation algorithms.</p></div>","PeriodicalId":15774,"journal":{"name":"Journal of environmental sciences","volume":"139 ","pages":"Pages 320-333"},"PeriodicalIF":6.9,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49746743","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Sustainable management of campus fallen leaves through low-temperature pyrolysis and application in Pb immobilization 低温热解对校园落叶的可持续管理及其在Pb固定化中的应用
IF 6.9 Q1 Environmental Science Pub Date : 2024-05-01 Epub Date: 2023-06-07 DOI: 10.1016/j.jes.2023.05.043
Rongli Tan , Ke Li , Yue Sun , Xiaoliang Fan , Zhengtao Shen , Lingyi Tang

Realizing campus sustainability requires the environmental-friendly and economical treatment of tremendous fallen leaves. Producing fallen leaf biochar at a low temperature is a candidate approach. In this study, six common types of fallen leaves on the campus were pyrolyzed at 300 °C. The obtained biochars were characterized and the adsorption mechanisms of lead (Pb) by the fallen leaf biochars were investigated. The adsorption capacity of leaf biochar for Pb was relatively high, up to 209 mg/g (Yulania denudata leaf biochar). Adsorption of Pb onto active sites was the rate-limiting step for most leaf biochars. But for Platanus leaf biochar, intraparticle diffusion of Pb2+ dominated owing to the lowest adsorption capacity. However, the highest exchangeable Pb fraction (27%) indicated its potential for removing aqueous Pb2+. Ginkgo and Prunus cerasifera leaf biochar immobilized Pb by surface complexation and precipitation as lead oxalate. Hence, they were suitable for soil heavy metal remediation. This study shed the light on the sustainable utilization of campus fallen leaves and the application of fallen leaf biochars in heavy metal remediation.

实现校园可持续发展需要对大量落叶进行环保和经济的处理。在低温下生产落叶生物炭是一种可行的方法。在这项研究中,校园里六种常见类型的落叶在300°C下被热解。对所获得的生物炭进行了表征,并研究了落叶生物炭对铅的吸附机理。叶用生物炭对Pb的吸附量较高,可达209mg/g(光叶生物炭)。Pb在活性位点上的吸附是大多数叶片生物炭的限速步骤。但对于Platanus叶生物炭,由于吸附能力最低,Pb2+的颗粒内扩散占主导地位。然而,最高的可交换Pb组分(27%)表明了其去除水性Pb2+的潜力。银杏和樱桃叶生物炭以草酸铅的形式通过表面络合沉淀固定化铅。因此,它们适合于土壤重金属修复。本研究为校园落叶的可持续利用及落叶生物炭在重金属修复中的应用提供了依据。
{"title":"Sustainable management of campus fallen leaves through low-temperature pyrolysis and application in Pb immobilization","authors":"Rongli Tan ,&nbsp;Ke Li ,&nbsp;Yue Sun ,&nbsp;Xiaoliang Fan ,&nbsp;Zhengtao Shen ,&nbsp;Lingyi Tang","doi":"10.1016/j.jes.2023.05.043","DOIUrl":"https://doi.org/10.1016/j.jes.2023.05.043","url":null,"abstract":"<div><p>Realizing campus sustainability requires the environmental-friendly and economical treatment of tremendous fallen leaves. Producing fallen leaf biochar at a low temperature is a candidate approach. In this study, six common types of fallen leaves on the campus were pyrolyzed at 300 °C. The obtained biochars were characterized and the adsorption mechanisms of lead (Pb) by the fallen leaf biochars were investigated. The adsorption capacity of leaf biochar for Pb was relatively high, up to 209 mg/g (<em>Yulania denudata</em> leaf biochar). Adsorption of Pb onto active sites was the rate-limiting step for most leaf biochars. But for <em>Platanus</em> leaf biochar, intraparticle diffusion of Pb<sup>2+</sup> dominated owing to the lowest adsorption capacity. However, the highest exchangeable Pb fraction (27%) indicated its potential for removing aqueous Pb<sup>2+</sup>. <em>Ginkgo</em> and <em>Prunus cerasifera</em> leaf biochar immobilized Pb by surface complexation and precipitation as lead oxalate. Hence, they were suitable for soil heavy metal remediation. This study shed the light on the sustainable utilization of campus fallen leaves and the application of fallen leaf biochars in heavy metal remediation.</p></div>","PeriodicalId":15774,"journal":{"name":"Journal of environmental sciences","volume":"139 ","pages":"Pages 281-292"},"PeriodicalIF":6.9,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49746419","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Compositional evolution for mixed aerosols containing gluconic acid and typical nitrate and the effect of multiply factors on hygroscopicity 含葡萄糖酸和典型硝酸盐混合气溶胶的组分演化及多因素对吸湿性的影响
IF 6.9 Q1 Environmental Science Pub Date : 2024-05-01 Epub Date: 2022-11-12 DOI: 10.1016/j.jes.2022.10.050
Yue Zhu, Shufeng Pang, Yunhong Zhang

The aging process of atmospheric aerosols usually leads to a mixture of inorganic salts and organic compounds of anthropogenic origin. In organic compounds, polyhydroxy organic acids are important components, however, the study on composition and hygroscopic properties of the mixture containing inorganics and polyhydroxy organic acids is scanty. In this study, gluconic acid, the proxy of polyhydroxy organic acids, is mixed with the representative nitrate (Mg(NO3)2, Ca(NO3)2) to form aerosols. ATR–FTIR and optical microscopy are employed to study the component changes and hygroscopicity as a function of relative humidity. As relative humidity fluctuates, the FTIR–ATR spectra display that the internal mixed gluconic acid (CH2(CH)4(OH)5COOH) and nitrate can react to release acidic gases, forming relevant gluconate and further affecting the hygroscopicity. The specific presentation is particles cannot be recovered to their original size after the dehydration–hydration process and there will be some disparities in GF for mixed particles. For the gluconic acid–Ca(NO3)2/Mg(NO3)2 mixtures with molar ratios of 1:1, higher degree of reaction resulting in the production of large amounts of gluconate should be responsible to the lower hygroscopicity compared to ZSR model. For 1:2 gluconic acid–nitrate mixed systems (with higher nitrate content), the hygroscopicity of mixtures are higher than the ZSR prediction. A possible reason could be ‘salt-promoting effect’ on the organic fractions of the surplus inorganic salt in the mixture. These data can improve the chemical composition list evaluation, in turn hygroscopic properties and phase state of atmospheric aerosol, and then the climate effect.

大气气溶胶的老化过程通常导致人为来源的无机盐和有机化合物的混合物。在有机化合物中,多羟基有机酸是重要的组分,但对含有无机物和多羟基有机酸类的混合物的组成和吸湿性能的研究很少。在本研究中,将多羟基有机酸的替代物葡萄糖酸与代表性硝酸盐(Mg(NO3)2,Ca(NO3,2)混合形成气溶胶。ATR–FTIR和光学显微镜用于研究组分变化和吸湿性作为相对湿度的函数。随着相对湿度的波动,FTIR–ATR光谱显示,内部混合的葡萄糖酸(CH2(CH)4(OH)5COOH)和硝酸盐可以反应释放酸性气体,形成相关的葡萄糖酸盐,并进一步影响吸湿性。具体表现为颗粒在脱水-水合过程后无法恢复到原始尺寸,混合颗粒的GF会有一些差异。对于摩尔比为1:1的葡萄糖酸-Ca(NO3)2/Mg(NO2)2混合物,与ZSR模型相比,产生大量葡萄糖酸的反应程度越高,吸湿性越低。对于1:2葡萄糖酸-硝酸盐混合体系(硝酸盐含量较高),混合物的吸湿性高于ZSR预测。一个可能的原因可能是对混合物中多余无机盐的有机部分的“促盐作用”。这些数据可以改善化学成分清单的评估,进而改善大气气溶胶的吸湿性和相态,进而改善气候效应。
{"title":"Compositional evolution for mixed aerosols containing gluconic acid and typical nitrate and the effect of multiply factors on hygroscopicity","authors":"Yue Zhu,&nbsp;Shufeng Pang,&nbsp;Yunhong Zhang","doi":"10.1016/j.jes.2022.10.050","DOIUrl":"https://doi.org/10.1016/j.jes.2022.10.050","url":null,"abstract":"<div><p>The aging process of atmospheric aerosols usually leads to a mixture of inorganic salts and organic compounds of anthropogenic origin. In organic compounds, polyhydroxy organic acids are important components, however, the study on composition and hygroscopic properties of the mixture containing inorganics and polyhydroxy organic acids is scanty. In this study, gluconic acid, the proxy of polyhydroxy organic acids, is mixed with the representative nitrate (Mg(NO<sub>3</sub>)<sub>2</sub>, Ca(NO<sub>3</sub>)<sub>2</sub>) to form aerosols. ATR–FTIR and optical microscopy are employed to study the component changes and hygroscopicity as a function of relative humidity. As relative humidity fluctuates, the FTIR–ATR spectra display that the internal mixed gluconic acid (CH<sub>2</sub>(CH)<sub>4</sub>(OH)<sub>5</sub>COOH) and nitrate can react to release acidic gases, forming relevant gluconate and further affecting the hygroscopicity. The specific presentation is particles cannot be recovered to their original size after the dehydration–hydration process and there will be some disparities in GF for mixed particles. For the gluconic acid–Ca(NO<sub>3</sub>)<sub>2</sub>/Mg(NO<sub>3</sub>)<sub>2</sub> mixtures with molar ratios of 1:1, higher degree of reaction resulting in the production of large amounts of gluconate should be responsible to the lower hygroscopicity compared to ZSR model. For 1:2 gluconic acid–nitrate mixed systems (with higher nitrate content), the hygroscopicity of mixtures are higher than the ZSR prediction. A possible reason could be ‘salt-promoting effect’ on the organic fractions of the surplus inorganic salt in the mixture. These data can improve the chemical composition list evaluation, in turn hygroscopic properties and phase state of atmospheric aerosol, and then the climate effect.</p></div>","PeriodicalId":15774,"journal":{"name":"Journal of environmental sciences","volume":"139 ","pages":"Pages 206-216"},"PeriodicalIF":6.9,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49746552","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 1
Controllable chemical redox reactions to couple microbial degradation for organic contaminated sites remediation: A review 可控化学氧化还原反应耦合微生物降解在有机污染场地修复中的研究进展
IF 6.9 Q1 Environmental Science Pub Date : 2024-05-01 Epub Date: 2023-06-20 DOI: 10.1016/j.jes.2023.06.012
Bin Chen , Jiang Xu , Lizhong Zhu

Global environmental concern over organic contaminated sites has been progressively conspicuous during the process of urbanization and industrial restructuring. While traditional physical or chemical remediation technologies may significantly destroy the soil structure and function, coupling moderate chemical degradation with microbial remediation becomes a potential way for the green, economic, and efficient remediation of contaminated sites. Hence, this work systematically elucidates why and how to couple chemical technology with microbial remediation, mainly focused on the controllable redox reactions of organic contaminants. The rational design of materials structure, selective generation of reactive oxygen species, and estimation of degradation pathway are described for chemical oxidation. Meanwhile, current progress on efficient and selective reductions of organic contaminants (i.e., dechlorination, defluorination, -NO2 reduction) is introduced. Combined with the microbial remediation of contaminated sites, several consideration factors of how to couple chemical and microbial remediation are proposed based on both fundamental and practical points of view. This review will advance the understanding and development of chemical-microbial coupled remediation for organic contaminated sites.

在城市化和产业结构调整过程中,全球对有机污染场地的环境关注日益突出。虽然传统的物理或化学修复技术可能会严重破坏土壤结构和功能,但将适度的化学降解与微生物修复相结合,成为污染场地绿色、经济、高效修复的潜在途径。因此,本工作系统地阐述了为什么以及如何将化学技术与微生物修复相结合,主要集中在有机污染物的可控氧化还原反应上。介绍了化学氧化材料结构的合理设计、活性氧的选择性生成和降解途径的估计。同时,介绍了目前在高效选择性还原有机污染物(即脱氯、脱氟、-NO2还原)方面的进展。结合污染场地的微生物修复,从基础和实践两个角度提出了如何将化学修复与微生物修复相结合的几个考虑因素。这篇综述将促进对有机污染场地化学-微生物联合修复的理解和发展。
{"title":"Controllable chemical redox reactions to couple microbial degradation for organic contaminated sites remediation: A review","authors":"Bin Chen ,&nbsp;Jiang Xu ,&nbsp;Lizhong Zhu","doi":"10.1016/j.jes.2023.06.012","DOIUrl":"https://doi.org/10.1016/j.jes.2023.06.012","url":null,"abstract":"<div><p>Global environmental concern over organic contaminated sites has been progressively conspicuous during the process of urbanization and industrial restructuring. While traditional physical or chemical remediation technologies may significantly destroy the soil structure and function, coupling moderate chemical degradation with microbial remediation becomes a potential way for the green, economic, and efficient remediation of contaminated sites. Hence, this work systematically elucidates why and how to couple chemical technology with microbial remediation, mainly focused on the controllable redox reactions of organic contaminants. The rational design of materials structure, selective generation of reactive oxygen species, and estimation of degradation pathway are described for chemical oxidation. Meanwhile, current progress on efficient and selective reductions of organic contaminants (i.e., dechlorination, defluorination, -NO<sub>2</sub> reduction) is introduced. Combined with the microbial remediation of contaminated sites, several consideration factors of how to couple chemical and microbial remediation are proposed based on both fundamental and practical points of view. This review will advance the understanding and development of chemical-microbial coupled remediation for organic contaminated sites.</p></div>","PeriodicalId":15774,"journal":{"name":"Journal of environmental sciences","volume":"139 ","pages":"Pages 428-445"},"PeriodicalIF":6.9,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49746628","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 1
Distribution of per- and polyfluoroalkyl substances in blood, serum, and urine of patients with liver cancer and associations with liver function biomarkers 肝癌患者血液、血清和尿液中全氟烷基和多氟烷基物质的分布及其与肝功能生物标志物的关系
IF 6.9 Q1 Environmental Science Pub Date : 2024-05-01 Epub Date: 2023-05-25 DOI: 10.1016/j.jes.2023.05.026
Cao Dai , Lin Peng , Yanjie Li , Zhendong Li , Da Chen , Fei Wang , Nan Lin

Studies have shown that per- and polyfluoroalkyl substances (PFASs) may be hepatotoxic in animals or humans. However, data on clinical epidemiology are very limited. In this study, 21 PFASs were determined in patients with liver diseases, with the highest median concentrations detected in the serum sample (26.7 ng/mL), followed by blood (10.7 ng/mL) and urine (5.02 ng/mL). Higher total PFAS concentrations were found in hepatocellular carcinoma (HCC) patients compared to non-HCC patients, with significant discrepancies in serum and blood samples. Besides, significant correlations were also found among PFAS concentrations and age, gender, body mass index (BMI), and liver function biomarkers levels. For example, PFAS concentrations are significantly higher in males than in females; Several serum PFASs concentrations increase with age and BMI, while the serum perfluorohexane sulfonic acid (PFHxS) concentrations are negatively correlated with age. In addition, multiple regression models adjusted for age, gender and BMI found that increased serum perfluorobutane sulfonic acid (PFBS), perfluoroheptane sulfonic acid (PFHpS) and perfluorohexylphosphonic acid (PFHxPA) conentrations are correlated with elevated alkaline phosphatase (ALP), aspartate aminotransferase (AST), and alpha-fetoprotein (AFP) (p < 0.05). Our results provide epidemiological support for the future study on the potential clinical hepatotoxicity of PFAS.

研究表明,全氟烷基和多氟烷基物质(PFAS)可能对动物或人类具有肝毒性。然而,有关临床流行病学的数据非常有限。在这项研究中,在肝病患者中检测到21种PFAS,血清样本中检测到的中位浓度最高(26.7 ng/mL),其次是血液(10.7 ng/mL)和尿液(5.02 ng/mL)。与非肝细胞癌患者相比,肝细胞癌(HCC)患者的PFAS总浓度更高,血清和血液样本存在显著差异。此外,PFAS浓度与年龄、性别、体重指数(BMI)和肝功能生物标志物水平之间也存在显著相关性。例如,男性的全氟辛烷磺酸浓度明显高于女性;一些血清PFASs浓度随着年龄和BMI的增加而增加,而血清全氟己烷磺酸(PFHxS)浓度与年龄呈负相关。此外,经年龄、性别和BMI调整的多元回归模型发现,血清全氟丁烷磺酸(PFBS)、全氟庚烷磺酸(PFHpS)和全氟己基膦酸(PFHxPA)浓度的增加与碱性磷酸酶(ALP)、天冬氨酸氨基转移酶(AST),和甲胎蛋白(AFP)(p<0.05)。我们的结果为未来PFAS潜在临床肝毒性的研究提供了流行病学支持。
{"title":"Distribution of per- and polyfluoroalkyl substances in blood, serum, and urine of patients with liver cancer and associations with liver function biomarkers","authors":"Cao Dai ,&nbsp;Lin Peng ,&nbsp;Yanjie Li ,&nbsp;Zhendong Li ,&nbsp;Da Chen ,&nbsp;Fei Wang ,&nbsp;Nan Lin","doi":"10.1016/j.jes.2023.05.026","DOIUrl":"https://doi.org/10.1016/j.jes.2023.05.026","url":null,"abstract":"<div><p>Studies have shown that per- and polyfluoroalkyl substances (PFASs) may be hepatotoxic in animals or humans. However, data on clinical epidemiology are very limited. In this study, 21 PFASs were determined in patients with liver diseases, with the highest median concentrations detected in the serum sample (26.7 ng/mL), followed by blood (10.7 ng/mL) and urine (5.02 ng/mL). Higher total PFAS concentrations were found in hepatocellular carcinoma (HCC) patients compared to non-HCC patients, with significant discrepancies in serum and blood samples. Besides, significant correlations were also found among PFAS concentrations and age, gender, body mass index (BMI), and liver function biomarkers levels. For example, PFAS concentrations are significantly higher in males than in females; Several serum PFASs concentrations increase with age and BMI, while the serum perfluorohexane sulfonic acid (PFHxS) concentrations are negatively correlated with age. In addition, multiple regression models adjusted for age, gender and BMI found that increased serum perfluorobutane sulfonic acid (PFBS), perfluoroheptane sulfonic acid (PFHpS) and perfluorohexylphosphonic acid (PFHxPA) conentrations are correlated with elevated alkaline phosphatase (ALP), aspartate aminotransferase (AST), and alpha-fetoprotein (AFP) (<em>p</em> &lt; 0.05). Our results provide epidemiological support for the future study on the potential clinical hepatotoxicity of PFAS.</p></div>","PeriodicalId":15774,"journal":{"name":"Journal of environmental sciences","volume":"139 ","pages":"Pages 418-427"},"PeriodicalIF":6.9,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49746626","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Experimental and theoretical insight into carbamazepine degradation by chlorine‐based advanced oxidation processes: Efficiency, energy consumption, mechanism and DBPs formation 氯基高级氧化工艺降解卡马西平的实验和理论研究:效率、能耗、机理和dbp的形成
IF 6.9 Q1 Environmental Science Pub Date : 2024-05-01 Epub Date: 2023-05-22 DOI: 10.1016/j.jes.2023.05.012
Chunwei Liu , Zuo Tong How , Yue Ju , Li Feng , Xuefeng Ren , Mohamed Gamal El-Din

Chlorine has been widely used in different advanced oxidation processes (AOPs) for micropollutants removal. In this study, different chlorine-based AOPs, namely medium pressure (MP) UV/chlorine, low pressure (LP) UV/chlorine, and in-situ chlorination, were compared for carbamazepine (CBZ) removal efficiency, energy consumption, and disinfection by-products (DBPs) formation. All three processes could achieve nearly 100% CBZ removal, while the reaction time needed by in-situ chlorination was double the time required by UV/chlorine processes. The energy consumed per magnitude of CBZ removed (EE/O) of MP UV/chlorine was 13 times higher than that of LP UV/chlorine, and relative to that of in-situ chlorination process. Accordingly, MP and LP UV/chlorine processes generated one to two orders of magnitude more hydroxyl radicals (OH) and reactive chlorine species (RCS) than in-situ chlorination. Besides, RCS were the dominant reactive species, contributing to 78.3%, 75.6%, and 71.6% of CBZ removal in MP, LP UV/chlorine, and in-situ chlorination, respectively. According to the Gibbs free energy barriers between CBZ and RCS/OH calculated based on density functional theory (DFT), RCS had more reaction routes with CBZ and showed lower energy barrier in the main CBZ degradation pathways like epoxidation and formation of iminostilbene. When applied to secondary wastewater effluent, UV/chlorine and in-situ chlorination produced overall DBPs ranging from 104.77 to 135.41 µg/L. However, the production of chlorate during UV/chlorine processes was 15 times higher than that during in-situ chlorination.

氯已被广泛用于不同的高级氧化工艺(AOP)中,用于去除微污染物。在本研究中,比较了不同的氯基AOP,即中压(MP)UV/氯、低压(LP)UV/氯气和原位氯化,对卡马西平(CBZ)的去除效率、能耗和消毒副产物(DBP)的形成进行了比较。所有三种工艺都可以实现近100%的CBZ去除,而原位氯化所需的反应时间是UV/氯工艺所需时间的两倍。MP UV/氯每去除CBZ量值(EE/O)所消耗的能量是LP UV/氯的13倍,并且相对于原位氯化过程。因此,MP和LP紫外线/氯工艺产生的羟基自由基(•OH)和活性氯物种(RCS)比原位氯化多一到两个数量级。此外,RCS是主要的反应物种,在MP、LP UV/氯和原位氯化中对CBZ的去除率分别为78.3%、75.6%和71.6%。根据基于密度泛函理论(DFT)计算的CBZ和RCS/•OH之间的吉布斯自由能垒,RCS与CBZ的反应路线较多,在环氧化和亚氨基二苯形成等主要CBZ降解途径中表现出较低的能垒。当应用于二级废水时,紫外线/氯和原位氯化产生的总DBP范围为104.77至135.41µg/L。然而,紫外线/氯化过程中氯酸盐的产量是原位氯化过程的15倍。
{"title":"Experimental and theoretical insight into carbamazepine degradation by chlorine‐based advanced oxidation processes: Efficiency, energy consumption, mechanism and DBPs formation","authors":"Chunwei Liu ,&nbsp;Zuo Tong How ,&nbsp;Yue Ju ,&nbsp;Li Feng ,&nbsp;Xuefeng Ren ,&nbsp;Mohamed Gamal El-Din","doi":"10.1016/j.jes.2023.05.012","DOIUrl":"https://doi.org/10.1016/j.jes.2023.05.012","url":null,"abstract":"<div><p><span><span>Chlorine has been widely used in different advanced oxidation processes (AOPs) for </span>micropollutants removal. In this study, different chlorine-based AOPs, namely medium pressure (MP) UV/chlorine, low pressure (LP) UV/chlorine, and </span><em>in-situ</em> chlorination, were compared for carbamazepine (CBZ) removal efficiency, energy consumption, and disinfection by-products (DBPs) formation. All three processes could achieve nearly 100% CBZ removal, while the reaction time needed by <em>in-situ</em> chlorination was double the time required by UV/chlorine processes. The energy consumed per magnitude of CBZ removed (EE/O) of MP UV/chlorine was 13 times higher than that of LP UV/chlorine, and relative to that of <em>in-situ</em><span> chlorination process. Accordingly, MP and LP UV/chlorine processes generated one to two orders of magnitude more hydroxyl radicals (</span><sup>•</sup>OH) and reactive chlorine species (RCS) than <em>in-situ</em> chlorination. Besides, RCS were the dominant reactive species, contributing to 78.3%, 75.6%, and 71.6% of CBZ removal in MP, LP UV/chlorine, and <em>in-situ</em><span> chlorination, respectively. According to the Gibbs free energy barriers between CBZ and RCS/</span><sup>•</sup><span><span>OH calculated based on density functional theory (DFT), RCS had more reaction routes with CBZ and showed lower energy barrier in the main CBZ degradation pathways like </span>epoxidation and formation of iminostilbene. When applied to secondary wastewater effluent, UV/chlorine and </span><em>in-situ</em> chlorination produced overall DBPs ranging from 104.77 to 135.41 µg/L. However, the production of chlorate during UV/chlorine processes was 15 times higher than that during <em>in-situ</em> chlorination.</p></div>","PeriodicalId":15774,"journal":{"name":"Journal of environmental sciences","volume":"139 ","pages":"Pages 72-83"},"PeriodicalIF":6.9,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49745963","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 1
Efficient degradation of aqueous dichloromethane by an enhanced microbial electrolysis cell: Degradation kinetics, microbial community and metabolic mechanisms 增强型微生物电解池对二氯甲烷水溶液的有效降解:降解动力学、微生物群落和代谢机制
IF 6.9 Q1 Environmental Science Pub Date : 2024-05-01 Epub Date: 2023-05-29 DOI: 10.1016/j.jes.2023.05.029
Meng Wu , Di Zhao , Bing Gu , Ziru Wang , Jun Hu , Zhiliang Yu , Jianming Yu

Dichloromethane (DCM) has been listed as a toxic and harmful water pollutant, and its removal needs attention. Microbial electrolysis cells (MECs) are viewed as a promising alternative for pollutant removal, which can be strengthened from two aspects: microbial inoculation and acclimation. In this study, the MEC for DCM degradation was inoculated with the active sludge enhanced by Methylobacterium rhodesianum H13 (strain H13) and then acclimated in the form of a microbial fuel cell (MFC). Both the introduction of strain H13 and the initiation in MFC form significantly promoted DCM degradation. The degradation kinetics were fitted by the Haldane model, with Vmax, Kh, Ki and vmax values of 103.2 mg/L/hr, 97.8 mg/L, 268.3 mg/L and 44.7 mg/L/hr/cm2, respectively. The cyclic voltammogram implies that DCM redox reactions became easier with the setup of MEC, and the electrochemical impedance spectrogram shows that the acclimated and enriched microbes reduced the charge transfer resistance from the electrode to the electrolyte. In the biofilm, the dominant genera shifted from Geobacter to Hyphomicrobium in acclimation stages. Moreover, Methylobacterium played an increasingly important role. DCM metabolism mainly occurred through the hydrolytic glutathione S-transferase pathway, given that the gene dcmA was identified rather than the dhlA and P450/MO. The exogenous electrons facilitated the reduction of GSSG, directly or indirectly accelerating the GSH-catalyzed dehalogenation. This study provides support for the construction of an efficient and stable MEC for DCM removal in water environment.

二氯甲烷(DCM)已被列为有毒有害的水污染物,其去除需要注意。微生物电解池(MECs)被认为是一种很有前途的污染物去除替代方案,它可以从微生物接种和驯化两个方面得到加强。在本研究中,用罗得岛甲基杆菌H13(菌株H13)增强的活性污泥接种用于DCM降解的MEC,然后以微生物燃料电池(MFC)的形式驯化。菌株H13的引入和MFC形式的引发都显著促进了DCM的降解。降解动力学通过Haldane模型拟合,Vmax、Kh、Ki和Vmax值分别为103.2 mg/L、97.8 mg/L、268.3 mg/L和44.7 mg/L/hr/cm2。循环伏安图表明,随着MEC的设置,DCM氧化还原反应变得更容易,电化学阻抗谱图显示,驯化和富集的微生物降低了从电极到电解质的电荷转移电阻。在生物膜中,优势属在驯化阶段从Geobacter转移到Hyphomicrobium。此外,甲基杆菌发挥了越来越重要的作用。DCM代谢主要通过水解谷胱甘肽S-转移酶途径发生,因为鉴定的基因是dcmA,而不是dhlA和P450/MO。外源电子促进GSSG的还原,直接或间接加速GSH催化的脱卤反应。本研究为构建高效稳定的水环境DCM去除MEC提供了支持。
{"title":"Efficient degradation of aqueous dichloromethane by an enhanced microbial electrolysis cell: Degradation kinetics, microbial community and metabolic mechanisms","authors":"Meng Wu ,&nbsp;Di Zhao ,&nbsp;Bing Gu ,&nbsp;Ziru Wang ,&nbsp;Jun Hu ,&nbsp;Zhiliang Yu ,&nbsp;Jianming Yu","doi":"10.1016/j.jes.2023.05.029","DOIUrl":"https://doi.org/10.1016/j.jes.2023.05.029","url":null,"abstract":"<div><p>Dichloromethane (DCM) has been listed as a toxic and harmful water pollutant, and its removal needs attention. Microbial electrolysis cells (MECs) are viewed as a promising alternative for pollutant removal, which can be strengthened from two aspects: microbial inoculation and acclimation. In this study, the MEC for DCM degradation was inoculated with the active sludge enhanced by <em>Methylobacterium rhodesianum</em> H13 (strain H13) and then acclimated in the form of a microbial fuel cell (MFC). Both the introduction of strain H13 and the initiation in MFC form significantly promoted DCM degradation. The degradation kinetics were fitted by the Haldane model, with <em>V</em><sub>max</sub>, <em>K</em><sub>h</sub>, <em>K</em><sub>i</sub> and <em>v</em><sub>max</sub> values of 103.2 mg/L/hr, 97.8 mg/L, 268.3 mg/L and 44.7 mg/L/hr/cm<sup>2</sup>, respectively. The cyclic voltammogram implies that DCM redox reactions became easier with the setup of MEC, and the electrochemical impedance spectrogram shows that the acclimated and enriched microbes reduced the charge transfer resistance from the electrode to the electrolyte. In the biofilm, the dominant genera shifted from <em>Geobacter</em> to <em>Hyphomicrobium</em> in acclimation stages. Moreover, <em>Methylobacterium</em> played an increasingly important role. DCM metabolism mainly occurred through the hydrolytic glutathione <em>S</em>-transferase pathway, given that the gene <em>dcmA</em> was identified rather than the <em>dhlA</em> and P450/MO. The exogenous electrons facilitated the reduction of GSSG, directly or indirectly accelerating the GSH-catalyzed dehalogenation. This study provides support for the construction of an efficient and stable MEC for DCM removal in water environment.</p></div>","PeriodicalId":15774,"journal":{"name":"Journal of environmental sciences","volume":"139 ","pages":"Pages 150-159"},"PeriodicalIF":6.9,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49764491","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Ecological impacts of the expansion of offshore wind farms on trophic level species of marine food chain 海上风电场扩张对海洋食物链营养级物种的生态影响
IF 6.9 Q1 Environmental Science Pub Date : 2024-05-01 Epub Date: 2023-05-18 DOI: 10.1016/j.jes.2023.05.002
Lijing Wang , Bangguo Wang , Wenxi Cen , Rui Xu , Yuwei Huang , Xin Zhang , Yinghui Han , Yuanxun Zhang

The global demand for renewable energy has resulted in a rapid expansion of offshore wind farms (OWFs) and increased attention to the ecological impacts of OWFs on the marine ecosystem. Previous reviews mainly focused on the OWFs’ impacts on individual species like birds, bats, or mammals. This review collected numerous field-measured data and simulated results to summarize the ecological impacts on phytoplankton, zooplankton, zoobenthos, fishes, and mammals from each trophic level and also analyze their interactions in the marine food chain. Phytoplankton and zooplankton are positively or adversely affected by the ‘wave effect’, ‘shading effect’, oxygen depletion and predation pressure, leading to a ± 10% fluctuation of primary production. Although zoobenthos are threatened transiently by habitat destruction with a reduction of around 60% in biomass in the construction stage, their abundance exhibited an over 90% increase, dominated by sessile species, due to the ‘reef effect’ in the operation stage. Marine fishes and mammals are to endure the interferences of noise and electromagnetic, but they are also aggregated around OWFs by the ‘reef effect’ and ‘reserve effect’. Furthermore, the complexity of marine ecosystem would increase with a promotion of the total system biomass by 40% through trophic cascade effects strengthen and resource partitioning alternation triggered by the proliferation of filter-feeders. The suitable site selection, long-term monitoring, and life-cycle-assessment of ecological impacts of OWFs that are lacking in current literature have been described in this review, as well as the carbon emission and deposition.

全球对可再生能源的需求导致海上风电场的快速扩张,并越来越关注海上风电场对海洋生态系统的生态影响。以前的综述主要集中在OWF对鸟类、蝙蝠或哺乳动物等单个物种的影响上。本综述收集了大量现场测量数据和模拟结果,总结了各营养级对浮游植物、浮游动物、底栖动物、鱼类和哺乳动物的生态影响,并分析了它们在海洋食物链中的相互作用。浮游植物和浮游动物受到“波浪效应”、“遮荫效应”、氧气消耗和捕食压力的积极或消极影响,导致初级生产力波动±10%。尽管底栖动物在施工阶段暂时受到栖息地破坏的威胁,生物量减少了约60%,但由于作业阶段的“珊瑚礁效应”,它们的丰度增加了90%以上,主要是固着物种。海洋鱼类和哺乳动物要承受噪声和电磁干扰,但它们也会通过“珊瑚礁效应”和“储备效应”聚集在OWF周围。此外,通过滤食性动物增殖引发的营养级联效应增强和资源分配交替,海洋生态系统的复杂性将随着总系统生物量增加40%而增加。本文介绍了目前文献中缺乏的OWF生态影响的合适选址、长期监测和生命周期评估,以及碳排放和沉积。
{"title":"Ecological impacts of the expansion of offshore wind farms on trophic level species of marine food chain","authors":"Lijing Wang ,&nbsp;Bangguo Wang ,&nbsp;Wenxi Cen ,&nbsp;Rui Xu ,&nbsp;Yuwei Huang ,&nbsp;Xin Zhang ,&nbsp;Yinghui Han ,&nbsp;Yuanxun Zhang","doi":"10.1016/j.jes.2023.05.002","DOIUrl":"https://doi.org/10.1016/j.jes.2023.05.002","url":null,"abstract":"<div><p>The global demand for renewable energy has resulted in a rapid expansion of offshore wind farms (OWFs) and increased attention to the ecological impacts of OWFs on the marine ecosystem. Previous reviews mainly focused on the OWFs’ impacts on individual species like birds, bats, or mammals. This review collected numerous field-measured data and simulated results to summarize the ecological impacts on phytoplankton, zooplankton, zoobenthos, fishes, and mammals from each trophic level and also analyze their interactions in the marine food chain. Phytoplankton and zooplankton are positively or adversely affected by the ‘wave effect’, ‘shading effect’, oxygen depletion and predation pressure, leading to <em>a</em> ± 10% fluctuation of primary production. Although zoobenthos are threatened transiently by habitat destruction with a reduction of around 60% in biomass in the construction stage, their abundance exhibited an over 90% increase, dominated by sessile species, due to the ‘reef effect’ in the operation stage. Marine fishes and mammals are to endure the interferences of noise and electromagnetic, but they are also aggregated around OWFs by the ‘reef effect’ and ‘reserve effect’. Furthermore, the complexity of marine ecosystem would increase with a promotion of the total system biomass by 40% through trophic cascade effects strengthen and resource partitioning alternation triggered by the proliferation of filter-feeders. The suitable site selection, long-term monitoring, and life-cycle-assessment of ecological impacts of OWFs that are lacking in current literature have been described in this review, as well as the carbon emission and deposition.</p></div>","PeriodicalId":15774,"journal":{"name":"Journal of environmental sciences","volume":"139 ","pages":"Pages 226-244"},"PeriodicalIF":6.9,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49745966","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 1
Aluminum exposure impairs oocyte quality via subcellular structure disruption and DNA damage-related apoptosis in mice 铝暴露通过亚细胞结构破坏和DNA损伤相关凋亡损害小鼠卵母细胞质量
IF 6.9 Q1 Environmental Science Pub Date : 2024-05-01 Epub Date: 2023-04-19 DOI: 10.1016/j.jes.2023.04.007
Hongge Li , Jingcai Liu , Weihua Nong , Mengying Shen , Sheng Dou , Shaochen Sun , Junli Wang

Aluminum (Al) can lead to an exposure of creature in varieties ways for its universality, and it could disturb normal physiological metabolism, with the damage to multisystem including reproduction. Since the oocyte quality is critical for female reproduction, we inspected the toxicity of Al on mouse oocyte maturation. We constructed in vitro exposure mouse model, and we found that 5 mmol/L Al had adverse effects on oocyte maturation by impairing organelle and cytoskeleton. Aberrant spindle and misaligned chromosomes which might be considered to be caused by elevated levels of acetylation, as well as abnormal distribution of actin dynamics could hinder normal meiosis of oocytes. Organelle dysfunction indicated that Al affected proteins synthesis, transport and digestion, which would further damage oocyte maturation. In order to explore the mechanism of Al toxicity, our further investigation demonstrated that Al caused mitochondrial dysfunction and imbalance calcium homeostasis, resulting in limited energy supply. Moreover, high level of reactive oxygen species, DNA damage and apoptosis caused by oxidative stress were also the manifestation of Al toxicity on oocytes. In conclusion, our study provided the evidence that Al exposure affected oocyte quality through its effects on spindle organization, actin dynamics, organelle function and the induction of DNA damage-related apoptosis with mouse model.

铝(Al)具有普遍性,可导致生物以多种方式暴露,并干扰正常的生理代谢,对包括生殖在内的多系统造成损害。由于卵母细胞质量对雌性生殖至关重要,我们检测了铝对小鼠卵母细胞成熟的毒性。我们构建了体外暴露小鼠模型,发现5mmol/L的Al通过损害细胞器和细胞骨架对卵母细胞成熟有不利影响。纺锤体异常和染色体错位可能被认为是由乙酰化水平升高引起的,以及肌动蛋白动力学的异常分布可能会阻碍卵母细胞的正常减数分裂。细胞器功能障碍表明Al影响蛋白质的合成、运输和消化,进而损害卵母细胞的成熟。为了探索铝的毒性机制,我们的进一步研究表明,铝导致线粒体功能障碍和钙稳态失衡,导致能量供应有限。此外,高水平的活性氧、氧化应激引起的DNA损伤和细胞凋亡也是Al对卵母细胞毒性的表现。总之,我们的研究提供了证据,证明铝暴露通过影响小鼠模型的纺锤体组织、肌动蛋白动力学、细胞器功能和诱导DNA损伤相关的细胞凋亡来影响卵母细胞的质量。
{"title":"Aluminum exposure impairs oocyte quality via subcellular structure disruption and DNA damage-related apoptosis in mice","authors":"Hongge Li ,&nbsp;Jingcai Liu ,&nbsp;Weihua Nong ,&nbsp;Mengying Shen ,&nbsp;Sheng Dou ,&nbsp;Shaochen Sun ,&nbsp;Junli Wang","doi":"10.1016/j.jes.2023.04.007","DOIUrl":"https://doi.org/10.1016/j.jes.2023.04.007","url":null,"abstract":"<div><p><span>Aluminum (Al) can lead to an exposure of creature in varieties ways for its universality, and it could disturb normal physiological metabolism, with the damage to multisystem including reproduction. Since the oocyte quality is critical for female reproduction, we inspected the toxicity of Al on mouse oocyte maturation. We constructed </span><em>in vitro</em><span> exposure mouse model, and we found that 5 mmol/L Al had adverse effects on oocyte maturation by impairing organelle<span><span> and cytoskeleton. Aberrant spindle and misaligned chromosomes which might be considered to be caused by elevated levels of acetylation, as well as abnormal distribution of actin dynamics could hinder normal meiosis of oocytes. Organelle dysfunction indicated that Al affected </span>proteins synthesis<span><span>, transport and digestion, which would further damage oocyte maturation. In order to explore the mechanism of Al toxicity, our further investigation demonstrated that Al caused mitochondrial dysfunction and imbalance calcium homeostasis, resulting in limited energy supply. Moreover, high level of </span>reactive oxygen species<span>, DNA damage and apoptosis caused by oxidative stress were also the manifestation of Al toxicity on oocytes. In conclusion, our study provided the evidence that Al exposure affected oocyte quality through its effects on spindle organization, actin dynamics, organelle function and the induction of DNA damage-related apoptosis with mouse model.</span></span></span></span></p></div>","PeriodicalId":15774,"journal":{"name":"Journal of environmental sciences","volume":"139 ","pages":"Pages 308-319"},"PeriodicalIF":6.9,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49746426","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Mechanistic insight into Cr(VI) retention by Si-containing ferrihydrite 含硅水合铁对Cr(VI)截留的机理研究
IF 6.9 Q1 Environmental Science Pub Date : 2024-05-01 Epub Date: 2023-06-03 DOI: 10.1016/j.jes.2023.05.040
Ying Hu , Qiang Xue , Honghan Chen , Huaming Guo , Kenneth C. Carroll , Song Wang

Hexavalent chromium [Cr(VI)] causes serious harm to the environment due to its high toxicity, solubility, and mobility. Ferrihydrites (Fh) are the main adsorbent and trapping agent of Cr(VI) in soils and aquifers, and they usually coexist with silicate (Si), forming Si-containing ferrihydrite (Si-Fh) mixtures. However, the mechanism of Cr(VI) retention by Si-Fh mixtures is poorly understood. In this study, the behaviors and mechanisms of Cr(VI) adsorption onto Si-Fh with different Si/Fe molar ratios was investigated. Transmission electron microscope, Fourier transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and other techniques were used to characterize Si-Fh and Cr(VI)-loading of Si-Fh. The results show that specific surface area of Si-Fh increases gradually with increasing Si/Fe ratios, but Cr(VI) adsorption on Si-Fh decreases with increasing Si/Fe ratios. This is because with an increase in Si/Fe molar ratio, the point of zero charge of Si-Fh gradually decreases and electrostatic repulsion between Si-Fh and Cr(VI) increases. However, the complexation of Cr(VI) is enhanced due to the increase in adsorbed hydroxyl (A-OH-) on Si-Fh with increasing Si/Fe molar ratio, which partly counteracts the effect of the electrostatic repulsion. Overall, the increase in the electrostatic repulsion has a greater impact on adsorption than the additional complexation with Si-Fh. Density functional theory calculation further supports this observation, showing the increases in electron variation of bonding atoms and reaction energies of inner spherical complexes with the increase in Si/Fe ratio.

六价铬[Cr(VI)]具有较高的毒性、溶解性和流动性,对环境造成严重危害。水铁矿(Fh)是土壤和含水层中Cr(VI)的主要吸附剂和捕集剂,它们通常与硅酸盐(Si)共存,形成含硅水铁矿(Si-Fh)混合物。然而,人们对Si-Fh混合物保留Cr(VI)的机理知之甚少。在本研究中,研究了不同Si/Fe摩尔比的Si-Fh对Cr(VI)的吸附行为和机理。利用透射电子显微镜、傅立叶变换红外光谱、X射线衍射、X射线光电子能谱等技术对Si Fh和Cr(VI)负载Si Fh进行了表征。结果表明,Si-Fh的比表面积随着Si/Fe比的增加而逐渐增加,但Cr(VI)在Si-Fh上的吸附量随着Si/Fe比的增加逐渐减小。这是因为随着Si/Fe摩尔比的增加,Si-Fh的零电荷点逐渐降低,并且Si-Fh和Cr(VI)之间的静电排斥增加。然而,随着Si/Fe摩尔比的增加,Si-Fh上吸附的羟基(A-OH-)增加,Cr(VI)的络合作用增强,这部分抵消了静电排斥的影响。总的来说,静电排斥的增加对吸附的影响比与Si-Fh的额外络合更大。密度泛函理论计算进一步支持了这一观察结果,表明键合原子的电子变化和内球形配合物的反应能随着Si/Fe比的增加而增加。
{"title":"Mechanistic insight into Cr(VI) retention by Si-containing ferrihydrite","authors":"Ying Hu ,&nbsp;Qiang Xue ,&nbsp;Honghan Chen ,&nbsp;Huaming Guo ,&nbsp;Kenneth C. Carroll ,&nbsp;Song Wang","doi":"10.1016/j.jes.2023.05.040","DOIUrl":"https://doi.org/10.1016/j.jes.2023.05.040","url":null,"abstract":"<div><p>Hexavalent chromium [Cr(VI)] causes serious harm to the environment due to its high toxicity, solubility, and mobility. Ferrihydrites (Fh) are the main adsorbent and trapping agent of Cr(VI) in soils and aquifers, and they usually coexist with silicate (Si), forming Si-containing ferrihydrite (Si-Fh) mixtures. However, the mechanism of Cr(VI) retention by Si-Fh mixtures is poorly understood. In this study, the behaviors and mechanisms of Cr(VI) adsorption onto Si-Fh with different Si/Fe molar ratios was investigated. Transmission electron microscope, Fourier transform infrared spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and other techniques were used to characterize Si-Fh and Cr(VI)-loading of Si-Fh. The results show that specific surface area of Si-Fh increases gradually with increasing Si/Fe ratios, but Cr(VI) adsorption on Si-Fh decreases with increasing Si/Fe ratios. This is because with an increase in Si/Fe molar ratio, the point of zero charge of Si-Fh gradually decreases and electrostatic repulsion between Si-Fh and Cr(VI) increases. However, the complexation of Cr(VI) is enhanced due to the increase in adsorbed hydroxyl (A-OH-) on Si-Fh with increasing Si/Fe molar ratio, which partly counteracts the effect of the electrostatic repulsion. Overall, the increase in the electrostatic repulsion has a greater impact on adsorption than the additional complexation with Si-Fh. Density functional theory calculation further supports this observation, showing the increases in electron variation of bonding atoms and reaction energies of inner spherical complexes with the increase in Si/Fe ratio.</p></div>","PeriodicalId":15774,"journal":{"name":"Journal of environmental sciences","volume":"139 ","pages":"Pages 217-225"},"PeriodicalIF":6.9,"publicationDate":"2024-05-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49746556","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 2
期刊
Journal of environmental sciences
全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
0
微信
客服QQ
Book学术公众号 扫码关注我们
反馈
×
意见反馈
请填写您的意见或建议
请填写您的手机或邮箱
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
现在去查看 取消
×
提示
确定
Book学术官方微信
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术
文献互助 智能选刊 最新文献 互助须知 联系我们:info@booksci.cn
Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。
Copyright © 2023 Book学术 All rights reserved.
ghs 京公网安备 11010802042870号 京ICP备2023020795号-1