Pub Date : 2024-11-19DOI: 10.1016/j.jhazmat.2024.136572
Xiao Chen, Xiao-Nan Wu, Jing-Chun Feng, Bin Wang, Can-Rong Li, Yi-Lei Lin, Yong-Ji Huang, Song Zhong, Xiao-Chun Zhang, Jun-Lin Hu, Si Zhang
Marine microplastics pose a significant threat to ecosystems, and deep-sea regions serve as critical sinks for these pollutants. Among these regions, cold seeps harbor relatively high concentrations of microplastics. However, research on the aging of microplastics under low-temperature, dark, methane-abundant, and high-pressure conditions remains limited. Seawater and sediment were collected from various Haima cold seepage sites to simulate seepage environments in 200-mL high-pressure reactors. Four types of microplastics at high concentrations of around (approximately 10%) were cultured and monitored over two months to explore how they aged. The key findings are as follows: (1) Compared to areas of weak seepage, methane seepage accelerated microplastic aging, as evidenced by increased surface roughness, enhanced C-O and (C=O)-O bond formation, increased microbial colonization, and reduced contact angles. (2) Microplastic aging is more pronounced in sediments than in seawater, with biodegradable polylactic acid (PLA) exhibiting the most significant aging characteristics and carbon contribution. (3) Aged microplastics induce greater disturbances in inorganic nutrient levels than in organic matter, impacting nitrogen cycle processes involving nitrate, nitrite, and ammonium. This study results reveal the fundamental aging characteristics of microplastics in extremely deep seas and highlight their potential ecological effects.
{"title":"Methane seepage leads to a specific microplastic aging process in the simulated cold seep environment","authors":"Xiao Chen, Xiao-Nan Wu, Jing-Chun Feng, Bin Wang, Can-Rong Li, Yi-Lei Lin, Yong-Ji Huang, Song Zhong, Xiao-Chun Zhang, Jun-Lin Hu, Si Zhang","doi":"10.1016/j.jhazmat.2024.136572","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136572","url":null,"abstract":"Marine microplastics pose a significant threat to ecosystems, and deep-sea regions serve as critical sinks for these pollutants. Among these regions, cold seeps harbor relatively high concentrations of microplastics. However, research on the aging of microplastics under low-temperature, dark, methane-abundant, and high-pressure conditions remains limited. Seawater and sediment were collected from various Haima cold seepage sites to simulate seepage environments in 200-mL high-pressure reactors. Four types of microplastics at high concentrations of around (approximately 10%) were cultured and monitored over two months to explore how they aged. The key findings are as follows: (1) Compared to areas of weak seepage, methane seepage accelerated microplastic aging, as evidenced by increased surface roughness, enhanced C-O and (C=O)-O bond formation, increased microbial colonization, and reduced contact angles. (2) Microplastic aging is more pronounced in sediments than in seawater, with biodegradable polylactic acid (PLA) exhibiting the most significant aging characteristics and carbon contribution. (3) Aged microplastics induce greater disturbances in inorganic nutrient levels than in organic matter, impacting nitrogen cycle processes involving nitrate, nitrite, and ammonium. This study results reveal the fundamental aging characteristics of microplastics in extremely deep seas and highlight their potential ecological effects.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"58 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671040","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}
As the economic center of southern China, the Pearl River Delta region (PRDR) pays special attention to public health issues. During the pandemic, intensive disinfection was carried out in the city to prevent the spread of the virus, which resulted in disinfectant residuals elevating and produced large amounts of toxic disinfection byproducts (DBPs) in the urban water environment. For the purpose of surveying the concentration and distribution of urban water DBPs during the outbreak, 57 samples were collected from three urban water matrices in the PRDR, and were analyzed for the common seven types of DBPs, to elucidate their occurrence and ecological risk. Total 31 DBPs were detected, and the average concentrations of various DBPs in the three matrices were in the order of: surface water (1.9-27.5 μg/L) < effluent from wastewater treatment plant (30.5-114.8 μg/L) < hospital wastewater (5.5-168.9 μg/L). Both trihalomethanes (THMs) and haloacetic acids (HAAs) were the two most major DBPs in all three water categories. By comparing the concentration levels of DBPs in different areas, the concentration levels of DBPs in PRDR were not high. In some hospital wastewater, the TOC content may be able to be used as an associative indicator of DBPs content. The results of the risk quotient indicate that HAAs and haloacetonitriles (HANs) pose some ecological risk.
{"title":"Occurrence and ecological risk of disinfection byproducts in urban waterbody during the pandemic in the Pearl River Delta","authors":"Huazhi Wu, Lin Zhang, Pengran Guo, Yanping Zhao, Yumei Song, Xuerong Zhang, Yongqian Lei, Jingwei Xu","doi":"10.1016/j.jhazmat.2024.136550","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136550","url":null,"abstract":"As the economic center of southern China, the Pearl River Delta region (PRDR) pays special attention to public health issues. During the pandemic, intensive disinfection was carried out in the city to prevent the spread of the virus, which resulted in disinfectant residuals elevating and produced large amounts of toxic disinfection byproducts (DBPs) in the urban water environment. For the purpose of surveying the concentration and distribution of urban water DBPs during the outbreak, 57 samples were collected from three urban water matrices in the PRDR, and were analyzed for the common seven types of DBPs, to elucidate their occurrence and ecological risk. Total 31 DBPs were detected, and the average concentrations of various DBPs in the three matrices were in the order of: surface water (1.9-27.5<!-- --> <!-- -->μg/L) < effluent from wastewater treatment plant (30.5-114.8<!-- --> <!-- -->μg/L) < hospital wastewater (5.5-168.9<!-- --> <!-- -->μg/L). Both trihalomethanes (THMs) and haloacetic acids (HAAs) were the two most major DBPs in all three water categories. By comparing the concentration levels of DBPs in different areas, the concentration levels of DBPs in PRDR were not high. In some hospital wastewater, the TOC content may be able to be used as an associative indicator of DBPs content. The results of the risk quotient indicate that HAAs and haloacetonitriles (HANs) pose some ecological risk.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"7 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671044","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 : 2024-11-19DOI: 10.1016/j.jhazmat.2024.136571
YeoJin Ju, Kyung-Woo Park, Eunhye Kwon, Dugin Kaown, Seong Chun Jun, Jiwon Park, Kang-Kun Lee
The distribution of uranium (U) concentrations, which reached up to 322 µg/L, was found to correlate with the pattern of fractures within the natural barrier system (NBS). Analysis of the vertical distribution of dissolved oxygen (DO), dissolved organic carbon (DOC), tritium (3H), microbial communities, and H2O and SO42– isotopes revealed insights into oxic water infiltration within the heterogeneous fractured system. Their distribution showed that the average infiltration depth at the KURT site is 200 m, while in external areas with a high frequency of fractures, oxic conditions extended down to 495 m. The SO42– isotopes suggested the potential for microbial sulfate reduction to play a role in regulating radionuclide mobility in the deep geological system. At approximately 500 m, genera capable of thriving under harsh conditions of low DO and high heavy metal concentrations, such as Novosphingobium, Comamonadaceae_uc, and Desulfuromonas_g2, were identified. These findings indicate hydrogeological variability and microbial adaptation within the deep NBS, highlighting the importance of understanding the deep geological environment for evaluating microbiome performance in regulating toxic radionuclides within repository systems. Overall, this study emphasizes the pivotal role of age tracers, stable isotopes, and microbiome in enhancing the assessment of the long-term stability of fractured granite barriers.
{"title":"Evaluating Radionuclide Mobility in Groundwater Recharge Areas of Fractured Natural Barrier Systems using Multiple Isotopes and Microbial Indicators","authors":"YeoJin Ju, Kyung-Woo Park, Eunhye Kwon, Dugin Kaown, Seong Chun Jun, Jiwon Park, Kang-Kun Lee","doi":"10.1016/j.jhazmat.2024.136571","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136571","url":null,"abstract":"The distribution of uranium (U) concentrations, which reached up to 322<!-- --> <!-- -->µg/L, was found to correlate with the pattern of fractures within the natural barrier system (NBS). Analysis of the vertical distribution of dissolved oxygen (DO), dissolved organic carbon (DOC), tritium (<sup>3</sup>H), microbial communities, and H<sub>2</sub>O and SO<sub>4</sub><sup>2–</sup> isotopes revealed insights into oxic water infiltration within the heterogeneous fractured system. Their distribution showed that the average infiltration depth at the KURT site is 200<!-- --> <!-- -->m, while in external areas with a high frequency of fractures, oxic conditions extended down to 495<!-- --> <!-- -->m. The SO<sub>4</sub><sup>2–</sup> isotopes suggested the potential for microbial sulfate reduction to play a role in regulating radionuclide mobility in the deep geological system. At approximately 500<!-- --> <!-- -->m, genera capable of thriving under harsh conditions of low DO and high heavy metal concentrations, such as <em>Novosphingobium</em>, <em>Comamonadaceae_uc</em>, and <em>Desulfuromonas_g2</em>, were identified. These findings indicate hydrogeological variability and microbial adaptation within the deep NBS, highlighting the importance of understanding the deep geological environment for evaluating microbiome performance in regulating toxic radionuclides within repository systems. Overall, this study emphasizes the pivotal role of age tracers, stable isotopes, and microbiome in enhancing the assessment of the long-term stability of fractured granite barriers.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"250 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671045","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}
This study investigated the application risk and value of Cd-enriched poplar wood, focusing on its wood properties, leaching characteristics, and brown rot resistance. The results indicated that Cd deposition in cell walls significantly inhibited brown rot fungi, thereby enhancing decay resistance. Furthermore, the extent of improvement in brown rot resistance was linked to wood density: the higher the density of Cd-enriched poplar wood, the stronger its resistance to brown rot. As the Cd concentration increased, the Cd distribution abundance and the wood crystallinity gradually increased. Structural changes were observed, including fluctuating microfibril angle and double wall thickness of fibers and vessels. Cd concentrations exceeding 50 mg/kg altered the chemical composition of the cell walls. The binding form of Cd in wood cell wall showed a trend of bound Cd ＞ free Cd ＞ residual Cd. Cd leaching occurred under cyclic soaking in water, which may lead to secondary contamination. However, under the condition of 75% relative humidity, Cd leaching was negligible, suggesting potential for safer use in controlled environments. These findings provide valuable insights into the management and application of Cd-enriched wood, especially in contexts where decay resistance is critical or in water-exposed environments.
{"title":"Application risk and value of Cd-enriched poplar wood: wood properties, leaching characteristics and brown rot resistance","authors":"Jing Qian, Manman Lu, Shixia Cui, Taoyu Han, Stavros Avramidis, Shengquan Liu, Jiejie Sun","doi":"10.1016/j.jhazmat.2024.136591","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136591","url":null,"abstract":"This study investigated the application risk and value of Cd-enriched poplar wood, focusing on its wood properties, leaching characteristics, and brown rot resistance. The results indicated that Cd deposition in cell walls significantly inhibited brown rot fungi, thereby enhancing decay resistance. Furthermore, the extent of improvement in brown rot resistance was linked to wood density: the higher the density of Cd-enriched poplar wood, the stronger its resistance to brown rot. As the Cd concentration increased, the Cd distribution abundance and the wood crystallinity gradually increased. Structural changes were observed, including fluctuating microfibril angle and double wall thickness of fibers and vessels. Cd concentrations exceeding 50<!-- --> <!-- -->mg/kg altered the chemical composition of the cell walls. The binding form of Cd in wood cell wall showed a trend of bound Cd ＞ free Cd ＞ residual Cd. Cd leaching occurred under cyclic soaking in water, which may lead to secondary contamination. However, under the condition of 75% relative humidity, Cd leaching was negligible, suggesting potential for safer use in controlled environments. These findings provide valuable insights into the management and application of Cd-enriched wood, especially in contexts where decay resistance is critical or in water-exposed environments.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"53 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673564","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}
The MnaNbTi2Ox (a = 0.6-0.9) catalysts for NH3 selective catalytic reduction denitration were prepared using the co-precipitation method. Among them, Mn0.7NbTi2Ox exhibits well low-temperature catalytic performance, wide activity temperature range (180-480 ℃), and worthy resistance to SO2 even with H2O. XRD was used to investigate the structure of MnaNbTi2Ox, in which Mn and Nb oxides highly dispersed in the MnaNbTi2Ox catalysts and Nb can dope into the crystal lattice of TiO2. XRF and XPS results show Nb can affect the transfer of electrons to Mn4+, and changing the Mn/Nb ratio can regulate the Mn4+ content on the MnaNbTi2Ox catalysts. H2-TPR, NH3 and NO oxidation results verify that Nb inhibits the oxidation capacity of MnaNbTi2Ox, and altering the Mn/Nb ratio can get appropriate oxidation property, which facilitates low-temperature NH3 activation and limit non-selective oxidation for NH3. In-situ DRIFTS results show Nb-OH bonds can provide new Brønsted acid sites, and both Lewis and Brønsted acid sites are active. Furthermore, Nb addition prevents sulphate deposition on the catalyst. The effect of Mn/Nb on catalytic performance, N2O formation and inhibition, SO2 poisoning, SO2 effect on NH3-SCR, and the enhancement of SO2 tolerance are also analyzed.
{"title":"Modulating NH3 oxidation and inhibiting sulfate deposition to improve NH3-SCR denitration performance by controlling Mn/Nb ratio over MnaNbTi2Ox (a = 0.6-0.9) catalysts","authors":"Yushi Li, Xuesong Leng, Zhiping Zhang, Xiaoyu Niu, Yujun Zhu","doi":"10.1016/j.jhazmat.2024.136568","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136568","url":null,"abstract":"The Mn<sub>a</sub>NbTi<sub>2</sub>O<sub>x</sub> (a = 0.6-0.9) catalysts for NH<sub>3</sub> selective catalytic reduction denitration were prepared using the co-precipitation method. Among them, Mn<sub>0.7</sub>NbTi<sub>2</sub>O<sub>x</sub> exhibits well low-temperature catalytic performance, wide activity temperature range (180-480 ℃), and worthy resistance to SO<sub>2</sub> even with H<sub>2</sub>O. XRD was used to investigate the structure of Mn<sub>a</sub>NbTi<sub>2</sub>O<sub>x</sub>, in which Mn and Nb oxides highly dispersed in the Mn<sub>a</sub>NbTi<sub>2</sub>O<sub>x</sub> catalysts and Nb can dope into the crystal lattice of TiO<sub>2</sub>. XRF and XPS results show Nb can affect the transfer of electrons to Mn<sup>4+</sup>, and changing the Mn/Nb ratio can regulate the Mn<sup>4+</sup> content on the Mn<sub>a</sub>NbTi<sub>2</sub>O<sub>x</sub> catalysts. H<sub>2</sub>-TPR, NH<sub>3</sub> and NO oxidation results verify that Nb inhibits the oxidation capacity of Mn<sub>a</sub>NbTi<sub>2</sub>O<sub>x</sub>, and altering the Mn/Nb ratio can get appropriate oxidation property, which facilitates low-temperature NH<sub>3</sub> activation and limit non-selective oxidation for NH<sub>3</sub>. <em>In-situ</em> DRIFTS results show Nb-OH bonds can provide new Brønsted acid sites, and both Lewis and Brønsted acid sites are active. Furthermore, Nb addition prevents sulphate deposition on the catalyst. The effect of Mn/Nb on catalytic performance, N<sub>2</sub>O formation and inhibition, SO<sub>2</sub> poisoning, SO<sub>2</sub> effect on NH<sub>3</sub>-SCR, and the enhancement of SO<sub>2</sub> tolerance are also analyzed.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"1 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671035","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 : 2024-11-19DOI: 10.1016/j.jhazmat.2024.136562
Mingdong Zhang, Qisheng Hong, Yuan Aocheng, Yan Zhang, Xiaoying Huang, Meiling Feng, Jingli Mu
Radionickel ion (63Ni2+) remediation is critical for public health and the environment, but selectively capturing of Ni2+ from complex environments like seawater presents a challenge. Metal sulfide ion exchangers (MSIEs) are emerging as efficient adsorbents for radionuclides; however, the study of MSIEs for selectively removing Ni2+ is still in its infancy. Herein, the layered metal sulfide K2Cu2Sn2S6 (CTS-1) with a unique sandwich-like anionic framework was synthesized by the hydrothermal method for the first time, representing a novel approach in the selective capture of Ni2+ from complex environments. Single-crystal structural analysis confirmed the sandwich-like framework, in which a [Cu-S] sublayer is sandwiched by two [Sn-S] sublayers with parallel grooves. The charge-balancing K+ ions are located within these grooves. Due to its special structure, CTS-1 exhibits remarkable adsorption capacities for Ni2+ with rapid kinetics (a high rate constant k2 of 7.26×10−2 g/(mg·min)), broad pH durability (removal rates >97% at pH 3–12), and high selectivity (separation factors for Ni2+ >700 against various cations). Impressively, it can efficiently remove Ni2+ from multiple complex environments, achieving a 90.28% removal rate even in seawater (C0Ni ~5 mg/L). CTS-1 is environmentally friendly and suitable for use in fixed-bed columns for the practical application. Moreover, Ni2+ ions are captured through ion exchange with K+, and the high selectivity stems from the strong affinity of S2− for Ni2+ and the trapping effect of the grooves within the structure. In summary, this pioneering study demonstrates the highly selective capture of Ni2+ by a sandwich-like layered MSIE, potentially inspiring the development of efficient scavengers for radionuclides.
{"title":"Highly selective capture of Ni2+ from complex environments by a sandwich-like layered metal sulfide ion exchanger","authors":"Mingdong Zhang, Qisheng Hong, Yuan Aocheng, Yan Zhang, Xiaoying Huang, Meiling Feng, Jingli Mu","doi":"10.1016/j.jhazmat.2024.136562","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136562","url":null,"abstract":"Radionickel ion (<sup>63</sup>Ni<sup>2+</sup>) remediation is critical for public health and the environment, but selectively capturing of Ni<sup>2+</sup> from complex environments like seawater presents a challenge. Metal sulfide ion exchangers (MSIEs) are emerging as efficient adsorbents for radionuclides; however, the study of MSIEs for selectively removing Ni<sup>2+</sup> is still in its infancy. Herein, the layered metal sulfide K<sub>2</sub>Cu<sub>2</sub>Sn<sub>2</sub>S<sub>6</sub> (CTS-1) with a unique sandwich-like anionic framework was synthesized by the hydrothermal method for the first time, representing a novel approach in the selective capture of Ni<sup>2+</sup> from complex environments. Single-crystal structural analysis confirmed the sandwich-like framework, in which a [Cu-S] sublayer is sandwiched by two [Sn-S] sublayers with parallel grooves. The charge-balancing K<sup>+</sup> ions are located within these grooves. Due to its special structure, CTS-1 exhibits remarkable adsorption capacities for Ni<sup>2+</sup> with rapid kinetics (a high rate constant <em>k</em><sub>2</sub> of 7.26×10<sup>−2</sup> g/(mg·min)), broad pH durability (removal rates >97% at pH 3–12), and high selectivity (separation factors for Ni<sup>2+</sup> >700 against various cations). Impressively, it can efficiently remove Ni<sup>2+</sup> from multiple complex environments, achieving a 90.28% removal rate even in seawater (<em>C</em><sub>0</sub><sup>Ni</sup> ~5<!-- --> <!-- -->mg/L). CTS-1 is environmentally friendly and suitable for use in fixed-bed columns for the practical application. Moreover, Ni<sup>2+</sup> ions are captured through ion exchange with K<sup>+</sup>, and the high selectivity stems from the strong affinity of S<sup>2−</sup> for Ni<sup>2+</sup> and the trapping effect of the grooves within the structure. In summary, this pioneering study demonstrates the highly selective capture of Ni<sup>2+</sup> by a sandwich-like layered MSIE, potentially inspiring the development of efficient scavengers for radionuclides.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"64 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671042","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}
Nerve and blister agents are among the deadliest chemicals posing a major threat to the society, and the development of materials that can rapidly decontaminate them under solvent-free ambient conditions is a major societal challenge. In this paper, layered double hydroxides (ZnAlxZr1-x-LDH) with varying Zr4+ doping content were synthesized and the decontamination properties of nerve and blister agents were investigated under ambient conditions. The results show that, compared to ZnAl-LDH, the ZnAl0.4Zr0.6-LDH with the highest amount of Zr4+ dopant reduced the decontamination reaction half-life of sarin (GB) and soman (GD) by 10 and 9 times, respectively. Mechanism studies revealed that ZnAl0.4Zr0.6-LDH employs the synergistic effect of Lewis acid-base sites to catalyze the decomposition of GB and GD into hydrolysis products and surface-bound hydrolysis products. The study also showed that under ambient conditions, ZnAl0.4Zr0.6-LDH demonstrated superior decontamination performance for the sulfur mustard (HD) simulant 2-chloroethyl ethyl sulfide (CEES) compared to ZnAl-LDH, effectively catalyzing the detoxification of CEES into dehydrohalogenation (EVS) and 1,2-bis-(ethylthio) ethane (BETE). ZnAl0.4Zr0.6-LDH also had satisfactory decontamination performance against HD. This work provides not only a green and efficient catalyst with potential for practical applications but also new insights for constructing broad-spectrum, highly efficient self-detoxifying materials.
{"title":"Synergistic effect of Lewis acid-base sites in Zr4+-doped layered double hydroxides promotes rapid decontamination of nerve and blister agents under ambient conditions","authors":"Chengcheng Huang, Ying Yang, Xin Hu, Qian Wang, Hongchen Fu, Pingjing Wang, Yunshan Zhou, Lijuan Zhang, Yuxu Zhong","doi":"10.1016/j.jhazmat.2024.136565","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136565","url":null,"abstract":"Nerve and blister agents are among the deadliest chemicals posing a major threat to the society, and the development of materials that can rapidly decontaminate them under solvent-free ambient conditions is a major societal challenge. In this paper, layered double hydroxides (ZnAl<sub>x</sub>Zr<sub>1-x</sub>-LDH) with varying Zr<sup>4+</sup> doping content were synthesized and the decontamination properties of nerve and blister agents were investigated under ambient conditions. The results show that, compared to ZnAl-LDH, the ZnAl<sub>0.4</sub>Zr<sub>0.6</sub>-LDH with the highest amount of Zr<sup>4+</sup> dopant reduced the decontamination reaction half-life of sarin (GB) and soman (GD) by 10 and 9 times, respectively. Mechanism studies revealed that ZnAl<sub>0.4</sub>Zr<sub>0.6</sub>-LDH employs the synergistic effect of Lewis acid-base sites to catalyze the decomposition of GB and GD into hydrolysis products and surface-bound hydrolysis products. The study also showed that under ambient conditions, ZnAl<sub>0.4</sub>Zr<sub>0.6</sub>-LDH demonstrated superior decontamination performance for the sulfur mustard (HD) simulant 2-chloroethyl ethyl sulfide (CEES) compared to ZnAl-LDH, effectively catalyzing the detoxification of CEES into dehydrohalogenation (EVS) and 1,2-bis-(ethylthio) ethane (BETE). ZnAl<sub>0.4</sub>Zr<sub>0.6</sub>-LDH also had satisfactory decontamination performance against HD. This work provides not only a green and efficient catalyst with potential for practical applications but also new insights for constructing broad-spectrum, highly efficient self-detoxifying materials.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"18 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142670995","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 : 2024-11-19DOI: 10.1016/j.jhazmat.2024.136578
Yibo Yan, Yong Yang
The identification of factors that affect changes in the heavy metal content of soil is the basis for reducing or preventing soil heavy metal pollution. In this research, 16 environmental factors were selected, and the influences of soil heavy metal spatial distribution factors and the synergy amongst space factors were evaluated using a geographic detector (GD) and the extreme gradient boosting (XGBoost)-Shapley additive explanations (SHAP) model. Three heavy metal elements, namely, Cd, Cu and Pb, in the study region were examined. The following results were obtained. (1) XGBoost demonstrated high accuracy in predicting the spatial distributions of soil heavy metals, with each heavy metal having an R2 value of over 0.6. (2) Geological type map (Geomap) and enterprise density considerably affected the concentrations of Cd, Cu and Pb in soil in the GD and XGBoost-SHAP models. In addition, cross-detection revealed strong explanatory power when natural and human factors were combined. (3) Under the same geological background, the different trends of gross domestic product effects on heavy metals indicated that pollution control measures were effective in economically developed areas, and the economy and the environment could be balanced. Meanwhile, the interaction between the normalised difference vegetation index and enterprise density showed that vegetation could alleviate heavy metal pollution in the region. This study supports strategic decision-making, serving as a reference for the global management of soil heavy metal contamination, sustainable ecological development and assurance of people’s health and well-being.
{"title":"Revealing the Synergistic Spatial Effects in Soil Heavy Metal Pollution with Explainable Machine Learning Models","authors":"Yibo Yan, Yong Yang","doi":"10.1016/j.jhazmat.2024.136578","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136578","url":null,"abstract":"The identification of factors that affect changes in the heavy metal content of soil is the basis for reducing or preventing soil heavy metal pollution. In this research, 16 environmental factors were selected, and the influences of soil heavy metal spatial distribution factors and the synergy amongst space factors were evaluated using a geographic detector (GD) and the extreme gradient boosting (XGBoost)-Shapley additive explanations (SHAP) model. Three heavy metal elements, namely, Cd, Cu and Pb, in the study region were examined. The following results were obtained. (1) XGBoost demonstrated high accuracy in predicting the spatial distributions of soil heavy metals, with each heavy metal having an <em>R</em><sup>2</sup> value of over 0.6. (2) Geological type map (Geomap) and enterprise density considerably affected the concentrations of Cd, Cu and Pb in soil in the GD and XGBoost-SHAP models. In addition, cross-detection revealed strong explanatory power when natural and human factors were combined. (3) Under the same geological background, the different trends of gross domestic product effects on heavy metals indicated that pollution control measures were effective in economically developed areas, and the economy and the environment could be balanced. Meanwhile, the interaction between the normalised difference vegetation index and enterprise density showed that vegetation could alleviate heavy metal pollution in the region. This study supports strategic decision-making, serving as a reference for the global management of soil heavy metal contamination, sustainable ecological development and assurance of people’s health and well-being.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"250 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671100","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 : 2024-11-19DOI: 10.1016/j.jhazmat.2024.136593
Zheyu Shen, Yixin Yang, Yue Gu, Zhonglong Wang, Shifa Wang
Widespread application of hydrazine results in serious harm on the natural environments and human health because of its highly toxic, mutagenic, carcinogenic and teratogenic properties. Hence, it is very emergent to develop a convenient and efficient method for detection of hydrazine existed in real environments and living organisms. In this work, a novel ratiometric fluorescent probe PKZ-IN from the natural monoterpenoid 2-hydroxy-3-pinanone was designed and synthesized to detect trace hydrazine. The detection performance of probe PKZ-IN for hydrazine was investigated, and the results showed that this probe possessed excellent performance including large Stokes shift (211 nm), fast response time (<30 s), remarkable emission shift (136 nm), and a wide pH range (5−13). This probe was successfully used to detect hydrazine existed in three different soil samples (humus soil, sandy soil and loess soil). In addition, probe PKZ-IN was also used to prepare nanofibrous membrane for detecting gaseous hydrazine qualitatively and quantitively by the mobile phone platform. Furthermore, PKZ-IN was successfully applied in living organisms and plants imaging for detection of the residual hydrazine.
{"title":"Carbazole-pyrimidine-based novel ratiometric fluorescent probe with large Stokes shift for detection of hydrazine in real environments and organisms","authors":"Zheyu Shen, Yixin Yang, Yue Gu, Zhonglong Wang, Shifa Wang","doi":"10.1016/j.jhazmat.2024.136593","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136593","url":null,"abstract":"Widespread application of hydrazine results in serious harm on the natural environments and human health because of its highly toxic, mutagenic, carcinogenic and teratogenic properties. Hence, it is very emergent to develop a convenient and efficient method for detection of hydrazine existed in real environments and living organisms. In this work, a novel ratiometric fluorescent probe <strong>PKZ-IN</strong> from the natural monoterpenoid 2-hydroxy-3-pinanone was designed and synthesized to detect trace hydrazine. The detection performance of probe <strong>PKZ-IN</strong> for hydrazine was investigated, and the results showed that this probe possessed excellent performance including large Stokes shift (211<!-- --> <!-- -->nm), fast response time (<30<!-- --> <!-- -->s), remarkable emission shift (136<!-- --> <!-- -->nm), and a wide pH range (5−13). This probe was successfully used to detect hydrazine existed in three different soil samples (humus soil, sandy soil and loess soil). In addition, probe <strong>PKZ-IN</strong> was also used to prepare nanofibrous membrane for detecting gaseous hydrazine qualitatively and quantitively by the mobile phone platform. Furthermore, <strong>PKZ-IN</strong> was successfully applied in living organisms and plants imaging for detection of the residual hydrazine.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"197 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142673568","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 : 2024-11-19DOI: 10.1016/j.jhazmat.2024.136577
Pu Sun, Jibo Wang, Xingbin Li, Chang Wei, Zhigan Deng, Minting Li
The phase transformation characteristics of lead sulfate (PbSO4) in a sulfuric acid (H2SO4) system were studied, focusing on the effects of temperature, H2SO4 concentration, ferric iron (Fe3+) concentration, sodium sulfate (Na2SO4), and potassium sulfate (K2SO4). The conversion of PbSO4 was analyzed by characterizing the composition and structure of the solid product through XRD, SEM/BSE-EDS, and FT-IR. The results indicated that the effect of temperature on PbSO4 transformation was influenced by H2SO4 concentration. The temperature threshold for PbSO4 conversion to lead jarosite (Pb-J) decreased from 150 to 90℃ as H2SO4 concentration decreased from 20 to 5 g/L. At 150℃, the amount of jarosite generated decreased significantly from 86.04 to 9.76%. Subsequently, when H2SO4 concentration exceeded 40 g/L, PbSO4 was essentially unchanged. Concurrently, Pb-J formation correlated with the partial formation of hydronium jarosite (H-J). The production of jarosite was inhibited when the solution pH was ~ 0.3 or lower. Furthermore, the increase in Fe3+ concentration facilitated Pb-J formation, whereas Na2SO4 and K2SO4 inhibited Pb-J formation, leading to the formation of potassium jarosite (K-J) and sodium jarosite (Na-J), respectively. This study provided insights into regulating PbSO4 conversion during sulfide ore oxygen pressure leaching.
{"title":"Phase conversion characteristics of lead sulfate in ferric sulfate medium","authors":"Pu Sun, Jibo Wang, Xingbin Li, Chang Wei, Zhigan Deng, Minting Li","doi":"10.1016/j.jhazmat.2024.136577","DOIUrl":"https://doi.org/10.1016/j.jhazmat.2024.136577","url":null,"abstract":"The phase transformation characteristics of lead sulfate (PbSO<sub>4</sub>) in a sulfuric acid (H<sub>2</sub>SO<sub>4</sub>) system were studied, focusing on the effects of temperature, H<sub>2</sub>SO<sub>4</sub> concentration, ferric iron (Fe<sup>3+</sup>) concentration, sodium sulfate (Na<sub>2</sub>SO<sub>4</sub>), and potassium sulfate (K<sub>2</sub>SO<sub>4</sub>). The conversion of PbSO<sub>4</sub> was analyzed by characterizing the composition and structure of the solid product through XRD, SEM/BSE-EDS, and FT-IR. The results indicated that the effect of temperature on PbSO<sub>4</sub> transformation was influenced by H<sub>2</sub>SO<sub>4</sub> concentration. The temperature threshold for PbSO<sub>4</sub> conversion to lead jarosite (Pb-J) decreased from 150 to 90℃ as H<sub>2</sub>SO<sub>4</sub> concentration decreased from 20 to 5<!-- --> <!-- -->g/L. At 150℃, the amount of jarosite generated decreased significantly from 86.04 to 9.76%. Subsequently, when H<sub>2</sub>SO<sub>4</sub> concentration exceeded 40<!-- --> <!-- -->g/L, PbSO<sub>4</sub> was essentially unchanged. Concurrently, Pb-J formation correlated with the partial formation of hydronium jarosite (H-J). The production of jarosite was inhibited when the solution pH was ~ 0.3 or lower. Furthermore, the increase in Fe<sup>3+</sup> concentration facilitated Pb-J formation, whereas Na<sub>2</sub>SO<sub>4</sub> and K<sub>2</sub>SO<sub>4</sub> inhibited Pb-J formation, leading to the formation of potassium jarosite (K-J) and sodium jarosite (Na-J), respectively. This study provided insights into regulating PbSO<sub>4</sub> conversion during sulfide ore oxygen pressure leaching.","PeriodicalId":361,"journal":{"name":"Journal of Hazardous Materials","volume":"229 1","pages":""},"PeriodicalIF":13.6,"publicationDate":"2024-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142671037","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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