Pub Date : 2024-11-16DOI: 10.1016/j.jhazmat.2024.136540
Hairong Ma, Anna N. Khusnutdinova, Sofia Lemak, Tatyana N. Chernikova, Olga V. Golyshina, David Almendral, Manuel Ferrer, Peter N. Golyshin, Alexander F. Yakunin
Enzyme-based depolymerization of plastics, including polyesters, has emerged as a promising approach for plastic waste recycling and reducing environmental plastic pollution. Currently, most of the known polyester-degrading enzymes are represented by a few natural and engineered PETases from the carboxylesterase family V. To identify novel groups of polyesterases, we selected 25 proteins from the carboxylesterase family IV, which share 22% to 80% sequence identity to the metagenomic thermophilic polyesterase IS12. All purified proteins were found to be active against chromogenic para-nitrophenyl esters with a preference for short acyl chains. Screening for polyesterase activity using emulsified polyesters demonstrated the presence of hydrolytic activity against bis(benzoyloxyethyl) terephthalate (3PET), polycaprolactone (PCL), and polylactic acid (PLA) in all tested proteins. Biochemical characterization of four selected polyesterases revealed high thermostability in CBA10055, whereas the mesophilic GEN0105 exhibited higher polyesterase activity. Two ancestral variants of GEN0105 showed higher thermostability and activity against PCL and PLA, but reduced activity with amorphous PET. Furthermore, six established PETases were found to be highly active against PCL and PLA. Thus, our results indicate that polyesterase activity is widespread in the family IV carboxylesterases, and that most polyesterases are promiscuous being able to degrade different polyesters.
以酶为基础的塑料（包括聚酯）解聚已成为塑料废物回收利用和减少环境塑料污染的一种有前途的方法。目前，大多数已知的聚酯降解酶都是以羧基酯酶家族 V 中的几种天然和工程 PET 酶为代表的。为了确定新的聚酯酶群，我们从羧基酯酶家族 IV 中挑选了 25 种蛋白质，它们与元基因组嗜热聚酯酶 IS12 有 22% 至 80% 的序列相同性。研究发现，所有纯化的蛋白质都对发色性对硝基苯酯具有活性，并偏好短酰基链。利用乳化聚酯进行的聚酯酶活性筛选表明，所有测试蛋白质都具有水解对苯二酸二（苯甲酰氧乙基）酯（3PET）、聚己内酯（PCL）和聚乳酸（PLA）的活性。四种所选聚酯酶的生化特征表明，CBA10055 具有很高的热稳定性，而中嗜性 GEN0105 则表现出更高的聚酯酶活性。GEN0105 的两个祖先变体对 PCL 和聚乳酸表现出更高的热稳定性和活性，但对无定形 PET 的活性降低。此外，还发现六种已建立的 PET 酶对 PCL 和 PLA 具有较高的活性。因此，我们的研究结果表明，聚酯酶活性广泛存在于羧基酯酶家族 IV 中，而且大多数聚酯酶具有杂合性，能够降解不同的聚酯。
{"title":"Polyesterase activity is widespread in the family IV carboxylesterases from bacteria","authors":"Hairong Ma, Anna N. Khusnutdinova, Sofia Lemak, Tatyana N. Chernikova, Olga V. Golyshina, David Almendral, Manuel Ferrer, Peter N. Golyshin, Alexander F. Yakunin","doi":"10.1016/j.jhazmat.2024.136540","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136540","url":null,"abstract":"Enzyme-based depolymerization of plastics, including polyesters, has emerged as a promising approach for plastic waste recycling and reducing environmental plastic pollution. Currently, most of the known polyester-degrading enzymes are represented by a few natural and engineered PETases from the carboxylesterase family V. To identify novel groups of polyesterases, we selected 25 proteins from the carboxylesterase family IV, which share 22% to 80% sequence identity to the metagenomic thermophilic polyesterase IS12. All purified proteins were found to be active against chromogenic <em>para</em>-nitrophenyl esters with a preference for short acyl chains. Screening for polyesterase activity using emulsified polyesters demonstrated the presence of hydrolytic activity against bis(benzoyloxyethyl) terephthalate (3PET), polycaprolactone (PCL), and polylactic acid (PLA) in all tested proteins. Biochemical characterization of four selected polyesterases revealed high thermostability in CBA10055, whereas the mesophilic GEN0105 exhibited higher polyesterase activity. Two ancestral variants of GEN0105 showed higher thermostability and activity against PCL and PLA, but reduced activity with amorphous PET. Furthermore, six established PETases were found to be highly active against PCL and PLA. Thus, our results indicate that polyesterase activity is widespread in the family IV carboxylesterases, and that most polyesterases are promiscuous being able to degrade different polyesters.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"98 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642881","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 : 2024-11-16DOI: 10.1016/j.jhazmat.2024.136538
Vera N. de Ruijter, Xinyi Xie, Albert A. Koelmans
Whether microplastics cause different effects than inert natural particles, and how to create relevant testing materials, are key questions in microplastics research. We prepared Environmentally Relevant Microplastic (ERMP) and Mineral Microparticle (ERMS) mixtures with similar levels of polydispersity and tested their 28-day chronic effects on the reproduction and growth of L. variegatus at two different organic matter (OM) contents (average and enriched). Additionally L. variegatus was exposed to ERMP and ERMS to study the particle egestion for 14 days. We observed no differences in growth or reproduction between ERMP and ERMS at particle concentrations of up to 10% (v/v). In contrast, organisms exposed to enriched OM content increased their growth with 30% and increased reproduction with 20%. For ERMP with an enriched OM content, reproduction was reduced with an effect threshold EC50 of 13.68 ± 5.54% (v/v). After 14 days of exposure to 5% ERMP, the egestion of faecal pellets was higher compared to exposure to 5% ERMS, suggesting that in order to acquire the same amount of nutrition, L. variegatus is spending more energy. With this study, we demonstrate that refinements in the manufacturing of environmentally diverse particle mixtures can contribute to a more realistic testing of particle effects.
{"title":"Microplastics versus natural mineral particles. How to create and test them while maintaining environmental relevance","authors":"Vera N. de Ruijter, Xinyi Xie, Albert A. Koelmans","doi":"10.1016/j.jhazmat.2024.136538","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136538","url":null,"abstract":"Whether microplastics cause different effects than inert natural particles, and how to create relevant testing materials, are key questions in microplastics research. We prepared Environmentally Relevant Microplastic (ERMP) and Mineral Microparticle (ERMS) mixtures with similar levels of polydispersity and tested their 28-day chronic effects on the reproduction and growth of <em>L. variegatus</em> at two different organic matter (OM) contents (average and enriched). Additionally <em>L. variegatus</em> was exposed to ERMP and ERMS to study the particle egestion for 14 days. We observed no differences in growth or reproduction between ERMP and ERMS at particle concentrations of up to 10% (v/v). In contrast, organisms exposed to enriched OM content increased their growth with 30% and increased reproduction with 20%. For ERMP with an enriched OM content, reproduction was reduced with an effect threshold EC<sub>50</sub> of 13.68 ± 5.54% (v/v). After 14 days of exposure to 5% ERMP, the egestion of faecal pellets was higher compared to exposure to 5% ERMS, suggesting that in order to acquire the same amount of nutrition, <em>L. variegatus</em> is spending more energy. With this study, we demonstrate that refinements in the manufacturing of environmentally diverse particle mixtures can contribute to a more realistic testing of particle effects.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"128 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642828","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}
Foodborne and waterborne bacterial infections caused by Escherichia coli (E. coli) pose a serious threat to public health and safety. Therefore, there is an urgent need to develop a fast and accurate diagnostic device for early detection and prevention of bacterial contamination. In this study, we designed a visual cotton fabric-based detection biosensor that can target enzymes produced by E. coli metabolism and induce color changes. In addition, the system can be integrated with the naked eye, smartphones, and small spectrometers to analyze the generated signals for qualitative, semi-quantitative, and quantitative detection. The platform achieved a minimum detection limit of 537 cfu/mL for E. coli, a wide detection range of 102-106 cfu/mL, and a minimum detection time as low as 20 mins. The detection results of complex environmental samples showed that the system has excellent anti-ion interference and anti-pH interference behavior. This visual detection biosensor has great commercial application potential and can be widely used in real-time on-site detection due to its rapid, portable, anti-interference, and low-cost advantages.
{"title":"Fabric-based visualization biosensor for real-time environmental monitoring and food safety","authors":"Jiaqi Zhang, Jizhen Zhang, Senlin Gu, Lipei Ren, Dong Wang, Christopher Hurren","doi":"10.1016/j.jhazmat.2024.136559","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136559","url":null,"abstract":"Foodborne and waterborne bacterial infections caused by <em>Escherichia coli</em> (<em>E. coli</em>) pose a serious threat to public health and safety. Therefore, there is an urgent need to develop a fast and accurate diagnostic device for early detection and prevention of bacterial contamination. In this study, we designed a visual cotton fabric-based detection biosensor that can target enzymes produced by <em>E. coli</em> metabolism and induce color changes. In addition, the system can be integrated with the naked eye, smartphones, and small spectrometers to analyze the generated signals for qualitative, semi-quantitative, and quantitative detection. The platform achieved a minimum detection limit of 537 cfu/mL for <em>E. coli</em>, a wide detection range of 10<sup>2</sup>-10<sup>6</sup> cfu/mL, and a minimum detection time as low as 20<!-- --> <!-- -->mins. The detection results of complex environmental samples showed that the system has excellent anti-ion interference and anti-pH interference behavior. This visual detection biosensor has great commercial application potential and can be widely used in real-time on-site detection due to its rapid, portable, anti-interference, and low-cost advantages.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"75 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642823","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}
Catalytic combustion is widely regarded as the most efficient technique for removing soot particulates from diesel engine exhaust, with its efficiency largely dependent on the performance of catalysts. In this study, a series of YMn1-xCoxO5-ζ catalysts were synthesized using a hydrothermal method to investigate their catalytic properties in soot oxidation. Among these catalysts, YMCo-0.2 exhibited the highest catalytic activity, achieving 90% soot conversion at 392 °C and demonstrating robust tolerance in the presence of water vapour and SO2. Structural characterisation revealed that Co doping did not alter the fundamental crystal structure of YMn2O5 mullite. Through some characterization comprehensive analysis, and DFT calculations further supported the experimental findings, indicate that Co substitution significantly increased the lattice oxygen mobility and surface active oxygen content. Compared to the surface lattice oxygens at other positions, the weakening of the Mn-O bond results in the lattice oxygens in the Co-O-Mn4+ sites in the catalysts exhibiting higher reactivity. Additionally, the catalyst displayed strong NO and O2 adsorption and activation capabilities, indicating its potential for efficient NOx-assisted soot combustion. This study provides insights for designing and optimizing mullite catalysts for soot combustion.
Environmental implications
The catalytic removal of soot particles from diesel exhaust is crucial for protecting both environmental quality and human health. In this work, cobalt (Co) doping into YMn2O5 mullite decreased the strength of Mn-O bond and increased the adsorption capacity of NO, which was beneficial to soot combustion reaction. This research enriches the application of mullite in the field of environmental catalysis.
催化燃烧被广泛认为是去除柴油发动机尾气中烟尘颗粒的最有效技术，其效率在很大程度上取决于催化剂的性能。本研究采用水热法合成了一系列 YMn1-xCoxO5-ζ 催化剂，以研究它们在烟尘氧化中的催化性能。在这些催化剂中，YMCo-0.2 表现出最高的催化活性，在 392 °C 时可实现 90% 的烟尘转化率，并在水蒸气和二氧化硫存在下表现出强大的耐受性。结构表征显示，掺入 Co 并没有改变 YMn2O5 莫来石的基本晶体结构。通过一些表征综合分析和 DFT 计算进一步支持了实验结果，表明掺入 Co 能显著提高晶格氧迁移率和表面活性氧含量。与其他位置的表面晶格氧相比，Mn-O 键的弱化导致催化剂中 Co-O-Mn4+ 位点的晶格氧表现出更高的反应活性。此外，催化剂还具有很强的 NO 和 O2 吸附和活化能力，这表明催化剂具有高效燃烧 NOx 烟尘的潜力。这项研究为设计和优化用于烟尘燃烧的莫来石催化剂提供了启示。环境意义催化去除柴油机尾气中的烟尘颗粒对保护环境质量和人类健康至关重要。在这项工作中，钴（Co）掺杂到 YMn2O5 莫来石中降低了 Mn-O 键的强度，提高了对 NO 的吸附能力，有利于烟尘燃烧反应。这项研究丰富了莫来石在环境催化领域的应用。
{"title":"Enhanced NOx-assisted soot combustion by cobalt doping to weaken mullite Mn-O bonds for lattice oxygen activation","authors":"Qilong Guo, Yaodi Liu, Xinran Zhang, Yupu Xu, Panpan Liu, Changsen Zhang","doi":"10.1016/j.jhazmat.2024.136474","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136474","url":null,"abstract":"Catalytic combustion is widely regarded as the most efficient technique for removing soot particulates from diesel engine exhaust, with its efficiency largely dependent on the performance of catalysts. In this study, a series of YMn<sub>1-x</sub>Co<sub>x</sub>O<sub>5-ζ</sub> catalysts were synthesized using a hydrothermal method to investigate their catalytic properties in soot oxidation. Among these catalysts, YMCo-0.2 exhibited the highest catalytic activity, achieving 90% soot conversion at 392 °C and demonstrating robust tolerance in the presence of water vapour and SO<sub>2</sub>. Structural characterisation revealed that Co doping did not alter the fundamental crystal structure of YMn<sub>2</sub>O<sub>5</sub> mullite. Through some characterization comprehensive analysis, and DFT calculations further supported the experimental findings, indicate that Co substitution significantly increased the lattice oxygen mobility and surface active oxygen content. Compared to the surface lattice oxygens at other positions, the weakening of the Mn-O bond results in the lattice oxygens in the Co-O-Mn<sup>4+</sup> sites in the catalysts exhibiting higher reactivity. Additionally, the catalyst displayed strong NO and O<sub>2</sub> adsorption and activation capabilities, indicating its potential for efficient NO<sub>x</sub>-assisted soot combustion. This study provides insights for designing and optimizing mullite catalysts for soot combustion.<h3>Environmental implications</h3>The catalytic removal of soot particles from diesel exhaust is crucial for protecting both environmental quality and human health. In this work, cobalt (Co) doping into YMn<sub>2</sub>O<sub>5</sub> mullite decreased the strength of Mn-O bond and increased the adsorption capacity of NO, which was beneficial to soot combustion reaction. This research enriches the application of mullite in the field of environmental catalysis.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"197 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642826","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 : 2024-11-16DOI: 10.1016/j.jhazmat.2024.136513
Xiang Chen , Tao Guo , Tiezhu Yan , Yunrong Dai , Lifeng Yin
Peroxymonosulfate (PMS) activation generates potent reactive oxygen species (ROS) such as sulfate radical (SO4·–) and hydroxyl radical (·OH), which play a key role in organic pollutant degradation. However, controlling the generation of these free radicals remains challenging. In this study, various metal (Co, Ni, and Cu)-doped nitrogen carbon compounds (NCs) were synthesized, and their performance in PMS activation under electric field regulation was explored to modulate ROS production for selective pollutant degradation. Bisphenol A (BPA), a readily degradable compound, and ibuprofen (IBU), a recalcitrant pollutant, were chosen as model pollutants to assess degradation efficiency. All catalysts achieved over 95 % BPA removal without the electric field, but the application of an electric field significantly accelerated BPA degradation, achieving complete removal within 3 min. In contrast, IBU degradation showed significant variation depending on the catalyst used and the electric field intensity, with Cu-NC demonstrating the highest performance, enhancing the degradation rate by 3.78-fold. Mechanistic studies revealed that the electric field altered the electron density on the catalyst surface, shifting ROS production from SO4·– to·OH in Co-NC systems. The findings could provide valuable insights into PMS activation under electric field regulation, offering a novel strategy for enhancing micropollutant removal through controlled ROS generation.
{"title":"Selective generation of hydroxyl and sulfate radicals under electric field regulation for micropollutants degradation: Mechanism and structure-activity relationship","authors":"Xiang Chen , Tao Guo , Tiezhu Yan , Yunrong Dai , Lifeng Yin","doi":"10.1016/j.jhazmat.2024.136513","DOIUrl":"10.1016/j.jhazmat.2024.136513","url":null,"abstract":"<div><div>Peroxymonosulfate (PMS) activation generates potent reactive oxygen species (ROS) such as sulfate radical (SO<sub>4</sub><sup>·–</sup>) and hydroxyl radical (·OH), which play a key role in organic pollutant degradation. However, controlling the generation of these free radicals remains challenging. In this study, various metal (Co, Ni, and Cu)-doped nitrogen carbon compounds (NCs) were synthesized, and their performance in PMS activation under electric field regulation was explored to modulate ROS production for selective pollutant degradation. Bisphenol A (BPA), a readily degradable compound, and ibuprofen (IBU), a recalcitrant pollutant, were chosen as model pollutants to assess degradation efficiency. All catalysts achieved over 95 % BPA removal without the electric field, but the application of an electric field significantly accelerated BPA degradation, achieving complete removal within 3 min. In contrast, IBU degradation showed significant variation depending on the catalyst used and the electric field intensity, with Cu-NC demonstrating the highest performance, enhancing the degradation rate by 3.78-fold. Mechanistic studies revealed that the electric field altered the electron density on the catalyst surface, shifting ROS production from SO<sub>4</sub><sup>·–</sup> to·OH in Co-NC systems. The findings could provide valuable insights into PMS activation under electric field regulation, offering a novel strategy for enhancing micropollutant removal through controlled ROS generation.</div></div>","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"481 ","pages":"Article 136513"},"PeriodicalIF":12.2,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642827","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 : 2024-11-16DOI: 10.1016/j.jhazmat.2024.136532
Fan Wu, Abdul Haleem, Mohib Ullah, Li Chen, Hao Li, Jianming Pan
Recovering precious metals such as palladium from secondary resources faces significant challenges, including the scarcity of efficient adsorbents capable of withstanding harsh acidic conditions and needing materials with high selectivity, mechanical stability, and scalability. In response to these challenges, we developed highly porous cryogels functionalized with sulfonic and amidoxime groups, achieving a unique combination of hydrophilicity, flexibility, and selectivity for Pd(II) ions. Using a redox cryopolymerization method, these cryogels attained a gel fraction of 100% and a maximum adsorption capacity of 425.3 mg g-1 at 318 K, as the Langmuir isotherm model fitted. This work also combined 3D printing technology with cryopolymerization to create a highly selective, high mechanical strength and customizable shape adsorption material, overcoming traditional adsorption materials' limitations in acid conditions. This innovative combination fills the gap in selective palladium recovery in customizable super macroporous materials, offering a sustainable solution for precious metal recovery and setting a foundation for broader applications in adsorption separation.
{"title":"Fabrication of superporous cryogels with amidoxime chelation sites and customizable 3D printing for targeted palladium recovery from secondary resources","authors":"Fan Wu, Abdul Haleem, Mohib Ullah, Li Chen, Hao Li, Jianming Pan","doi":"10.1016/j.jhazmat.2024.136532","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136532","url":null,"abstract":"Recovering precious metals such as palladium from secondary resources faces significant challenges, including the scarcity of efficient adsorbents capable of withstanding harsh acidic conditions and needing materials with high selectivity, mechanical stability, and scalability. In response to these challenges, we developed highly porous cryogels functionalized with sulfonic and amidoxime groups, achieving a unique combination of hydrophilicity, flexibility, and selectivity for Pd(II) ions. Using a redox cryopolymerization method, these cryogels attained a gel fraction of 100% and a maximum adsorption capacity of 425.3<!-- --> <!-- -->mg<!-- --> <!-- -->g<sup>-1</sup> at 318<!-- --> <!-- -->K, as the Langmuir isotherm model fitted. This work also combined 3D printing technology with cryopolymerization to create a highly selective, high mechanical strength and customizable shape adsorption material, overcoming traditional adsorption materials' limitations in acid conditions. This innovative combination fills the gap in selective palladium recovery in customizable super macroporous materials, offering a sustainable solution for precious metal recovery and setting a foundation for broader applications in adsorption separation.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"1 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-16","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642824","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 : 2024-11-15DOI: 10.1016/j.jhazmat.2024.136519
Xiaoyan Tu, Jiajia Yuan, Shuxia Xu, Xinfeng Zhang
The monitoring of glyphosate residual in environmental samples is critically important due to its high environmental risk. Here, we reported a low background dual-ligand and fast response copper-based metal organic framework (Cu-MOF) nanoprobe for imaging glyphosate in plant tissue, rapid screening of glyphosate-contaminated samples, and sensitive detection of glyphosate in environmental samples. The Cu-MOF nanoprobe was prepared with 2-Aminoisophthalic Acid (AIA) and trimesic acid (H3BTC) as ligands, and Cu2+ as a metal node. Thanking to both ligand-to-metal charge transfer (LMCT) and photoinduced electron transfer (PET) effects, the fluorescence of ligand AIA could be fully quenched in Cu-AIA/BTC probe. Upon the addition of glyphosate, it competed with the ligands in Cu-AIA/BTC probe, causing the collapse of MOF structure and the release of ligand AIA with obvious fluorescence recovery. This nanoprobe exhibited a desirable linear response for glyphosate in the concentration range of 0.1-80 μM, with a low detection limit of 33 nM, much lower than the maximum contaminant level (4.1 μM) set by the U.S. Environmental Protection Agency (EPA). Furthermore, it was also successfully applied for plant tissue imaging, fast screening of glyphosate-contaminated samples and monitoring of the degradation of glyphosate on tea leaves and in soil, indicating the broad application prospect of the nanoprobe.
{"title":"Low background dual-ligand Cu-MOF nanoprobe for plant tissue imaging and fast screening as well as sensitive detection of glyphosate in environmental samples","authors":"Xiaoyan Tu, Jiajia Yuan, Shuxia Xu, Xinfeng Zhang","doi":"10.1016/j.jhazmat.2024.136519","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136519","url":null,"abstract":"The monitoring of glyphosate residual in environmental samples is critically important due to its high environmental risk. Here, we reported a low background dual-ligand and fast response copper-based metal organic framework (Cu-MOF) nanoprobe for imaging glyphosate in plant tissue, rapid screening of glyphosate-contaminated samples, and sensitive detection of glyphosate in environmental samples. The Cu-MOF nanoprobe was prepared with 2-Aminoisophthalic Acid (AIA) and trimesic acid (H<sub>3</sub>BTC) as ligands, and Cu<sup>2+</sup> as a metal node. Thanking to both ligand-to-metal charge transfer (LMCT) and photoinduced electron transfer (PET) effects, the fluorescence of ligand AIA could be fully quenched in Cu-AIA/BTC probe. Upon the addition of glyphosate, it competed with the ligands in Cu-AIA/BTC probe, causing the collapse of MOF structure and the release of ligand AIA with obvious fluorescence recovery. This nanoprobe exhibited a desirable linear response for glyphosate in the concentration range of 0.1-80<!-- --> <!-- -->μM, with a low detection limit of 33<!-- --> <!-- -->nM, much lower than the maximum contaminant level (4.1<!-- --> <!-- -->μM) set by the U.S. Environmental Protection Agency (EPA). Furthermore, it was also successfully applied for plant tissue imaging, fast screening of glyphosate-contaminated samples and monitoring of the degradation of glyphosate on tea leaves and in soil, indicating the broad application prospect of the nanoprobe.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"247 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642831","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 : 2024-11-15DOI: 10.1016/j.jhazmat.2024.136514
Xiao Yang, Jiayi Du, Chao Jia, Tian Yang, Shuai Shao
Groundwater is vital for agricultural cities, but intensive farming and fertilizer use have increased contamination risks, particularly for non-carcinogenic health hazards. This study reveals the sources of contaminants in groundwater, their health impacts, and targeted strategies in such cities. The study analyzed 115 groundwater samples, with the main groundwater chemical type being HCO₃-Na·Ca. Significant exceedances were found in Mg²⁺, HCO₃−, F−, total hardness (TH), and Mn, with HCO₃− and Mg²⁺ surpassing standards in nearly all samples. The average Comprehensive Environmental Water Quality Index (CEWQI) was 100.68, indicating that overall groundwater quality in the study area is good. High-quality water is mainly found near reservoirs and rivers, while urban and eastern regions have relatively poorer water quality. The proportion of groundwater unsuitable for drinking is low. Monte Carlo risk assessments revealed that F− and NO₃− pose non-carcinogenic risks to both adults and children, with NO₃− presenting a higher potential health risk. The Positive Matrix Factorization (PMF) model identified that groundwater pollution primarily results from natural geological processes and human activities, with agriculture being the major anthropogenic factor. AI-based zoning strategies highlighted industrial areas and high-fluoride zones as critical areas requiring enhanced prevention and control measures.
{"title":"Unravelling integrated groundwater management in pollution-prone agricultural cities: a synergistic approach combining probabilistic risk, source apportionment and artificial intelligence","authors":"Xiao Yang, Jiayi Du, Chao Jia, Tian Yang, Shuai Shao","doi":"10.1016/j.jhazmat.2024.136514","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136514","url":null,"abstract":"Groundwater is vital for agricultural cities, but intensive farming and fertilizer use have increased contamination risks, particularly for non-carcinogenic health hazards. This study reveals the sources of contaminants in groundwater, their health impacts, and targeted strategies in such cities. The study analyzed 115 groundwater samples, with the main groundwater chemical type being HCO₃-Na·Ca. Significant exceedances were found in Mg²⁺, HCO₃<sup>−</sup>, F<sup>−</sup>, total hardness (TH), and Mn, with HCO₃<sup>−</sup> and Mg²⁺ surpassing standards in nearly all samples. The average Comprehensive Environmental Water Quality Index (CEWQI) was 100.68, indicating that overall groundwater quality in the study area is good. High-quality water is mainly found near reservoirs and rivers, while urban and eastern regions have relatively poorer water quality. The proportion of groundwater unsuitable for drinking is low. Monte Carlo risk assessments revealed that F<sup>−</sup> and NO₃<sup>−</sup> pose non-carcinogenic risks to both adults and children, with NO₃<sup>−</sup> presenting a higher potential health risk. The Positive Matrix Factorization (PMF) model identified that groundwater pollution primarily results from natural geological processes and human activities, with agriculture being the major anthropogenic factor. AI-based zoning strategies highlighted industrial areas and high-fluoride zones as critical areas requiring enhanced prevention and control measures.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"12 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142642878","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 : 2024-11-15DOI: 10.1016/j.jhazmat.2024.136520
Jie Zhou , Xiaolei Hu , Zhengkun Luo , Xiaodong Li , Wei-xian Zhang , Zilong Deng
A poriferous nZVI aerogel (nZVI@UiO-66-NH2/TCNF) was elaborately constructed by in-situ deposition of nZVI on UiO-66-NH2 and coupling with a bio-based TEMPO oxidized cellulose nanofiber (TCNF) substrate, followed by freeze-drying process for p-chloronitrobenzene (p-CNB) degradation. With degradation efficiency of above 85 % within 3 h under a wide pH range of 3–9, the nZVI@UiO-66-NH2/TCNF aerogel presented better p-CNB removal performance than other developed aerogels. Extended to 24 h, superior p-CNB removal performance (99.83 %) and 4-chloroaniline (p-CAN) selectivity (98.84 %) were successfully achieved. This could be attributed to 1) the facilitated mass transfer via concentration-gradient driving force with buffering and drag-reducing hydrated shear layer from porous channels of hydrophilic TCNF; 2) the enhanced adhesion of p-CNB onto UiO-66-NH2 and accelerated electron transfer by Fe-O-Zr bonds, synergistically improving the nitro- reduction of p-CNB using nZVI. This work pioneered a unique paradigm, providing nZVI with both solid bio-based moldability and highly-selective removal for the treatment of chloronitrobenzene containing wastewater.
{"title":"Nanocellulose encapsulated nZVI@UiO-66-NH2 aerogel for high-efficiency p-chloronitrobenzene removal with selective reduction","authors":"Jie Zhou , Xiaolei Hu , Zhengkun Luo , Xiaodong Li , Wei-xian Zhang , Zilong Deng","doi":"10.1016/j.jhazmat.2024.136520","DOIUrl":"10.1016/j.jhazmat.2024.136520","url":null,"abstract":"<div><div>A poriferous nZVI aerogel (nZVI@UiO-66-NH<sub>2</sub>/TCNF) was elaborately constructed by in-situ deposition of nZVI on UiO-66-NH<sub>2</sub> and coupling with a bio-based TEMPO oxidized cellulose nanofiber (TCNF) substrate, followed by freeze-drying process for p-chloronitrobenzene (p-CNB) degradation. With degradation efficiency of above 85 % within 3 h under a wide pH range of 3–9, the nZVI@UiO-66-NH<sub>2</sub>/TCNF aerogel presented better p-CNB removal performance than other developed aerogels. Extended to 24 h, superior p-CNB removal performance (99.83 %) and 4-chloroaniline (p-CAN) selectivity (98.84 %) were successfully achieved. This could be attributed to 1) the facilitated mass transfer via concentration-gradient driving force with buffering and drag-reducing hydrated shear layer from porous channels of hydrophilic TCNF; 2) the enhanced adhesion of p-CNB onto UiO-66-NH<sub>2</sub> and accelerated electron transfer by Fe-O-Zr bonds, synergistically improving the nitro- reduction of p-CNB using nZVI. This work pioneered a unique paradigm, providing nZVI with both solid bio-based moldability and highly-selective removal for the treatment of chloronitrobenzene containing wastewater.</div></div>","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"481 ","pages":"Article 136520"},"PeriodicalIF":12.2,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637807","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 : 2024-11-15DOI: 10.1016/j.jhazmat.2024.136526
Rong Liu, Kun Wu, Xuan Sun, Yucheng Liu, Yuchen Wang, Jiacheng Liu, Zhihua Li
This study focused on two Mn-oxide-containing adsorbents for As(Ⅲ) removal, namely granular iron-manganese composite oxide (GFMO) and granular iron-manganese-copper composite oxide (GFMCO). The comparative experiments results demonstrated that GFMCO exhibited superior performance in As(Ⅲ) removal and a more obvious Mn(II) release compared to GFMO. Furthermore, this study explored the approaches for the control of manganese release during As(Ⅲ) removal, identifying sodium hypochlorite (NaClO) oxidation followed by manganese sand filtration as the most effective method for capturing released Mn(Ⅱ) in water. Manganese sand columns effectively captured released Mn(Ⅱ) from effluent, while chlorine oxidation significantly improved manganese removal. The positive effect of copper on Mn(Ⅱ) removal by oxidants was also assessed. In addition, the solution pH significantly impacted manganese removal efficiency, with alkaline conditions being the most conducive. Moreover, the presence of sulfite notably accelerated manganese release. Characterization of the adsorption columns indicated that the manganese element undergoes release, migration, and speciation transformation within the filter systems, where redox reactions, adsorption processes, and autocatalytic oxidation processes were all involved. Not only NaClO oxidation but also autocatalytic oxidation with newly-formed Mn oxides contributed to the transformation Mn(Ⅱ) to Mn oxides, promoting the stabilization of Mn element in manganese sand filtration columns. This study provides valuable insights into the stability of Mn-oxide-containing adsorbents for As(Ⅲ) removal in the filter system and highlights on engineered approaches to control the transformation and migration of released manganese ions.
{"title":"Insights into the stability assessment and reaction mechanisms of Mn-oxide-containing adsorbents for As(Ⅲ) removal in filter columns: Migration laws and stabilization mechanisms of Mn element","authors":"Rong Liu, Kun Wu, Xuan Sun, Yucheng Liu, Yuchen Wang, Jiacheng Liu, Zhihua Li","doi":"10.1016/j.jhazmat.2024.136526","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136526","url":null,"abstract":"This study focused on two Mn-oxide-containing adsorbents for As(Ⅲ) removal, namely granular iron-manganese composite oxide (GFMO) and granular iron-manganese-copper composite oxide (GFMCO). The comparative experiments results demonstrated that GFMCO exhibited superior performance in As(Ⅲ) removal and a more obvious Mn(II) release compared to GFMO. Furthermore, this study explored the approaches for the control of manganese release during As(Ⅲ) removal, identifying sodium hypochlorite (NaClO) oxidation followed by manganese sand filtration as the most effective method for capturing released Mn(Ⅱ) in water. Manganese sand columns effectively captured released Mn(Ⅱ) from effluent, while chlorine oxidation significantly improved manganese removal. The positive effect of copper on Mn(Ⅱ) removal by oxidants was also assessed. In addition, the solution pH significantly impacted manganese removal efficiency, with alkaline conditions being the most conducive. Moreover, the presence of sulfite notably accelerated manganese release. Characterization of the adsorption columns indicated that the manganese element undergoes release, migration, and speciation transformation within the filter systems, where redox reactions, adsorption processes, and autocatalytic oxidation processes were all involved. Not only NaClO oxidation but also autocatalytic oxidation with newly-formed Mn oxides contributed to the transformation Mn(Ⅱ) to Mn oxides, promoting the stabilization of Mn element in manganese sand filtration columns. This study provides valuable insights into the stability of Mn-oxide-containing adsorbents for As(Ⅲ) removal in the filter system and highlights on engineered approaches to control the transformation and migration of released manganese ions.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"75 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142637764","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}
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