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An in-situ biochar-enhanced anaerobic membrane bioreactor for swine wastewater treatment under various organic loading rates 原位生物炭强化厌氧膜生物反应器在不同有机负荷率下处理猪废水的方法
IF 5.9 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-05-23 DOI: 10.1016/j.jes.2024.05.020
Nianwen Chen , Xinbo Zhang , Qing Du , Huizhong Wang , Zhiwen Wang , Junzhi Ren , Hongxia Li , Wenshan Guo , Huu Hao Ngo

A biochar-assisted anaerobic membrane bioreactor (BC-AnMBR) was conducted to evaluate the performance in treating swine wastewater with different organic loading rates (OLR) ranging from 0.38 to 1.13 kg-COD/(m3.d). Results indicated that adding spent coffee grounds biochar (SCG-BC) improved the organic removal efficiency compared to the conventional AnMBR, with an overall COD removal rate of > 95.01%. Meanwhile, methane production of up to 0.22 LCH4/gCOD with an improvement of 45.45% was achieved under a high OLR of 1.13 kg-COD/(m3.d). Furthermore, the transmembrane pressure (TMP) in the BC-AnMBR system was stable at 4.5 kPa, and no irreversible membrane fouling occurred within 125 days. Microbial community analysis revealed that the addition of SCG-BC increased the relative abundance of autotrophic methanogenic archaea, particularly Methanosarcina (from 0.11% to 11.16%) and Methanothrix (from 16.34% to 24.05%). More importantly, Desulfobacterota and Firmicutes phylum with direct interspecific electron transfer (DIET) capabilities were also enriched with autotrophic methanogens. Analysis of the electron transfer pathway showed that the concentration of c-type cytochromes increased by 38.60% in the presence of SCG-BC, and thus facilitated the establishment of DIET and maintained high activity of the electron transfer system even at high OLR. In short, the BC-AnMBR system performs well under various OLR conditions and is stable in the recovery energy system for swine wastewater.

研究人员对生物炭辅助厌氧膜生物反应器(BC-AnMBR)处理不同有机负荷率(OLR)(0.38 至 1.13 kg-COD/(m3.d))猪场废水的性能进行了评估。结果表明,与传统的 AnMBR 相比,添加废咖啡渣生物炭(SCG-BC)提高了有机物去除效率,总体 COD 去除率为 95.01%。同时,在 1.13 kg-COD/(m3.d) 的高 OLR 条件下,甲烷产量高达 0.22 LCH4/gCOD,提高了 45.45%。此外,BC-AnMBR 系统的跨膜压力(TMP)稳定在 4.5 kPa,并且在 125 天内没有发生不可逆的膜堵塞。微生物群落分析表明,添加 SCG-BC 增加了自养型甲烷古菌的相对丰度,尤其是 Methanosarcina(从 0.11% 增加到 11.16%)和 Methanothrix(从 16.34% 增加到 24.05%)。更重要的是,具有直接种间电子传递(DIET)能力的脱硫菌门(Desulfobacterota)和真菌门(Firmicutes)也富集了自养型甲烷菌。对电子传递途径的分析表明,在 SCG-BC 的存在下,c 型细胞色素的浓度增加了 38.60%,从而促进了 DIET 的建立,即使在高 OLR 下也能保持电子传递系统的高活性。总之,BC-AnMBR 系统在各种 OLR 条件下表现良好,在猪废水回收能源系统中具有稳定性。
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引用次数: 0
Assessing the effectiveness and mechanisms of Fe/PS, Fe/H2O2, and O3 treatment for water disinfection: Spotlight on VBNC bacteria 评估Fe/PS、Fe/H2O2和O3处理水消毒的效果和机制:聚焦 VBNC 细菌
2区 环境科学与生态学 Pub Date : 2024-05-22 DOI: 10.1016/j.jes.2024.05.023
Zheng Qi , Zaihui Huang , Chunguang Liu

Advanced oxidation processes (AOPs) exhibit significant potential for water disinfection due to their generation of large quantities of highly oxidizing free radicals. However, the neglect of viable but nonculturable (VBNC) cells obscures their true disinfection efficacy and potential environmental health risks. Therefore, the study evaluated the disinfection effectiveness and mechanisms of typical AOPs, including Fe/H2O2, Fe/persulfate (PS), and O3, from the perspective of the production of VBNC bacteria. The results indicate that Fe/PS exhibits the strongest bacterial inactivation rate (99.94%), and the cells lose their ability to reactivate. Fe/H2O2 and O3 induce more cells to enter the VBNC state compared to Fe/PS. Moreover, different AOPs result in varying levels of free radical production and utilization efficiency, with SO4•− and O3 exhibiting greater selectivity in deactivating bacteria compared to HO. The inhibition of VBNC bacteria production by Fe/PS treatment may be attributed to the combined action of HO and SO4•− on microorganisms, leading to oxidative stress and metabolic disruption in bacteria through the inhibition of biofilm formation and aminoacyl-tRNA biosynthesis (p < 0.05), thereby causing direct bacterial death rather than entry into the VBNC state. In contrast, Fe/H2O2 and O3 result in the upregulation of the metabolism of alanine, aspartate, and glutamate, as well as styrene degradation capacity by the bacteria, leading to the production of more VBNC bacteria. Overall, the study offers insights into mitigating potential biological risks in water disinfection and developing environmentally friendly and efficient disinfection technologies.

高级氧化工艺(AOPs)可产生大量高度氧化自由基,因此在水消毒方面具有巨大潜力。然而,由于忽略了可存活但不可培养的细胞(VBNC),因此掩盖了其真正的消毒功效和潜在的环境健康风险。因此,本研究从 VBNC 细菌产生的角度评估了典型 AOP 的消毒效果和机制,包括 Fe/H2O2、Fe/过硫酸盐(PS)和 O3。结果表明,Fe/PS 的细菌灭活率最高(99.94%),细胞失去了再活化能力。与 Fe/PS 相比,Fe/H2O2 和 O3 能诱导更多的细胞进入 VBNC 状态。此外,不同的 AOP 会导致不同程度的自由基产生和利用效率,与 HO- 相比,SO4- 和 O3 在使细菌失活方面表现出更大的选择性。Fe/PS 处理对 VBNC 细菌产生的抑制作用可能是由于 HO- 和 SO4- 对微生物的联合作用,通过抑制生物膜的形成和氨基酰-tRNA 的生物合成(p < 0.05),导致细菌氧化应激和代谢紊乱,从而直接导致细菌死亡,而不是进入 VBNC 状态。与此相反,Fe/H2O2 和 O3 会导致细菌的丙氨酸、天冬氨酸和谷氨酸代谢以及苯乙烯降解能力上调,从而产生更多的 VBNC 细菌。总之,这项研究为减轻水消毒中潜在的生物风险和开发环境友好型高效消毒技术提供了启示。
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引用次数: 0
Risk assessment of difenoconazole pollution in carp (Cyprinus carpio): Involvement of liver metabolism disorder and IP3R-Sig1R mediated mitochondrial Ca2+ overload 苯醚甲环唑污染鲤鱼的风险评估:肝脏代谢紊乱与 IP3R-Sig1R 介导的线粒体 Ca2+ 超载的关系
2区 环境科学与生态学 Pub Date : 2024-05-22 DOI: 10.1016/j.jes.2024.05.028
Feixue Liu , Tianmeng Zhang , Yeyun Ma , Jingquan Dong , Yong Sun

Environmental residues of the fungicide difenoconazole (DFZ) have been shown to pose a threat to mammals. However, the risk assessment of DFZ for cultured carp remains unclear. The aim of this study was to investigate the adverse effects of DFZ on carp liver and their molecular mechanisms by simulating the environmental contamination concentrations of DFZ. Our results showed that DFZ induced structural damage in the liver, including edema, vacuolation, and congestion. In addition, DFZ residues were detected in liver tissues. Mechanistically, DFZ causes mitochondrial dysfunction by promoting Ca2+ transfer from the endoplasmic reticulum (ER) to mitochondria via IP3R, leading to the onset of ROS burst and apoptosis, and the inhibition of Nrf2 antioxidant function by DFZ also results in uncontrolled ROS. Mitophagy was also activated intracellularly to counteract mitochondrial damage. Interestingly, treatment with 2-APB alleviated mitochondrial dysfunction, restored the mitochondrial membrane potential, and inhibited apoptosis by blocking the translocation of Ca2+ from the ER to the mitochondria. Metabolomic analysis revealed that DFZ disrupted energy metabolism in carp liver, whereas 2-APB reversed DFZ-induced metabolic alterations. In conclusion, the present study elucidates the threat of DFZ to carp liver and highlights the mechanism of damage, thereby helping to explain the impact of agriculture on the aquatic environment.

环境中残留的杀菌剂苯醚甲环唑(DFZ)已被证明会对哺乳动物造成威胁。然而,DFZ 对养殖鲤鱼的风险评估仍不明确。本研究旨在通过模拟 DFZ 的环境污染浓度,研究 DFZ 对鲤鱼肝脏的不良影响及其分子机制。结果表明,DFZ 会导致肝脏结构损伤,包括水肿、空泡化和充血。此外,在肝脏组织中还检测到了 DFZ 残留。从机理上讲,DFZ通过IP3R促进Ca2+从内质网(ER)转移到线粒体,从而引起线粒体功能障碍,导致ROS爆发和细胞凋亡,DFZ对Nrf2抗氧化功能的抑制也导致ROS失控。细胞内的丝裂噬也被激活,以对抗线粒体损伤。有趣的是,用 2-APB 处理可缓解线粒体功能障碍,恢复线粒体膜电位,并通过阻断 Ca2+ 从 ER 向线粒体的转运抑制细胞凋亡。代谢组学分析表明,DFZ 破坏了鲤鱼肝脏的能量代谢,而 2-APB 逆转了 DFZ 诱导的代谢改变。总之,本研究阐明了 DFZ 对鲤鱼肝脏的威胁,并强调了其损害机制,从而有助于解释农业对水生环境的影响。
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引用次数: 0
Plasmid-mediated transfer of antibiotic resistance genes and biofilm formation in a simulated drinking water distribution system under chlorine pressure 氯压力下模拟饮用水分配系统中质粒介导的抗生素耐药基因转移和生物膜的形成
2区 环境科学与生态学 Pub Date : 2024-05-22 DOI: 10.1016/j.jes.2024.05.021
Yexing Wang , Yingyu Zhang , Xiuneng Zhu , Yulin Tang , Yongji Zhang

The effects of disinfectants and plasmid-based antibiotic resistance genes (ARGs) on the growth of microorganisms and the plasmid-mediated transfer of ARGs in the water and biofilm of the drinking water distribution system under simulated conditions were explored. The heterotrophic plate count of the water in reactors with 0.1 mg/L NaClO and NH2Cl was higher than in the control groups. There was no similar phenomenon in biofilm. In the water of reactors containing NaClO, the aphA and bla genes were lower than in the antibiotic resistant bacteria group, while both genes were higher in the water of reactors with NH2Cl than in the control group. Chloramine may promote the transfer of ARGs in the water phase. Both genes in the biofilm of the reactors containing chlorine were lower than the control group. Correlation analysis between ARGs and water quality parameters revealed that the copy numbers of the aphA gene were significantly positively correlated with the copy numbers of the bla gene in water and significantly negatively correlated in biofilm (p < 0.05). The results of the sequencing assay showed that bacteria in the biofilm, in the presence of disinfectant, were primarily Gram-negative. 1.0 mg/L chlorine decreased the diversity of the community in the biofilm. The relative abundance of some bacteria that may undergo transfer increased in the biofilm of the reactor containing 0.1 mg/L chlorine.

在模拟条件下,探讨了消毒剂和基于质粒的抗生素耐药基因(ARGs)对饮用水输配系统水和生物膜中微生物生长和质粒介导的 ARGs 转移的影响。在加入 0.1 mg/L NaClO 和 NH2Cl 的反应器中,水中的异养菌板计数高于对照组。生物膜中没有类似现象。在含有 NaClO 的反应器中,phA 和 bla 基因的含量低于抗生素耐药菌组,而在含有 NH2Cl 的反应器中,这两种基因的含量均高于对照组。氯胺可能会促进 ARGs 在水相中的转移。含氯反应器生物膜中的这两种基因均低于对照组。ARGs 与水质参数的相关性分析表明,水中 aphA 基因的拷贝数与 bla 基因的拷贝数呈显著正相关,而在生物膜中则呈显著负相关(p <0.05)。测序分析结果表明,在有消毒剂存在的情况下,生物膜中的细菌主要是革兰氏阴性菌。1.0 毫克/升氯降低了生物膜中群落的多样性。在含 0.1 毫克/升氯的反应器生物膜中,一些可能发生转移的细菌的相对丰度有所增加。
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引用次数: 0
Diversity and dynamic response of anaerobic ammonia oxidation granular sludge 厌氧氨氧化颗粒污泥的多样性和动态响应
2区 环境科学与生态学 Pub Date : 2024-05-19 DOI: 10.1016/j.jes.2024.05.016
Jiahong Ye , Xiang Li , Yan Yuan , Yayi Wang , Yong Huang , Jun Ma , Han Wang , Pengze Dang , Pei-ling Xu

Red anaerobic ammonia oxidation (Anammox) granular sludge (AnGS) has been reported in successfully operating Anammox systems, and its color is associated with sludge activity. However, in long-term operating systems, AnGS exhibits different sensory colors, physical structures, community structures, and denitrification performance, but the relationship between them has not yet been elucidated. The AnGS of the Anammox system, which has been in operation for more than a decade, can be divided into two main categories: red and white. The specific Anammox activity (SAA) in conventional red AnGS increased continuously as the particle size increased from <0.51 mm to 6.02 ± 0.84 mm. The SAA of white AnGS were slightly lower than those of red AnGS with similarly-size granules but significantly higher than AnGS with smaller red granules. Compared with red AnGS, the extracellular polymeric substances of white AnGS were significantly reduced, mainly due to the higher intracellular iron content, resulting in lower heme c concentration. Thus, heme c may prove not to be an evaluative tool for measuring Anammox activity. Red and white AnGS, whether through self-aggregation or adsorption by hydroxyl apatite and other carriers, will face the fate of internal voids during particle size growth. White AnGS exhibited a more complex microbial community than red AnGS. Candidatus Brocadia was abundant in red AnGS and the abundance increased with increasing granule size. Candidatus Kuenenia and Candidatus Jettenia made significant contributions to denitrification in white AnGS. This study provides a new perspective on particle selection for anammox engineering applications.

据报道,在成功运行的厌氧氨氧化(Anammox)系统中,颗粒污泥(AnGS)呈红色,其颜色与污泥活性有关。然而,在长期运行的系统中,颗粒污泥的感官颜色、物理结构、群落结构和反硝化性能各不相同,但它们之间的关系尚未阐明。运行了十多年的 Anammox 系统的 AnGS 可分为两大类:红色和白色。传统红色 AnGS 的特定 Anammox 活性(SAA)随着粒径从 0.51 毫米增加到 6.02 ± 0.84 毫米而持续增加。白色 AnGS 的 SAA 略低于颗粒大小相似的红色 AnGS,但明显高于红色颗粒较小的 AnGS。与红色 AnGS 相比,白色 AnGS 的细胞外聚合物质明显减少,这主要是由于细胞内铁含量较高,导致血红素 c 浓度较低。因此,血红素 c 可能并不是衡量 Anammox 活性的评价工具。红色和白色 AnGS,无论是通过自我聚集还是被羟基磷灰石和其他载体吸附,在粒径增长过程中都将面临内部空隙的命运。与红色 AnGS 相比,白色 AnGS 的微生物群落更为复杂。 红色 AnGS 中含有大量的 Candidatus Brocadia,其数量随着颗粒大小的增加而增加。这项研究为选择颗粒进行anammox工程应用提供了一个新的视角。
{"title":"Diversity and dynamic response of anaerobic ammonia oxidation granular sludge","authors":"Jiahong Ye ,&nbsp;Xiang Li ,&nbsp;Yan Yuan ,&nbsp;Yayi Wang ,&nbsp;Yong Huang ,&nbsp;Jun Ma ,&nbsp;Han Wang ,&nbsp;Pengze Dang ,&nbsp;Pei-ling Xu","doi":"10.1016/j.jes.2024.05.016","DOIUrl":"https://doi.org/10.1016/j.jes.2024.05.016","url":null,"abstract":"<div><p>Red anaerobic ammonia oxidation (Anammox) granular sludge (AnGS) has been reported in successfully operating Anammox systems, and its color is associated with sludge activity. However, in long-term operating systems, AnGS exhibits different sensory colors, physical structures, community structures, and denitrification performance, but the relationship between them has not yet been elucidated. The AnGS of the Anammox system, which has been in operation for more than a decade, can be divided into two main categories: red and white. The specific Anammox activity (SAA) in conventional red AnGS increased continuously as the particle size increased from &lt;0.51 mm to 6.02 ± 0.84 mm. The SAA of white AnGS were slightly lower than those of red AnGS with similarly-size granules but significantly higher than AnGS with smaller red granules. Compared with red AnGS, the extracellular polymeric substances of white AnGS were significantly reduced, mainly due to the higher intracellular iron content, resulting in lower heme c concentration. Thus, heme c may prove not to be an evaluative tool for measuring Anammox activity. Red and white AnGS, whether through self-aggregation or adsorption by hydroxyl apatite and other carriers, will face the fate of internal voids during particle size growth. White AnGS exhibited a more complex microbial community than red AnGS. <em>Candidatus Brocadia</em> was abundant in red AnGS and the abundance increased with increasing granule size. <em>Candidatus Kuenenia</em> and <em>Candidatus Jettenia</em> made significant contributions to denitrification in white AnGS. This study provides a new perspective on particle selection for anammox engineering applications.</p></div>","PeriodicalId":15788,"journal":{"name":"Journal of Environmental Sciences-china","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-05-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141084586","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"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
Asymmetric oxygen vacancy promotes CO-SCR performance on defect-engineered Rh/CeCuOx catalyst 不对称氧空位促进了缺陷工程 Rh/CeCuOx 催化剂的 CO-SCR 性能
2区 环境科学与生态学 Pub Date : 2024-05-18 DOI: 10.1016/j.jes.2024.05.002
Qian Wang , Xinyu Han , Kaiting Chen , Kaijie Liu , Xiangguang Yang , Yibo Zhang

Selective catalytic reduction of NOx with CO (CO-SCR) is a process that purifies both NO and CO pollutants through a catalytic reaction. Specifically, the cleavage of NO on the catalyst surface is crucial for promoting the reaction. During the reaction, the presence of oxygen vacancies can extract oxygen from NO, thereby facilitating the cleavage of NO on the catalyst surface. Thus, the formation of oxygen vacancies is key to accelerating the CO-SCR reaction, with different types of oxygen vacancies being more conducive to their generation. In this study, Rh/CeCuOx catalysts were synthesized using the co-crystallization and impregnation methods, and asymmetric oxygen vacancies were induced through hydrogen thermal treatment. This structural modification was aimed at regulating the behavior of NO on the catalyst surface. The Rh/Ce0.95Cu0.05Ox-H2 catalyst exhibited the best performance in CO-SCR, achieving above 90% NO conversion at 162 °C. Various characterization techniques showed that the H2 treatment effectively reduced some of the CuO and Rh2O3, creating asymmetric oxygen vacancies that accelerated the cleavage of NO on the catalyst surface, rather than forming difficult-to-decompose nitrates. This study offers a novel approach to constructing oxygen vacancies in new CO-SCR catalysts.

一氧化氮与一氧化碳的选择性催化还原(CO-SCR)是一种通过催化反应同时净化一氧化氮和一氧化碳污染物的工艺。具体来说,催化剂表面 NO 的裂解是促进反应的关键。在反应过程中,氧空位的存在可以从 NO 中提取氧气,从而促进催化剂表面 NO 的裂解。因此,氧空位的形成是加速 CO-SCR 反应的关键,不同类型的氧空位更有利于其生成。本研究采用共晶法和浸渍法合成了 Rh/CeCuOx 催化剂,并通过氢热处理诱导了不对称氧空位。这种结构改性旨在调节催化剂表面 NO 的行为。Rh/Ce0.95Cu0.05Ox-H2 催化剂在 CO-SCR 中表现出了最佳性能,在 162 °C 时实现了 90% 以上的 NO 转化率。各种表征技术表明,H2 处理有效地还原了部分 CuO 和 Rh2O3,产生了不对称氧空位,加速了催化剂表面 NO 的裂解,而不是形成难以分解的硝酸盐。这项研究为在新型 CO-SCR 催化剂中构建氧空位提供了一种新方法。
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引用次数: 0
Tailoring C-defect O-doping and n-π* transition awakened porous ultra-thin carbon nitride for efficient peroxymonosulfate activation: Performances and mechanism insight 定制 C 缺陷 O 掺杂和 n-π* 过渡唤醒多孔超薄氮化碳,实现高效过一硫酸盐活化:性能和机理洞察
2区 环境科学与生态学 Pub Date : 2024-05-17 DOI: 10.1016/j.jes.2024.05.012
Meng Tai , Guangbo Che , Tianyu Zhou , Honghui Teng , Chunbo Liu , Bo Hu

Integrating photocatalysis technology with peroxymonosulfate oxidation possesses huge potential for degrading stubborn pollutant. Herein, a porous ultra-thin carbon nitride with C-defect O-doping and advanced n-π* transition was customized by one-pot thermal-induced polymerization of molten urea assisted with paraformaldehyde. Via visible-light coupling peroxymonosulfate activation, the DCN-100 can completely photodegrade 2,4-dichlorophenol, and rate constant is 136.6 and 37.9 times that of CN and DCN-100 without peroxymonosulfate. The light-absorption of DCN-100 surpasses 550 nm, specific surface area rises from 45.03 to 98.58 m2/g, and charge behaviors are significantly improved. The effects of paraformaldehyde amount, PMS dosage, pH, 2,4-dichlorophenol concentration, different water-body, wavelength and recycling times on photodegradation performance were explored in detail. Via capture experiments, ESR, LC-MS, Fukui-function, TEXT toxicity assessment and DFT theoretical calculation, the main active substances, degradation pathway, intermediate toxicity and enhanced activity mechanism of DCN-100 were clarified. The research provides a cost-effective, high-efficiency and environmental-friendly photocatalysts to activate peroxymonosulfate for water remediating.

将光催化技术与过氧化单硫酸盐氧化技术相结合,在降解顽固污染物方面具有巨大潜力。本文通过熔融尿素与多聚甲醛的一锅热诱导聚合,定制了一种具有C缺陷O掺杂和高级n-π*转变的多孔超薄氮化碳。通过可见光耦合过氧单硫酸盐活化,DCN-100 可完全光降解 2,4-二氯苯酚,速率常数分别是无过氧单硫酸盐的 CN 和 DCN-100 的 136.6 倍和 37.9 倍。DCN-100 的光吸收波长超过 550 nm,比表面积从 45.03 m2/g 上升到 98.58 m2/g,电荷行为明显改善。详细探讨了多聚甲醛用量、PMS用量、pH值、2,4-二氯苯酚浓度、不同水体、波长和循环时间对光降解性能的影响。通过捕获实验、ESR、LC-MS、福井函数、TEXT毒性评估和DFT理论计算,阐明了DCN-100的主要活性物质、降解途径、中间毒性和活性增强机理。该研究为活化过硫酸盐进行水质修复提供了一种经济、高效、环保的光催化剂。
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引用次数: 0
Porphyrinic based hydrogen-bonded organic framework/TiO2 nanocomposites for efficient photocatalytic degradation of sulfadiazine 基于卟啉的氢键有机框架/二氧化钛纳米复合材料用于高效光催化降解磺胺嘧啶
2区 环境科学与生态学 Pub Date : 2024-05-17 DOI: 10.1016/j.jes.2024.05.015
Chunying Li , Yu Zhang , Mengfei Tian , Naveed Ahmad , Kaitao Jia , Zidan Luo , Bin Qiao , Jiabo Cheng , Chunjian Zhao

Porphyrinic hydrogen-bonded organic frameworks (porph-HOFs) have emerged as highly promising materials in the realm of photocatalysis due to their remarkable attributes, including low density, high surface area, efficient visible light absorption, and notable chemical stability. However, the rapid recombination of photogenerated charges remains a significant concern. In this work, a novel HOF-based photocatalyst, PFC-72/TiO2 was successfully designed with visible light response and high electron transfer capability. This involved bonding TiO2 nanoparticles to the PFC-72 framework synthesized using cobalt porphyrin as organic ligand and introducing bridging molecules 4-mercaptopyridine (4-PySH). Moreover, sulfadiazine (SDZ), a highly prevalent antibiotic, was effectively degraded from wastewater using PFC-72/TiO2. The high specific surface area of PFC-72 significantly improved the dispersion of TiO2 in PFC-72/TiO2, providing more active sites and improving the ability to adsorb SDZ. Characterizations and density functional theory analysis further confirmed that the photosensitization effect of porph-HOF extended the response range of TiO2 in PFC-72/TiO2 and reduced the recombination efficiency of photogenerated charges, consequently enhancing photocatalytic performance. Additionally, due to significantly improved robustness of PFC-72 and its axial coordination interaction with 4-PySH, PFC-72/TiO2 displayed excellent stability and recyclability. Consequently, optimized PFC-72/TiO2 exhibited a remarkable SDZ removal efficiency of 93.73% within 120 min, maintaining consistent photoactivity even after undergoing four cycles. Furthermore, intermediate products and degradation pathways were proposed based on UPLC-MS/MS.

卟啉氢键有机框架(porph-HOFs)因其低密度、高比表面积、高效吸收可见光和显著的化学稳定性等显著特性,已成为光催化领域极具前景的材料。然而,光生电荷的快速重组仍然是一个重大问题。在这项工作中,我们成功设计了一种新型的基于 HOF 的光催化剂 PFC-72/TiO2,它具有可见光响应和高电子转移能力。这包括将 TiO2 纳米颗粒与以卟啉钴为有机配体合成的 PFC-72 框架结合,并引入桥接分子 4-巯基吡啶 (4-PySH)。此外,PFC-72/TiO2 还能有效降解废水中的磺胺嘧啶(SDZ),这是一种非常普遍的抗生素。PFC-72 的高比表面积显著改善了 TiO2 在 PFC-72/TiO2 中的分散性,提供了更多的活性位点,提高了吸附 SDZ 的能力。表征和密度泛函理论分析进一步证实,porph-HOF 的光敏效应扩大了 PFC-72/TiO2 中 TiO2 的响应范围,降低了光生电荷的重组效率,从而提高了光催化性能。此外,由于 PFC-72 的稳健性及其与 4-PySH 的轴向配位相互作用得到明显改善,PFC-72/TiO2 显示出卓越的稳定性和可回收性。因此,优化后的 PFC-72/TiO2 在 120 分钟内对 SDZ 的去除率高达 93.73%,即使经过四次循环也能保持稳定的光活性。此外,还根据 UPLC-MS/MS 提出了中间产物和降解途径。
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引用次数: 0
Facile synthesis of boron-doped porous biochar as a metal-free adsorbent for efficient removal of aqueous tetracycline antibiotics 掺硼多孔生物炭的简易合成,作为无金属吸附剂高效去除水体中的四环素类抗生素
2区 环境科学与生态学 Pub Date : 2024-05-17 DOI: 10.1016/j.jes.2024.04.044
Lu Xu , Yuetong Qi , Shaolei He , Chengzhi Wang , Xin Jin , Qize Wang , Kai Wang , Pengkang Jin

This study introduced a microwave-assisted pyrolysis method for the rapid and efficient preparation of boron-doped porous biochar. The resulting biochar exhibited a large specific surface area (933.39 m2/g), a rich porous structure (1.044 cm3/g), and abundant active sites. Consequently, the prepared boron-doped porous biochar exhibited higher efficiency in adsorbing tetracycline with a maximum adsorption capacity of 413.223 mg/g, which significantly exceeded that of unmodified biochar and most commercial and reported adsorbents. The correlation analysis between the adsorption capacity and adsorbent characteristics revealed that the formation of the –BCO2 group enhanced π–π electron donor–acceptor interactions between boron-doped porous biochar and tetracycline. This mechanism mainly contributed to the enhanced adsorption of tetracycline by boron-doped porous biochar. Additionally, the as-prepared boron-doped porous biochar exhibited broad applications in removing antibiotics (tetracycline), phenolics (bisphenol A), and dyes (methylene blue and rhodamine B). Moreover, the boron-doped porous biochar exhibited satisfactory stability, and its adsorption capacity can be nearly completely regenerated through simple heat treatment. This study provides new insights into the effectiveness of boron-doped carbonaceous materials in removing antibiotic contaminants.

本研究采用微波辅助热解方法快速高效地制备了掺硼多孔生物炭。制备出的生物炭具有较大的比表面积(933.39 m2/g)、丰富的多孔结构(1.044 cm3/g)和丰富的活性位点。因此,制备的掺硼多孔生物炭吸附四环素的效率更高,最大吸附容量为 413.223 mg/g,大大超过了未改性生物炭和大多数商业及报道的吸附剂。吸附容量与吸附剂特性之间的相关性分析表明,-BCO2 基团的形成增强了掺硼多孔生物炭与四环素之间的 π-π 电子供体-受体相互作用。这一机制是掺硼多孔生物炭吸附四环素能力增强的主要原因。此外,制备的掺硼多孔生物炭在去除抗生素(四环素)、酚类化合物(双酚 A)和染料(亚甲基蓝和罗丹明 B)方面具有广泛的应用前景。此外,掺硼多孔生物炭还表现出令人满意的稳定性,通过简单的热处理,其吸附能力几乎可以完全再生。这项研究为掺硼碳质材料去除抗生素污染物的有效性提供了新的见解。
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引用次数: 0
Lanthanum hydroxide showed best application potential in La-based materials based on its stable phosphate adsorption properties in complex water environments 氢氧化镧在复杂的水环境中具有稳定的磷酸盐吸附特性,显示出 La 基材料的最佳应用潜力
2区 环境科学与生态学 Pub Date : 2024-05-17 DOI: 10.1016/j.jes.2024.05.014
Linjuan Zhu , Yao Zhang , Shuo Xu , Baoyou Shi , Haotian Hao , Yili Wang

Three lanthanum morphology materials encompassing all lanthanum composites were synthesized by the direct precipitation method, and their phosphate adsorption order was determined as La2(CO3)3 > La(OH)3 > La2O3. Further comparison of the adsorption performance between La2(CO3)3 and La(OH)3 revealed that the former exhibited a twofold higher rate of adsorption compared to the latter. The presence of SO42−, HCO3, Mg2+, and HA in the water led to a decrease in the phosphate adsorption of La2(CO3)3 and La(OH)3, while Ca2+ enhances the adsorption of phosphoric acid by both materials. Compared to La2(CO3)3, La(OH)3 exhibited stronger resistance against coexisting ions. The pH was the limiting factor for phosphate adsorption in both cases, and their adsorption capacity decreased significantly as the pH increased. The phosphate adsorption mechanism of La2(CO3)3 was ligand exchange to form inner-sphere complexes, while the phosphate adsorption mechanism of La(OH)3 involved ligand exchange, inner-sphere complexation, and electrostatic attraction. The stability of La(OH)3 exhibited superior performance compared to that of La2(CO3)3 over 5 adsorption-desorption cycles. Although La2(CO3)3 had a higher initial phosphate adsorption capacity than La(OH)3, its phosphate adsorption capacity decreased by 40% after five adsorption-desorption cycles, while that of La(OH)3 decreased by 2.3%. Additionally, the amount of La(OH)3 adsorbed after five cycles was 25.6% higher than that of La2(CO3)3. Therefore, La(OH)3 performs better regeneration adsorption than La2(CO3)3. Furthermore, a smaller dosage of La(OH)3 was required compared to La2(CO3)3 in a test aimed at lowering the actual phosphate concentration in water to 0.5 mg/L. In summary, La(OH)3 is a more suitable substrate for cyclic adsorption for phosphorus removal than La2(CO3)3 and has better potential for practical application. In conclusion, La(OH)3 proves to be a more suitable substrate for cyclic adsorption in phosphorus removal compared to La2(CO3)3 and exhibits superior potential for practical application.

通过直接沉淀法合成了三种镧形态材料,包括所有镧复合材料,并确定了它们的磷酸盐吸附顺序为 La2(CO3)3 > La(OH)3 > La2O3。进一步比较 La2(CO3)3 和 La(OH)3 的吸附性能发现,前者的吸附率是后者的两倍。水中 SO42-、HCO3-、Mg2+ 和 HA 的存在导致 La2(CO3)3 和 La(OH)3 对磷酸盐的吸附量减少,而 Ca2+ 则增强了这两种材料对磷酸的吸附。与 La2(CO3)3 相比,La(OH)3 对共存离子的抗性更强。pH 值是这两种材料吸附磷酸盐的限制因素,随着 pH 值的升高,它们的吸附能力明显下降。La2(CO3)3 的磷酸盐吸附机理是配体交换形成内球络合物,而 La(OH)3 的磷酸盐吸附机理涉及配体交换、内球络合和静电吸引。与 La2(CO3)3 相比,La(OH)3 在 5 次吸附-解吸循环中表现出更高的稳定性。虽然 La2(CO3)3 的初始磷酸盐吸附容量高于 La(OH)3,但经过 5 次吸附-解吸循环后,其磷酸盐吸附容量下降了 40%,而 La(OH)3 则下降了 2.3%。此外,经过五个循环后,La(OH)3 的吸附量比 La2(CO3)3 高出 25.6%,因此,La(OH)3 的再生吸附性能优于 La2(CO3)3。此外,在一项旨在将水中实际磷酸盐浓度降至 0.5 mg/L 的试验中,与 La2(CO3)3 相比,La(OH)3 的用量更少。总之,与 La2(CO3)3 相比,La(OH)3 是一种更适合循环吸附除磷的基质,具有更好的实际应用潜力。总之,与 La2(CO3)3 相比,La(OH)3 被证明是一种更适合循环吸附除磷的基质,并具有更好的实际应用潜力。
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引用次数: 0
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Journal of Environmental Sciences-china
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