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Optimization of Fenton-like reaction pathways using Ov-containing ZnO@nitrogen-rich porous carbon: the electron transfer and 1O2 triggered non-radical process 利用含 Ov 的 ZnO@ 富氮多孔碳优化 Fenton-like 反应途径:电子转移和 1O2 触发的非自由基过程
IF 8.131 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-22 DOI: 10.1039/d4en00749b
Zhenfeng Zhang, Tianli Xiong, Haihao Peng, Honglin Zhang, Siying He, Xuran Liu, Yanan Liu, Wenyi Feng, Zhaohui Yang, Weiping Xiong
With the development of persulfate-based Fenton-like catalysis, how to control the PDS reaction pathway is a great challenge. Herein, we prepared catalysts with nitrogen-rich porous carbon (NPC) layers and oxygen vacancy (Ov) sites for PDS activation to degrade sulfamethazine (SMZ). Results revealed that the ZnO@NPC/PDS system exhibited only non-radical pathways, which comprised the singlet oxygen (1O2) and electron transfer process. The intrinsic mechanism underlying the production of active species was further verified by comparing the results of the ZnO@NPC/PDS and ZnO@NPC-Etch/PDS systems, Raman analysis and DFT calculations. Adsorption of PDS by carbon layers resulted in the formation of a catalyst–PDS complex, which not only elongated the S–O bond and accelerated the decomposition of PDS to generate 1O2 but also provided access for electron transfer. Meanwhile, Ov sites increased electron density and electron migration strength, which promoted more electron transfer from Ovs to PDS molecules through nitrogen-rich porous carbon layers. Moreover, the ZnO@NPC/PDS system could maintain a degradation rate of >90% for SMZ in real water matrixes. T. E. S. T software prediction and toxicity tests were used to investigate environmental implications of degradation intermediates, which showed reduced ecological toxicity compared with SMZ. This work fabricated the ZnO@NPC/PDS system and explored the interaction between nitrogen-rich porous carbon layers and Ov to regulate the occurrence of non-radical pathways, which could provide a strategy to control the PDS reaction pathway.
随着基于过硫酸盐的 Fenton-like 催化技术的发展,如何控制 PDS 反应途径是一个巨大的挑战。在此,我们制备了具有富氮多孔碳(NPC)层和氧空位(Ov)的催化剂,用于活化 PDS 以降解磺胺二甲嘧啶(SMZ)。结果表明,ZnO@NPC/PDS体系只表现出非自由基途径,包括单线态氧(1O2)和电子转移过程。通过比较 ZnO@NPC/PDS 和 ZnO@NPC-Etch/PDS 系统、拉曼分析和 DFT 计算的结果,进一步验证了活性物种产生的内在机制。碳层对 PDS 的吸附导致催化剂-PDS 复合物的形成,这不仅拉长了 S-O 键,加速 PDS 分解生成 1O2,还为电子转移提供了通道。同时,Ov位点增加了电子密度和电子迁移强度,促进了更多电子通过富氮多孔碳层从Ov转移到PDS分子。此外,ZnO@NPC/PDS 系统在实际水基质中对 SMZ 的降解率可达 90%。利用 T. E. S. T 软件预测和毒性测试研究了降解中间产物对环境的影响,结果表明与 SMZ 相比,降解中间产物的生态毒性有所降低。这项工作制备了 ZnO@NPC/PDS 系统,并探索了富氮多孔碳层与 Ov 之间的相互作用,以调节非自由基途径的发生,从而为控制 PDS 反应途径提供了一种策略。
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引用次数: 0
Salt-Resistant Catalyst Fe-Bi@γ-Al2O3 for Catalytic Ozonation of High-Salt Simulated Wastewater 用于高盐模拟废水催化臭氧处理的耐盐催化剂 Fe-Bi@γ-Al2O3
IF 3.8 4区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-11-22 DOI: 10.1007/s11270-024-07652-x
Lei Guo, Xingwang Yang, Yanhua Xu, Jun Zhou, Wenquan Sun, Yongjun Sun

In order to study the effects of common ionic components in wastewater on the catalytic performance and salt resistance of the Fe-Bi@γ-Al2O3 catalyst, hydroquinone was selected as the target organic pollutant. Five factors, namely cation species, anion species, total hardness, total alkalinity, and TDS were studied to investigate the effects of different ionic components on the degradation of hydroquinone by the Fe-Bi@γ-Al2O3 catalyst. K+ and Na+ had basically no effect on the COD removal rate, and the COD removal rates were 81.43% and 83.81%, respectively, with no significant change from the COD removal rate from raw water (85.24%), Cu2+ and Al3+ had some inhibitory effect on the COD removal rate, and the COD removal rate was 68.57% and 70.00%, respectively. While, the presence of Fe3+, Cl, Br and SiO32− had a significant inhibitory effect on the COD removal rate, and the COD removal rate was 61.90%, 51.90%, 55.71% and 60.48%. The concentration of Ca2+ was 50 mg/L and Mg2+ was 200 mg/L, the COD removal rate was 57.62% and 60.48%, respectively due to water hardness. The alkalinity had an inhibitory effect on the treatment effect of simulated waste water, when the OH concentration was 1500 mg/L, the COD removal rate was 49.05%. The higher the TDS concentration, the more obvious was the inhibitory effect on the COD removal rate, and the COD removal rate was 41.43% when the TDS was 50,000 mg/L. The intermediates and possible degradation mechanisms after catalytic ozone oxidation of hydroquinone-simulated wastewater by Fe-Bi@γ-Al2O3 were investigated by UV spectroscopy scanning, 3D fluorescence spectroscopy scanning, and GC–MS scanning.

为了研究废水中常见离子成分对Fe-Bi@γ-Al2O3催化剂催化性能和耐盐性的影响,选择对苯二酚作为目标有机污染物。研究了阳离子种类、阴离子种类、总硬度、总碱度和 TDS 五个因素,考察了不同离子组分对 Fe-Bi@γ-Al2O3 催化剂降解对苯二酚的影响。K+和Na+对COD的去除率基本没有影响,COD去除率分别为81.43%和83.81%,与原水的COD去除率(85.24%)相比没有显著变化;Cu2+和Al3+对COD的去除率有一定的抑制作用,COD去除率分别为68.57%和70.00%。而 Fe3+、Cl-、Br- 和 SiO32- 的存在对 COD 去除率有明显的抑制作用,COD 去除率分别为 61.90%、51.90%、55.71% 和 60.48%。当 Ca2+ 浓度为 50 mg/L 和 Mg2+ 浓度为 200 mg/L 时,由于水硬度的影响,COD 去除率分别为 57.62% 和 60.48%。碱度对模拟废水的处理效果有抑制作用,当 OH 浓度为 1500 mg/L 时,COD 去除率为 49.05%。TDS 浓度越高,对 COD 去除率的抑制作用越明显,当 TDS 为 50,000 mg/L 时,COD 去除率为 41.43%。通过紫外光谱扫描、三维荧光光谱扫描和气相色谱-质谱扫描研究了 Fe-Bi@γ-Al2O3 催化臭氧氧化对苯二酚模拟废水后的中间产物及可能的降解机理。
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引用次数: 0
Facet-Dependent Hematite Reactivity in Cr(Ⅵ) Removal with Fe(Ⅱ) 铁(Ⅱ)去除铬(Ⅵ)的反应活性与赤铁矿的面相有关
IF 8.131 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-22 DOI: 10.1039/d4en00733f
Shengnan Zhang, Lingyi Li, Junxue Li, Wei Cheng
Hematite displays diverse crystal structures and often coexists with Fe(Ⅱ), both of which are crucial in controlling the fate and mobility of Cr(Ⅵ). However, the mechanisms underlying Cr(Ⅵ) removal in the presence of Fe(Ⅱ) on various hematite facets remain elusive. This study aims to elucidate the facet-dependent reactivity of hematite nanocrystals in conjunction with Fe(Ⅱ) for the removal Cr(Ⅵ) from aqueous solutions. Hematite nanoplates (HNPs), predominantly composed of {001} facets, and nanorods (HNRs), exposing both {001} and {110} facets, were synthesized and characterized. Their Cr(VI) removal capabilities were evaluated in hematite-Cr(VI) and hematite-Fe(II)-Cr(VI) systems, as well as the Fe(II)-Cr(VI) system. The adsorption of Fe(Ⅱ) and Cr(VI) on hematite surfaces was highly dependent on the crystal facets and pH, with HNRs demonstrating superior Cr(Ⅵ) adsorption over HNPs, especially under acidic conditions. Neutral pH favored Fe(II)-Cr(VI) redox reactions and Fe(II) adsorption. The hematite-Fe(Ⅱ) couple displayed a synergistic effect in removing Cr(Ⅵ) under acidic conditions, which was not observed under neutral conditions. The presence of Fe(Ⅱ) notably enhanced Cr(Ⅵ) adsorption onto hematite, and bound Fe(Ⅱ) facilitated electron transfer, accelerating Cr(Ⅵ) reduction. HNRs-Fe(Ⅱ) exhibited higher Cr(Ⅵ) removal efficiency than HNPs-Fe(Ⅱ) due to their lower free corrosion potential and improved electron transport properties. This research underscores the potential of facet engineering in optimizing hematite nanocrystals for environmental remediation, specifically in Cr(Ⅵ)-contaminated environments.
赤铁矿的晶体结构多种多样,而且经常与铁(Ⅱ)共存,这两种元素对控制铬(Ⅵ)的去向和流动性至关重要。然而,不同赤铁矿面上的铁(Ⅱ)存在时,铬(Ⅵ)的去除机制仍不明确。本研究旨在阐明赤铁矿纳米晶体与 Fe(Ⅱ)在去除水溶液中的 Cr(Ⅵ)方面的反应性。研究人员合成并鉴定了主要由{001}面组成的赤铁矿纳米板(HNPs)和同时具有{001}面和{110}面的纳米棒(HNRs)。在赤铁矿-铬(VI)和赤铁矿-铁(II)-铬(VI)体系以及铁(II)-铬(VI)体系中评估了它们去除铬(VI)的能力。赤铁矿表面对铁(Ⅱ)和铬(Ⅵ)的吸附在很大程度上取决于晶面和 pH 值,其中 HNRs 比 HNPs 更好地吸附了铬(Ⅵ),尤其是在酸性条件下。中性 pH 有利于铁(Ⅱ)-铬(Ⅵ)氧化还原反应和铁(Ⅱ)的吸附。在酸性条件下,赤铁矿-Fe(Ⅱ)耦合物在去除铬(Ⅵ)方面显示出协同效应,而在中性条件下却观察不到这种效应。Fe(Ⅱ)的存在明显增强了赤铁矿对 Cr(Ⅵ)的吸附,结合的 Fe(Ⅱ)促进了电子转移,加速了 Cr(Ⅵ)的还原。与 HNPs-Fe(Ⅱ)相比,HNRs-Fe(Ⅱ)具有更低的自由腐蚀电位和更好的电子传递特性,因而具有更高的铬(Ⅵ)去除效率。这项研究强调了刻面工程在优化赤铁矿纳米晶体的环境修复方面的潜力,特别是在受(Ⅵ)铬污染的环境中。
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引用次数: 0
Emerging investigator series: CeO2/CuO nanostructured composite with enhanced antimicrobial properties and low cytotoxicity to human keratinocytes in vitro 新晋研究人员系列:CeO2/CuO 纳米结构复合材料在体外具有更强的抗菌性能和对人类角质细胞的低细胞毒性
IF 8.131 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-22 DOI: 10.1039/d4en00501e
Svetlana Vihodceva, Andris Šutka, Mairis Iesalnieks, Liga Orlova, Arturs Pludonis, Maarja Otsus, Mariliis Sihtmäe, Heiki Vija, Alexandra Nefedova, Angela Ivask, Anne Kahru, Kaja Kasemets
This research presents a synthesis method for the CeO<small><sub>2</sub></small>/CuO nanostructured composite, which has potential applications as an antimicrobial material in the production of antimicrobial surface coatings, for example, for high-touch surfaces. The antimicrobial efficacy, mode of action, and potential cytotoxicity of CeO<small><sub>2</sub></small>/CuO towards the human immortalized keratinocyte cell line <em>in vitro</em> were studied compared to those of CuO, CeO<small><sub>2</sub></small>, and ionic Cu (a solubility control). The used synthesis method resulted in a CeO<small><sub>2</sub></small>/CuO nanostructured composite with a mean particle size of 27 nm and a specific surface area of 80.3 m<small><sup>2</sup></small> g<small><sup>−1</sup></small>. The composite had a significant proportion (54%) of non-lattice oxygen species, highlighting the presence of substantial surface defects crucial for generating reactive oxygen species (ROS). The antimicrobial properties of CeO<small><sub>2</sub></small>/CuO, CuO, and CeO<small><sub>2</sub></small> were assessed at six concentrations from 1 to 1000 mg L<small><sup>−1</sup></small> in deionized water. The CeO<small><sub>2</sub></small>/CuO composite exhibited antibacterial efficacy at a minimum bactericidal concentration (MBC) of 100 mg L<small><sup>−1</sup></small> towards <em>Escherichia coli</em> already after 2 h of contact and towards <em>Pseudomonas aeruginosa</em> and <em>Staphylococcus aureus</em> after 4 h of contact, whereas after 24 h of exposure, the antibacterial efficacy to all three bacterial strains was evident already at a MBC = 10 mg L<small><sup>−1</sup></small>. Fungi <em>Candida albicans</em> proved less susceptible than bacteria (24 h MBC = 100 mg L<small><sup>−1</sup></small>). Thus, the CeO<small><sub>2</sub></small>/CuO composite showed significant antibacterial efficacy against Gram-negative and Gram-positive bacteria, being at the same time safe to human keratinocytes <em>in vitro</em> in the case of which even 1000 mg L<small><sup>−1</sup></small> caused no harmful effects after 2 h exposure and 500 mg L<small><sup>−1</sup></small> caused no cytotoxicity after 24 h exposure. CeO<small><sub>2</sub></small>/CuO caused abiotic and biotic ROS production in all the tested environments. ROS production in deionized water was the most remarkable. Shedding of Cu-ions from CeO<small><sub>2</sub></small>/CuO was moderate and depended on the test environment, varying from 0.3 to 1 mg L<small><sup>−1</sup></small>, and considering the MBC of ionic Cu for microorganisms was not the main contributor to the antimicrobial activity of CeO<small><sub>2</sub></small>/CuO. The CeO<small><sub>2</sub></small>/CuO composite exhibited no acute toxicity to the environmentally relevant bacterium <em>Vibrio fischeri</em>. These findings indicate that CeO<small><sub>2</sub></small>/CuO's high ROS production is its primary antimicrobial mechanism and that due to its low cytotoxicit
本研究提出了一种 CeO2/CuO 纳米结构复合材料的合成方法,这种复合材料可作为抗菌材料用于生产抗菌表面涂层,例如用于高接触表面。研究了 CeO2/CuO 与 CuO、CeO2 和离子铜(溶解度对照)相比,在体外对人类永生角质细胞系的抗菌功效、作用模式和潜在细胞毒性。采用的合成方法得到了 CeO2/CuO 纳米结构复合材料,其平均粒径为 27 nm,比表面积为 80.3 m2 g-1。该复合材料中的非晶格氧物种占很大比例(54%),这表明存在大量表面缺陷,而这些缺陷对活性氧物种(ROS)的产生至关重要。评估了 CeO2/CuO、CuO 和 CeO2 在去离子水中 1 至 1000 mg L-1 六种浓度下的抗菌特性。CeO2/CuO 复合材料在最低杀菌浓度(MBC)为 100 mg L-1 时,接触 2 小时后对大肠杆菌就有抗菌效果,接触 4 小时后对绿脓杆菌和金黄色葡萄球菌也有抗菌效果,而接触 24 小时后,MBC = 10 mg L-1 时对所有三种细菌菌株都有明显的抗菌效果。真菌白色念珠菌的敏感性低于细菌(24 小时的 MBC = 100 毫克/升)。因此,CeO2/CuO 复合材料对革兰氏阴性菌和革兰氏阳性菌具有显著的抗菌效果,同时在体外对人类角质细胞也是安全的,即使接触 1000 毫克 L-1 也不会在 2 小时后产生有害影响,接触 500 毫克 L-1 也不会在 24 小时后产生细胞毒性。CeO2/CuO 在所有测试环境中都会产生非生物和生物 ROS。在去离子水中产生的 ROS 最为显著。从 CeO2/CuO 中脱落的铜离子不多,取决于测试环境,从 0.3 到 1 mg L-1 不等,考虑到离子铜对微生物的 MBC,这并不是 CeO2/CuO 抗菌活性的主要因素。CeO2/CuO 复合材料对环境相关细菌 Vibrio fischeri 没有急性毒性。这些研究结果表明,CeO2/CuO 产生大量 ROS 是其主要的抗菌机制,而且由于其对人类角质细胞的细胞毒性较低,因此可被视为一种很有前途的抗菌剂。
{"title":"Emerging investigator series: CeO2/CuO nanostructured composite with enhanced antimicrobial properties and low cytotoxicity to human keratinocytes in vitro","authors":"Svetlana Vihodceva, Andris Šutka, Mairis Iesalnieks, Liga Orlova, Arturs Pludonis, Maarja Otsus, Mariliis Sihtmäe, Heiki Vija, Alexandra Nefedova, Angela Ivask, Anne Kahru, Kaja Kasemets","doi":"10.1039/d4en00501e","DOIUrl":"https://doi.org/10.1039/d4en00501e","url":null,"abstract":"This research presents a synthesis method for the CeO&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;/CuO nanostructured composite, which has potential applications as an antimicrobial material in the production of antimicrobial surface coatings, for example, for high-touch surfaces. The antimicrobial efficacy, mode of action, and potential cytotoxicity of CeO&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;/CuO towards the human immortalized keratinocyte cell line &lt;em&gt;in vitro&lt;/em&gt; were studied compared to those of CuO, CeO&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;, and ionic Cu (a solubility control). The used synthesis method resulted in a CeO&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;/CuO nanostructured composite with a mean particle size of 27 nm and a specific surface area of 80.3 m&lt;small&gt;&lt;sup&gt;2&lt;/sup&gt;&lt;/small&gt; g&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt;. The composite had a significant proportion (54%) of non-lattice oxygen species, highlighting the presence of substantial surface defects crucial for generating reactive oxygen species (ROS). The antimicrobial properties of CeO&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;/CuO, CuO, and CeO&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt; were assessed at six concentrations from 1 to 1000 mg L&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt; in deionized water. The CeO&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;/CuO composite exhibited antibacterial efficacy at a minimum bactericidal concentration (MBC) of 100 mg L&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt; towards &lt;em&gt;Escherichia coli&lt;/em&gt; already after 2 h of contact and towards &lt;em&gt;Pseudomonas aeruginosa&lt;/em&gt; and &lt;em&gt;Staphylococcus aureus&lt;/em&gt; after 4 h of contact, whereas after 24 h of exposure, the antibacterial efficacy to all three bacterial strains was evident already at a MBC = 10 mg L&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt;. Fungi &lt;em&gt;Candida albicans&lt;/em&gt; proved less susceptible than bacteria (24 h MBC = 100 mg L&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt;). Thus, the CeO&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;/CuO composite showed significant antibacterial efficacy against Gram-negative and Gram-positive bacteria, being at the same time safe to human keratinocytes &lt;em&gt;in vitro&lt;/em&gt; in the case of which even 1000 mg L&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt; caused no harmful effects after 2 h exposure and 500 mg L&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt; caused no cytotoxicity after 24 h exposure. CeO&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;/CuO caused abiotic and biotic ROS production in all the tested environments. ROS production in deionized water was the most remarkable. Shedding of Cu-ions from CeO&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;/CuO was moderate and depended on the test environment, varying from 0.3 to 1 mg L&lt;small&gt;&lt;sup&gt;−1&lt;/sup&gt;&lt;/small&gt;, and considering the MBC of ionic Cu for microorganisms was not the main contributor to the antimicrobial activity of CeO&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;/CuO. The CeO&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;/CuO composite exhibited no acute toxicity to the environmentally relevant bacterium &lt;em&gt;Vibrio fischeri&lt;/em&gt;. These findings indicate that CeO&lt;small&gt;&lt;sub&gt;2&lt;/sub&gt;&lt;/small&gt;/CuO's high ROS production is its primary antimicrobial mechanism and that due to its low cytotoxicit","PeriodicalId":73,"journal":{"name":"Environmental Science: Nano","volume":"34 1","pages":""},"PeriodicalIF":8.131,"publicationDate":"2024-11-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142684497","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Human Footprints on Sediment Quality in the Shadegan International Wetland, Northwest of the Persian Gulf 人类足迹对波斯湾西北部沙德甘国际湿地沉积物质量的影响
IF 3.8 4区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-11-21 DOI: 10.1007/s11270-024-07609-0
Kourosh Sabbagh, Hamed Haghnazar, Renato Somma, Karen H. Johannesson, Mojtaba Pourakbar, Ehsan Aghayani

This study focuses on assessing the contamination of surficial sediments in the Shadegan International Wetland, southwest of the Persian Gulf, identifying heavy metal concentrations, evaluating pollution levels using multi-element indices, and determining pollution sources through statistical analyses. Sediment samples were collected from fifteen sites across the wetland and analyzed for the concentrations of six heavy metal(loid)s including Arsenic (As), Chromium (Cr), Copper (Cu), Nickel (Ni), Lead (Pb), and Zinc (Zn). The results revealed moderate to considerable contamination of sediments with heavy metals such as Cr, Ni, Pb, and Zn, with concentrations exceeding local background levels. Multivariate statistical techniques, including Correlation Matrix and Principal Component Analysis, identified common pollution sources, such as municipal wastewater, industrial effluents, and agricultural runoff. Pollution indices, including the Modified Pollution Index (MPI), the Aggregative Toxicity Index (ATI), the Ecological Contamination Index (ECI), the Contamination Severity Index (CSI), the Toxic Risk Index (TRI), and the Total Toxic Units (STU), were employed to assess pollution severity, revealing moderate to heavy pollution levels in certain areas, primarily attributed to anthropogenic activities. The Safe-Heart indicator, a novel visualization tool introduced in this study, provided a comprehensive overview of sediment pollution, highlighting areas of high contamination and underscoring the urgent need for remediation measures to safeguard the wetland ecosystem and aquatic organisms.

本研究的重点是评估波斯湾西南部沙德甘国际湿地表层沉积物的污染情况,确定重金属浓度,使用多元素指数评估污染程度,并通过统计分析确定污染源。从整个湿地的 15 个地点收集了沉积物样本,并分析了六种重金属的浓度,包括砷 (As)、铬 (Cr)、铜 (Cu)、镍 (Ni)、铅 (Pb) 和锌 (Zn)。结果显示,沉积物受到铬、镍、铅和锌等重金属的中度至严重污染,浓度超过了当地的背景水平。相关矩阵和主成分分析等多元统计技术确定了常见的污染源,如城市污水、工业废水和农业径流。污染指数包括修正污染指数 (MPI)、综合毒性指数 (ATI)、生态污染指数 (ECI)、污染严重程度指数 (CSI)、毒性风险指数 (TRI) 和总毒性单位 (STU),用于评估污染严重程度,揭示了某些地区的中度至重度污染水平,主要归因于人为活动。本研究中引入的新型可视化工具 "安全心脏 "指标提供了沉积物污染的全面概况,突出了高污染区域,并强调了采取补救措施以保护湿地生态系统和水生生物的迫切需要。
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引用次数: 0
Optimizing oxygen vacancy concentration and electronic transport processes in a MnxCo/CeO2 nanoreactor: regulation mechanism of the radical to non-radical pathway 优化 MnxCo/CeO2 纳米反应器中的氧空位浓度和电子传输过程:自由基到非自由基途径的调节机制
IF 8.131 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-21 DOI: 10.1039/d4en00892h
Hailan Qin, Jiahao Wang, Siyuan Di, Yunkang Liu, Pin Chen, Min Liu, Qiuyue Zhang, Shukui Zhu
Enhancing the efficiency of electron transfer and augmenting the utilization rate of peroxymonosulfate (PMS) pose challenges for advanced oxidation processes (AOPs). A high-performance bimetallic-doped catalyst (MnCo/CeO2) with an appropriate concentration of oxygen vacancies (OVs) was successfully designed using a straightforward synthesis strategy. It primarily activates PMS through non-radical pathways. Systemic characterization, experiments, and theoretical calculations have demonstrated that reasonable OVs and the Mn/Co bimetallic doping strategy effectively modulated the surface spatial electron structure and greatly improved interfacial electron transfer processes (ETP). Ultimately, MnCo/CeO2 exhibits a remarkable ciprofloxacin (CIP) removal efficiency of 93.71% (k = 0.03501 min−1) within 50 min (after 5 cycles, 89%), which is 5.03 times faster than that of traditional CeO2 (k = 0.00696 min−1), and the possible degradation pathway as well as toxicity of intermediate products were identified using LC-MS, Fukui function analysis, and toxicity evaluation. This work proposes a feasible strategy for designing bimetallic-doped metallic oxide catalysts, which have great application potential for the degradation of organic contaminants under actual harsh environmental conditions.
提高电子转移效率和过一硫酸盐(PMS)的利用率是高级氧化工艺(AOPs)面临的挑战。采用简单的合成策略,成功设计出了一种具有适当氧空位(OVs)浓度的高性能双金属掺杂催化剂(MnCo/CeO2)。它主要通过非自由基途径活化 PMS。系统表征、实验和理论计算表明,合理的氧空位和 Mn/Co 双金属掺杂策略有效地调节了表面空间电子结构,大大改善了界面电子转移过程 (ETP)。最终,MnCo/CeO2 在 50 分钟内对环丙沙星(CIP)的去除率达到 93.71%(k = 0.03501 min-1),是传统 CeO2(k = 0.00696 min-1)的 5.03 倍,并通过 LC-MS、福井函数分析和毒性评价确定了中间产物的可能降解途径和毒性。这项工作为设计双金属掺杂金属氧化物催化剂提出了可行的策略,在实际恶劣环境条件下降解有机污染物方面具有巨大的应用潜力。
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引用次数: 0
Electrochemical investigation of an antipyretic drug in plant extracts and environmental samples at the O-MWCNT/CuO nanostructure modified glassy carbon electrode 在 O-MWCNT/CuO 纳米结构修饰的玻璃碳电极上对植物提取物和环境样品中解热镇痛药物的电化学研究
IF 8.131 2区 环境科学与生态学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-11-21 DOI: 10.1039/d4en00454j
Yesurajan Allwin Richard, Sebastinbaskar Aniu Lincy, An-Ya Lo, Chelliah Koventhan, Venkataraman Dharuman, Shakkthivel Piraman
Opened multiwalled carbon nanotubes (O-MWCNT) were prepared by unzipping MWCNTs using Hummers' method and decorated with CuO to form a nanohybrid (O-MWCNT/CuO) through a simple co-precipitation technique, aimed at developing a novel electrochemical sensor. The O-MWCNT/CuO composite was used to modify a glassy carbon electrode (GCE) for the sensitive detection of the antipyretic drug acetaminophen (ACT) in various matrices. O-MWCNT/CuO was characterized using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), UV-visible spectroscopy, cyclic voltammetry (CV), linear sweep voltammetry (LSV) and electrochemical impedance spectroscopy (EIS), which confirmed the successful formation of the nanocomposite as well as its electrical conductivity and catalytic properties. The sensor demonstrates a wide linear detection range (0.005–1450 μM), with a low detection limit (LOD) of 7.2 nM and excellent sensitivity of 0.019 μA cm−2 μM−1. Additionally, the sensor demonstrated good stability (maintaining performance over 65 cycles) and selectivity in various co-interfering compounds. Notably, the electrochemical sensor was applied for the detection of ACT in environmental water samples, pharmaceutical formulations, human biological fluids, and fenugreek plant extracts, achieving good recovery rates (97.37–100.20%) with relative standard deviations (RSD) ranging from 1.0% to 3.3%, using the standard addition method. The novelty of this work lies in the development of a highly sensitive, stable, and selective GCE-modified sensor for ACT detection, with promising applications in real-world sample analysis.
利用 Hummers 方法将多壁碳纳米管拉开,制备出开放式多壁碳纳米管(O-MWCNT),并通过简单的共沉淀技术用氧化铜装饰形成纳米杂化物(O-MWCNT/CuO),旨在开发一种新型电化学传感器。O-MWCNT/CuO 复合材料被用来修饰玻璃碳电极 (GCE),以灵敏检测各种基质中的解热镇痛药对乙酰氨基酚 (ACT)。利用 X 射线衍射 (XRD)、傅立叶变换红外光谱 (FT-IR)、扫描电子显微镜 (SEM)、透射电子显微镜 (TEM)、紫外可见光谱、循环伏安法 (CV)、线性扫描伏安法 (LSV) 和电化学阻抗光谱 (EIS) 对 O-MWCNT/CuO 进行了表征,证实了纳米复合材料的成功形成及其导电性和催化特性。该传感器的线性检测范围很宽(0.005-1450 μM),检测限(LOD)低至 7.2 nM,灵敏度高达 0.019 μA cm-2 μM-1。此外,该传感器还具有良好的稳定性(可在 65 个循环周期内保持性能)和对各种共干扰化合物的选择性。值得注意的是,该电化学传感器被用于检测环境水样、药物制剂、人体生物液和葫芦巴植物提取物中的 ACT,采用标准添加法,实现了良好的回收率(97.37%-100.20%),相对标准偏差(RSD)为 1.0%-3.3%。这项工作的创新之处在于开发出了一种高灵敏度、高稳定性和高选择性的 GCE 修饰型 ACT 检测传感器,有望在实际样品分析中得到应用。
{"title":"Electrochemical investigation of an antipyretic drug in plant extracts and environmental samples at the O-MWCNT/CuO nanostructure modified glassy carbon electrode","authors":"Yesurajan Allwin Richard, Sebastinbaskar Aniu Lincy, An-Ya Lo, Chelliah Koventhan, Venkataraman Dharuman, Shakkthivel Piraman","doi":"10.1039/d4en00454j","DOIUrl":"https://doi.org/10.1039/d4en00454j","url":null,"abstract":"Opened multiwalled carbon nanotubes (O-MWCNT) were prepared by unzipping MWCNTs using Hummers' method and decorated with CuO to form a nanohybrid (O-MWCNT/CuO) through a simple co-precipitation technique, aimed at developing a novel electrochemical sensor. The O-MWCNT/CuO composite was used to modify a glassy carbon electrode (GCE) for the sensitive detection of the antipyretic drug acetaminophen (ACT) in various matrices. O-MWCNT/CuO was characterized using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), transmission electron microscopy (TEM), UV-visible spectroscopy, cyclic voltammetry (CV), linear sweep voltammetry (LSV) and electrochemical impedance spectroscopy (EIS), which confirmed the successful formation of the nanocomposite as well as its electrical conductivity and catalytic properties. The sensor demonstrates a wide linear detection range (0.005–1450 μM), with a low detection limit (LOD) of 7.2 nM and excellent sensitivity of 0.019 μA cm<small><sup>−2</sup></small> μM<small><sup>−1</sup></small>. Additionally, the sensor demonstrated good stability (maintaining performance over 65 cycles) and selectivity in various co-interfering compounds. Notably, the electrochemical sensor was applied for the detection of ACT in environmental water samples, pharmaceutical formulations, human biological fluids, and fenugreek plant extracts, achieving good recovery rates (97.37–100.20%) with relative standard deviations (RSD) ranging from 1.0% to 3.3%, using the standard addition method. The novelty of this work lies in the development of a highly sensitive, stable, and selective GCE-modified sensor for ACT detection, with promising applications in real-world sample analysis.","PeriodicalId":73,"journal":{"name":"Environmental Science: Nano","volume":"19 1","pages":""},"PeriodicalIF":8.131,"publicationDate":"2024-11-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142678205","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Source Apportionment of Hydrocarbons in Ghana's Coastal Sediments: Utilizing Hydrocarbons Ratios and Advanced Statistical Methods 加纳沿海沉积物中碳氢化合物的来源分配:利用碳氢化合物比率和先进的统计方法
IF 3.8 4区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-11-20 DOI: 10.1007/s11270-024-07588-2
Ebenezer Aquisman Asare, Dickson Abdul-Wahab, Anita Asamoah, Rafeah Wahi, Zainab Ngaini, Charles Kofi Klutse, Omolayo Ajoke Omorinoye

This study presents a comprehensive analysis of hydrocarbon pollution in Ghana's coastal sediments, with a focus on aliphatic hydrocarbons and polycyclic aromatic hydrocarbons. The primary objectives were to identify the sources of hydrocarbon pollution, assess its extent, and understand its implications for environmental management and policy. A total of 15 samples were collected from 5 sampling spots. Soxhlet extraction technique was applied. Analysis was conducted by gas chromatography/flame ionization detector for aliphatic hydrocarbons and gas chromatography/mass spectrometry for polycyclic aromatic hydrocarbons. Isomeric ratios, such as the carbon preference index, low molecular weight to high molecular weight n-alkanes, etc., were used to infer the sources of n-alkanes. Polycyclic aromatic hydrocarbons diagnostic ratios, including Benzo[b + k]fluoranthene/Benzo[a]pyrene, Phenanthrene/Anthracene, etc., were used to predict PAHs sources into petrogenic and pyrogenic sources. The study also utilized statistical tools like principal component analysis-absolute principal component scores-multiple linear regression for a detailed source appointment. The type of aliphatic hydrocarbon detected in samples ranged from C10H22 to C33H68. Concerning aliphatic hydrocarbon, C21H44 has the highest average presence at 5.224 μg/kg of dry mass in sediment samples whereas, C10H22 shows the lowest mean concentration of 1.953 µg/kg of dry mass. The mean concentrations of the polycyclic aromatic hydrocarbons detected in samples ranged from 0.544 µg/kg for Anthracene to 2.168 µg/kg for Acenaphthene. Primary findings revealed a mix of petrogenic and pyrogenic sources in the coastal sediments, evidenced by the varying aliphatic hydrocarbons and polycyclic aromatic hydrocarbons ratios. Notably, the presence of carcinogenic PAHs highlighted potential health risks. The APCS-MLR analysis identified specific sources influencing hydrocarbon pollution. These include crude oil, urban runoff, atmospheric deposition, etc. This research contributes to a better understanding of coastal sediment pollution, serving as a foundation for future environmental policies and sustainable coastal management strategies in Ghana.

本研究对加纳沿海沉积物中的碳氢化合物污染进行了全面分析,重点是脂肪族碳氢化合物和多环芳烃。主要目标是确定碳氢化合物污染的来源,评估其程度,并了解其对环境管理和政策的影响。共从 5 个采样点采集了 15 个样本。采用索氏提取技术。采用气相色谱/火焰离子化检测器分析脂肪族碳氢化合物,采用气相色谱/质谱分析多环芳烃。利用碳偏好指数、低分子量与高分子量正构烷烃等异构体比率来推断正构烷烃的来源。多环芳烃诊断比率,包括苯并[b + k]荧蒽/苯并[a]芘、菲/蒽等,用于预测多环芳烃的石油来源和热源来源。研究还利用主成分分析-绝对主成分得分-多元线性回归等统计工具进行了详细的来源划分。样本中检测到的脂肪烃类型从 C10H22 到 C33H68 不等。关于脂肪烃,C21H44 在沉积物样本中的平均含量最高,为 5.224 微克/千克(干重),而 C10H22 的平均含量最低,为 1.953 微克/千克(干重)。在样本中检测到的多环芳烃的平均浓度从 0.544 微克/千克(蒽)到 2.168 微克/千克(苊)不等。主要研究结果表明,沿海沉积物中既有岩石源,也有热源,这从不同的脂肪族碳氢化合物和多环芳烃比例中可见一斑。值得注意的是,致癌多环芳烃的存在突显了潜在的健康风险。APCS-MLR 分析确定了影响碳氢化合物污染的具体来源。这些污染源包括原油、城市径流、大气沉降等。这项研究有助于更好地了解沿海沉积物污染,为加纳未来的环境政策和可持续沿海管理战略奠定基础。
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引用次数: 0
Preparation and Characterization of a Novel Ca-Fe-Si-S Composite for the Simultaneous Stabilization of Heavy Metals in Arsenic Slag 制备新型 Ca-Fe-Si-S 复合材料并确定其特性,以同时稳定砷渣中的重金属
IF 3.8 4区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-11-20 DOI: 10.1007/s11270-024-07616-1
Ge Zhang, Huifen Yang, Xingjie Lin, Yu Miao, Chi Zhang, Fangze Li, Zhikun Pang, Xin Xin

In this work, a novel Ca-Fe-Si-S composite was prepared from thermal desorption residue through FeSO4 impregnation-pyrolysis. The characteristics and modification process of the composite were specified through a series of analytical methods. And stabilization experiments were conducted to investigate the performance of prepared materials. The optimal Ca–Fe–Si–S composite was obtained at impregnation ratio of 10%, pyrolysis temperature of 900℃ and pyrolysis time of 60 min. The modification process included the dissolution of calcium hydroxide, the formation of gypsum and ferrous silicate, the dehydration of gypsum, the reduction decomposition of calcium sulfate, the decomposition of calcium carbonate and the solid reaction at high temperature. The obtained optimal Ca–Fe–Si–S composite was a multifunctional material mainly composed of high contents of Ca, Fe, Si, S, which corresponding to FeS, CaS, Ca2SiO4, Ca3Al2(SiO4)3, Ca3Fe2(SiO4)3, Ca5(SiO4)2SO4. The application of 5% optimal Ca–Fe–Si–S composite successfully lowed the leaching concentrations of As, Zn, Cu, Cd in arsenic slag to meet the discharging standard. Meanwhile, the non-specifically bound and specifically bound of As totally decreased by 3.72%, and the acid extractable species of Zn, Cu, Cd reduced by 11.20%, 29.37%, 2.76% respectively. The distribution of stable species for heavy metals significantly increased as united results of surface complexation, chemical precipitation and ion/anion exchange reactions between the prepared composite and heavy metals. The findings of this research provide an effective material for the simultaneous stabilization of multiple heavy metals.

本研究利用热脱附残余物通过 FeSO4 浸渍-热解制备了一种新型 Ca-Fe-Si-S 复合材料。通过一系列分析方法明确了该复合材料的特性和改性过程。并通过稳定化实验研究了制备材料的性能。在浸渍率为 10%、热解温度为 900℃、热解时间为 60 分钟的条件下,获得了最佳的 Ca-Fe-Si-S 复合材料。改性过程包括氢氧化钙的溶解、石膏和硅酸亚铁的形成、石膏的脱水、硫酸钙的还原分解、碳酸钙的分解以及高温下的固体反应。获得的最佳 Ca-Fe-Si-S 复合材料是一种多功能材料,主要由高含量的 Ca、Fe、Si、S 组成,分别对应 FeS、CaS、Ca2SiO4、Ca3Al2(SiO4)3、Ca3Fe2(SiO4)3、Ca5(SiO4)2SO4。5% 的最佳 Ca-Fe-Si-S 复合材料的应用成功降低了砷渣中 As、Zn、Cu、Cd 的浸出浓度,达到了排放标准。同时,As 的非特异性结合和特异性结合完全减少了 3.72%,Zn、Cu、Cd 的酸萃取物种分别减少了 11.20%、29.37% 和 2.76%。由于制备的复合材料与重金属之间发生了表面络合、化学沉淀和离子/阴离子交换反应,重金属的稳定种类分布明显增加。这项研究成果为同时稳定多种重金属提供了一种有效的材料。
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引用次数: 0
Water Quality Assessment, Possible Pollution Source Identification from Anthropogenically Stressed River Yamuna, India using Hydrochemical, Water Quality Indices and Multivariate Statistics Analysis 利用水化学、水质指数和多元统计分析对印度亚穆纳河进行水质评估和可能的污染源鉴定
IF 3.8 4区 环境科学与生态学 Q2 ENVIRONMENTAL SCIENCES Pub Date : 2024-11-20 DOI: 10.1007/s11270-024-07649-6
Vikas Kumar, Absar Alam, Jeetendra Kumar, Venkatesh Ramrao Thakur, Vijay Kumar, Saket K. Srivastava, Dharm Nath Jha, Basanta Kumar Das

For effective and sustainable water management, assessing the water quality and identifying potential sources that threaten the river system are crucial steps. In the present study, spatiotemporal variation of 20 hydrochemical variables, water quality indices, and multivariate statistics were applied to evaluate the quality of Yamuna River water. In the middle and lower stretch, the levels of electric conductivity (EC), total dissolved solids (TDS), turbidity, dissolved organic matter (DOM), chemical oxygen demand (COD), and nutrients were higher than in the upper stretch. Based on the trophic state index, the upper, middle, and lower stretches were mesotrophic, moderate, and low eutrophic in nature, respectively. In the drinking water category, the water quality index (WQI) ranged from almost good (upper stretch) to inappropriate (middle and lower stretch). Nemerow pollution index (PINemerow) and the comprehensive pollution index (CPI) indicated that most sites were strongly and moderately polluted, respectively. Various point and nonpoint sources of pollution deteriorated the quality of Yamuna water. Spatial cluster analysis divided eleven stations into three groups based on water variables similarity. Discriminate analysis indicated that water temperature, flow, turbidity, pH, dissolved oxygen (DO), magnesium hardness (Mg-H) and COD were the most influencing variables seasonally, while water flow, pH, chloride (Clˉ), DO, Mg-H, and nitrate–N were for spatial variation in Yamuna water quality. Five potential sources were identified using principal component analysis (PCA); anthropogenic, natural, agricultural non-point sources, metrological, and seasonal factors. This study emphasizes the importance of using multivariate statistical techniques to identify variability patterns and develop management plans to improve river water quality by identifying the key variables responsible for maximum deterioration.

Graphical Abstract

为了有效和可持续地管理水资源,评估水质和确定威胁河流系统的潜在来源是至关重要的步骤。本研究采用 20 个水化学变量的时空变化、水质指数和多元统计来评估亚穆纳河水质。在中下游,电导率 (EC)、溶解性总固体 (TDS)、浊度、溶解性有机物 (DOM)、化学需氧量 (COD) 和营养物质的含量均高于上游。根据营养状态指数,上段、中段和下段分别为中营养型、中营养型和低营养型。在饮用水类别中,水质指数(WQI)从基本良好(上游)到不适宜(中游和下游)不等。尼默罗污染指数(PINemerow)和综合污染指数(CPI)分别表明,大多数地点受到严重污染和中度污染。各种点源和非点源污染导致亚穆纳河水质恶化。空间聚类分析根据水体变量的相似性将 11 个站点分为三组。判别分析表明,水温、流量、浊度、pH 值、溶解氧 (DO)、镁硬度 (Mg-H) 和化学需氧量是对亚穆纳河水质影响最大的季节性变量,而水流量、pH 值、氯化物 (Clˉ)、溶解氧、镁硬度 (Mg-H) 和硝酸盐-氮是亚穆纳河水质空间变化的影响因素。利用主成分分析(PCA)确定了五个潜在来源:人为、自然、农业非点源、气象和季节因素。这项研究强调了使用多元统计技术确定变异模式和制定管理计划的重要性,通过确定造成最大恶化的关键变量来改善河流水质。
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