六溴环十二烷(HBCD)对H4细胞和SK-N-AS细胞脱碘酶2和3表达的影响

六溴环十二烷(hexabromocyclododecane,HBCD)与多溴联苯醚(polybrominated diethyl ethers,PBDEs)复合污染体系,对人类健康尤其神经系统所造成的潜在危害及其机制一直是笔者课题组的研究方向。HBCD是广泛使用的溴化阻燃剂,与PBDEs一样,会通过干扰内分泌系统、影响甲状腺激素分泌及损伤神经系统,对生物体产生发育神经毒性。作为系列研究之一,本研究以H4人脑神经胶质瘤细胞和SK-N-AS人神经母细胞瘤细胞为体外生物模型,通过观察HBCD对H4细胞Ⅱ型脱碘酶(Dio2)和SK-N-AS细胞Ⅲ型脱碘酶(Dio3)表达的调控,初步探讨了HBCD对神经系统局部甲状腺激素水平的潜在影响。H4细胞和SK-N-AS细胞分别暴露于0、1、3和9μmol·L-1HBCD 24 h后,采用MTT法检测细胞活力,Western Blot和RT-PCR法分别分析Dio2和Dio3蛋白和基因的表达,酶联免疫吸附测定(ELISA)法检测H4细胞脑源性神经细胞营养因子(BDNF)的分泌。结果表明,HBCD以剂量依赖方式降低H4细胞和SK-N-AS细胞生存率,引起H4细胞Dio2蛋白和基因表达下调,而致SK-N-AS细胞Dio3蛋白和基因表达上调。此外,HBCD还降低H4细胞BDNF的分泌。这表明,HBCD很可能通过影响神经和胶质细胞脱碘酶的表达,影响脑局部甲状腺激素水平,从而引起神经系统损伤及发育神经毒性。     

Characterization of CANON reactor performance and microbial community shifts with elevated COD/N ratios under a continuous aeration mode

COD/N at low ratios (0–0.82) improved N removals of CANON. CANON performance decreased after COD/N up to 0.82. The relative abundance of AOB decreased continuously with increasing COD/N. AOB outcompeted at a high COD load led to CANON failure. The relative abundance of AnAOB decreased and increased with increasing COD/N. The effects of increasing COD/N on nitrogen removal performance and microbial structure were investigated in a SBR adopting a completely autotrophic nitrogen removal over nitrite process with a continuous aeration mode (DO at approximately 0.15–0.2 mg/L). As the COD/N increased from 0.1 to≤0.59, the nitrogen removal efficiency (NRE) increased from 88.7% to 95.5%; while at COD/N ratios of 0.59–0.82, the NRE remained at 90.7%–95.5%. As the COD/N increased from 0.82 to 1.07, the NRE decreased continuously until reaching 60.1%. Nitrosomonas sp. (AOB) and Candidatus Jettenia (anammox bacteria) were the main functional genera in the SBR. As the COD/N increased from 0.10 to 1.07, the relative abundance of Nitrosomonas decreased from 13.4% to 2.0%, while that of Candidatus Jettenia decreased from 35% to 9.9% with COD/N<0.82 then increased to 45.4% at a COD/N of 1.07. Aerobic heterotrophic bacteria outcompeted AOB at high COD loadings (650 mg/L) because of oxygen competition, which ultimately led to deteriorated nitrogen removal performance.     

Enhanced catalytic oxidation of 2,4-dichlorophenol via singlet oxygen dominated peroxymonosulfate activation on CoOOH@Bi2O3 composite

• Bi₂O₃ cannot directly activate PMS. • Bi₂O₃ loading increased the specific surface area and conductivity of CoOOH. • Larger specific surface area provided more active sites for PMS activation. • Faster electron transfer rate promoted the generation of reactive oxygen species. • ¹O₂ was identified as dominant ROS in the CoOOH@Bi₂O₃/PMS system. Cobalt oxyhydroxide (CoOOH) has been turned out to be a high-efficiency catalyst for peroxymonosulfate (PMS) activation. In this study, CoOOH was loaded on bismuth oxide (Bi₂O₃) using a facile chemical precipitation process to improve its catalytic activity and stability. The result showed that the catalytic performance on the 2,4-dichlorophenol (2,4-DCP) degradation was significantly enhanced with only 11 wt% Bi₂O₃ loading. The degradation rate in the CoOOH@Bi₂O₃/PMS system (0.2011 min⁻¹) was nearly 6.0 times higher than that in the CoOOH/PMS system (0.0337 min⁻¹). Furthermore, CoOOH@Bi₂O₃ displayed better stability with less Co ions leaching (16.4% lower than CoOOH) in the PMS system. These phenomena were attributed to the Bi₂O₃ loading which significantly increased the conductivity and specific surface area of the CoOOH@Bi₂O₃ composite. Faster electron transfer facilitated the redox reaction of Co (III) / Co (II) and thus was more favorable for reactive oxygen species (ROS) generation. Meanwhile, larger specific surface area furnished more active sites for PMS activation. More importantly, there were both non-radical (¹O₂) and radicals (SO₄⁻•, O₂⁻•, and OH•) in the CoOOH@Bi₂O₃/PMS system and ¹O₂ was the dominant one. In general, this study provided a simple and practical strategy to enhance the catalytic activity and stability of cobalt oxyhydroxide in the PMS system.     

Experimental and computational assessment of 1,4-Dioxane degradation in a photo-Fenton reactive ceramic membrane filtration process

• 1,4-Dioxane was degraded via the photo-Fenton reactive membrane filtration. • Degradation efficiency and AQY were both enhanced in photocatalytic membrane. • There is a tradeoff between photocatalytic degradation and membrane permeation flux. • Degradation pathways of 1,4-Dioxane is revealed by DFT analysis. The present study evaluated a photo-Fenton reactive membrane that achieved enhanced 1,4-Dioxane removal performance. As a common organic solvent and stabilizer, 1,4-Dioxane is widely used in a variety of industrial products and poses negative environmental and health impacts. The membrane was prepared by covalently coating photocatalyst of goethite (α-FeOOH) on a ceramic porous membrane as we reported previously. The effects of UV irradiation, H₂O₂ and catalyst on the removal efficiency of 1,4-Dioxane in batch reactors were first evaluated for optimized reaction conditions, followed by a systematical investigation of 1,4-Dioxane removal in the photo-Fenton membrane filtration mode. Under optimized conditions, the 1,4-Dioxane removal rate reached up to 16% with combination of 2 mmol/L H₂O₂ and UV₃₆₅ irradiation (2000 µW/cm²) when the feed water was filtered by the photo-Fenton reactive membrane at a hydraulic retention time of 6 min. The removal efficiency and apparent quantum yield (AQY) were both enhanced in the filtration compared to the batch mode of the same photo-Fenton reaction. Moreover, the proposed degradation pathways were analyzed by density functional theory (DFT) calculations, which provided a new insight into the degradation mechanisms of 1,4-Dioxane in photo-Fenton reactions on the functionalized ceramic membrane.     

4-氯-3-甲基苯酚(PCMC)暴露对成年斑马鱼内源性物质的影响

建立了4-氯-3-甲基苯酚（PCMC）的水生生物斑马鱼暴露毒理学模型,研究了斑马鱼PCMC暴露后内源性代谢物的变化.同时,在斑马鱼PCMC半数致死浓度LC₅₀的基础上,以1/10 LC₅₀为暴露浓度进行代谢组学分析.最后,经超高效液相色谱串联三重四级杆飞行时间质谱（UHPLC-Triple-TOF-MS）检测,结合主成分分析（PCA）和正交偏最小二乘法判别分析（OPLS-DA）进行代谢谱分析.结果发现,空白对照组和暴露组在代谢水平上有明显差异.进一步分析后筛选出9种上调物质和11种下调物质作为潜在生物标志物,主要包括氨基酸、嘌呤、糖类和脂质.根据差异代谢物生理功能分析发现,PCMC主要通过影响嘌呤代谢、甘油磷脂代谢、淀粉和蔗糖代谢、组氨酸代谢、丙酮酸代谢及苯丙氨酸、酪氨酸和色氨酸的生物合成,对斑马鱼的心血管系统、神经系统、蛋白代谢和能量代谢等方面产生毒性效应.本研究建立的代谢组学方法能全面评价氯酚类消毒剂对水生生物的毒性效应,为进一步阐明氯酚类消毒剂的毒性机制提供了理论基础.     

Effect of the addition of organic carbon sources on nitrous oxide emission in anaerobic-aerobic (low dissolved oxygen) sequencing batch reactors

The effect of additional organic carbon sources on the production of nitrous oxide (N₂O) in anaerobic-aerobic (low dissolved oxygen) real wastewater treatment system was investigated. In this paper, three laboratory-scale sequencing batch reactors (SBRs) (SBR-1, SBR-2 and SBR-3) were operating under an anaerobic-aerobic (low dissolved oxygen, 0.15–0.45 mg·L^-1) configuration. The SBRs were ‘long-term cultured’ respectively with a single municipal wastewater sample, sodium acetate, and a waste-activated sludge alkaline fermentation liquid as the additional carbon sources of real wastewater. Off-gas analysis showed that N₂O was emitted into the atmosphere during the aerobic (low dissolved oxygen) period in the three SBRs, and the order of N₂O emission rate was SBR-2>SBR-1>SBR-3. It was observed that the higher poly-β-hydroxyvalerate fraction of polyhydroxyalkanoates, the lower glycogen transformation and less nitrite accumulation was in SBR-3, while the opposite behavior was observed in SBR-2. Further research indicated that the interaction of the factors above potentially affected the N₂O emission in the anaerobic-aerobic (low dissolved oxygen) system.     

沸石负载对叔丁基杯[4]芳烃乙酸对铀的吸附行为

以对叔丁基杯[4]芳烃与溴乙酸乙酯为主要反应底物合成了对叔丁基杯[4]芳烃乙酸,然后将其负载在沸石上,红外光谱显示合成物具有杯[4]芳烃乙酸的特征结构,扫描电镜分析表明对叔丁基杯[4]芳烃乙酸成功负载于沸石之上,且分布均匀,分散性良好.通过静态吸附实验,结果表明在pH值 4,对叔丁基杯[4]芳烃乙酸/沸石的负载比0.025/1,吸附剂用量0.5g,铀初始质量浓度10mg/L,吸附时间30min时,沸石在负载了对叔丁基杯[4]芳烃乙酸后,对溶液中铀的吸附率从30%左右提高到93%.沸石和负载沸石吸附动力学行为均符合准二级动力学模型,但负载沸石对铀的吸附速率明显高于沸石.沸石和负载沸石吸附等温式都符合Langmuir吸附等温线,说明都为单分子层吸附;由此推导出的最大吸附量Qm从16.8919提高到32.5733mg/g,这主要是因为沸石负载了对叔丁基杯[4]芳烃乙酸增加了吸附点位.吸附铀前后的红外光谱表明,负载沸石对铀的去除主要依靠对叔丁基杯[4]芳烃乙酸与铀的强络合作用和Si—O和Al—O的吸附作用,两种作用的协同加快了吸附速率,增加了吸附容量.     

太湖典型湖区沉积物外源有机质贡献率研究

采用稳定同位素示踪法,分析了太湖竺山湾和南部湖区苕溪港区域表层沉积物碳和氮同位素分布特征,并利用“端元混合法”计算确定了陆源输入对湖泊沉积物有机质的贡献. 结果表明:① δ13C值在南部湖区要高于竺山湾,竺山湾表现为从河道(-27.72‰)到湾内(-23.00‰)逐渐增大的趋势,南部研究区域也表现出同样的趋势,说明外源有机质的贡献不断减少;② δ15N值在陆源有机质中较低,而在内源有机质中较高,没有明显的梯度变化规律;③ C/N比表现为从外源到内源不断减小的趋势;④ 利用“端元混合法”计算外源有机质贡献率发现,δ13C和C/N比的结果较为相似:竺山湾入湖口的外源有机质贡献率为46.51%～52.51%,竺山湾外源有机质贡献率为27.61%～30.85%;而δ15N计算得到的外源有机质贡献率差异较大,竺山湾入湖口处为56.91%～97.47%,竺山湾为74.83%. 讨论认为含氮物质的多来源特征及N同位素分馏作用的复杂性都增加了有机质源解析的不确定性.      

不同SBR系统N2O排放及微生物群落比较

为了解污水脱氮中微生物群落对N₂O排放的影响,在相同的工艺条件下,研究了制药厂(A)和啤酒厂(B)2种不同来源污泥在SBR系统中的N₂O排放特性.结果发现:①A和B 2个系统总氮去除率在97.5%和98.6%的情况下,脱氮中N₂O态氮所占比例分别为6.35%和2.84%,相差2倍以上.②A系统的N₂O排放时期主要集中在好氧硝化段,而B系统则主要集中在缺氧反硝化段.③在1个脱氮周期内,A系统只有1个N₂O排放高峰,出现在好氧硝化段(第3小时);而B系统有2个N₂O排放高峰,分别出现在好氧硝化段(第3小时)和缺氧反硝化段(第6小时).采用PCR-DGGE技术分析微生物群落特征发现,A系统和B系统的微生物群落有明显差异,表明污水脱氮中微生物群落是影响N₂O排放的重要因素.通过优化微生物群落结构,可有效控制污水脱氮中N₂O排放.      

Benefits of supplementing an industrial waste anaerobic digester with energy crops for increased biogas production

Currently, there is increasing competition for waste as feedstock for the growing number of biogas plants. This has led to fluctuation in feedstock supply and biogas plants being operated below maximum capacity. The feasibility of supplementing a protein/lipid-rich industrial waste (pig manure, slaughterhouse waste, food processing and poultry waste) mesophilic anaerobic digester with carbohydrate-rich energy crops (hemp, maize and triticale) was therefore studied in laboratory scale batch and continuous stirred tank reactors (CSTR) with a view to scale-up to a commercial biogas process. Co-digesting industrial waste and crops led to significant improvement in methane yield per ton of feedstock and carbon-to-nitrogen ratio as compared to digestion of the industrial waste alone. Biogas production from crops in combination with industrial waste also avoids the need for micronutrients normally required in crop digestion. The batch co-digestion methane yields were used to predict co-digestion methane yield in full scale operation. This was done based on the ratio of methane yields observed for laboratory batch and CSTR experiments compared to full scale CSTR digestion of industrial waste. The economy of crop-based biogas production is limited under Swedish conditions; therefore, adding crops to existing industrial waste digestion could be a viable alternative to ensure a constant/reliable supply of feedstock to the anaerobic digester.