溴代阻燃剂对氧化亚铁硫杆菌浸提废旧电脑主板覆层铜的影响

以破碎至10~20目(0.84~2.00 mm)的废旧电脑主板颗粒为试验材料,分为未处理(未去除溴代阻燃剂的主板颗粒)、处理(去除30%溴代阻燃剂的主板颗粒)、加萃取物(处理主板颗粒和萃取物)、对照4组. 以CCl₄作为萃取剂,采用固液萃取技术,分析了在微生物作用下不同处理组中ρ(Cu2+)、ρ(Fe3+)、E_h(氧化还原电位)和pH的变化,以考察溴代阻燃剂对氧化亚铁硫杆菌(Thiobacillus ferrooxidans)浸Cu率的影响. 结果表明:随着浸提时间的增加,氧化亚铁硫杆菌对未处理、处理和加萃取物3组的浸Cu率不同,其中处理组最好,加萃取物组最差. 浸提过程中,ρ(Fe3+)、E_h和pH与微生物活性、浸Cu率显著相关,表现为微生物活性越好,ρ(Cu2+)和pH越大,ρ(Fe3+)和E_h越小. 浸提24和168 h,处理组的浸Cu率比未处理组分别提高了14.11%和17.37%; 而加萃取物组的浸Cu率比未处理组分别降低了27.69%和21.67%. 表明废旧电脑主板中的溴代阻燃剂是影响微生物浸Cu率的重要因素之一. 为进一步提高浸Cu率,必须考虑溴代阻燃剂对微生物生长的影响.      

全自养脱氮颗粒污泥的培养及脱氮性能的恢复与强化

采用交替限氧-厌氧和低充放比(30%)运行模式,在SBR反应器中成功启动全自养脱氮(CANON)工艺,启动过程经历常规硝化主导阶段、短程硝化主导阶段和全自养脱氮阶段,总氮去除速率和总氮去除效率分别达到(312±15)mg/(L·d)和(71.2±4.3)%.培养得到的污泥中颗粒污泥(粒径3300μm)和絮状污泥(粒径<300μm)体积分别占污泥总体积的39%和61%.在自养脱氮性能恶化的SBR反应器进水中长期添加适量N2H4,反应器脱氮性能得以恢复甚至强化,反应器总氮去除速率升高到(480±34)mg/(L·d),颗粒污泥的比例增加到污泥总体积的51%.     

舟山本岛大气污染输送过程的数值模拟分析

利用HYSPLIT-4后向轨迹模式和NCEP(美国国家环境预报中心)的2012年GDAS(全球资料同化系统)气象数据,结合NO₂、PM_2.5、PM₁₀和SO₂等常规大气污染物的质量浓度数据,对舟山本岛2012年4月、7月、10月和12月的大气污染输送过程进行了模拟,并通过聚类分析和潜在源区分析〔包括PSCF(潜在源贡献)和CWT(浓度权重轨迹)计算〕,确定大气污染传输路径及影响源区. 结果表明:舟山本岛气流后向轨迹呈明显的季节变化特征,4月主要受来自黄海海面气流轨迹的影响,其占总轨迹数的36.7%,ρ(PM₁₀)为(53.24±24.33)μg/m3;7月以途经琉球群岛和东海气流轨迹为主,占总轨迹数的48.4%,对ρ(NO₂)、ρ(PM_2.5)、ρ(PM₁₀)和ρ(SO₂)贡献分别为(24.63±6.33)、(28.60±4.83)、(52.89±18.76)和(8.67±3.11)μg/m3;10月气流轨迹主要来自于东海海面,占总轨迹数的49.2%;12月气流则主要来自辽宁南部和黄海,占总轨迹数的66.1%,对ρ(NO₂)、ρ(PM_2.5)、ρ(PM₁₀)和ρ(SO₂)贡献分别为(28.48±15.14)、(58.71±14.10)、(69.83±38.94)和(20.83±13.28)μg/m3. 舟山本岛PM_2.5的潜在源主要为毗邻城市间局地污染,集中于浙江沿海城市及杭州湾、上海等地.      

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。     

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.     

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.     

Fe3O4-MnO2复合材料催化降解水中有机污染物的研究进展

综述了Fe₃O₄-MnO₂复合材料催化降解水中有机污染物的研究进展,介绍了Fe₃O₄-MnO₂复合材料的负载方式,总结了Fe₃O₄-MnO₂复合材料在催化降解水中有机污染物方面的应用。同时,阐述了Fe₃O₄-MnO₂复合材料催化降解水中有机污染物的机理。指出：Fe₃O₄-MnO₂复合材料未来的研发方向是实现负载方式的多样性和提高复合材料的热稳定性,制备出形貌多样、结晶性能好、稳定性高、经济性好、功能多样的Fe₃O₄-MnO₂复合材料。     

水溶液中对叔辛基酚的紫外光降解研究

研究了185nm紫外光对薄液层中对叔辛基酚(4-OP)的作用规律,考察了初始浓度、液层厚度、光强等因素对4-OP的降解效果的影响.结果表明,用该方法降解水中4-OP,在4-OP初始浓度10mg/L,液层厚度为2mm,光照距离为10cm,光照45min后,去除率可达到95%以上,其降解过程符合表观一级反应动力学特征.