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Long-term straw removal and double-cropping system reduce soil cadmium content and uptake in rice: A four-year field analysis 长期清除稻草和双季稻制可降低土壤中的镉含量和水稻对镉的吸收:为期四年的实地分析
2区 环境科学与生态学 Pub Date : 2024-06-06 DOI: 10.1016/j.jes.2024.05.050
Beibei Tian, Yihao Yang, Anwei Chen, Liang Peng, Xiao Deng, Yang Yang, Qingru Zeng, Si Luo

Several studies have demonstrated that reintroducing crop straw to fields may intensify cadmium (Cd) contamination in agricultural soils. However, the specific effects of long-term straw management practices on Cd concentration and its bioavailability in soil-rice ecosystems remain unclear. In this context, to explore the influence of straw return (SR) and straw removal (NSR) on Cd accumulation in both soil and rice within a double-cropping system, we conducted a four-year field study. Our research study unveiled that NSR consistently decreased soil Cd concentration and its bioavailability by approximately 16.93%–27.30% and 8.23%–21.05% respectively across both study sites. Conversely, SR resulted in a substantial increase in soil Cd bioavailability, ranging from 38.64%–53.95%. Notably, compared to NSR, SR significantly increased total soil Cd by 5.47%–36.58% and increased Cd content in brown rice by 8.00%–100.24%. Remarkably, after four consecutive years of NSR, brown rice Cd concentration at the Changfeng site compiled with national safety standards (GB 2762–2022). Additionally, returning early rice straw significantly raised soil Cd bioavailability for the subsequent crop, more so than late rice straw did for the early rice the following year. The findings suggest that traditional double-cropping cultivation with straw removal can effectively mitigate Cd contamination risks in crops and farmland in Hunan Province.

多项研究表明,将农作物秸秆还田可能会加剧农业土壤中的镉(Cd)污染。然而,长期秸秆管理方法对土壤-水稻生态系统中镉浓度及其生物利用率的具体影响仍不清楚。在此背景下,为了探索秸秆还田(SR)和秸秆清除(NSR)对双季稻系统中土壤和水稻中镉积累的影响,我们开展了一项为期四年的田间研究。研究结果表明,在两个研究地点,秸秆还田持续降低了土壤中的镉浓度及其生物利用率,降幅分别约为 16.93%-27.30% 和 8.23%-21.05% 。相反,SR 则使土壤中镉的生物利用率大幅提高,范围从 38.64% 到 53.95%。值得注意的是,与 NSR 相比,SR 使土壤总镉显著增加了 5.47%-36.58%,使糙米中的镉含量增加了 8.00%-100.24%。值得注意的是,经过连续四年的 NSR 后,长丰基地的糙米镉浓度符合国家安全标准(GB 2762-2022)。此外,早稻秸秆还田显著提高了后茬作物的土壤镉生物利用率,比晚稻秸秆还田对第二年早稻的影响更大。研究结果表明,湖南省传统的双季稻种植与秸秆还田可有效降低农作物和农田的镉污染风险。
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引用次数: 0
Molecular biological mechanism of fillers with surface micro-electric field to enhance biodegradation of kitchen-oil wastewater 表面微电场填料促进厨房油污水生物降解的分子生物学机理
2区 环境科学与生态学 Pub Date : 2024-06-06 DOI: 10.1016/j.jes.2024.05.051
Tong Ren, Han Zhang , Chun Hu

The kitchen-oil wastewater is characterized by a high concentration of organic matter, complex composition and refractory pollutants, which make wastewater treatment more difficult. Based on the study of using micro-electric field characteristic catalyst HCLL-S8-M to enhance the electron transfer between microorganisms in kitchen-oil wastewater which further improved the COD removal rate, we focus on the microbial community, intracellular metabolism and extracellular respiration, and make an in-depth analysis of the molecular biological mechanisms to microbial treatment in wastewater. It is found that electroactive microorganisms are enriched on the material surface, and the expression levels of cytochrome c and riboflavin genes related to electron transfer are up-regulated, confirming that the surface micro-electric field structure could enhance the electron transfer between microbial species and improve the efficiency of wastewater degradation. This study provides a new idea for the treatment of refractory organic wastewater.

厨油废水具有有机物浓度高、成分复杂、污染物难处理等特点,给废水处理增加了难度。在研究利用微电场特性催化剂 HCLL-S8-M 增强厨油废水中微生物间的电子传递,进一步提高 COD 去除率的基础上,重点研究了微生物群落、胞内代谢和胞外呼吸,深入分析了废水中微生物处理的分子生物学机理。研究发现,电活性微生物在材料表面富集,与电子传递相关的细胞色素 c 和核黄素基因表达水平上调,证实了表面微电场结构可增强微生物物种间的电子传递,提高废水降解效率。这项研究为难降解有机废水的处理提供了新思路。
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引用次数: 0
Mechanism of nano-scale zero-valent iron modified biochar for enhancing low-nitrogen anammox process resistance to low temperatures 纳米级零价铁改性生物炭增强低氮厌氧工艺耐低温性的机理
2区 环境科学与生态学 Pub Date : 2024-06-06 DOI: 10.1016/j.jes.2024.05.049
Wenjing Chen , Lijin Zhang , Zirui Liu , Wenru Liu , Bin Lu , Haitao Zhao

Two anaerobic ammonia oxidation (anammox) systems, one with adding nano-scale zero-valent iron modified biochar (nZVI@BC) and the other with adding biochar, were constructed to explore the feasibility of nZVI@BC for enhancing the resistance of low-nitrogen anammox processes to low temperatures. The results showed that the average nitrogen removal efficiency with nZVI@BC addition at low temperatures was maintained at about 80%, while that with biochar addition gradually decreased to 69.49%. The heme-c content of biomass with nZVI@BC was significantly higher by 36.60%-91.45%. Additional, nZVI@BC addition resulted in more extracellular polymeric substances, better biomass granulation, and a higher abundance of anammox bacteria. In particularly, anammox genes hzsA/B/C, hzo and hdh played a pivotal role in maintaining nitrogen removal performance at 15°C. These findings suggest that nZVI@BC has the potential to enhance the resistance of low-nitrogen anammox processes to low temperatures, making it a valuable approach for practical applications in low-nitrogen and low-temperature wastewater treatment.

构建了两个厌氧氨氧化(anammox)系统,一个是添加纳米级零价铁改性生物炭(nZVI@BC)的系统,另一个是添加生物炭的系统,以探索 nZVI@BC 增强低氮氨氧化过程耐低温能力的可行性。结果表明,在低温条件下,添加 nZVI@BC 的平均脱氮效率保持在 80% 左右,而添加生物炭的平均脱氮效率则逐渐下降至 69.49%。加入 nZVI@BC 后,生物质中的血红素-c 含量显著提高了 36.60%-91.45% 。此外,添加 nZVI@BC 后,细胞外高分子物质增多,生物质颗粒化效果更好,氨氧化细菌的数量也更多。特别是,anammox 基因 hzsA/B/C、hzo 和 hdh 在保持 15°C 脱氮性能方面发挥了关键作用。这些研究结果表明,nZVI@BC 有潜力提高低氮安默氧工艺对低温的耐受性,使其成为低氮、低温废水处理实际应用中的一种有价值的方法。
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引用次数: 0
The compounding effect of re-adsorptionon on bioaccessibility of methylmercury in rice-based infant cereals by vitro digestion assessment 通过体外消化评估再吸附对米基婴儿谷物中甲基汞生物可及性的复合效应
2区 环境科学与生态学 Pub Date : 2024-06-06 DOI: 10.1016/j.jes.2024.05.052
Xin Wang , Wenbin Cui , Yingjun Wang , Yanbin Li , Bo Meng , Genique Nicolas , Michael Ojeda , Yong Cai

Considerable levels of methylmercury (MeHg) have been found rice-based infant cereals as a result of MeHg transfer from the rice as a raw material to the products, hence consumption of rice products may pose a potential health risk to infants who may receive cereals as the major diets and are susceptible to toxicity of MeHg. Determination of bioaccessibility of MeHg would provide a more accurate assessment of MeHg exposure through consumption of rice-based cereals, yet this information remains lacking. Further, the re-adsorption of methylmercury on the residual food will affect the accurate assessment of its bioaccessibility. Our goals in this work were 1) to determine the bioaccessibility of MeHg in infant rice cereals commonly available on the market by using a typical in vitro artificial gastrointestinal digestion model and 2) to evaluate the effects of MeHg re-adsorption on the in vitro assessment of MeHg bioaccessibility. The determined bioaccessibility of MeHg in the studied rice cereals after the standard dual-step (using gastric followed by intestinal juice) protocol ranged from 25% to 74%, a wide range comparable to that of fish samples observed here and in previous studies. The surprisingly higher bioaccessibility of MeHg in fish and rice cereals after the gastric step only, in comparison to after the complete two-step gastrointestinal digestion, suggests the re-adsorption of MeHg on the residual food. Separate experiments with spiked MeHg standards confirmed that the MeHg released by the acetic gastric juice was re-adsorbed on the residues during the intestinal step at neutral pH. This study provided first-hand data on the bioaccessibility of MeHg in infant rice cereals and methodological implications on using in vitro digestion to evaluate the bioaccessibility of MeHg and metal contaminants in general.

以大米为原料的婴幼儿谷类食品中甲基汞的含量相当高,这是因为甲基汞从作为原料的大米转移到了谷类食品中。测定甲基汞的生物可吸收性,可以更准确地评估食用以大米为主要原料的谷类食品摄入甲基汞的情况。此外,甲基汞在残留食物中的再吸附也会影响对其生物可及性的准确评估。我们这项工作的目标是:1)采用典型的体外人工胃肠道消化模型,测定市场上常见的婴幼儿米谷类食品中甲基汞的生物可及性;2)评估甲基汞再吸附对体外评估甲基汞生物可及性的影响。经过标准的两步法(先用胃液,再用肠液)后,所研究的稻米谷物中甲基汞的生物可及性从 25% 到 74%不等,范围之广与本研究和以往研究中观察到的鱼类样本相当。与经过完整的两步胃肠消化法相比,仅经过胃部消化后,鱼类和大米谷物中的甲基汞生物利用率更高,这表明甲基汞在残留食物中被重新吸附。用添加的甲基汞标准物质进行的单独实验证实,在中性 pH 值下,乙酸胃液释放的甲基汞在肠道消化过程中被残留物再次吸附。这项研究提供了有关婴幼儿米谷类食物中甲基汞生物可及性的第一手数据,以及使用体外消化法评估甲基汞和一般金属污染物生物可及性的方法学意义。
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引用次数: 0
Plant secretions and volatiles contribute to the evolution of bacterial antibiotic resistance in soil-crop system 植物分泌物和挥发性物质促进了土壤-作物系统中细菌抗生素耐药性的进化
2区 环境科学与生态学 Pub Date : 2024-05-31 DOI: 10.1016/j.jes.2024.05.039
Houyu Li , Qifan Yang , Wei Liu , Ruolan Li , Dandan Zhang , Guilong Zhang , Yan Xu

The exponential growth of antibiotic-resistant bacteria and antibiotic-resistant genes (ARGs) in soil-crop systems in recent years has posed a great challenge to ecological security and human health. While many studies have documented the residues of ARGs in soils and crops, but little is known about who drives the proliferation of ARGs in farming systems and what their underlying mechanisms are. Herein, we explored the occurrence and proliferating behavior of ARGs in soil-crop environments in terms of root secretions and plant volatiles. This review highlighted that plant root secretions and volatile organic compounds (VOCs) served as key substances mediating the development of antibiotic resistance in the soil-crop system. Still, there is controversy here as to plant root secretions promote the ARGs proliferation or inhibit. Some studies indicated that root secretions can suppress the colonization of ARGs, mainly attributed by the production of blunted metabolic enzymes and blocking of cellular exocytosis systems. Whereas the others have evidenced that root secretions can promote ARGs proliferation, primarily by altering the structure of microbial communities to influence species interactions and thus indirectly affect the proliferation of ARGs. Also, VOCs can act as molecular signals to convey antibiotic resistance information to their neighbors, which in turn drive the up-regulation of ARGs expression. Even so, the mechanism by which VOC-driven antibiotic resistance acquisition and proliferation need to be further probed. Overall, this review contributed to the development of products and technologies to impede the ARGs proliferation in agricultural environment.

近年来,土壤-作物系统中的抗生素细菌和抗生素基因(ARGs)呈指数级增长,对生态安全和人类健康构成了巨大挑战。虽然许多研究都记录了土壤和作物中 ARGs 的残留情况,但对于谁在农业系统中推动了 ARGs 的扩散及其内在机制却知之甚少。在此,我们从根系分泌物和植物挥发物的角度探讨了土壤-作物环境中 ARGs 的发生和增殖行为。这篇综述强调,植物根系分泌物和挥发性有机化合物(VOCs)是介导土壤-作物系统中抗生素耐药性发展的关键物质。不过,对于植物根系分泌物是促进还是抑制 ARGs 的增殖还存在争议。一些研究表明,根系分泌物可抑制 ARGs 的定殖,主要原因是根系分泌物产生的代谢酶和细胞外渗系统受阻。而其他研究则证明,根系分泌物可以促进 ARGs 的增殖,主要是通过改变微生物群落结构来影响物种间的相互作用,从而间接影响 ARGs 的增殖。此外,挥发性有机化合物还可以作为分子信号,向邻近的微生物传递抗生素抗性信息,进而推动 ARGs 表达的上调。尽管如此,VOC 驱动抗生素耐药性获得和增殖的机制仍有待进一步探究。总之,本综述有助于开发相关产品和技术,以阻止 ARGs 在农业环境中的扩散。
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引用次数: 0
One-step hydrothermal synthesis of CQDs/TiO2/NH2-MIL-125 for efficient photocatalytic production of H2O2 under visible light 在可见光下一步水热合成 CQDs/TiO2/NH2-MIL-125 以高效光催化产生 H2O2
IF 5.9 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-05-31 DOI: 10.1016/j.jes.2024.05.034
Jianhui Shi, Kaikai Pu, Ting Zhao, Jiating Shi, Na Zheng, Lijun Nie, Kunkun Xue, Yuhang Gao

NH2-MIL-125 and its derivatives are receiving more attention in various aspects of photocatalytic reactions, especially in the photocatalytic hydrogen peroxide (H2O2) production from water (H2O) and oxygen (O2), which is a promising and sustainable strategy. However, the generation of H2O2 from NH2-MIL-125 is far from satisfactory due to rapid photo-generated carriers recombination and poor surface electron transfer. In the work, the composite photocatalyst CQDs/TiO2/NH2-MIL-125 (C/T/NM) was designed for the first time by one-step hydrothermal method. TiO2 was in situ converted from partial NH2-MIL-125 (NM) during the successful loaded of Carbon quantum dots (CQDs) by hydrothermal process. The results indicated the type Ⅱ heterojunction was successfully constructed between the NM and TiO2 interface, which could promote the transmission of photo-generated electrons. In addition, the successful loaded of CQDs could effectively transfer and stored the photo-generated electrons to the photocatalyst surface to participate in the reaction, and further avoiding the recombination of photo-generated carriers. The C/T/NM composite photocatalyst achieved a H2O2 generation of 455 µmol/L for 5 hours under visible light without oxygen bubbling, which was 7.1 times superior to that of NM. The H2O2 generation rate reached 645.4 µM/(g·h), which was in priority in the reported literature under the same conditions. Finally, based on the active species capture experiments, energy band structure analysis and the photoelectrochemical measurements, a possible mechanism for the efficient H2O2 generation through C/T/NM had been proposed. This work provided new ideas for designing NH2-MIL-125 based composite photocatalysts for the production of H2O2.

NH2-MIL-125 及其衍生物在光催化反应的各个方面都受到了越来越多的关注,尤其是以水(H2O)和氧(O2)为原料光催化产生过氧化氢(H2O2),这是一种前景广阔的可持续策略。然而,由于光生载流子快速重组和表面电子传递不畅,NH2-MIL-125 生成 H2O2 的效果并不理想。该研究首次采用一步水热法设计了复合光催化剂 CQDs/TiO2/NH2-MIL-125(C/T/NM)。在水热法成功负载碳量子点(CQDs)的过程中,部分NH2-MIL-125(NM)原位转化出TiO2。结果表明,NM 与 TiO2 界面之间成功构建了Ⅱ型异质结,可促进光生电子的传输。此外,CQDs 的成功负载能有效地将光生电子转移并储存到光催化剂表面参与反应,进一步避免了光生载流子的重组。C/T/NM 复合光催化剂在可见光下无氧鼓泡 5 小时的 H2O2 生成量为 455 µmol/L,是 NM 的 7.1 倍。H2O2 生成速率达到 645.4 µM/(g-h),在相同条件下优先于文献报道。最后,根据活性物种捕获实验、能带结构分析和光电化学测量结果,提出了通过 C/T/NM 高效生成 H2O2 的可能机制。这项工作为设计基于 NH2-MIL-125 的复合光催化剂生产 H2O2 提供了新思路。
{"title":"One-step hydrothermal synthesis of CQDs/TiO2/NH2-MIL-125 for efficient photocatalytic production of H2O2 under visible light","authors":"Jianhui Shi,&nbsp;Kaikai Pu,&nbsp;Ting Zhao,&nbsp;Jiating Shi,&nbsp;Na Zheng,&nbsp;Lijun Nie,&nbsp;Kunkun Xue,&nbsp;Yuhang Gao","doi":"10.1016/j.jes.2024.05.034","DOIUrl":"https://doi.org/10.1016/j.jes.2024.05.034","url":null,"abstract":"<div><p>NH<sub>2</sub>-MIL-125 and its derivatives are receiving more attention in various aspects of photocatalytic reactions, especially in the photocatalytic hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) production from water (H<sub>2</sub>O) and oxygen (O<sub>2</sub>), which is a promising and sustainable strategy. However, the generation of H<sub>2</sub>O<sub>2</sub> from NH<sub>2</sub>-MIL-125 is far from satisfactory due to rapid photo-generated carriers recombination and poor surface electron transfer. In the work, the composite photocatalyst CQDs/TiO<sub>2</sub>/NH<sub>2</sub>-MIL-125 (C/T/NM) was designed for the first time by one-step hydrothermal method. TiO<sub>2</sub> was in situ converted from partial NH<sub>2</sub>-MIL-125 (NM) during the successful loaded of Carbon quantum dots (CQDs) by hydrothermal process. The results indicated the type Ⅱ heterojunction was successfully constructed between the NM and TiO<sub>2</sub> interface, which could promote the transmission of photo-generated electrons. In addition, the successful loaded of CQDs could effectively transfer and stored the photo-generated electrons to the photocatalyst surface to participate in the reaction, and further avoiding the recombination of photo-generated carriers. The C/T/NM composite photocatalyst achieved a H<sub>2</sub>O<sub>2</sub> generation of 455 µmol/L for 5 hours under visible light without oxygen bubbling, which was 7.1 times superior to that of NM. The H<sub>2</sub>O<sub>2</sub> generation rate reached 645.4 µM/(g·h), which was in priority in the reported literature under the same conditions. Finally, based on the active species capture experiments, energy band structure analysis and the photoelectrochemical measurements, a possible mechanism for the efficient H<sub>2</sub>O<sub>2</sub> generation through C/T/NM had been proposed. This work provided new ideas for designing NH<sub>2</sub>-MIL-125 based composite photocatalysts for the production of H<sub>2</sub>O<sub>2</sub>.</p></div>","PeriodicalId":15788,"journal":{"name":"Journal of Environmental Sciences-china","volume":null,"pages":null},"PeriodicalIF":5.9,"publicationDate":"2024-05-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141481621","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
Effects of nitrate (NO3−) stress-induced exacerbated cadmium (Cd2+) toxicity on the inflammatory response, oxidative defense, and apoptosis in juvenile Japanese flounder (Paralichthys olivaceus) 硝酸盐(NO3-)应激引起的镉(Cd2+)毒性加剧对日本鲽(Paralichthys olivaceus)幼鱼炎症反应、氧化防御和细胞凋亡的影响
2区 环境科学与生态学 Pub Date : 2024-05-31 DOI: 10.1016/j.jes.2024.05.036
Jiachen Yu , Jie Lian , Yingying Wan , Xiangyuan Li , Pengfei Liu , Qing Ji , Suyue Zhou , Nianhao Zheng , Xingqiang Wang

Due to the discharge of industrial wastewater, urban domestic sewage, and intensive marine aquaculture tailwater, nitrate (NO3) pollution has emerged as a significant issue in offshore waters. Nitrate pollution affects aquatic life and may interact with other pollutants, leading to comprehensive toxicity. Cadmium (Cd2+) is the most widespread metal contaminant, adversely affecting aquatic life in the coastal waters of China. Despite this, few studies have focused on the synergistic toxicity of NO3 and Cd2+ in marine organisms. This study conducted a 30-day exposure experiment on marine Japanese flounder (Paralichthys olivaceus) to explore the synergistic toxicity of NO3 and Cd2+. Our results demonstrated that the exposure to Cd2+ alone induced slight histopathological changes in the liver. However, malformations such as hepatic vacuolar degeneration and sinusoid dilatation were exacerbated under co-exposure. Moreover, co-exposure induced the downregulation of antioxidants and the upregulation of the product malonaldehyde (MDA) from lipid peroxidation, indicating potent oxidative stress in the liver. The increased mRNA expression of IL-8, TNF-α, and IL-1β, along with the decreased expression level of TGF-β, indicated a synergistic inflammatory response in the organisms. Furthermore, the co-exposure led to an abnormal expression of P53, caspase-3, caspase-9, Bcl-2, and Bax, and disturbed the apoptosis in the liver through TUNEL staining analysis. Overall, our results imply that co-exposure synergistically affects inflammation, redox status, and apoptosis in flounders. Therefore, the findings from this study provide valuable perspectives on the ecological risk assessment of marine teleosts co-exposure to NO3 and Cd2+.

由于工业废水、城市生活污水和集约化海水养殖尾水的排放,硝酸盐(NO3-)污染已成为近海水域的一个重要问题。硝酸盐污染会影响水生生物,并可能与其他污染物相互作用,导致综合毒性。镉(Cd2+)是最普遍的金属污染物,对中国近海水域的水生生物造成了不利影响。尽管如此,很少有研究关注 NO3- 和 Cd2+ 对海洋生物的协同毒性。本研究对日本鲽(Paralichthys olivaceus)进行了为期 30 天的暴露实验,以探讨 NO3- 和 Cd2+ 的协同毒性。结果表明,单独暴露于 Cd2+ 会引起肝脏轻微的组织病理学变化。然而,在同时暴露的情况下,肝空泡变性和窦状扩张等畸形会加剧。此外,共同暴露诱导抗氧化剂下调,脂质过氧化产物丙二醛(MDA)上调,表明肝脏中存在强大的氧化应激。IL-8、TNF-α 和 IL-1β 的 mRNA 表达量增加,而 TGF-β 的表达量减少,这表明生物体内存在协同炎症反应。此外,共同暴露导致 P53、caspase-3、caspase-9、Bcl-2 和 Bax 表达异常,并通过 TUNEL 染色分析干扰了肝脏中的细胞凋亡。总之,我们的研究结果表明,共同暴露会协同影响比目鱼的炎症、氧化还原状态和细胞凋亡。因此,本研究的结果为共同暴露于 NO3- 和 Cd2+ 的海洋远洋鱼类的生态风险评估提供了有价值的视角。
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引用次数: 0
Effects of batch and continuous-flow operation on biotreatment of Mn(II)-containing mine drainage 分批和连续流操作对含锰(II)矿井排水生物处理的影响
2区 环境科学与生态学 Pub Date : 2024-05-31 DOI: 10.1016/j.jes.2024.05.038
Obey Gotore , Miho Watanabe , Kunihiro Okano , Naoyuki Miyata , Taiki Katayama , Tetsuo Yasutaka , Yuki Semoto , Takaya Hamai

The biotreatment of mine drainage containing dissolved manganese (Mn) using Mn(II)-oxidizing bacteria is challenging. Sequencing-batch (SBRs) and continuous-flow reactors (CFRs) packed with limestones and inoculated with the mine-drainage microbial community were compared to determine the removal efficiency of Mn(II) from mine drainage. Mn(II) removal in CFRs was 11.4%±0.0% (mean ± standard deviation) in the first two weeks and; it slightly increased to 13.6%±0.0% after four weeks, and more than 94% of Mn(II) was removed under the steady-state treatment phase. The performance of SBRs was more effective, wherein 24.4%±0.1% of Mn was removed in the first two weeks, and in four weeks, surpassed 66.6%±0.2%. Rapid Mn(II) removal observed in the start-up of SBR resulted from higher microbial metabolic activities. The adenosine triphosphate (ATP) content of the microbial community was four-fold more than in CFR, but comparable during the steady-state phase. The Mn-oxide deposits occurring in the SBR and CFR at steady-state were mixed phases of birnessite and woodruffite, and the average Mn oxidation valence in the SBR (+3.73) was slightly higher than that in the CFR (+3.54). During the start-up treatment, the closest relatives of Methyloversatilis, Methylibium, and Curvibacter dominated the SBR, whereas putative Mn oxidizers were associated with Hyphomicrobium, Pedobacter, Pedomicrobium, Terricaulis sp., Sulfuritalea, and Terrimonas organisms. The growth of potential Mn-oxidizing genera, including Mesorhizobium, Rhodococcus, Hydrogenophaga, Terricaulis sp., and ‘Candidatus Manganitrophus-noduliformans’ was observed under the steady state. The SBR operation was effective as a prior start-up treatment for mine drainage-containing Mn(II), through which the CFR performed well as posterior bio-treatment.

利用锰(II)氧化细菌对含有溶解锰(Mn)的矿井排水进行生物处理具有挑战性。为了确定矿井排水中锰(II)的去除效率,我们对装有石灰石并接种了矿井排水微生物群落的序批式反应器(SBR)和连续流反应器(CFR)进行了比较。前两周,CFR 对锰(II)的去除率为 11.4%±0.0%(平均值±标准偏差),四周后略有上升,达到 13.6%±0.0%,在稳态处理阶段,锰(II)的去除率超过 94%。SBR 的性能更为有效,前两周的锰去除率为 24.4%±0.1%,四周后超过 66.6%±0.2%。在 SBR 启动过程中观察到的 Mn(II) 快速去除是由于微生物代谢活动较高所致。微生物群落的三磷酸腺苷 (ATP) 含量是 CFR 的四倍,但在稳态阶段与 CFR 相当。在稳态阶段,SBR 和 CFR 中出现的氧化锰沉积物为桦木石和木屑石的混合相,SBR 中的平均氧化锰价(+3.73)略高于 CFR 中的氧化锰价(+3.54)。在启动处理过程中,Methyloversatilis、Methylibium 和 Curvibacter 的近亲在 SBR 中占主导地位,而推定的锰氧化剂则与 Hyphomicrobium、Pedobacter、Pedomicrobium、Terricaulis sp.、Sulfuritalea 和 Terrimonas 生物有关。在稳定状态下,观察到了潜在锰氧化菌属的生长,包括 Mesorhizobium、Rhodococcus、Hydrogenophaga、Terricaulis sp.和 "Candidatus Manganitrophus-noduliformans"。SBR 操作作为含锰(II)矿井排水的先期启动处理是有效的,通过该操作,CFR 作为后置生物处理效果良好。
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引用次数: 0
Depolymerization of lignin over heterogeneous Co-NC catalyst 在异相 Co-NC 催化剂上对木质素进行氧化还原中性解聚反应
IF 5.9 2区 环境科学与生态学 Q1 ENVIRONMENTAL SCIENCES Pub Date : 2024-05-24 DOI: 10.1016/j.jes.2024.05.025
Fei Song , Kai Du , Huamei Yang , Qi Luo , Yuxuan Liu , Qian Qiang , Yangming Ding , Qingda An , Changzhi Li

Green and atom-economic depolymerization of lignin remains a great challenge due to its complex non-repetitive structure and the inert property for chemo-digestion. A redox-neutral lignin depolymerization system without the use of extra oxidant and/or reductant over a Co-NC catalyst has been developed in this work, providing the first non-noble metal heterogeneous catalytic system for redox-neutral valorization of lignin. Mechanistic studies based on control reactions and deuterium labeling experiments suggest that the reaction proceeds via a metal-catalyzed dehydrogenation of Cα-OH to afford a carbonyl intermediate, followed by Cβ-O bond cleavage (via hydrogenolysis) to afford monophenols and aromatic ketone products. The hydrogen used for the cleavage of the Cβ-O bond originates from the alcohol moiety in the substrate, and the cascade dehydrogenation and hydrogenolysis steps are highly coupled, rendering it an efficient and atom-economic process.

由于木质素具有复杂的非重复性结构和化学消化的惰性,因此对其进行绿色和原子经济的解聚仍然是一项巨大的挑战。本研究开发了一种无需使用额外氧化剂和/或还原剂的 Co-NC 催化剂氧化还原中性木质素解聚系统,为木质素氧化还原中性价化提供了首个非贵金属异相催化系统。基于对照反应和氘标记实验的机理研究表明,该反应是通过金属催化 Cα-OH 脱氢生成羰基中间体,然后 Cβ-O 键裂解(通过氢解)生成单酚和芳香酮产物。用于 Cβ-O 键裂解的氢来自底物中的醇分子,级联脱氢和氢解步骤高度耦合,使其成为一种高效、原子经济的工艺。
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引用次数: 0
Overlooked formation of chlorinated coupling byproducts during phenol degradation with ferrate(VI) oxidation technology 利用六价铬铁氧化技术降解苯酚过程中被忽视的氯化偶联副产品的形成
2区 环境科学与生态学 Pub Date : 2024-05-24 DOI: 10.1016/j.jes.2024.05.024
Dan Tao , Yuxin Zhou , Laura Carter , Chengxuan Tian , Na Qin , Kehao Li , Fan Zhang

Currently, ferrate(VI) oxidation technology (FOT) has been regarded as one of the most promising options for the degradation of emerging organic pollutants. However, the role and transformation of chloride ions (Cl) in FOT have not been well explored. The current study aims to investigate the formation of chlorinated phenolic byproducts upon ferrate(VI) oxidation processes. The obtained results indicate that chlorides suffering ferrate(VI) attack will be transformed to active chlorine species (ACS), which will subsequently lead to the formation of highly toxic aromatic chlorinated byproducts. The identified byproducts include common chlorinated phenolic derivatives, as well as complex chlorinated oligomer byproducts with ether structures (mainly dimers and trimers). While the formation of common chlorophenols can be ascribed to the electrophilic substitution reactions mediated by ACS, the oligomer byproducts are generated via coupling reactions between chlorinated phenoxy radicals. ECOSAR software predicts that the generated chlorinated oligomer byproducts exhibit high ecotoxicological effects. As a whole, the above findings shed light on the potential risk of FOT in real practice.

目前,铁酸(VI)氧化技术(FOT)已被视为降解新出现的有机污染物的最有前途的方法之一。然而,氯离子(Cl-)在 FOT 中的作用和转化尚未得到很好的探讨。本研究旨在调查在六价铬铁氧化过程中氯化酚类副产物的形成。研究结果表明,受到六价铬铁侵蚀的氯化物会转化为活性氯物种(ACS),进而形成剧毒的芳香族氯化副产品。已确定的副产品包括常见的氯化酚衍生物,以及具有醚结构(主要是二聚体和三聚体)的复杂氯化低聚物副产品。普通氯酚的形成可归因于由 ACS 介导的亲电取代反应,而低聚物副产品则是通过氯化苯氧自由基之间的偶联反应生成的。根据 ECOSAR 软件预测,生成的氯化低聚物副产物具有较高的生态毒理效应。总之,上述发现揭示了 FOT 在实际应用中的潜在风险。
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Journal of Environmental Sciences-china
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