Pub Date : 2024-09-27DOI: 10.1016/j.jhazmat.2024.135989
Lansen Yang, Pengfei Li, Ligai Bai, Jiankun Cao, Hongyuan Yan
The accumulation of perfluorocarboxylic acids (PFCAs) in environment and foods represents a significant threat to public health due to the long-term ingestion of contaminated food. This study introduces a novel adsorbent, the hierarchical porous hydrophilic molecularly imprinted resin (HPHMIR), which was synthesized by integrating molecular imprinting techniques with hydrophilic resins. The HPHMIR, characterized by its extensive mesoporous structure (average pore width ~9.71 nm) and favorable imprinting factors (2.6–5.0), facilitates the effective adsorption of PFCAs from complex matrices through multiple interaction mechanisms, including hydrogen bonding and electrostatic interactions. This innovative material was employed in a 96-well plate format for solid-phase extraction (SPE), and combined with LC-MS/MS, a high-throughput method for the determination of PFCAs in milk was developed. The proposed method demonstrated exceptional performance, including excellent linearity (0.48–240 ng mL−1; r ≥ 0.9986), low detection limits (0.04–0.11 ng mL−1), high precision (relative standard deviation ≤ 9.9%), and satisfactory recovery (75.7–118.1%). These results highlight the efficacy of the method in extracting trace levels of PFCAs from complicated sample matrices, presenting a promising alternative for monitoring PFCA contamination and advancing public health standards.
由于长期摄入受污染的食物，全氟羧酸（PFCAs）在环境和食物中的积累对公众健康构成了重大威胁。本研究介绍了一种新型吸附剂--分层多孔亲水性分子印迹树脂（HPHMIR），它是通过将分子印迹技术与亲水性树脂相结合而合成的。HPHMIR 具有广泛的介孔结构（平均孔宽约为 9.71 nm）和良好的印迹因子（2.6-5.0），可通过多种相互作用机制（包括氢键和静电作用）从复杂基质中有效吸附全氟辛烷磺酸。将这种创新材料用于 96 孔板固相萃取（SPE），并结合 LC-MS/MS，开发了一种高通量测定牛奶中 PFCAs 的方法。该方法线性关系良好（0.48-240 ng mL-1; r ≥ 0.9986），检出限低（0.04-0.11 ng mL-1），精密度高（相对标准偏差≤9.9%），回收率高（75.7-118.1%）。这些结果凸显了该方法从复杂样品基质中提取痕量全氟辛烷磺酸的功效，为监测全氟辛烷磺酸污染和提高公共卫生标准提供了一种可行的替代方法。
{"title":"Innovative hierarchical porous hydrophilic molecularly imprinted resin for high-throughput detection of perfluorocarboxylic acids in milk using 96-well plate SPE-LC-MS/MS","authors":"Lansen Yang, Pengfei Li, Ligai Bai, Jiankun Cao, Hongyuan Yan","doi":"10.1016/j.jhazmat.2024.135989","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.135989","url":null,"abstract":"The accumulation of perfluorocarboxylic acids (PFCAs) in environment and foods represents a significant threat to public health due to the long-term ingestion of contaminated food. This study introduces a novel adsorbent, the hierarchical porous hydrophilic molecularly imprinted resin (HPHMIR), which was synthesized by integrating molecular imprinting techniques with hydrophilic resins. The HPHMIR, characterized by its extensive mesoporous structure (average pore width ~9.71<!-- --> <!-- -->nm) and favorable imprinting factors (2.6–5.0), facilitates the effective adsorption of PFCAs from complex matrices through multiple interaction mechanisms, including hydrogen bonding and electrostatic interactions. This innovative material was employed in a 96-well plate format for solid-phase extraction (SPE), and combined with LC-MS/MS, a high-throughput method for the determination of PFCAs in milk was developed. The proposed method demonstrated exceptional performance, including excellent linearity (0.48–240<!-- --> <!-- -->ng<!-- --> <!-- -->mL<sup>−1</sup>; <em>r</em> ≥ 0.9986), low detection limits (0.04–0.11<!-- --> <!-- -->ng<!-- --> <!-- -->mL<sup>−1</sup>), high precision (relative standard deviation ≤ 9.9%), and satisfactory recovery (75.7–118.1%). These results highlight the efficacy of the method in extracting trace levels of PFCAs from complicated sample matrices, presenting a promising alternative for monitoring PFCA contamination and advancing public health standards.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325923","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 : 2024-09-26DOI: 10.1016/j.jhazmat.2024.135967
Krzysztof B. Bec, Justyna Grabska, Frank Pfeifer, Heinz W. Siesler, Christian W. Huck
Contamination by microplastics, a global environmental concern, demands effective monitoring. While current methods focus on characterizing the smallest particles, their low throughput hinders practical assessment. Miniaturized near-infrared (NIR) spectroscopy offers high-throughput capabilities and rapid on-site analysis, potentially filling this gap. However, diverse sensor characteristics result in significant differences among handheld NIR spectrometers. This study characterizes the analytical performance of these instruments for identifying soil microplastics, comparing miniaturized devices MicroNIR 1700ES, NeoSpectra Scanner, microPHAZIR, nanoFTIR-NIR, NIR-S-G1, and SCiO sensor against a reference benchtop instrument, the NIRFlex N-500. Detection of common polymers, ABS, EVAC, HDPE, LDPE, PA6, PMMA, POM, PET, PS, PTFE, and SBR, at low concentrations (0.75% w/w) was possible without sample preparation. Sensor selection proved crucial; FT instruments N-500 and NeoSpectra Scanner provided the most accurate analysis, while other handheld instruments faced various challenges. Covariance analysis, Principal Component Analysis (PCA), and mid-level data fusion revealed that miniaturized NIR spectrometers can successfully screen microplastics on-site. However, the ability of each sensor to discriminate certain groups of polymers strongly depends on its spectral characteristics. This study demonstrates the importance of sensor selection in the development of portable NIR spectroscopy for environmental monitoring of microplastics.
{"title":"Rapid on-site analysis of soil microplastics using miniaturized NIR spectrometers: Key aspect of instrumental variation","authors":"Krzysztof B. Bec, Justyna Grabska, Frank Pfeifer, Heinz W. Siesler, Christian W. Huck","doi":"10.1016/j.jhazmat.2024.135967","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.135967","url":null,"abstract":"Contamination by microplastics, a global environmental concern, demands effective monitoring. While current methods focus on characterizing the smallest particles, their low throughput hinders practical assessment. Miniaturized near-infrared (NIR) spectroscopy offers high-throughput capabilities and rapid on-site analysis, potentially filling this gap. However, diverse sensor characteristics result in significant differences among handheld NIR spectrometers. This study characterizes the analytical performance of these instruments for identifying soil microplastics, comparing miniaturized devices MicroNIR 1700ES, NeoSpectra Scanner, microPHAZIR, nanoFTIR-NIR, NIR-S-G1, and SCiO sensor against a reference benchtop instrument, the NIRFlex N-500. Detection of common polymers, ABS, EVAC, HDPE, LDPE, PA6, PMMA, POM, PET, PS, PTFE, and SBR, at low concentrations (0.75% w/w) was possible without sample preparation. Sensor selection proved crucial; FT instruments N-500 and NeoSpectra Scanner provided the most accurate analysis, while other handheld instruments faced various challenges. Covariance analysis, Principal Component Analysis (PCA), and mid-level data fusion revealed that miniaturized NIR spectrometers can successfully screen microplastics on-site. However, the ability of each sensor to discriminate certain groups of polymers strongly depends on its spectral characteristics. This study demonstrates the importance of sensor selection in the development of portable NIR spectroscopy for environmental monitoring of microplastics.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321268","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 : 2024-09-26DOI: 10.1016/j.jhazmat.2024.135978
Qian Zhao, Zhenduo Yang, Ziyuan Zhou, Yuewei Yang, Wei Wang
The widespread use of S-metolachlor (ME) in agriculture to suppress weeds and boost crop yields, particularly in cultivating Vigna angularis, is well established. However, the application of organosilicon adjuvants with herbicides has potential threats to non-target crops. This study investigates the toxicity symptoms and mechanisms when V. angularis is exposed to ME in conjunction with a common organosilicon adjuvant. Results indicate that ME inhibits the growth of V. angularis seedlings, and adding adjuvants could aggravate the negative effects of ME. According to the growth index of seedlings, the adjuvant increased the toxicity of ME by 84-96%. Additionally, the chlorophyll content, root permeability, and antioxidant indicators in the seedlings were also adversely affected. Integrated metabolomics and transcriptomics analyses reveal that differentially abundant metabolites (DAMs) and differentially expressed genes (DEGs) are mainly enriched in four ways: "lysine degradation," "ABC transporters," "phenylalanine metabolism," and "monoterpenoid biosynthesis." The metabolic pathways and gene regulatory network involving 11 DAMs and 22 DEGs are associated with the physiological processes affected by ME and the adjuvant. This study provides guidance for the application of herbicides and their adjuvants in agricultural production to minimize adverse effects on non-target crops.
在农业中广泛使用 S-甲草胺（ME）来抑制杂草和提高作物产量，尤其是在栽培木樨（Vigna angularis）时。然而，除草剂中有机硅佐剂的应用对非目标作物有潜在威胁。本研究调查了当 Vigna angularis 接触 ME 和一种常见的有机硅佐剂时的毒性症状和机制。结果表明，ME 会抑制 V. angularis 幼苗的生长，而添加佐剂会加剧 ME 的负面影响。根据幼苗的生长指数，佐剂会使 ME 的毒性增加 84-96%。此外，幼苗的叶绿素含量、根系渗透性和抗氧化指标也受到了不利影响。代谢组学和转录组学的综合分析表明，差异丰度代谢物（DAMs）和差异表达基因（DEGs）主要富集在四个方面："赖氨酸降解"、"ABC 转运体"、"苯丙氨酸代谢 "和 "单萜生物合成"。涉及11个DAMs和22个DEGs的代谢途径和基因调控网络与受ME和佐剂影响的生理过程有关。这项研究为除草剂及其佐剂在农业生产中的应用提供了指导，以尽量减少对非目标作物的不利影响。
{"title":"Toxicity Mechanism of Organosilicon Adjuvant in Combination with S-metolachlor on Vigna angularis","authors":"Qian Zhao, Zhenduo Yang, Ziyuan Zhou, Yuewei Yang, Wei Wang","doi":"10.1016/j.jhazmat.2024.135978","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.135978","url":null,"abstract":"The widespread use of <em>S</em>-metolachlor (ME) in agriculture to suppress weeds and boost crop yields, particularly in cultivating <em>Vigna angularis</em>, is well established. However, the application of organosilicon adjuvants with herbicides has potential threats to non-target crops. This study investigates the toxicity symptoms and mechanisms when <em>V. angularis</em> is exposed to ME in conjunction with a common organosilicon adjuvant. Results indicate that ME inhibits the growth of <em>V. angularis</em> seedlings, and adding adjuvants could aggravate the negative effects of ME. According to the growth index of seedlings, the adjuvant increased the toxicity of ME by 84-96%. Additionally, the chlorophyll content, root permeability, and antioxidant indicators in the seedlings were also adversely affected. Integrated metabolomics and transcriptomics analyses reveal that differentially abundant metabolites (DAMs) and differentially expressed genes (DEGs) are mainly enriched in four ways: \"lysine degradation,\" \"ABC transporters,\" \"phenylalanine metabolism,\" and \"monoterpenoid biosynthesis.\" The metabolic pathways and gene regulatory network involving 11 DAMs and 22 DEGs are associated with the physiological processes affected by ME and the adjuvant. This study provides guidance for the application of herbicides and their adjuvants in agricultural production to minimize adverse effects on non-target crops.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321325","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 : 2024-09-26DOI: 10.1016/j.jhazmat.2024.135863
Danxing Yang, Wen Fang, Hao Zhang, Xueyuan Gu, Haiyi Chen, Haitao Sun, Jun Luo
Rainfall runoff can mobilize heavy metals in industrial soils, posing environmental risks. The mobility and distribution of heavy metals in different industrial soil layers are often overlooked. This study employed dynamic leaching experiments in layered soil columns with DGT (the diffusive gradients in thin films) measurements and DIFS (DGT-induced fluxes in soils and sediments) model to describe the migration, availability, and resupply ability of metals at different depths in surface and deep soil columns of industrial soils. Results showed significantly higher available concentrations (CDGT and CSoln) of Ni and Cd in surface soils compared to deep soils, likely due to the differences in soil physiochemical properties (contamination, pH, and soil texture). Continuous leaching promoted the migration of available Ni and Cd in surface soils. Maximum values of RNi (0.79–0.91) and RCd (0.75–0.80) were observed in the top layer (0–4 cm) of the surface soil, consistent with the trends of RFe. Combined DGT and DIFS model analysis implied higher potential availability and resupply of Ni and Cd in surface soil columns. These findings highlight the importance of considering dynamic leaching effects on heavy metal transport, availability, and release in industrial soils.
{"title":"Migration and Availability of Ni and Cd in Industrial Soils Under Different Leaching Conditions: Insights from DGT and DIFS Models","authors":"Danxing Yang, Wen Fang, Hao Zhang, Xueyuan Gu, Haiyi Chen, Haitao Sun, Jun Luo","doi":"10.1016/j.jhazmat.2024.135863","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.135863","url":null,"abstract":"Rainfall runoff can mobilize heavy metals in industrial soils, posing environmental risks. The mobility and distribution of heavy metals in different industrial soil layers are often overlooked. This study employed dynamic leaching experiments in layered soil columns with DGT (the diffusive gradients in thin films) measurements and DIFS (DGT-induced fluxes in soils and sediments) model to describe the migration, availability, and resupply ability of metals at different depths in surface and deep soil columns of industrial soils. Results showed significantly higher available concentrations (<em>C</em><sub>DGT</sub> and <em>C</em><sub>Soln</sub>) of Ni and Cd in surface soils compared to deep soils, likely due to the differences in soil physiochemical properties (contamination, pH, and soil texture). Continuous leaching promoted the migration of available Ni and Cd in surface soils. Maximum values of <em>R</em><sub>Ni</sub> (0.79–0.91) and <em>R</em><sub>Cd</sub> (0.75–0.80) were observed in the top layer (0–4<!-- --> <!-- -->cm) of the surface soil, consistent with the trends of <em>R</em><sub>Fe</sub>. Combined DGT and DIFS model analysis implied higher potential availability and resupply of Ni and Cd in surface soil columns. These findings highlight the importance of considering dynamic leaching effects on heavy metal transport, availability, and release in industrial soils.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142325284","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 : 2024-09-26DOI: 10.1016/j.jhazmat.2024.135983
Sengyang Wang, Guangyu Li, Xiang Ji, Yang Wang, Bo Xu, Jianfeng Tang, Chuanbo Guo
The Eastern Route of China's South-to-North Water Diversion Project (SNWDP-ER) traverses through impounded lakes that are potentially vulnerable to heavy metals (HMs) contamination although the understanding remains elusive. This study employed machine learning approaches, including super-clustering of Self-Organizing Map (SOM) and Robust Principal Component Analysis (RPCA), to elucidate the spatiotemporal patterns and assess ecological risks associated with HMs in the surface sediments of Gao-Bao-Shaobo Lake (GBSL) and Dongping Lake (DPL). We collected 184 surface sediments from 47 stations across the two important impounded lakes over four seasons. The results revealed higher HMs concentrations in the south-central GBSL and west-central DPL, with a notable increase in contamination in autumn. The comprehensive risk assessment, utilizing various indicators such as the Sediment Quality Guidelines (SQGs), Improved Potential Ecological Risk Index (IPERI), Geo-accumulation Index (Igeo), Contamination Factor (CF), and Enrichment Factor (EF), identified arsenic (As), cadmium (Cd), nickel (Ni), and chromium (Cr) as primary contaminants of concern. Positive Matrix Factorization (PMF) model, coupled with Spearman analysis attributed over 70% of HMs pollution to anthropogenic activities. This research provides a nuanced understanding of HMs pollution in the context of large-scale water diversion projects and offers a scientific basis for targeted pollution mitigation strategies.
中国南水北调东线工程（SNWDP-ER）穿越了可能易受重金属（HMs）污染的蓄水湖泊，但人们对重金属污染的认识仍很模糊。本研究采用机器学习方法，包括自组织图超聚类（SOM）和鲁棒性主成分分析（RPCA），来阐明高宝-邵伯湖（GBSL）和东平湖（DPL）表层沉积物中重金属的时空模式并评估其生态风险。我们在这两个重要的蓄水湖泊的 47 个站位采集了 184 份表层沉积物，历时四个季节。结果表明，高沙湖中南部和东平湖中西部的 HMs 浓度较高，且秋季污染明显加重。综合风险评估采用了各种指标，如沉积物质量准则 (SQGs)、潜在生态风险改进指数 (IPERI)、地质累积指数 (Igeo)、污染因子 (CF) 和富集因子 (EF)，确定砷 (As)、镉 (Cd)、镍 (Ni) 和铬 (Cr) 为主要污染物。正矩阵因式分解（PMF）模型和斯皮尔曼分析将 70% 以上的 HMs 污染归因于人为活动。这项研究让人们对大规模引水工程中的 HMs 污染有了细致入微的了解，并为制定有针对性的污染缓解战略提供了科学依据。
{"title":"Machine learning-driven assessment of heavy metal contamination in the impounded Lakes of China's South-to-North Water Diversion Project: Identifying spatiotemporal patterns and ecological risks","authors":"Sengyang Wang, Guangyu Li, Xiang Ji, Yang Wang, Bo Xu, Jianfeng Tang, Chuanbo Guo","doi":"10.1016/j.jhazmat.2024.135983","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.135983","url":null,"abstract":"The Eastern Route of China's South-to-North Water Diversion Project (SNWDP-ER) traverses through impounded lakes that are potentially vulnerable to heavy metals (HMs) contamination although the understanding remains elusive. This study employed machine learning approaches, including super-clustering of Self-Organizing Map (SOM) and Robust Principal Component Analysis (RPCA), to elucidate the spatiotemporal patterns and assess ecological risks associated with HMs in the surface sediments of Gao-Bao-Shaobo Lake (GBSL) and Dongping Lake (DPL). We collected 184 surface sediments from 47 stations across the two important impounded lakes over four seasons. The results revealed higher HMs concentrations in the south-central GBSL and west-central DPL, with a notable increase in contamination in autumn. The comprehensive risk assessment, utilizing various indicators such as the Sediment Quality Guidelines (SQGs), Improved Potential Ecological Risk Index (IPERI), Geo-accumulation Index (Igeo), Contamination Factor (CF), and Enrichment Factor (EF), identified arsenic (As), cadmium (Cd), nickel (Ni), and chromium (Cr) as primary contaminants of concern. Positive Matrix Factorization (PMF) model, coupled with Spearman analysis attributed over 70% of HMs pollution to anthropogenic activities. This research provides a nuanced understanding of HMs pollution in the context of large-scale water diversion projects and offers a scientific basis for targeted pollution mitigation strategies.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142324853","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 : 2024-09-26DOI: 10.1016/j.jhazmat.2024.135985
Wang Yao, Huifang Xing, Shan Ni, Yafeng Liu, Wengjie Wang, Huizhou Liu, Liangrong Yang
Extracting uranium from water is crucial for environmental protection and the sustainable nuclear power industry. However, high-efficiency extraction and mild desorption condition still poses significant challenges. Herein, a polyoxometalate-based metal-organic framework (POMOF) for high-performance uranium extraction is prepared by in situ confined encapsulating H3[PW12O40] (PW12) into MIL-101(Cr). The highly dispersed PW12 enables adsorption sites to be sufficiently exposed, supports the pore structure of MIL-101(Cr), while being protected by spatial confinement. Furthermore, its abundant oxygen groups form high-affinity coordination with uranium and provide the pH-dependent conformation switch to achieve selective adsorption and instantaneous structural transformation. The assembly of structure and function makes POMOF exhibit substantial synergistic stability and adsorption capacity. Consequently, the constructed MIL-101(Cr)@PW12 exhibits excellent uranium adsorption ability of 461.88 mg/g, as well as superior selectivity towards a wide variety of metal ions. Remarkably, instantaneous desorption can be achieved in 2 s under mild desorption conditions of 0.005 mol/L HCl, and the adsorption capacity remained at 94.30% after 8 adsorption cycles. POMOF demonstrates the vast potential for uranium capture from water and offers new insight into designing structure and functional synergistic materials for the selective adsorption and instantaneous desorption of uranium.
{"title":"In-situ Assembly of Polyoxometalate-Based Metal-Organic Framework for High-Efficiency Recovery of Uranium","authors":"Wang Yao, Huifang Xing, Shan Ni, Yafeng Liu, Wengjie Wang, Huizhou Liu, Liangrong Yang","doi":"10.1016/j.jhazmat.2024.135985","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.135985","url":null,"abstract":"Extracting uranium from water is crucial for environmental protection and the sustainable nuclear power industry. However, high-efficiency extraction and mild desorption condition still poses significant challenges. Herein, a polyoxometalate-based metal-organic framework (POMOF) for high-performance uranium extraction is prepared by in situ confined encapsulating H<sub>3</sub>[PW<sub>12</sub>O<sub>40</sub>] (PW<sub>12</sub>) into MIL-101(Cr). The highly dispersed PW<sub>12</sub> enables adsorption sites to be sufficiently exposed, supports the pore structure of MIL-101(Cr), while being protected by spatial confinement. Furthermore, its abundant oxygen groups form high-affinity coordination with uranium and provide the pH-dependent conformation switch to achieve selective adsorption and instantaneous structural transformation. The assembly of structure and function makes POMOF exhibit substantial synergistic stability and adsorption capacity. Consequently, the constructed MIL-101(Cr)@PW<sub>12</sub> exhibits excellent uranium adsorption ability of 461.88<!-- --> <!-- -->mg/g, as well as superior selectivity towards a wide variety of metal ions. Remarkably, instantaneous desorption can be achieved in 2<!-- --> <!-- -->s under mild desorption conditions of 0.005<!-- --> <!-- -->mol/L HCl, and the adsorption capacity remained at 94.30% after 8 adsorption cycles. POMOF demonstrates the vast potential for uranium capture from water and offers new insight into designing structure and functional synergistic materials for the selective adsorption and instantaneous desorption of uranium.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142324886","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}
Exposure to tobacco smoke and essential metals is linked with metabolic syndrome (MS). However, the joint effect of them on MS in older adults and the underlying mechanisms are still unclear. This large-scale study measured the urinary concentrations of 8 nicotine metabolites and 8 essential metals in 4564 older adults from Shenzhen, China. The biomarker of insulin resistance, triglyceride-glucose index (TyG), was also calculated. Restricted cubic splines (RCS), Bayesian kernel machine regression and quantile-based g-computation were used to access the single and joint effects of urinary nicotine metabolites and essential metals on MS and insulin resistance. Mediation analysis was performed to investigate the role of TyG in these relationships.Single urinary nicotine metabolite and essential metal had non-linear relationships with MS in RCS. The overall effect of urinary nicotine metabolites and essential metals was positively associated with MS. Urinary zinc (52.2%) and copper (20.1%) were the major contributors to MS, whereas molybdenum had a negative association with MS. TyG mediated 64.7% of the overall effect of urinary nicotine metabolites and essential metals on MS. Overall, the mixture of urinary nicotine metabolites and essential metals had a dose-response relationship with MS. Insulin resistance was as a crucial mediated pathway in this association.
接触烟草烟雾和基本金属与代谢综合征（MS）有关。然而，它们对老年人代谢综合征的共同影响及其内在机制仍不清楚。这项大规模研究测量了中国深圳 4564 名老年人尿液中 8 种尼古丁代谢物和 8 种必需金属的浓度。同时还计算了胰岛素抵抗的生物标志物--甘油三酯-葡萄糖指数（TyG）。利用限制立方样条（RCS）、贝叶斯核机器回归和基于量子的 g 计算方法，研究了尿液中尼古丁代谢物和必需金属对 MS 和胰岛素抵抗的单一和联合影响。尿中尼古丁代谢物和必需金属与RCS中的MS存在非线性关系。尿液中尼古丁代谢物和必需金属的总体效应与 MS 呈正相关。尿液中的锌（52.2%）和铜（20.1%）是导致多发性硬化的主要因素，而钼与多发性硬化呈负相关。在尿液中尼古丁代谢物和必需金属对多发性硬化症的总体影响中，64.7%是由TyG介导的。总体而言，尿液中尼古丁代谢物和必需金属的混合物与多发性硬化呈剂量反应关系。胰岛素抵抗是这一关联的关键介导途径。
{"title":"Associations of urinary nicotine metabolites and essential metals with metabolic syndrome in older adults: The mediation effect of insulin resistance","authors":"Zhihui Guo, Peiyi Liu, Tian Li, Erwei Gao, Junye Bian, Xiaohu Ren, Benhong Xu, Xiao Chen, Haiyan Huang, Jianjun Liu, Xifei Yang, Shaoyou Lu","doi":"10.1016/j.jhazmat.2024.135969","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.135969","url":null,"abstract":"Exposure to tobacco smoke and essential metals is linked with metabolic syndrome (MS). However, the joint effect of them on MS in older adults and the underlying mechanisms are still unclear. This large-scale study measured the urinary concentrations of 8 nicotine metabolites and 8 essential metals in 4564 older adults from Shenzhen, China. The biomarker of insulin resistance, triglyceride-glucose index (TyG), was also calculated. Restricted cubic splines (RCS), Bayesian kernel machine regression and quantile-based g-computation were used to access the single and joint effects of urinary nicotine metabolites and essential metals on MS and insulin resistance. Mediation analysis was performed to investigate the role of TyG in these relationships.Single urinary nicotine metabolite and essential metal had non-linear relationships with MS in RCS. The overall effect of urinary nicotine metabolites and essential metals was positively associated with MS. Urinary zinc (52.2%) and copper (20.1%) were the major contributors to MS, whereas molybdenum had a negative association with MS. TyG mediated 64.7% of the overall effect of urinary nicotine metabolites and essential metals on MS. Overall, the mixture of urinary nicotine metabolites and essential metals had a dose-response relationship with MS. Insulin resistance was as a crucial mediated pathway in this association.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142324848","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 : 2024-09-26DOI: 10.1016/j.jhazmat.2024.135968
Xiaoxin Zhao, Shuoqi Huang, Qi Yao, Rui He, Hao Wang, Zhaodan Xu, Wang Xing, Dali Liu
Sugar beet (Beta vulgaris L.) shows potential as an energy crop for cadmium (Cd) phytoremediation. To elucidate its in vivo response strategy to Cd exposure, seedlings were treated with 1, 3, and 5 mmol/L CdCl2 (Cd-1, Cd-3, and Cd-5) for 6 h, using 0 mmol/L CdCl2 (Cd-0) as the control. The results showed that Cd-3 promoted a unique “hormesis” effect, leading to enhanced growth performance, increased levels of chlorophyll, soluble protein, and SOD activity, and reduced MDA content in sugar beet, compared to Cd-1, Cd-5, and even Cd-0. GO and KEGG enrichments and PPI network of transcriptomic analysis revealed that the differentially expressed genes (DEGs) were primarily involved in lipid metabolism, cellular protein catabolism, and photosynthesis. Notably, the MAPK signaling pathway was significantly enriched only under Cd-3, with the up-regulation of ABA-related core gene BvPYL9 and an increase in ABA content after 6 h of Cd exposure. Furthermore, overexpression of BvPYL9 in Arabidopsis thaliana (OE-1 and OE-2) resulted in enhanced growth (fresh weight, dry weight, root length), as well as higher ABA and soluble protein contents. Cd-induced transcriptional responses of BvPYL9 were also evident in OE-1 and OE-2, especially at 10 µmol/L, indicated by qRT-PCR. These findings suggest that ABA-mediated MAPK signaling pathway is activated in response to Cd toxicity, with BvPYL9 being a key factor in the cascade effects for the Cd-induced hormesis in sugar beet.
{"title":"ABA-regulated MAPK signaling pathway promotes hormesis in sugar beet under cadmium exposure","authors":"Xiaoxin Zhao, Shuoqi Huang, Qi Yao, Rui He, Hao Wang, Zhaodan Xu, Wang Xing, Dali Liu","doi":"10.1016/j.jhazmat.2024.135968","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.135968","url":null,"abstract":"Sugar beet (<em>Beta vulgaris</em> L.) shows potential as an energy crop for cadmium (Cd) phytoremediation. To elucidate its <em>in vivo</em> response strategy to Cd exposure, seedlings were treated with 1, 3, and 5<!-- --> <!-- -->mmol/L CdCl<sub>2</sub> (Cd-1, Cd-3, and Cd-5) for 6<!-- --> <!-- -->h, using 0<!-- --> <!-- -->mmol/L CdCl<sub>2</sub> (Cd-0) as the control. The results showed that Cd-3 promoted a unique “hormesis” effect, leading to enhanced growth performance, increased levels of chlorophyll, soluble protein, and SOD activity, and reduced MDA content in sugar beet, compared to Cd-1, Cd-5, and even Cd-0. GO and KEGG enrichments and PPI network of transcriptomic analysis revealed that the differentially expressed genes (DEGs) were primarily involved in lipid metabolism, cellular protein catabolism, and photosynthesis. Notably, the MAPK signaling pathway was significantly enriched only under Cd-3, with the up-regulation of ABA-related core gene <em>BvPYL9</em> and an increase in ABA content after 6<!-- --> <!-- -->h of Cd exposure. Furthermore, overexpression of <em>BvPYL9</em> in <em>Arabidopsis thaliana</em> (OE-1 and OE-2) resulted in enhanced growth (fresh weight, dry weight, root length), as well as higher ABA and soluble protein contents. Cd-induced transcriptional responses of <em>BvPYL9</em> were also evident in OE-1 and OE-2, especially at 10 µmol/L, indicated by qRT-PCR. These findings suggest that ABA-mediated MAPK signaling pathway is activated in response to Cd toxicity, with <em>BvPYL9</em> being a key factor in the cascade effects for the Cd-induced hormesis in sugar beet.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142324851","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}
Current total concentration-based methods for source attribution and risk assessment often overestimate metal risks, thereby impeding the formulation of effective risk management strategies. This study aims to develop a framework for source-specific risk assessment based on metal bioavailability in surface river sediments from a human-dominated seaward catchment in eastern China. Metal bioavailability was quantified using chemical fractionation results, and source apportionment was conducted using the positive matrix factorization (PMF) model. Risk assessment integrated these findings using two indices: the Potential Ecological Risk Index (PERI) and the Mean Probable Effect Concentration Quotient (mPEC-Q), with uncertainty addressed via Monte Carlo simulations. Results indicated that average total concentrations of Cu, Pb, Zn, Cr, Hg, Cd, and As exceeded their respective background levels by 1.63 to 15.00 times. The residual fraction constituted the majority, accounting for 53.84% to 77.79% of total concentrations, suggesting significant natural origins. However, source apportionment revealed a predominant contribution from anthropogenic activities, including industrial smelting, agricultural practices, and atmospheric deposition. The contributions were found to vary between 5.35% and 40.03% when the total concentration was adjusted to bioavailable content. Total concentration-based PERI/mPEC-Q assessments indicated high/moderate risk levels, decreasing to considerable/low risk levels with bioavailability adjustment. Hg and Cd were identified as priority metals. Further incorporating source appointment parameters into the risk assessment, industrial smelting was identified as the primary contributor, accounting for 66.06% of total risk by total concentration and 65.63% by bioavailability. This underscores the role of bioavailability in mitigating risk overestimation. Monte Carlo simulations validated industrial smelting as a major risk contributor. This study emphasizes the importance of considering bioavailability in the source-risk assessment of sediment-metals, crucial for targeted risk management in urbanized catchment areas.
{"title":"Source-risk and uncertainty assessment of trace metals in surface sediments of a human-dominated seaward catchment in eastern China","authors":"Fangli Wang, Zihan Yu, Yali Zhang, Runxiang Ni, Zhi Li, Shaojing Li, Ningning Song, Jun Liu, Haiying Zong, Wei Jiao, Hongtao Shi","doi":"10.1016/j.jhazmat.2024.135960","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.135960","url":null,"abstract":"Current total concentration-based methods for source attribution and risk assessment often overestimate metal risks, thereby impeding the formulation of effective risk management strategies. This study aims to develop a framework for source-specific risk assessment based on metal bioavailability in surface river sediments from a human-dominated seaward catchment in eastern China. Metal bioavailability was quantified using chemical fractionation results, and source apportionment was conducted using the positive matrix factorization (PMF) model. Risk assessment integrated these findings using two indices: the Potential Ecological Risk Index (<em>PERI</em>) and the Mean Probable Effect Concentration Quotient (<em>mPEC-Q</em>), with uncertainty addressed via Monte Carlo simulations. Results indicated that average total concentrations of Cu, Pb, Zn, Cr, Hg, Cd, and As exceeded their respective background levels by 1.63 to 15.00 times. The residual fraction constituted the majority, accounting for 53.84% to 77.79% of total concentrations, suggesting significant natural origins. However, source apportionment revealed a predominant contribution from anthropogenic activities, including industrial smelting, agricultural practices, and atmospheric deposition. The contributions were found to vary between 5.35% and 40.03% when the total concentration was adjusted to bioavailable content. Total concentration-based <em>PERI</em>/<em>mPEC-Q</em> assessments indicated high/moderate risk levels, decreasing to considerable/low risk levels with bioavailability adjustment. Hg and Cd were identified as priority metals. Further incorporating source appointment parameters into the risk assessment, industrial smelting was identified as the primary contributor, accounting for 66.06% of total risk by total concentration and 65.63% by bioavailability. This underscores the role of bioavailability in mitigating risk overestimation. Monte Carlo simulations validated industrial smelting as a major risk contributor. This study emphasizes the importance of considering bioavailability in the source-risk assessment of sediment-metals, crucial for targeted risk management in urbanized catchment areas.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142324852","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 : 2024-09-26DOI: 10.1016/j.jhazmat.2024.135964
Xinxin Shi, Zhuolin Ma, Stanislav A. Evlashin, Fedor S. Fedorov, Julian Shi, Yang Liu, Weihuang Zhu, Pengfei Guo, Tinglin Huang, Gang Wen
Extremely limited organic carbon sources and aerobic environment in micro-polluted reservoir water make conventional denitrification exceptionally challenging. As a result, total nitrogen (TN) concentration in most reservoir waters exceeds standard value year-round. In this study, for the first time, we constructed a mini water-lifting and aeration system (mini-WLAS) to remove nitrate in actual reservoir water. In the mini-WLAS, H2 was produced through electrolysis of reservoir water without adding any electrolyte, and the ascending water flow carried the generated H2 from lower layer to upper bacteria layer. The maximum denitrification rate reached 0.29 mg (L·d)-1 under dissolved oxygen (DO) concentration of 6-8 mg L-1, 6.04 times higher than that of the control group. There is almost no accumulation of NH4+-N, NO2--N, and N2O, and the concentration of CODMn decreased by 55.2%. More importantly, the pH stayed near-neutral steadily throughout the whole process. Microbial community analysis showed that the abundances of hydrogenotrophic denitrifying bacteria (HDB) were 2 orders higher than those in the control system. Some HDB could work under aerobic conditions, providing an explanation for the excellent denitrification performance under high DO. This study provides a novel perspective for TN removal from reservoir water.
{"title":"Hydrogen Generated by Electrochemical Water Splitting as Electron Donor for Nitrate Removal from Micro-Polluted Reservoir Water","authors":"Xinxin Shi, Zhuolin Ma, Stanislav A. Evlashin, Fedor S. Fedorov, Julian Shi, Yang Liu, Weihuang Zhu, Pengfei Guo, Tinglin Huang, Gang Wen","doi":"10.1016/j.jhazmat.2024.135964","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.135964","url":null,"abstract":"Extremely limited organic carbon sources and aerobic environment in micro-polluted reservoir water make conventional denitrification exceptionally challenging. As a result, total nitrogen (TN) concentration in most reservoir waters exceeds standard value year-round. In this study, for the first time, we constructed a mini water-lifting and aeration system (mini-WLAS) to remove nitrate in actual reservoir water. In the mini-WLAS, H<sub>2</sub> was produced through electrolysis of reservoir water without adding any electrolyte, and the ascending water flow carried the generated H<sub>2</sub> from lower layer to upper bacteria layer. The maximum denitrification rate reached 0.29<!-- --> <!-- -->mg (L·d)<sup>-1</sup> under dissolved oxygen (DO) concentration of 6-8<!-- --> <!-- -->mg<!-- --> <!-- -->L<sup>-1</sup>, 6.04 times higher than that of the control group. There is almost no accumulation of NH<sub>4</sub><sup>+</sup>-N, NO<sub>2</sub><sup>-</sup>-N, and N<sub>2</sub>O, and the concentration of COD<sub>Mn</sub> decreased by 55.2%. More importantly, the pH stayed near-neutral steadily throughout the whole process. Microbial community analysis showed that the abundances of hydrogenotrophic denitrifying bacteria (HDB) were 2 orders higher than those in the control system. Some HDB could work under aerobic conditions, providing an explanation for the excellent denitrification performance under high DO. This study provides a novel perspective for TN removal from reservoir water.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":null,"pages":null},"PeriodicalIF":13.6,"publicationDate":"2024-09-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142321270","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：