Pub Date : 2024-09-30DOI: 10.1016/j.jhazmat.2024.135994
Daofen Huang, Haoran Dong, Xing Li, Long Li, Junmin Deng, Junyang Xiao, Jie Dong, Shuangjie Xiao
The ultraviolet (UV)/chlorine process has been widely applied for water treatment. However, the transformation of microplastic-leached dissolved organic matter (MP-DOM) in advanced treatment of real wastewater remains unclear. Here, we investigated alterations in the photoproperties of MP-DOM leached from biodegradable and conventional microplastics (MPs) and their subsequent effects on the degradation of sulfamethazine (SMT) by the UV/chlorine process. Spectroscopy was used to assess photophysical properties, focusing on changes in light absorption capacity, functional groups, and fluorescence components, while photochemical properties were determined by calculating the apparent quantum yields of reactive intermediates (ΦRIs). For photophysical properties, our findings revealed that the degree of molecular structure modification, functional group changes, and fluorescence characteristics during UV/chlorine treatment are closely linked to the type of MPs. For photochemical properties, the ΦRIs increased with higher chlorine dosages due to the formation of new functionalities. Both singlet oxygen (1O2) and hydroxyl radicals (•OH) formation were strongly correlated with excited triplet state of DOM (3DOM*) in the UV/chlorine treatment. Additionally, we found that the four types of MP-DOM inhibit the degradation of SMT and elucidated the mechanisms behind this inhibition. We also proposed degradation pathways for SMT and assessed the ecotoxicity of the resulting intermediates. This study provides important insights into how the characteristics and transformation of MP-DOM affect contaminant degradation, which is critical for evaluating the practical application of UV-based advanced oxidation processes (UV-AOPs).
{"title":"Transformation of dissolved organic matter leached from biodegradable and conventional microplastics under UV/chlorine treatment and the subsequent effect on contaminant removal","authors":"Daofen Huang, Haoran Dong, Xing Li, Long Li, Junmin Deng, Junyang Xiao, Jie Dong, Shuangjie Xiao","doi":"10.1016/j.jhazmat.2024.135994","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.135994","url":null,"abstract":"The ultraviolet (UV)/chlorine process has been widely applied for water treatment. However, the transformation of microplastic-leached dissolved organic matter (MP-DOM) in advanced treatment of real wastewater remains unclear. Here, we investigated alterations in the photoproperties of MP-DOM leached from biodegradable and conventional microplastics (MPs) and their subsequent effects on the degradation of sulfamethazine (SMT) by the UV/chlorine process. Spectroscopy was used to assess photophysical properties, focusing on changes in light absorption capacity, functional groups, and fluorescence components, while photochemical properties were determined by calculating the apparent quantum yields of reactive intermediates (<em>Φ</em><sub>RIs</sub>). For photophysical properties, our findings revealed that the degree of molecular structure modification, functional group changes, and fluorescence characteristics during UV/chlorine treatment are closely linked to the type of MPs. For photochemical properties, the <em>Φ</em><sub>RIs</sub> increased with higher chlorine dosages due to the formation of new functionalities. Both singlet oxygen (<sup>1</sup>O<sub>2</sub>) and hydroxyl radicals (•OH) formation were strongly correlated with excited triplet state of DOM (<sup>3</sup>DOM*) in the UV/chlorine treatment. Additionally, we found that the four types of MP-DOM inhibit the degradation of SMT and elucidated the mechanisms behind this inhibition. We also proposed degradation pathways for SMT and assessed the ecotoxicity of the resulting intermediates. This study provides important insights into how the characteristics and transformation of MP-DOM affect contaminant degradation, which is critical for evaluating the practical application of UV-based advanced oxidation processes (UV-AOPs).","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142360523","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}
Considering the unexpected nuclear power waste emission and potential nuclear leakage, the exploration of robust materials for the effective capture and storage of radioactive iodine is of great importance but still remains a challenge. In this work, we report the rational synthesis of functionalized NH2-UiO-66-on-ZIF-67 architecture to enhance the static adsorption and retention of volatile iodine. Such MOF-on-MOF heterostructures was fabricated through seeding ZIF-67 core on the surface of NH2-UiO-66 satellite via a facile polyvinylpyrrolidone (PVP) regulated internal extended growth strategies. NH2-UiO-66-on-ZIF-67 exhibited unique core-satellite structure, which significantly promotes the binding interactions with iodine through synergizing of the N-rich imidazole moieties and surface functionalized amino groups within the porosity channels. As a result, the as fabricated NH2-UiO-66-on-ZIF-67 achieves enhanced mass diffusion and high capture capacity of 3600 mg g–1 for iodine vapor under static sorption conditions. Moreover, water vapor in humid conditions (relative humidity of 18%) has almost no effect on the static iodine adsorption performance of the material. This study sheds light on a reliable MOF-on-MOF hybrid strategy for effective radioiodine treatment to ensure the safety nuclear waste management.
{"title":"Construction of heterogeneous MOF-on-MOF for highly efficient gaseous iodine sequestration under static conditions","authors":"Linshuai Liu, Nannan Wang, Chunlin He, Yuezhou Wei, Jingjing Wang, Xinpeng Wang","doi":"10.1016/j.jhazmat.2024.136017","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136017","url":null,"abstract":"Considering the unexpected nuclear power waste emission and potential nuclear leakage, the exploration of robust materials for the effective capture and storage of radioactive iodine is of great importance but still remains a challenge. In this work, we report the rational synthesis of functionalized NH<sub>2</sub>-UiO-66-on-ZIF-67 architecture to enhance the static adsorption and retention of volatile iodine. Such MOF-on-MOF heterostructures was fabricated through seeding ZIF-67 core on the surface of NH<sub>2</sub>-UiO-66 satellite via a facile polyvinylpyrrolidone (PVP) regulated internal extended growth strategies. NH<sub>2</sub>-UiO-66-on-ZIF-67 exhibited unique core-satellite structure, which significantly promotes the binding interactions with iodine through synergizing of the N-rich imidazole moieties and surface functionalized amino groups within the porosity channels. As a result, the as fabricated NH<sub>2</sub>-UiO-66-on-ZIF-67 achieves enhanced mass diffusion and high capture capacity of 3600<!-- --> <!-- -->mg<!-- --> <!-- -->g<sup>–1</sup> for iodine vapor under static sorption conditions. Moreover, water vapor in humid conditions (relative humidity of 18%) has almost no effect on the static iodine adsorption performance of the material. This study sheds light on a reliable MOF-on-MOF hybrid strategy for effective radioiodine treatment to ensure the safety nuclear waste management.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142360541","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}
Pub Date : 2024-09-30DOI: 10.1016/j.jhazmat.2024.136015
Guojian Wu, Chenxing Du, Chuanyi Peng, Zitong Qiu, Si Li, Wenjuan Chen, Huimin Qiu, Zhi Zheng, Zhiwei Lu, Yizhong Shen
The intelligently efficient, reliable, economical and portable onsite assay toward pyrethroid pesticides (PPs) residues is critical for food safety analysis and environmental pollution traceability. Here, a fluorescent nanozyme Cu-ATP@[Ru(bpy)3]2+ with laccase-like activity was designed to develop a versatile machine learning-assisted colorimetric and fluorescence dual-modal assay for efficient onsite intelligent decision recognition and quantification of PPs residues. In the presence of alkaline phosphatase (ALP), the laccase-like activity of Cu-ATP@[Ru(bpy)3]2+ was enhanced to oxidize colorless o-phenylenediamine (OPD) into dark-yellow 2,3-diaminophenazine (DAP) via electron transfer, appearing a new yellow fluorescence at 550 nm. Meanwhile, the red fluorescence of Cu-ATP@[Ru(bpy)3]2+ at 600 nm was quenched due to the internal filter effect (IFE) of DAP towards Cu-ATP@[Ru(bpy)3]2+. However, the selective inhibition of PPs toward ALP activity enabled to observe a dual-modal response of PPs concentration-dependent decrease in colorimetric signal and enhancement in the fluorescence intensity ratio of F600 nm/F550 nm. On this basis, both the colorimetric and fluorescence images were captured and processed with a home-made WeChat applet-installed smartphone to extract the corresponding image color information, thus achieving machine learning-assisted onsite real-time and dynamic intelligent decision recognition and quantification of PPs residues in real samples, which shows a promising potential in safeguarding food safety and environmental health.
{"title":"Machine learning-assisted laccase-like activity nanozyme for intelligently onsite real-time and dynamic analysis of pyrethroid pesticides","authors":"Guojian Wu, Chenxing Du, Chuanyi Peng, Zitong Qiu, Si Li, Wenjuan Chen, Huimin Qiu, Zhi Zheng, Zhiwei Lu, Yizhong Shen","doi":"10.1016/j.jhazmat.2024.136015","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136015","url":null,"abstract":"The intelligently efficient, reliable, economical and portable onsite assay toward pyrethroid pesticides (PPs) residues is critical for food safety analysis and environmental pollution traceability. Here, a fluorescent nanozyme Cu-ATP@[Ru(bpy)<sub>3</sub>]<sup>2+</sup> with laccase-like activity was designed to develop a versatile machine learning-assisted colorimetric and fluorescence dual-modal assay for efficient onsite intelligent decision recognition and quantification of PPs residues. In the presence of alkaline phosphatase (ALP), the laccase-like activity of Cu-ATP@[Ru(bpy)<sub>3</sub>]<sup>2+</sup> was enhanced to oxidize colorless <em>o</em>-phenylenediamine (OPD) into dark-yellow 2,3-diaminophenazine (DAP) via electron transfer, appearing a new yellow fluorescence at 550<!-- --> <!-- -->nm. Meanwhile, the red fluorescence of Cu-ATP@[Ru(bpy)<sub>3</sub>]<sup>2+</sup> at 600<!-- --> <!-- -->nm was quenched due to the internal filter effect (IFE) of DAP towards Cu-ATP@[Ru(bpy)<sub>3</sub>]<sup>2+</sup>. However, the selective inhibition of PPs toward ALP activity enabled to observe a dual-modal response of PPs concentration-dependent decrease in colorimetric signal and enhancement in the fluorescence intensity ratio of <em>F</em><sub>600 nm</sub>/<em>F</em><sub>550 nm</sub>. On this basis, both the colorimetric and fluorescence images were captured and processed with a home-made WeChat applet-installed smartphone to extract the corresponding image color information, thus achieving machine learning-assisted onsite real-time and dynamic intelligent decision recognition and quantification of PPs residues in real samples, which shows a promising potential in safeguarding food safety and environmental health.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142330237","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}
Pub Date : 2024-09-30DOI: 10.1016/j.jhazmat.2024.136002
Xin Zhang, Yanjun Zhang, Yu Zhang, Yuxiang Cheng, Qiangbin Liu, Hao Deng, Yongjie Ma, Lin Bai, Lei Liu
During nuclear accidents, large quantities of radionuclides will be released into the environment, posing serious health hazards to local residents. The screening of high-risk nuclides is critical for the development of subsequent nuclear emergency response measures. In order to overcome the shortcomings of traditional screening methods, a machine learning method was proposed to screen high-risk nuclides and predict their contamination to groundwater more effectively. The performances of Support Vector Machine (SVM), Random Forest (RF) and Back Propagation Neural Network (BPNN) algorithms were compared, and sensitivity analyses of the initial leakage concentration ratio (C0/Cp), distribution coefficient (Kd) and decay coefficient () on the model outputs were performed. Results showed that RF classification model achieved the highest prediction accuracy for screening high-risk nuclides. The contribution of the input parameters ranked as Kd > > C0/Cp. BPNN regression model was found to be the best for predicting when high-risk nuclides would pollute groundwater. The output was negatively correlated with C0/Cp and positively correlated with Kd and , with the parameter influence ranking as Kd > C0/Cp > . The contribution of Kd mainly came from itself, and the contribution of C0/Cp and mainly due to their interaction with other parameters.
{"title":"High-risk nuclide screening and parameter sensitivity analysis based on numerical simulation and machine learning","authors":"Xin Zhang, Yanjun Zhang, Yu Zhang, Yuxiang Cheng, Qiangbin Liu, Hao Deng, Yongjie Ma, Lin Bai, Lei Liu","doi":"10.1016/j.jhazmat.2024.136002","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136002","url":null,"abstract":"During nuclear accidents, large quantities of radionuclides will be released into the environment, posing serious health hazards to local residents. The screening of high-risk nuclides is critical for the development of subsequent nuclear emergency response measures. In order to overcome the shortcomings of traditional screening methods, a machine learning method was proposed to screen high-risk nuclides and predict their contamination to groundwater more effectively. The performances of Support Vector Machine (SVM), Random Forest (RF) and Back Propagation Neural Network (BPNN) algorithms were compared, and sensitivity analyses of the initial leakage concentration ratio (<em>C</em><sub><em>0</em></sub><em>/C</em><sub><em>p</em></sub>), distribution coefficient (<em>K</em><sub><em>d</em></sub>) and decay coefficient (<span><math><mi is=\"true\" mathvariant=\"bold-italic\">λ</mi></math></span>) on the model outputs were performed. Results showed that RF classification model achieved the highest prediction accuracy for screening high-risk nuclides. The contribution of the input parameters ranked as <em>K</em><sub><em>d</em></sub> > <span><math><mi is=\"true\">λ</mi></math></span> > <em>C</em><sub><em>0</em></sub><em>/C</em><sub><em>p</em></sub>. BPNN regression model was found to be the best for predicting when high-risk nuclides would pollute groundwater. The output was negatively correlated with <em>C</em><sub><em>0</em></sub><em>/C</em><sub><em>p</em></sub> and positively correlated with <em>K</em><sub><em>d</em></sub> and <span><math><mi is=\"true\">λ</mi></math></span>, with the parameter influence ranking as <em>K</em><sub><em>d</em></sub> > <em>C</em><sub><em>0</em></sub><em>/C</em><sub><em>p</em></sub> > <span><math><mi is=\"true\">λ</mi></math></span>. The contribution of <em>K</em><sub><em>d</em></sub> mainly came from itself, and the contribution of <em>C</em><sub><em>0</em></sub><em>/C</em><sub><em>p</em></sub> and <span><math><mi is=\"true\">λ</mi></math></span> mainly due to their interaction with other parameters.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142360526","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}
Pub Date : 2024-09-29DOI: 10.1016/j.jhazmat.2024.136004
Abbas Motalebizadeh, Somayeh Fardindoost, Mina Hoorfar
In this study, we developed a method for the on-site selective detection and quantification of microplastics in various water matrices using fluorescence-tagged peptides combined with electrochemical impedance spectroscopy (EIS). Among the types of plastics found in seawater, polystyrene (PS) microplastics were selected. Fluorometry, scanning electron microscopy (SEM), and Raman spectroscopy were used to verify the specific interaction of these peptides with PS spherical particles of different sizes (ranging from 0.1 to 250 µm). Principal component analysis (PCA) was employed to determine the effects of temperature (25-65 °C), incubation time (5 and 10 minutes), and particle size on plastic-peptide bonding efficiency, based on fluorescence intensity. For each water type (pure, tap, NaCl (0.5 M), and seawater), EIS plots (Nyquist and Bode) were generated. Significant factors affecting the EIS response, including particle size, shape, and material, were analyzed by measuring electrical parameters for different microplastic concentrations (50 ppb to 20 ppm). The EIS parameters changed with increasing plastic concentration, determining a limit of detection (LOD) of 50 ppb (ng/mL) for pure and tap water and 400 ppb for saline water, as the lowest concentration producing a significant change in EIS parameters compared to the baseline. The sensor proved highly effective for detecting microplastics in low ionic strength environments such as pure and tap water. However, in high ionic strength environments like saline and seawater, the detection capability diminished, likely due to the masking effect of ions on the EIS response.
在这项研究中，我们开发了一种利用荧光标记肽结合电化学阻抗光谱（EIS）对各种水基质中的微塑料进行现场选择性检测和定量的方法。在海水中发现的塑料类型中，选择了聚苯乙烯（PS）微塑料。利用荧光测定法、扫描电子显微镜（SEM）和拉曼光谱来验证这些肽与不同大小（0.1 至 250 微米）的 PS 球形颗粒之间的特定相互作用。根据荧光强度，采用主成分分析法（PCA）确定温度（25-65 °C）、培养时间（5 和 10 分钟）和颗粒大小对塑料肽键合效率的影响。对于每种水（纯水、自来水、NaCl（0.5 M）和海水），都生成了 EIS 图（奈奎斯特图和博德图）。通过测量不同微塑料浓度（50 ppb 至 20 ppm）的电参数，分析了影响 EIS 响应的重要因素，包括颗粒大小、形状和材料。EIS 参数随着塑料浓度的增加而变化，纯水和自来水的检测限（LOD）为 50 ppb（纳克/毫升），盐水的检测限（LOD）为 400 ppb，这是 EIS 参数与基线相比发生显著变化的最低浓度。事实证明，在纯净水和自来水等低离子强度环境中，传感器能非常有效地检测微塑料。然而，在盐水和海水等高离子强度环境中，检测能力下降，这可能是由于离子对 EIS 响应的掩蔽效应。
{"title":"Selective On-Site Detection and Quantification of Polystyrene Microplastics in Water Using Fluorescence-Tagged Peptides and Electrochemical Impedance Spectroscopy","authors":"Abbas Motalebizadeh, Somayeh Fardindoost, Mina Hoorfar","doi":"10.1016/j.jhazmat.2024.136004","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136004","url":null,"abstract":"In this study, we developed a method for the on-site selective detection and quantification of microplastics in various water matrices using fluorescence-tagged peptides combined with electrochemical impedance spectroscopy (EIS). Among the types of plastics found in seawater, polystyrene (PS) microplastics were selected. Fluorometry, scanning electron microscopy (SEM), and Raman spectroscopy were used to verify the specific interaction of these peptides with PS spherical particles of different sizes (ranging from 0.1 to 250<!-- --> <!-- -->µm). Principal component analysis (PCA) was employed to determine the effects of temperature (25-65 °C), incubation time (5 and 10<!-- --> <!-- -->minutes), and particle size on plastic-peptide bonding efficiency, based on fluorescence intensity. For each water type (pure, tap, NaCl (0.5<!-- --> <!-- -->M), and seawater), EIS plots (Nyquist and Bode) were generated. Significant factors affecting the EIS response, including particle size, shape, and material, were analyzed by measuring electrical parameters for different microplastic concentrations (50 ppb to 20 ppm). The EIS parameters changed with increasing plastic concentration, determining a limit of detection (LOD) of 50 ppb (ng/mL) for pure and tap water and 400 ppb for saline water, as the lowest concentration producing a significant change in EIS parameters compared to the baseline. The sensor proved highly effective for detecting microplastics in low ionic strength environments such as pure and tap water. However, in high ionic strength environments like saline and seawater, the detection capability diminished, likely due to the masking effect of ions on the EIS response.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142330238","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}
Rapid urbanization in China has led to the disappearance of countless villages and the transformation of homestead land into cultivated land or grassland. The quality of homestead soil (HS) plays a pivotal role in land-use conversion and reuse strategies, so the current state of heavy metal pollution in HS deserves attention. This study determined the fraction contents, bioaccessibility, risks, and affecting factors of Hg, As, Cd, Pb, Cu, and Zn in HS by comparing them with soil in cultivated land (CS), grassland (GS), homestead-converted cultivated land (HCS), and homestead-converted grassland (HGS). Results demonstrate that the contents of the six metals exceed background values, especially for Cd and Hg, resulting in significant pollution and elevated ecological risk. Distinct from the dominant residual fraction of other metals, the extractable fraction of Cd shows the highest proportion, which also contributes most to the high values of the Risk Assessment Code and extreme pollution conditions in HS, GS, and CS. Moreover, pH shows predominantly negative relations with the effective available and potentially available contents, while the effects of organic carbon fractions are notably the opposite. Furthermore, CS and GS suggest higher non-carcinogenic and carcinogenic risks than in the converted soil. This study indicates that HS has a lower metal accumulation risk compared with cultivated land and grassland, and homestead conversion seems to restrict the bioaccessibility of metals in soil.
{"title":"Heavy metals in homestead soil: metal fraction contents, bioaccessibility, and risk assessment","authors":"Qingqing Cao, Jiaqi Zhao, Wen Ma, Dongxu Cui, Xiaoping Zhang, Jian Liu, Hao Chen","doi":"10.1016/j.jhazmat.2024.135933","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.135933","url":null,"abstract":"Rapid urbanization in China has led to the disappearance of countless villages and the transformation of homestead land into cultivated land or grassland. The quality of homestead soil (HS) plays a pivotal role in land-use conversion and reuse strategies, so the current state of heavy metal pollution in HS deserves attention. This study determined the fraction contents, bioaccessibility, risks, and affecting factors of Hg, As, Cd, Pb, Cu, and Zn in HS by comparing them with soil in cultivated land (CS), grassland (GS), homestead-converted cultivated land (HCS), and homestead-converted grassland (HGS). Results demonstrate that the contents of the six metals exceed background values, especially for Cd and Hg, resulting in significant pollution and elevated ecological risk. Distinct from the dominant residual fraction of other metals, the extractable fraction of Cd shows the highest proportion, which also contributes most to the high values of the Risk Assessment Code and extreme pollution conditions in HS, GS, and CS. Moreover, pH shows predominantly negative relations with the effective available and potentially available contents, while the effects of organic carbon fractions are notably the opposite. Furthermore, CS and GS suggest higher non-carcinogenic and carcinogenic risks than in the converted soil. This study indicates that HS has a lower metal accumulation risk compared with cultivated land and grassland, and homestead conversion seems to restrict the bioaccessibility of metals in soil.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142330239","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}
Pub Date : 2024-09-29DOI: 10.1016/j.jhazmat.2024.135993
Fang Bai, Jie Li, Tianli Li, Jun Sha, Jin Liu, Lin Li, Guofei Dai, Yunlu Jia, Lirong Song
The use of H2O2 to mitigate cyanobacterial blooms has gained popularity due to its selectivity. Previous research has shown that consecutive low-dose H2O2 are far more effective in suppressing cyanobacteria than a single higher dose, minimizing damage to co-existing organisms in the aquatic ecosystem. However, the underlying mechanism remains unclear. This study aimed to investigate the mechanism underlying this sensitivity by monitoring the progression from oxidative stress to cell death in Microcystis induced by consecutive low doses of H2O2 (3+5 mg/L, with an interval time of 4 hours). The initial application of H2O2 (3 mg/L) resulted in a rapid increase in the transcription of antioxidant genes (gpx, 2-cys prx, trxA and sod) within 1 h, and returned to baseline levels within 8 h. The addition of a second H2O2 led to a significant increase in glutathione peroxidase (gene and product) and glutathione within 24 h. The cell death following consecutive H2O2 stress was classified as regulated cell death (RCD), characterized by the upregulated metacaspase genes, increased caspase-like activity, modulation of the mazEF system, DNA fragmentation, cell vacuolization, and membrane disruption. Interestingly, the RCD process coincided with the fluctuation of glutathione cycle. Validation experiments demonstrated that exogenous glutathione can promote the gene expression and activity of metacaspase, while inhibition of glutathione biosynthesis led to decreased intracellular glutathione and suppressed metacaspase activity and gene expression. Therefore, glutathione may play a vital role in the connection between oxidative stress and RCD during consecutive H2O2 treatment. These results reveal the inherent vulnerability of Microcystis to consecutive oxidative stress, providing a biological mechanism for a sustainable strategy to mitigate cyanobacterial bloom.
{"title":"Unveiling the susceptibility mechanism of Microcystis to consecutive sub-lethal oxidative stress—Enhancing Oxidation Technology for Cyanobacterial Bloom Control","authors":"Fang Bai, Jie Li, Tianli Li, Jun Sha, Jin Liu, Lin Li, Guofei Dai, Yunlu Jia, Lirong Song","doi":"10.1016/j.jhazmat.2024.135993","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.135993","url":null,"abstract":"The use of H<sub>2</sub>O<sub>2</sub> to mitigate cyanobacterial blooms has gained popularity due to its selectivity. Previous research has shown that consecutive low-dose H<sub>2</sub>O<sub>2</sub> are far more effective in suppressing cyanobacteria than a single higher dose, minimizing damage to co-existing organisms in the aquatic ecosystem. However, the underlying mechanism remains unclear. This study aimed to investigate the mechanism underlying this sensitivity by monitoring the progression from oxidative stress to cell death in <em>Microcystis</em> induced by consecutive low doses of H<sub>2</sub>O<sub>2</sub> (3+5<!-- --> <!-- -->mg/L, with an interval time of 4<!-- --> <!-- -->hours). The initial application of H<sub>2</sub>O<sub>2</sub> (3<!-- --> <!-- -->mg/L) resulted in a rapid increase in the transcription of antioxidant genes (<em>gpx</em>, <em>2-cys prx</em>, <em>trxA</em> and <em>sod</em>) within 1<!-- --> <!-- -->h, and returned to baseline levels within 8<!-- --> <!-- -->h. The addition of a second H<sub>2</sub>O<sub>2</sub> led to a significant increase in glutathione peroxidase (gene and product) and glutathione within 24<!-- --> <!-- -->h. The cell death following consecutive H<sub>2</sub>O<sub>2</sub> stress was classified as regulated cell death (RCD), characterized by the upregulated metacaspase genes, increased caspase-like activity, modulation of the <em>mazEF</em> system, DNA fragmentation, cell vacuolization, and membrane disruption. Interestingly, the RCD process coincided with the fluctuation of glutathione cycle. Validation experiments demonstrated that exogenous glutathione can promote the gene expression and activity of metacaspase, while inhibition of glutathione biosynthesis led to decreased intracellular glutathione and suppressed metacaspase activity and gene expression. Therefore, glutathione may play a vital role in the connection between oxidative stress and RCD during consecutive H<sub>2</sub>O<sub>2</sub> treatment. These results reveal the inherent vulnerability of <em>Microcystis</em> to consecutive oxidative stress, providing a biological mechanism for a sustainable strategy to mitigate cyanobacterial bloom.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142330241","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}
Understanding how widely distributed microplastics (MPs) and diethyl phthalate (DEP) interact with crops remains limited, despite their significant implications for human exposure. We used physiology, transcriptomics, adsorption kinetics, and computational chemistry to assess rye’s molecular response to two sizes of MPs (200 nm and 5 μm) and DEP, both individually and in combination. Findings systematically highlight potential ecological risks from MPs and DEP, with ecotoxicity ranking as follows: CK (Control Check) < LMPs < SMPs < DEP < LMPs+DEP < SMPs+DEP. Fluorescence and scanning electron microscopy revealed SMP’s translocation ability in rye and its potential to disrupt leaf cells. DEP increased the negative charge on MPs, which enhanced their uptake by rye. DEP adsorption by MPs in hydroponics reduced DEP bioavailability in rye (18.17-46.91%). Molecular docking studies showed DEP interacted with chlorophyll, superoxide dismutase, and glutathione S-transferases proteins’ active sites. Transcriptomic analysis identified significant up-regulation of genes linked to mitogen-activated protein kinase signaling, phytohormones, and antioxidant systems in rye exposed to MPs and DEP, correlating with physiological changes. These findings deepen the understanding of how MPs can accumulate and translocate within rye, and their adsorption to DEP raises crop safety issues of greater environmental risk.
尽管微塑料（MPs）和邻苯二甲酸二乙酯（DEP）对人类暴露有重大影响，但人们对广泛分布的微塑料（MPs）和邻苯二甲酸二乙酯（DEP）如何与农作物相互作用的了解仍然有限。我们利用生理学、转录组学、吸附动力学和计算化学来评估黑麦对两种尺寸的微塑料（200 nm 和 5 μm）和邻苯二甲酸二乙酯（DEP）的分子反应。研究结果系统地强调了 MPs 和 DEP 的潜在生态风险，生态毒性排名如下：CK（对照检查）；LMPs；SMPs；DEP；LMPs+DEP；SMPs+DEP。荧光和扫描电子显微镜显示了 SMP 在黑麦中的迁移能力及其破坏叶片细胞的潜力。DEP 增加了 MPs 的负电荷，从而增强了黑麦对其的吸收。水培法中 MPs 对 DEP 的吸附降低了 DEP 在黑麦中的生物利用率（18.17%-46.91%）。分子对接研究表明，DEP 与叶绿素、超氧化物歧化酶和谷胱甘肽 S 转化酶蛋白的活性位点相互作用。转录组分析发现，在暴露于 MPs 和 DEP 的黑麦中，与丝裂原活化蛋白激酶信号转导、植物激素和抗氧化系统有关的基因明显上调，这与生理变化相关。这些发现加深了人们对 MPs 如何在黑麦中积累和转移的理解，而它们对 DEP 的吸附又提出了具有更大环境风险的作物安全问题。
{"title":"Revealing the bioavailability and phytotoxicity of different particle size microplastics on diethyl phthalate (DEP) in rye (Secale cereale L.)","authors":"Jinke Hu, Guozhang Bao, Xinyu Pan, Huixin Wang, Ningning Xing","doi":"10.1016/j.jhazmat.2024.135979","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.135979","url":null,"abstract":"Understanding how widely distributed microplastics (MPs) and diethyl phthalate (DEP) interact with crops remains limited, despite their significant implications for human exposure. We used physiology, transcriptomics, adsorption kinetics, and computational chemistry to assess rye’s molecular response to two sizes of MPs (200<!-- --> <!-- -->nm and 5 μm) and DEP, both individually and in combination. Findings systematically highlight potential ecological risks from MPs and DEP, with ecotoxicity ranking as follows: CK (Control Check) < LMPs < SMPs < DEP < LMPs+DEP < SMPs+DEP. Fluorescence and scanning electron microscopy revealed SMP’s translocation ability in rye and its potential to disrupt leaf cells. DEP increased the negative charge on MPs, which enhanced their uptake by rye. DEP adsorption by MPs in hydroponics reduced DEP bioavailability in rye (18.17-46.91%). Molecular docking studies showed DEP interacted with chlorophyll, superoxide dismutase, and glutathione S-transferases proteins’ active sites. Transcriptomic analysis identified significant up-regulation of genes linked to mitogen-activated protein kinase signaling, phytohormones, and antioxidant systems in rye exposed to MPs and DEP, correlating with physiological changes. These findings deepen the understanding of how MPs can accumulate and translocate within rye, and their adsorption to DEP raises crop safety issues of greater environmental risk.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329235","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}
Pub Date : 2024-09-28DOI: 10.1016/j.jhazmat.2024.135954
Hua Wang, Ran Wu, Haoyi Zheng, Yanxia Gong, Yong Yang, Yaxin Zhu, Lijuan Liu, Miaozhen Cai, Shaoting Du
Chiral herbicides applied to agricultural soils are typically mildly to moderately contaminated with heavy metals (HMs), necessitating a thorough investigation into their effects on soil HMs availability. This study evaluated the effect of the chiral herbicide napropamide (NAP) on HMs bioavailability in different soil types, including weakly alkaline clay in Northeast China, neutral sandy loam in Zhejiang, and weakly acidic clay loam in Sichuan, China. The results demonstrate significant differences in the availability of HMs (Cd, Pb, Zn, and Ni) in the soil following enantiomer treatments, with variation ranges of 4.57-45.67%, 5.03-96.21%, 2.92-52.30%, and 10.57-29.79%, respectively. Overall, R-NAP enhanced the bioavailability of HMs more effectively than S-NAP, specifically by significantly activating available iron 3.33-191.97% and markedly affecting soil pH and cation exchange capacity. Additionally, R-NAP influenced biotic processes by enriching dominant microbial communities, such as Chitinophaga, Niabella, and Promicromonospora, and by constructing more stable microbial networks. Notably, bioavailable Fe plays a dual regulatory role, affecting both the abiotic and biotic processes affected by soil NAP. In summary, although R-NAP is commonly used in agriculture, it poses a greater risk of HMs contamination in crops, highlighting the need for careful application and management. This study provides a fundamental theoretical basis for the judicious use of chiral herbicides in agricultural soils with mild-to-moderate HMs contamination.
农田土壤中施用的手性除草剂通常会受到轻度至中度的重金属（HMs）污染，因此有必要深入研究其对土壤中 HMs 可利用性的影响。本研究评估了手性除草剂萘草胺（NAP）对不同土壤类型中 HMs 生物利用率的影响，包括中国东北的弱碱性粘土、浙江的中性砂壤土和四川的弱酸性粘壤土。结果表明，对映体处理后，土壤中 HMs（镉、铅、锌和镍）的可利用性存在显著差异，变化范围分别为 4.57-45.67%、5.03-96.21%、2.92-52.30% 和 10.57-29.79%。总体而言，R-NAP 比 S-NAP 更有效地提高了 HMs 的生物利用率，特别是显著激活了可用铁 3.33-191.97%，并明显影响了土壤 pH 值和阳离子交换容量。此外，R-NAP 还通过丰富优势微生物群落（如 Chitinophaga、Niabella 和 Promicromonospora）以及构建更稳定的微生物网络来影响生物过程。值得注意的是，生物可利用铁发挥着双重调节作用，既影响非生物过程，也影响受土壤 NAP 影响的生物过程。总之，虽然 R-NAP 常用于农业，但它对作物造成 HMs 污染的风险更大，因此需要谨慎应用和管理。本研究为在轻度至中度 HMs 污染的农业土壤中合理使用手性除草剂提供了基本理论依据。
{"title":"Enhanced Mobilization of Soil Heavy Metals by the Enantioselective Herbicide R-Napropamide Compared to its S-Isomer: Analyses of Abiotic and Biotic Drivers","authors":"Hua Wang, Ran Wu, Haoyi Zheng, Yanxia Gong, Yong Yang, Yaxin Zhu, Lijuan Liu, Miaozhen Cai, Shaoting Du","doi":"10.1016/j.jhazmat.2024.135954","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.135954","url":null,"abstract":"Chiral herbicides applied to agricultural soils are typically mildly to moderately contaminated with heavy metals (HMs), necessitating a thorough investigation into their effects on soil HMs availability. This study evaluated the effect of the chiral herbicide napropamide (NAP) on HMs bioavailability in different soil types, including weakly alkaline clay in Northeast China, neutral sandy loam in Zhejiang, and weakly acidic clay loam in Sichuan, China. The results demonstrate significant differences in the availability of HMs (Cd, Pb, Zn, and Ni) in the soil following enantiomer treatments, with variation ranges of 4.57-45.67%, 5.03-96.21%, 2.92-52.30%, and 10.57-29.79%, respectively. Overall, <em>R</em>-NAP enhanced the bioavailability of HMs more effectively than <em>S</em>-NAP, specifically by significantly activating available iron 3.33-191.97% and markedly affecting soil pH and cation exchange capacity. Additionally, <em>R</em>-NAP influenced biotic processes by enriching dominant microbial communities, such as <em>Chitinophaga</em>, <em>Niabella</em>, and <em>Promicromonospora</em>, and by constructing more stable microbial networks. Notably, bioavailable Fe plays a dual regulatory role, affecting both the abiotic and biotic processes affected by soil NAP. In summary, although <em>R</em>-NAP is commonly used in agriculture, it poses a greater risk of HMs contamination in crops, highlighting the need for careful application and management. This study provides a fundamental theoretical basis for the judicious use of chiral herbicides in agricultural soils with mild-to-moderate HMs contamination.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142329234","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}
Pub Date : 2024-09-28DOI: 10.1016/j.jhazmat.2024.135988
Vangelis Soultanidis, Evangelos A. Voudrias
Asbestos-Containing Materials (ACMs) were widely used in the construction sector but, due to their harmful health effects, many countries have banned their use. ACMs are classified as hazardous and, in contact with water, produce potentially harmful leachates. The objective of this work was to determine the leaching behavior of 20 elements from two asbestos-cement materials and mine asbestos samples across the entire pH range and varying liquid-to-solid ratios (column tests). The pH-dependence tests showed consistent leaching patterns across the three materials. Geochemical speciation model (LeachXS) predictions were successful in most cases of the batch experiments and were improved by adjusting iron oxides concentration for some elements. Model predictions were successful for fewer elements in the column experiments. Depending on the pH, element release was controlled by respective solid phase dissolution, sorption onto iron oxides and substitution in ettringite. Some leaching concentrations exceeded the EU limits for granular non-hazardous waste landfills. Considering the strongly alkaline nature of monolithic asbestos-cement waste undergoing carbonation, we propose all three materials to be disposed of in non-hazardous waste landfills, according to EU legislation. A case study concluded that geochemical modeling of ACMs leaching is a useful tool in estimating element release under various environmental conditions.
{"title":"Leaching and geochemical modeling of asbestos-cement waste and mine asbestos","authors":"Vangelis Soultanidis, Evangelos A. Voudrias","doi":"10.1016/j.jhazmat.2024.135988","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.135988","url":null,"abstract":"Asbestos-Containing Materials (ACMs) were widely used in the construction sector but, due to their harmful health effects, many countries have banned their use. ACMs are classified as hazardous and, in contact with water, produce potentially harmful leachates. The objective of this work was to determine the leaching behavior of 20 elements from two asbestos-cement materials and mine asbestos samples across the entire pH range and varying liquid-to-solid ratios (column tests). The pH-dependence tests showed consistent leaching patterns across the three materials. Geochemical speciation model (LeachXS) predictions were successful in most cases of the batch experiments and were improved by adjusting iron oxides concentration for some elements. Model predictions were successful for fewer elements in the column experiments. Depending on the pH, element release was controlled by respective solid phase dissolution, sorption onto iron oxides and substitution in ettringite. Some leaching concentrations exceeded the EU limits for granular non-hazardous waste landfills. Considering the strongly alkaline nature of monolithic asbestos-cement waste undergoing carbonation, we propose all three materials to be disposed of in non-hazardous waste landfills, according to EU legislation. A case study concluded that geochemical modeling of ACMs leaching is a useful tool in estimating element release under various environmental conditions.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142328873","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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}
京公网安备 11010802042870号
京ICP备2023020795号-1
扫码关注我们
求助内容：
应助结果提醒方式：