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Efficient degradation of F-53B as PFOS alternative in water by plasma discharge: Feasibility and mechanism insights 等离子放电法高效降解水中的全氟辛烷磺酸替代品 F-53B:可行性和机理研究
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-29 DOI: 10.1016/j.jhazmat.2024.135069
Han Zhang, Yinyin Zhang, Luxiang Zhu, Yanan Liu
The frequent detection of 6:2 chlorinated polyfluorinated ether sulfonate (F-53B) in various environments has raised concerns owing to its comparable or even higher environmental persistence and toxicity than perfluorooctane sulfonate (PFOS). This study investigated the plasma degradation of F-53B for the first time using a water film plasma discharge system. The results revealed that F-53B demonstrated a higher rate constant but similar defluorination compared to PFOS, which could be ascribed to the introduction of the chlorine atom. Successful elimination (94.8–100 %) was attained at F-53B initial concentrations between 0.5 and 10 mg/L, with energy yields varying from 15.1 to 84.5 mg/kWh. The mechanistic exploration suggested that the decomposition of F-53B mainly occurred at the gas-liquid interface, where it directly reacted with reactive species generated by gas discharge. F-53B degradation pathways involving dechlorination, desulfonation, carboxylation, C-O bond cleavage, and stepwise CF elimination were proposed based on the identified byproducts and theoretical calculations. Furthermore, the demonstrated effectiveness in removing F-53B in various coexisting ions and water matrices highlighted the robust anti-interference ability of the treatment process. These findings provide mechanistic insights into the plasma degradation of F-53B, showcasing the potential of plasma processes for eliminating PFAS alternatives in water.
由于 6:2 氯化多氟醚磺酸盐(F-53B)具有与全氟辛烷磺酸(PFOS)相当甚至更高的环境持久性和毒性,因此在各种环境中频繁检测到该物质引起了人们的关注。本研究首次使用水膜等离子体放电系统对 F-53B 的等离子体降解进行了研究。结果显示,与全氟辛烷磺酸相比,F-53B 的速率常数更高,但脱氟效果相似,这可能是由于引入了氯原子。F-53B 的初始浓度在 0.5 至 10 毫克/升之间时,可成功消除(94.8%-100%),能量产量在 15.1 至 84.5 毫克/千瓦时之间。机理探索表明,F-53B 的分解主要发生在气液界面,在此与气体放电产生的反应物直接反应。根据确定的副产物和理论计算,提出了 F-53B 的降解途径,包括脱氯、脱硫、羧化、C-O 键裂解和逐步消除 CF。此外,在去除各种共存离子和水基质中的 F-53B 时所表现出的有效性突显了该处理工艺强大的抗干扰能力。这些研究结果提供了等离子体降解 F-53B 的机理见解,展示了等离子体工艺消除水中全氟辛烷磺酸替代品的潜力。
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引用次数: 0
Endoplasmic reticulum stress response modulator OsbZIP39 regulates cadmium accumulation via activating the expression of defensin-like gene OsCAL2 in rice 内质网应激反应调节器 OsbZIP39 通过激活水稻防御素样基因 OsCAL2 的表达调控镉积累
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-28 DOI: 10.1016/j.jhazmat.2024.135007
Jian Li, Ling-Yan Wang, Huan-Chao Huang, Wu Yang, Guang-Yi Dai, Zhi-Qiang Fang, Jun-Liang Zhao, Kuai-Fei Xia, Xuan Zeng, Meng-Ling He, Nan Yao, Ming-Yong Zhang
Accumulation of cadmium (Cd) in rice is not only harmful to the growth of plants but also poses a threat to human health. Exposure to Cd triggers unfolded protein response (UPR) within cells, a process that is still not completely understood. The study demonstrated that the lack of OsbZIP39, an essential endoplasmic reticulum (ER)-resident regulator of the UPR, resulted in decreased Cd intake and reduced Cd levels in the roots, stems, and grains of rice. Upon exposure to Cd stress, GFP-OsbZIP39 translocated from ER to nucleus, initiating UPR. Further investigation revealed that Cd treatment caused changes in sphingolipid levels in the membrane, influencing the localization and activation of OsbZIP39. Yeast one-hybrid and dual-LUC assays were conducted to validate the interaction between activated OsbZIP39 and the promoter of the defensin-like gene , resulting in an increase in its expression. Different variations were identified in the coding region of , which may explain the varying levels of Cd accumulation observed in the and subspecies. Under Cd treatment, OsbZIP39 exhibited a more significant enhancement in the transcription of compared to OsbZIP39. Our data suggest that OsbZIP39 positively regulates Cd uptake in rice, offering an encouraging objective for the cultivation of low-Cd rice.
镉(Cd)在水稻中的积累不仅对植物的生长有害,也对人类健康构成威胁。暴露于镉会引发细胞内的未折叠蛋白反应(UPR),而这一过程至今仍未完全明了。研究表明,缺乏 OsbZIP39(一种 UPR 的重要内质网(ER)驻留调节因子)会导致水稻根、茎和谷粒中的镉摄入量减少和镉含量降低。暴露于镉胁迫时,GFP-OsbZIP39从ER转位到细胞核,启动了UPR。进一步研究发现,镉处理引起膜中鞘脂水平的变化,影响了OsbZIP39的定位和活化。酵母单杂交和双LUC实验验证了活化的OsbZIP39与防御素样基因启动子之间的相互作用,从而增加了防御素样基因的表达。在OsbZIP39的编码区发现了不同的变异,这可能解释了在和亚种中观察到的不同程度的镉积累。与 OsbZIP39 相比,在镉处理条件下,OsbZIP39 的转录增强更为显著。我们的数据表明,OsbZIP39 能积极调节水稻对镉的吸收,这为低镉水稻的栽培提供了一个令人鼓舞的目标。
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引用次数: 0
Exposure to zinc and dialkyldimethyl ammonium compound alters bacterial community structure and resistance gene levels in partial sulfur autotrophic denitrification coupled with the Anammox process 暴露于锌和二烷基二甲基铵化合物会改变部分硫自养反硝化和 Anammox 过程中的细菌群落结构和抗性基因水平
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-28 DOI: 10.1016/j.jhazmat.2024.135070
Yukun Yuan, Jingfeng Gao, Zhiqi Wang, Hongxin Xu, Liqin Zeng, Xiaoyu Fu, Yifan Zhao
Dialkyldimethyl ammonium compound (DADMAC) is widely used in daily life as a typical disinfectant and often co-exists with the heavy metal zinc in sewage environments. This study investigated the effects of co-exposure to zinc (1 mg/L) and DADMAC (0.2–5 mg/L) on the performance, bacterial community, and resistance genes (RGs) in a partial sulfur autotrophic denitrification coupled with anaerobic ammonium oxidation (PSAD-Anammox) system in a sequencing batch moving bed biofilm reactor for 150 days. Co-exposure to zinc and low concentration (0.2 mg/L) DADMAC did not affect the nitrogen removal ability of the PASD-Anammox system, but increased the abundance and transmission risk of free RGs in water. Co-exposure to zinc and medium-to-high (2–5 mg/L) DADMAC led to fluctuations in and inhibition of nitrogen removal, which might be related to the enrichment of heterotrophic denitrifying bacteria dominated by Co-exposure to zinc and high concentration DADMAC (5 mg/L) stimulated the secretion of extracellular polymeric substances and increased the proliferation risk of intracellular RGs in sludge. This study provided insights into the application of PSAD-Anammox system and the ecological risks of wastewater containing zinc and DADMAC.
二烷基二甲基铵化合物(DADMAC)作为一种典型的消毒剂被广泛应用于日常生活中,并经常与重金属锌共存于污水环境中。本研究调查了在一个序批式移动床生物膜反应器中,锌(1 毫克/升)和 DADMAC(0.2-5 毫克/升)共同暴露 150 天对部分硫自养反硝化耦合厌氧氨氧化(PSAD-Anammox)系统的性能、细菌群落和抗性基因(RGs)的影响。同时接触锌和低浓度(0.2 毫克/升)DADMAC 不会影响 PASD-Anammox 系统的脱氮能力,但会增加水中游离 RG 的丰度和传播风险。同时暴露于锌和中高浓度(2-5 mg/L)DADMAC 会导致脱氮能力的波动和抑制,这可能与以异养反硝化细菌为主的富集有关;同时暴露于锌和高浓度 DADMAC(5 mg/L)会刺激细胞外聚合物质的分泌,增加污泥中细胞内 RGs 的增殖风险。这项研究为 PSAD-Anammox 系统的应用以及含锌和 DADMAC 废水的生态风险提供了启示。
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引用次数: 0
Ancestral sequence reconstruction of the prokaryotic three-domain laccases for efficiently degrading polyethylene 高效降解聚乙烯的原核生物三维长酶的祖先序列重建
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-28 DOI: 10.1016/j.jhazmat.2024.135012
Bo Zeng, Yishan Fu, Jiacai Ye, Penghui Yang, Shixiu Cui, Wenxuan Qiu, Yangyang Li, Taoxu Wu, Haiyun Zhang, Yachan Wang, Guocheng Du, Song Liu
Biodegradation of polyethylene (PE) plastics is environmentally friendly. To obtain the laccases that can efficiently degrade PE plastics, we generated 9 ancestral laccases from 23 bacterial three-domain laccases through ancestral sequence reconstruction. The optimal temperatures of the ancestral laccases were between 60 °C-80 °C, while their optimal pHs were at 3.0 or 4.0. Without substrate pretreatment and mediator addition, all the ancestral laccases can degrade low-density polyethylene (LDPE) films at pH 7.0 and 60 °C. Among them, Anc52, which shared low sequence identity (18 %−41.7 %) with the reported PE-degrading laccases, was the most effective for LDPE degradation. After the catalytic reactions at 90 °C for 14 h, Anc52 (0.2 mg/mL) induced clear wrinkles and deep pits on the PE film surface detected by scanning electron microscope, and its carbonyl and hydroxyl indices reached 2.08 and 2.42, respectively. Then, we identified the residues 203 and 288 critical for PE degradation through site-directed mutation on Anc52. Moreover, Anc52 be activated by heat treatment (60 °C and 90 °C) at pH 7.0, which gave it a high catalytic efficiency (/= 191.73 mM·s) and thermal stability (half-life at 70 °C = 13.70 h). The ancestral laccases obtained here could be good candidates for PE biodegradation.
生物降解聚乙烯(PE)塑料对环境无害。为了获得能高效降解聚乙烯塑料的长链蛋白酶,我们通过祖先序列重建从23种细菌三域长链蛋白酶中生成了9种祖先长链蛋白酶。祖先裂解酶的最适温度为 60 ℃-80 ℃,最适 pH 值为 3.0 或 4.0。在不进行底物预处理和添加介质的情况下,所有祖先裂解酶都能在pH值为7.0和温度为60 ℃的条件下降解低密度聚乙烯(LDPE)薄膜。其中,与已报道的聚乙烯降解拉克酶序列相同度较低(18 %-41.7 %)的 Anc52 对低密度聚乙烯降解最有效。在90 ℃下催化反应14 h后,扫描电子显微镜检测到Anc52(0.2 mg/mL)在聚乙烯薄膜表面产生了明显的皱纹和深坑,其羰基指数和羟基指数分别达到了2.08和2.42。随后,我们通过对 Anc52 的定点突变确定了对 PE 降解起关键作用的残基 203 和 288。此外,在 pH 值为 7.0 的条件下,通过热处理(60 ℃ 和 90 ℃)激活 Anc52,使其具有较高的催化效率(/= 191.73 mM-s)和热稳定性(70 ℃ 时的半衰期=13.70 h)。在此获得的祖先漆酶可能是聚乙烯生物降解的良好候选物。
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引用次数: 0
Are eco-friendly “green” tires also chemically green? Comparing metals, rubbers and selected organic compounds in green and conventional tires 生态友好型 "绿色 "轮胎的化学成分也是绿色的吗?比较绿色轮胎和传统轮胎中的金属、橡胶和特定有机化合物
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-28 DOI: 10.1016/j.jhazmat.2024.135042
Elisabeth S. Rødland, Gilberto Binda, Davide Spanu, Stefano Carnati, Laura Röhler Bjerke, Luca Nizzetto
Tires are a major source of synthetic and natural rubber particles, metals and organic compounds, in which several compounds are linked to negative environmental impact. Recent advances in material technology, coupled with focus on sustainability, have introduced a new range of tires, sold as “green, sustainable, and eco-friendly”. Although these “green” tires may have lower impact on the environment on a global scale, there is no current knowledge about the chemical composition of “green” tires, and whether they are more eco-friendly when considering the release of tire wear particles or tire-associated chemicals. Here we have investigated the chemical composition of nine “green” vehicle tires, one “green” bike tire and seven “conventional” vehicle tires. No significant difference was found between “green” and “conventional” tires tested in this study. For N-(1,3-dimethylbutyl)-N'-phenyl-p-phenylenediamine (6PPD), the average concentration in “green” tires were higher (16 ± 7.8 µg/mg) compared to “conventional” tires (8.7 ± 4.5 µg/mg). The relationship between metals, selected organic compounds and rubbers demonstrated large variation across brands, and lower variability between tires grouped according to their seasonal use. This study indicates that more work is needed to understand how the shift towards sustainable tires might change the chemical composition of tires.
轮胎是合成和天然橡胶颗粒、金属和有机化合物的主要来源,其中有几种化合物与对环境的负面影响有关。最近,材料技术的进步加上对可持续发展的关注,推出了一系列新的轮胎,以 "绿色、可持续和生态友好 "的名义销售。虽然这些 "绿色 "轮胎对全球环境的影响可能较小,但目前还不了解 "绿色 "轮胎的化学成分,也不知道在考虑轮胎磨损颗粒或轮胎相关化学物质的释放时,它们是否更环保。在此,我们调查了 9 个 "绿色 "汽车轮胎、1 个 "绿色 "自行车轮胎和 7 个 "传统 "汽车轮胎的化学成分。本研究中测试的 "绿色 "轮胎和 "传统 "轮胎之间没有发现明显差异。就 N-(1,3-二甲基丁基)-N'-苯基对苯二胺(6PPD)而言,"绿色 "轮胎中的平均浓度(16 ± 7.8 µg/mg)高于 "传统 "轮胎(8.7 ± 4.5 µg/mg)。金属、特定有机化合物和橡胶之间的关系表明,不同品牌轮胎之间的差异很大,而根据季节性使用情况分组的轮胎之间的差异较小。这项研究表明,要了解向可持续轮胎的转变会如何改变轮胎的化学成分,还需要做更多的工作。
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引用次数: 0
Mixotrophic aerobic denitrification facilitated by denitrifying bacterial-fungal communities assisted with iron in micro-polluted water: Performance, metabolic activity, functional genes abundance, and community co-occurrence 微污染水体中铁辅助反硝化细菌-真菌群落促进的混养需氧反硝化:性能、代谢活动、功能基因丰度和群落共存性
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-27 DOI: 10.1016/j.jhazmat.2024.135057
Ben Ma, Mengting Chu, Haihan Zhang, Kaige Chen, Fengrui Li, Xiang Liu, Dmitry B. Kosolapov, Wei Zhi, Zhongbing Chen, Jun Yang, Ye Deng, Raju Sekar, Tao Liu, Xiaoyan Liu, Tinglin Huang
Low-dosage nitrate pollutants can contribute to eutrophication in surface water bodies, such as lakes and reservoirs. This study employed assembled denitrifying bacterial-fungal communities as bio-denitrifiers, in combination with zero-valent iron (ZVI), to treat micro-polluted water. Immobilized bacterial-fungal mixed communities (IBFMC) reactors demonstrated their ability to reduce nitrate and organic carbon by over 43.2 % and 53.7 %, respectively. Compared to IBFMC reactors, IBFMC combined with ZVI (IBFMC@ZVI) reactors exhibited enhanced removal efficiencies for nitrate and organic carbon, reaching the highest of 31.55 % and 17.66 %, respectively. The presence of ZVI in the IBFMC@ZVI reactors stimulated various aspects of microbial activity, including the metabolic processes, electron transfer system activities, abundance of functional genes and enzymes, and diversity and richness of microbial communities. The contents of adenosine triphosphate and electron transfer system activities enhanced more than 5.6 and 1.43 folds in the IBFMC@ZVI reactors compared with IBFMC reactors. Furthermore, significant improvement of crucial genes and enzyme denitrification chains was observed in the IBFMC@ZVI reactors. Iron played a central role in enhancing microbial diversity and activity, and promoting the supply, and transfer of inorganic electron donors. This study presents an innovative approach for applying denitrifying bacterial-fungal communities combined with iron enhancing efficient denitrification in micro-polluted water.
低剂量硝酸盐污染物会导致湖泊和水库等地表水体富营养化。这项研究利用组装的反硝化细菌-真菌群落作为生物反硝化剂,并结合零价铁(ZVI)来处理微污染水体。固定化细菌-真菌混合群落(IBFMC)反应器证明了其降低硝酸盐和有机碳的能力,降低幅度分别超过 43.2% 和 53.7%。与 IBFMC 反应器相比,IBFMC 与 ZVI(IBFMC@ZVI)相结合的反应器对硝酸盐和有机碳的去除率更高,最高分别达到 31.55 % 和 17.66 %。IBFMC@ZVI 反应器中 ZVI 的存在刺激了微生物活动的各个方面,包括代谢过程、电子传递系统活动、功能基因和酶的丰度以及微生物群落的多样性和丰富度。与 IBFMC 反应器相比,IBFMC@ZVI 反应器中的三磷酸腺苷含量和电子传递系统活性分别提高了 5.6 倍和 1.43 倍以上。此外,在 IBFMC@ZVI 反应器中还观察到关键基因和酶反硝化链的明显改善。铁在提高微生物多样性和活性、促进无机电子供体的供应和转移方面发挥了核心作用。这项研究提出了一种创新方法,将反硝化细菌-真菌群落与铁结合起来,提高微污染水体的反硝化效率。
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引用次数: 0
Optimal biochar selection for cadmium pollution remediation in Chinese agricultural soils via optimized machine learning 通过优化机器学习为中国农业土壤镉污染修复优化生物炭选择
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-27 DOI: 10.1016/j.jhazmat.2024.135065
Zhaolin Du, Xuan Sun, Shunan Zheng, Shunyang Wang, Lina Wu, Yi An, Yongming Luo
Biochar is effective in mitigating heavy metal pollution, and cadmium (Cd) is the primary pollutant in agricultural fields. However, traditional trial-and-error methods for determining the optimal biochar remediation efficiency are time-consuming and inefficient because of the varied soil, biochar, and Cd pollution conditions. This study employed the machine learning method to predict the Cd immobilization efficiency of biochar in soil. The predictive accuracy of the random forest (RF) model was superior to that of the other common linear and nonlinear models. Furthermore, to improve the reliability and accuracy of the RF model, it was optimized by employing a root-mean-squared-error-based trial-and-error approach. With the aid of the optimized model, the empirical categories for soil Cd immobilization efficiency were biochar properties (60.96 %) > experimental conditions (19.6 %) ≈ soil properties (19.44 %). Finally, this study identified the optimal biochar properties for enhancing agricultural soil Cd remediation in different regions of China, which was beneficial for decision-making regarding nationwide agricultural soil remediation using biochar. The immobilization effect of alkaline biochar was pronounced in acidic soils with relatively high organic matter. This study provides insights into the immobilization mechanism and an approach for biochar selection for Cd immobilization in agricultural soil.
生物炭能有效缓解重金属污染,而镉(Cd)是农田中的主要污染物。然而,由于土壤、生物炭和镉污染条件各不相同,传统的试错法确定最佳生物炭修复效率既费时又低效。本研究采用机器学习方法预测生物炭在土壤中的镉固定效率。随机森林(RF)模型的预测精度优于其他常见的线性和非线性模型。此外,为了提高随机森林模型的可靠性和准确性,还采用了基于均方根误差的试错法对其进行了优化。在优化模型的帮助下,土壤镉固定效率的经验分类为生物炭特性(60.96 %)>实验条件(19.6 %)≈土壤特性(19.44 %)。最后,本研究确定了中国不同地区农田土壤镉修复的最佳生物炭性质,有利于全国范围内利用生物炭进行农田土壤修复的决策。在有机质相对较高的酸性土壤中,碱性生物炭的固定化效果明显。该研究为农业土壤中镉的固定化机制和生物炭的选择提供了启示。
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引用次数: 0
Development and standardization of spectrophotometric assay for quantification of thermal hydrolysis-origin melanoidins and its implication in antioxidant activity evaluation 开发和标准化分光光度法,用于定量分析热水解产生的黑色素及其在抗氧化活性评估中的作用
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-27 DOI: 10.1016/j.jhazmat.2024.135021
Yingying Li, Siwei Xiao, Qian Zhang, Nan Wang, Qing Yang, Jiuxiao Hao
Melanoidins are brown recalcitrant polymers originating from the thermal hydrolysis pretreatment (THP) of organic solid waste (OSW). Owing to their various formation pathways and complex structures, there is currently no reliable method to quantify melanoidins. In this study, a spectrophotometric method was developed to determine melanoidins concentration in different OSW. Three typical model Maillard reaction systems (glucose-glycine, glucose/fructose-20 amino acids, and dextran-bovine serum albumin) were used to acquire the characteristic peaks and establish standard curves. The results showed that a standard curve using glucose/fructose-20 amino acids model melanoidins at 280 nm was the optimal quantification method, because it had the best correlation with the physicochemical indicators of melanoidins and semi-quantification results calculated by excitation-emission matrix fluorescence. In addition, the applicability of the proposed method was evaluated using multiple real melanoidins samples extracted from thermally pretreated OSW under different THP conditions and food-derived melanoidins as well, demonstrating its validity and advantages. This study is the first to provide a simple, effective, and accurate method for quantifying THP-origin melanoidins from different sources. Remarkably, as a specific and important application scenario, the proposed quantification method was employed to investigate the concentration dependence of melanoidins antioxidation in thermally pretreated OSW.
类黑色素是有机固体废物(OSW)热水解预处理(THP)过程中产生的棕色难降解聚合物。由于其形成途径多样且结构复杂,目前尚无可靠的方法对类黑色素进行定量。本研究采用分光光度法测定了不同有机固体废物中的类黑色素的浓度。采用三种典型的 Maillard 反应体系(葡萄糖-甘氨酸、葡萄糖/果糖-20 氨基酸和葡聚糖-牛血清白蛋白)获取特征峰并建立标准曲线。结果表明,以葡萄糖/果糖-20 氨基酸为模型的标准曲线在 280 nm 波长处与黑色素的理化指标和激发-发射矩阵荧光计算的半定量结果的相关性最好,因此是最佳的定量方法。此外,研究人员还利用从不同 THP 条件下经热预处理的 OSW 提取的多个真实类黑色素样品以及从食品中提取的类黑色素样品对所提方法的适用性进行了评估,证明了该方法的有效性和优势。该研究首次提供了一种简单、有效、准确的方法,用于量化不同来源的 THP 源类黑色素。值得注意的是,作为一个具体而重要的应用场景,所提出的定量方法还被用于研究热预处理 OSW 中类黄酮抗氧化的浓度依赖性。
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引用次数: 0
Photo-induced protonation assisted nano primary battery for highly efficient immobilization of diverse heavy metal ions 光诱导质子化辅助纳米原电池用于高效固定各种重金属离子
IF 13.6 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-27 DOI: 10.1016/j.jhazmat.2024.135066
Hongjian Ge, Chaowen Chen, Sijia Li, Xinyue Guo, Jing Zhang, Pengqi Yang, Huan Xu, Jia Zhang, Zhengyan Wu
Highly-stable heavy metal ions (HMIs) appear long-term damage, while the existing remediation strategies struggle to effectively remove a variety of oppositely charged HMIs without releasing toxic substances. Here we construct an iron-copper primary battery-based nanocomposite, with photo-induced protonation effect, for effectively consolidating broad-spectrum HMIs. In FCPBN, Fe/Cu cell acts as the reaction impetus, and functional graphene oxide modified by carboxyl and UV-induced protonated 2-nitrobenzaldehyde serves as an auxiliary platform. Due to the groups and built-in electric fields under UV stimuli, FCPBN exhibits excellent affinity for ions, with a maximum adsorption rate constant of 974.26 g∙mg∙min and facilitated electrons transfer, assisting to reduce 9 HMIs including CrO, AsO, Cd in water from 0.03 to 3.89 ppb. The cost-efficiency, stability and collectability of the FCPBN during remediation, and the beneficial effects on polluted soil and the beings further demonstrate the splendid remediation performance without secondary pollution. This work is expected to remove multi-HMIs thoroughly and sustainably, which tackles an environmental application challenge.
高度稳定的重金属离子(HMIs)会造成长期损害,而现有的修复策略难以在不释放有毒物质的情况下有效去除各种带相反电荷的 HMIs。在此,我们构建了一种具有光诱导质子化效应的铁铜原电池基纳米复合材料,可有效固化广谱重金属离子。在 FCPBN 中,铁/铜电池是反应的动力,羧基修饰的功能性氧化石墨烯和紫外线诱导的质子化 2-硝基苯甲醛是辅助平台。在紫外光刺激下,由于基团和内置电场的作用,FCPBN 对离子表现出极佳的亲和力,最大吸附速率常数为 974.26 g∙mg∙min 并促进电子转移,可将水中的 CrO、AsO、Cd 等 9 种 HMIs 从 0.03 ppb 降至 3.89 ppb。FCPBN 在修复过程中的成本效益、稳定性和可收集性,以及对污染土壤和生物的有益影响,进一步证明了其出色的修复性能,且不会造成二次污染。这项工作有望彻底、可持续地去除多种 HMIs,从而解决环境应用难题。
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引用次数: 0
The reactivity of organic radicals in the performic, peracetic, perpropionic acids-based advanced oxidation process: A case study of sulfamethoxazole 以执行酸、过乙酸和过丙酸为基础的高级氧化过程中有机自由基的反应性:磺胺甲噁唑案例研究
IF 12.2 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL Pub Date : 2024-06-27 DOI: 10.1016/j.jhazmat.2024.135033
Siqi Deng , Zhengqiang Yang , Xinyi Yu , Mingxue Li , Haijie Cao

Advanced oxidation processes (AOPs) based on peracetic acid (PAA) displayed great potential in removing emerging contaminants by generating HO and organic radicals. Performic and perpropionic acids (PFA and PPA) also act as disinfectants, but their application potential has not been investigated yet. Here, we investigated the degradation mechanism and kinetics of sulfamethoxazole (SMX) by HO, RC(O)O species (including HC(O)O, CH3C(O)O and CH3CH2C(O)O) and RC(O)OO species (including HC(O)OO, CH3C(O)OO and CH3CH2C(O)OO). The results show that the calculated reaction rate constants of SMX follow the order of HC(O)O > CH3C(O)O > CH3CH2C(O)O > HO > HC(O)OO > CH3C(O)OO > CH3CH2C(O)OO. The reactivity towards SMX is strongly correlated with the redox potentials of reactive radicals. Hence, the RCOO species play dominant roles in the purification of SMX in PFA/PAA/PPA-based AOPs. The degradation of SMX mainly proceeds via addition at the benzene ring, the hydrogen abstraction from the -NH2 group as well as the single electron transfer reaction. This study highlights the fundamental aspects of PFA, PAA, and PPA in the purification of sulfamethoxazole and enhances the role of organic radicals in the AOPs based on organic peracetic acids.

基于过乙酸(PAA)的高级氧化工艺(AOPs)通过产生 HO 和有机自由基,在去除新出现的污染物方面显示出巨大的潜力。过甲酸和过丙酸(PFA 和 PPA)也可作为消毒剂,但其应用潜力尚未得到研究。在此,我们研究了 HO、RC(O)O 物种(包括 HC(O)O、CHC(O)O 和 CHCHC(O)O)和 RC(O)OO 物种(包括 HC(O)OO、CHC(O)OO 和 CHCHC(O)OO)对磺胺甲噁唑(SMX)的降解机理和动力学。结果表明,SMX 的计算反应速率常数遵循 HC(O)O > CHC(O)O > CHCHC(O)O > HO > HC(O)OO > CHC(O)OO > CHCHC(O)OO 的顺序。对 SMX 的反应性与活性自由基的氧化还原电位密切相关。因此,在基于 PFA/PAA/PPA 的 AOPs 中,RCOO 物种在净化 SMX 的过程中起着主导作用。SMX 的降解主要通过苯环上的加成反应、-NH 基团的氢抽取反应以及单电子转移反应进行。这项研究强调了 PFA、PAA 和 PPA 在磺胺甲噁唑纯化过程中的基本作用,并增强了有机自由基在基于有机过乙酸的 AOPs 中的作用。
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Journal of Hazardous Materials
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