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Occurrence and ecological risk of disinfection byproducts in urban waterbody during the pandemic in the Pearl River Delta 珠江三角洲大流行期间城市水体中消毒副产物的出现和生态风险
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-19 DOI: 10.1016/j.jhazmat.2024.136550
Huazhi Wu, Lin Zhang, Pengran Guo, Yanping Zhao, Yumei Song, Xuerong Zhang, Yongqian Lei, Jingwei Xu
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.
作为华南地区的经济中心,珠江三角洲地区对公共卫生问题尤为重视。疫情期间,为防止病毒传播,城市进行了密集消毒,导致消毒剂残留量升高,在城市水环境中产生了大量有毒的消毒副产物(DBPs)。为了调查疫情期间城市水体中 DBPs 的浓度和分布情况,我们从珠江三角洲地区的三个城市水体基质中采集了 57 个样本,并对常见的七种 DBPs 进行了分析,以阐明它们的出现和生态风险。共检测到 31 种 DBPs,三种基质中各种 DBPs 的平均浓度依次为:地表水(1.9-27.5 μg/L);污水处理厂出水(30.5-114.8 μg/L);医院废水(5.5-168.9 μg/L)。三卤甲烷(THMs)和卤乙酸(HAAs)是三类废水中最主要的两种 DBPs。通过比较不同地区的 DBPs 浓度水平,珠江三角洲地区的 DBPs 浓度水平并不高。在一些医院废水中,TOC 含量可作为 DBPs 含量的关联指标。风险商数的结果表明,HAAs 和卤代乙腈(HANs)具有一定的生态风险。
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引用次数: 0
Evaluating Radionuclide Mobility in Groundwater Recharge Areas of Fractured Natural Barrier Systems using Multiple Isotopes and Microbial Indicators 利用多种同位素和微生物指标评估断裂天然屏障系统地下水补给区的放射性核素流动性
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-19 DOI: 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.
铀(U)浓度高达 322 微克/升,其分布与天然屏障系统(NBS)内的裂缝形态相关。对溶解氧(DO)、溶解有机碳(DOC)、氚(3H)、微生物群落以及 H2O 和 SO42- 同位素的垂直分布分析揭示了异质断裂系统中的缺氧水渗透情况。SO42-同位素表明,微生物的硫酸盐还原作用有可能在深部地质系统中起到调节放射性核素流动性的作用。在约 500 米处,发现了能够在低溶解氧和高重金属浓度的恶劣条件下生长的菌属,如新磷酸盐菌属、科莫纳藻属 (Comamonadaceae_uc) 和脱硫单胞菌属 (Desulfuromonas_g2)。这些发现表明了深层 NBS 中的水文地质变异性和微生物适应性,突出了了解深层地质环境对于评估微生物组在调节储存库系统内有毒放射性核素方面的性能的重要性。总之,这项研究强调了年龄示踪剂、稳定同位素和微生物组在加强断裂花岗岩屏障长期稳定性评估方面的关键作用。
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引用次数: 0
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 通过控制 MnaNbTi2Ox(a = 0.6-0.9)催化剂上的锰/铌比来调节 NH3 氧化和抑制硫酸盐沉积,从而提高 NH3-SCR 脱硝性能
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-19 DOI: 10.1016/j.jhazmat.2024.136568
Yushi Li, Xuesong Leng, Zhiping Zhang, Xiaoyu Niu, Yujun Zhu
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.
采用共沉淀法制备了用于 NH3 选择性催化还原脱硝的 MnaNbTi2Ox(a = 0.6-0.9)催化剂。其中,Mn0.7NbTi2Ox 具有良好的低温催化性能、较宽的活性温度范围(180-480 ℃)以及即使在有 H2O 的情况下也能抵抗 SO2 的特性。XRD 被用来研究 MnaNbTi2Ox 的结构,其中 Mn 和 Nb 氧化物高度分散在 MnaNbTi2Ox 催化剂中,Nb 可以掺杂到 TiO2 的晶格中。XRF 和 XPS 结果表明,Nb 可以影响电子向 Mn4+ 的转移,改变 Mn/Nb 的比例可以调节 MnaNbTi2Ox 催化剂上 Mn4+ 的含量。H2-TPR、NH3 和 NO 氧化结果验证了 Nb 会抑制 MnaNbTi2Ox 的氧化能力,而改变 Mn/Nb 的比例可以获得适当的氧化性能,从而促进 NH3 的低温活化并限制 NH3 的非选择性氧化。原位 DRIFTS 结果表明,Nb-OH 键可以提供新的布氏酸位点,而且路易斯酸位点和布氏酸位点都很活跃。此外,铌的添加还能防止硫酸盐在催化剂上沉积。此外,还分析了 Mn/Nb 对催化性能、N2O 生成和抑制、二氧化硫中毒、二氧化硫对 NH3-SCR 的影响以及二氧化硫耐受性的增强等方面的影响。
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引用次数: 0
Highly selective capture of Ni2+ from complex environments by a sandwich-like layered metal sulfide ion exchanger 三明治状层状金属硫化物离子交换剂对复杂环境中 Ni2+ 的高选择性捕获
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-19 DOI: 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.
放射性镍离子(63Ni2+)的修复对公众健康和环境至关重要,但从海水等复杂环境中选择性地捕获 Ni2+ 却是一项挑战。金属硫化物离子交换剂(MSIEs)正在成为放射性核素的高效吸附剂;然而,对 MSIEs 选择性去除 Ni2+ 的研究仍处于起步阶段。本文首次采用水热法合成了具有独特夹层阴离子框架的层状金属硫化物 K2Cu2Sn2S6(CTS-1),为从复杂环境中选择性捕获 Ni2+ 提供了一种新方法。单晶结构分析证实了这种 "三明治 "式框架,其中一个[Cu-S]亚层被两个带有平行沟槽的[Sn-S]亚层夹住。电荷平衡的 K+ 离子位于这些沟槽中。由于其特殊的结构,CTS-1 对 Ni2+ 具有显著的吸附能力、快速的动力学特性(速率常数 k2 高达 7.26×10-2 g/(mg-min))、广泛的 pH 持久性(pH 值为 3-12 时的去除率为 97%)和高选择性(Ni2+ 与各种阳离子的分离系数为 700)。令人印象深刻的是,它能从多种复杂环境中高效去除 Ni2+,即使在海水(C0Ni ~5 mg/L)中也能达到 90.28% 的去除率。CTS-1 对环境友好,适合在固定床色谱柱中实际应用。此外,Ni2+ 离子是通过与 K+ 的离子交换捕获的,而高选择性则源于 S2- 对 Ni2+ 的强亲和力和结构内凹槽的捕获效应。总之,这项开创性的研究证明了三明治状层状 MSIE 对 Ni2+ 的高选择性捕获,可能会对开发高效的放射性核素清除剂有所启发。
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引用次数: 0
Synergistic effect of Lewis acid-base sites in Zr4+-doped layered double hydroxides promotes rapid decontamination of nerve and blister agents under ambient conditions 掺杂 Zr4+ 的层状双氢氧化物中路易斯酸碱位点的协同效应促进了环境条件下神经毒剂和水疱毒剂的快速净化
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-19 DOI: 10.1016/j.jhazmat.2024.136565
Chengcheng Huang, Ying Yang, Xin Hu, Qian Wang, Hongchen Fu, Pingjing Wang, Yunshan Zhou, Lijuan Zhang, Yuxu Zhong
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.
神经毒剂和水泡剂是对社会构成重大威胁的最致命化学物质之一,而开发可在无溶剂环境条件下快速净化神经毒剂和水泡剂的材料是一项重大的社会挑战。本文合成了不同 Zr4+ 掺杂含量的层状双氢氧化物(ZnAlxZr1-x-LDH),并研究了其在环境条件下对神经毒剂和水泡剂的去污性能。结果表明,与 ZnAl-LDH 相比,掺杂 Zr4+ 量最高的 ZnAl0.4Zr0.6-LDH 可使沙林(GB)和索曼(GD)的去污反应半衰期分别缩短 10 倍和 9 倍。机理研究表明,ZnAl0.4Zr0.6-LDH 利用路易斯酸碱位点的协同效应,将 GB 和 GD 催化分解为水解产物和表面结合型水解产物。研究还表明,在环境条件下,ZnAl0.4Zr0.6-LDH 对硫芥子气(HD)模拟物 2-氯乙基硫醚(CEES)的去污性能优于 ZnAl-LDH,能有效催化 CEES 解毒为脱氢卤化(EVS)和 1,2-双(乙硫基)乙烷(BETE)。ZnAl0.4Zr0.6-LDH 对 HD 的净化性能也令人满意。这项工作不仅提供了一种具有实际应用潜力的绿色高效催化剂,还为构建广谱、高效的自解毒材料提供了新的见解。
{"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}
引用次数: 0
Application risk and value of Cd-enriched poplar wood: wood properties, leaching characteristics and brown rot resistance 富含镉的杨木的应用风险和价值:木材特性、浸出特性和抗褐腐病能力
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-19 DOI: 10.1016/j.jhazmat.2024.136591
Jing Qian, Manman Lu, Shixia Cui, Taoyu Han, Stavros Avramidis, Shengquan Liu, Jiejie Sun
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.
本研究调查了富镉杨木的应用风险和价值,重点关注其木材特性、浸出特性和抗褐腐性。结果表明,镉沉积在细胞壁中能显著抑制褐腐真菌,从而增强抗腐烂性。此外,抗褐腐病能力的提高程度与木材密度有关:富含镉的杨木密度越高,抗褐腐病能力越强。随着镉浓度的增加,镉分布丰度和木材结晶度也逐渐增加。观察到的结构变化包括纤维和血管的微纤维角和双壁厚度的波动。镉浓度超过 50 毫克/千克会改变细胞壁的化学成分。镉在木材细胞壁中的结合形式呈现出结合镉 > 游离镉 > 残余镉的趋势。镉在水中循环浸泡时会发生浸出,这可能会导致二次污染。不过,在相对湿度为 75% 的条件下,镉的沥滤几乎可以忽略不计,这表明在受控环境中使用镉具有更安全的潜力。这些发现为富镉木材的管理和应用提供了有价值的启示,尤其是在对抗腐蚀性能要求很高的情况下或在暴露于水的环境中。
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引用次数: 0
Revealing the Synergistic Spatial Effects in Soil Heavy Metal Pollution with Explainable Machine Learning Models 用可解释的机器学习模型揭示土壤重金属污染的协同空间效应
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-19 DOI: 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.
确定影响土壤重金属含量变化的因素是减少或预防土壤重金属污染的基础。本研究选取了 16 个环境因子,利用地理检测器(GD)和极端梯度提升(XGBoost)-沙普利加性解释(SHAP)模型评估了土壤重金属空间分布因子的影响及空间因子间的协同作用。对研究区域的三种重金属元素,即镉、铜和铅进行了研究。结果如下(1) XGBoost 在预测土壤重金属空间分布方面表现出较高的准确性,每种重金属的 R2 值均超过 0.6。(2)在 GD 和 XGBoost-SHAP 模型中,地质类型图(Geomap)和企业密度对土壤中镉、铜和铅的浓度有很大影响。此外,当自然因素和人为因素相结合时,交叉探测显示出很强的解释力。(3)在相同的地质背景下,国内生产总值对重金属影响的不同趋势表明,经济发达地区的污染控制措施是有效的,经济与环境可以达到平衡。同时,归一化差异植被指数与企业密度的交互作用表明,植被可以缓解该地区的重金属污染。本研究有助于制定战略决策,为全球土壤重金属污染治理、生态可持续发展和保障人民健康福祉提供参考。
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引用次数: 0
Carbazole-pyrimidine-based novel ratiometric fluorescent probe with large Stokes shift for detection of hydrazine in real environments and organisms 基于咔唑-嘧啶的新型比率荧光探针,具有大斯托克斯位移,可用于检测实际环境和生物体中的肼
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-19 DOI: 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.
肼的广泛应用对自然环境和人类健康造成了严重危害,因为它具有剧毒、致突变、致癌和致畸等特性。因此,开发一种方便、高效的方法来检测实际环境和生物体中存在的肼是非常迫切的。本研究从天然单萜类化合物 2-hydroxy-3-pinanone 中设计并合成了一种新型比率荧光探针 PKZ-IN,用于检测痕量肼。研究了探针 PKZ-IN 对肼的检测性能,结果表明该探针具有优异的性能,包括较大的斯托克斯位移(211 nm)、快速的响应时间(30 s)、显著的发射位移(136 nm)和较宽的 pH 值范围(5-13)。该探针被成功用于检测三种不同土壤样品(腐殖土、沙土和黄土)中存在的肼。此外,探针 PKZ-IN 还被用于制备纳米纤维膜,以便通过手机平台对气态肼进行定性和定量检测。此外,PKZ-IN 还成功应用于生物体和植物成像中残留肼的检测。
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引用次数: 0
Phase conversion characteristics of lead sulfate in ferric sulfate medium 硫酸铅在硫酸铁介质中的相变特性
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-19 DOI: 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.
研究了硫酸(H2SO4)体系中硫酸铅(PbSO4)的相变特性,重点关注温度、H2SO4 浓度、铁(Fe3+)浓度、硫酸钠(Na2SO4)和硫酸钾(K2SO4)的影响。通过 XRD、SEM/BSE-EDS 和 FT-IR 表征固体产物的组成和结构,分析了 PbSO4 的转化情况。结果表明,温度对 PbSO4 转化的影响受 H2SO4 浓度的影响。当 H2SO4 浓度从 20 克/升降低到 5 克/升时,PbSO4 转化为硬玉铅(Pb-J)的温度阈值从 150℃降低到 90℃。在 150℃ 时,生成的金刚石数量从 86.04% 显著下降到 9.76%。随后,当 H2SO4 浓度超过 40 g/L 时,PbSO4 基本保持不变。同时,Pb-J 的形成与部分水合焦石棉(H-J)的形成相关。当溶液 pH 值约为 0.3 或更低时,酒石的生成受到抑制。此外,Fe3+ 浓度的增加促进了 Pb-J 的形成,而 Na2SO4 和 K2SO4 则抑制了 Pb-J 的形成,分别导致了钾金刚石(K-J)和钠金刚石(Na-J)的形成。该研究为硫化矿氧压浸出过程中 PbSO4 转化的调控提供了见解。
{"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}
引用次数: 0
How Rhodococcus ruber accelerated biodegradation of benzophenone-3 红葡萄球菌如何加速二苯甲酮-3 的生物降解
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-11-18 DOI: 10.1016/j.jhazmat.2024.136566
Fei Liu, Yue Ma, Wenxuan Li, Jue Cai, Haiyun Zhang, Fu Chen, Yongming Zhang, Bruce E. Rittmann
Benzophenone-3 (2-hydroxy-4-methoxybenzophenone, BP-3) poses risks to human health and natural ecosystems, and means to improve its biodegradation are necessary. When a small mass of Rhodococcus ruber, isolated from BP-3-acclimated biomass, was bioaugmented into the acclimated biomass, BP-3 removal was accelerated by 120%. The first step of BP-3 biodegradation generates either 2,5-dihydroxy-4-methoxybenzophenone (5-OH-BP-3) or benzophenone-1 (2,4-dihydoxybenzophenone, BP-1). BP-1 is generated by sequential demethylation, hydroxylation, and dehydrogenation reactions, while 5-OH-BP-3 is generated by one mono-oxygenation reaction. Of the two intermediates, 5-OH-BP-3 exhibited stronger inhibition than BP-1 or the original BP-3. Gene-completion mapping showed that R. ruber contains genes for demethylase, hydrolase, dehydrogenase, and mono-oxygenase reaction, which means that R. ruber could generate the less-toxic BP-1. Thus, bioaugmentation of R. ruber into BP-3-acclimated biomass eliminated the accumulation of 5-OH-BP-3 and, consequently, accelerated of BP-3 biodegradation via BP-1.
二苯甲酮-3(2-羟基-4-甲氧基二苯甲酮,BP-3)对人类健康和自然生态系统构成风险,因此有必要改善其生物降解。将从 BP-3 适应生物质中分离出的少量红球菌(Rhodococcus ruber)生物增殖到适应生物质中,BP-3 的去除速度加快了 120%。BP-3 生物降解的第一步是生成 2,5-二羟基-4-甲氧基二苯甲酮(5-OH-BP-3)或二苯甲酮-1(2,4-二羟基二苯甲酮,BP-1)。BP-1 是通过连续的脱甲基、羟基和脱氢反应生成的,而 5-OH-BP-3 则是通过一个单氧反应生成的。在这两种中间产物中,5-OH-BP-3 比 BP-1 或原始 BP-3 表现出更强的抑制作用。基因补全图谱显示,R. ruber 含有去甲基化酶、水解酶、脱氢酶和单加氧酶反应的基因,这意味着 R. ruber 可以生成毒性较低的 BP-1。因此,将 R. ruber 生物增殖到 BP-3 适应的生物质中,可消除 5-OH-BP-3 的积累,从而通过 BP-1 加速 BP-3 的生物降解。
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引用次数: 0
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Journal of Hazardous Materials
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