高效异养硝化-好氧反硝化菌Glutamicibacter sp.WS1低温下对多种氮源的脱氮特性及氮代谢机制

针对污水处理厂冬季生物脱氮效率低、出水水质不达标的问题,从活性污泥中分离出1株耐低温异养硝化-好氧反硝化菌株Glutamicibacter sp.WS1.采用PCR技术扩增该菌株的脱氮功能基因,研究其对不同氮源的低温脱氮效能,通过单因素实验探究环境因子对其低温好氧反硝化性能的影响,并利用氮平衡解析其氮代谢路径.结果表明,菌株WS1含有氮代谢相关的功能基因amoA、napA、nirS和nirK;在15℃低温条件下,菌株WS1在以NH₄⁺-N、NO₃^--N、NO₂^--N+NO₃^--N和NH₄⁺-N+NO₃^--N为氮源时,对各无机氮的去除率分别为100%、98.10%、99.87%+100%和100%+94.92%;菌株WS1的最佳反硝化条件：柠檬酸钠为碳源、C/N为16、pH为8、ρ（DO）为4.5~6.8 mg ·L^-1和温度为30℃;在低温（15℃）和低C/N （10）条件下,菌株WS1对NO₃^--N的去除率达到92.50%;异养硝化-好氧反硝化/好氧反硝化和同化作用是菌株WS1去除不同氮源底物的主要途径,其中大部分的无机氮（47%~56%）通过异养硝化-好氧反硝化/好氧反硝化作用转化为了气态氮.菌株WS1在低温污水脱氮领域具有广阔的应用前景.     

赤泥活化过一硫酸盐降解环丙沙星:性能和机制

为提高赤泥的综合利用及抗生素有机废水的深度处理,以赤泥（red mud,RM）为催化剂、环丙沙星（ciprofloxacin,CIP）为目标污染物,系统研究了RM活化过一硫酸盐（peroxymonosulfate,PMS）降解CIP的效果和机制.结果表明,含有Fe、Al和Ca等金属氧化物,具有较大比表面积（10.96 m²·g^-1）和复杂孔道结构的RM能够有效增强PMS对CIP的降解速率和效果.自由基捕获剂甲醇、叔丁醇和苯酚的抑制实验结果进一步说明,体系产生的SO₄^-·和HO·在RM表面与CIP发生氧化反应.温度、PMS浓度和RM投加量影响CIP的降解.温度升高反应速度加快,反应活化能为5.74 kJ·mol^-1; PMS浓度增加,体系产生更多SO₄^-·和HO·,CIP的降解率升高; RM存在最佳投加量1.0 g·L^-1.HPLC/MS/MS共检测到8种降解产物,CIP分子中的哌嗪环易受活性物质进攻,CIP主要通过2种途径进行降解.本研究表明RM是一种极具潜力的廉价催化剂,可用于活化过一硫酸盐处理含抗生素的污染废水.     

磺胺二甲基嘧啶(SM2)高效降解菌J2的分离筛选及降解特性研究

从城市污水处理厂活性污泥中分离得到一株能以磺胺二甲基嘧啶(SM2)为唯一碳源的菌株,经生理生化鉴定和16S rRNA基因序列同源性分析,将此菌鉴定为蜡样芽孢杆菌(Bacillus cereus),命名为J2.不同条件下的降解特性研究结果表明,J2菌株具有极高的SM2耐受性(100 mg·L~(-1))、较广的温度(20～30℃)和pH(6～8)适用范围;在温度30℃、pH=8.0、初始OD_(600)=0.1、SM2起始浓度为50 mg·L~(-1)的条件下,J2菌株在36 h内对SM2的降解率可达100%,降解效率远超目前已报道的其他SM2降解菌株,展现出了良好的应用潜力.J2菌株降解SM2过程中产生了5种主要中间代谢产物,分析推断其降解SM2的途径分为两条:①磺胺二甲基嘧啶分子首先在酶促反应作用下脱除SO_2,生成嘧啶环和苯胺环自由基,这两种自由基再经过环间耦合生成N-(4,6-二甲基嘧啶-2基)-1,4-二苯胺,该分子中的C—N键在活性氧物种的作用下断开生成苯胺和2-氨基-4,6-二甲基嘧啶;②在漆酶的作用下N~4键断裂,产生N-(3,5-二甲基嘧啶)-苯磺酰胺,之后N-(3,5-二甲基嘧啶)-苯磺酰胺的N—S键断裂,进一步形成2-氨基-4,6-二甲基嘧啶和苯亚砜.     

活性污泥降解四溴双酚A的特性、途径及毒性评估

电子行业典型污染物溴代阻燃剂对环境的污染引起了广泛关注.本文以产量最大、应用最广的典型溴代阻燃剂四溴双酚A(Tetrabromobisphenol A,TBBPA)为研究对象,考察了活性污泥降解四溴双酚A的特性、影响因素、降解途径并进行毒性评估.结果显示:活性污泥能有效降解水体中的TBBPA;在初始接菌量OD_(600)=0.77,TBBPA浓度为2.50 mg·L~(-1),温度为40℃,pH值为6.0时,经6 h反应后降解率可达58.46%,脱溴率达43.80%;在自然水体中活性污泥对TBBPA的降解受到抑制,尤其在腐殖质含量较高时;自然光能促进TBBPA降解,紫外光则抑制其降解活性;利用LC-Q-TOF-MS/MS检测到3种中间产物,推测TBBPA可能通过以下两种路径降解:①TBBPA发生甲基化和脱溴反应,产生甲基化的二溴双酚A,随后发生羟基化反应生成5-[1-(3-溴-4-甲氧基-苯基)-1-甲基-乙基]-2-甲氧基-苯酚;②TBBPA发生羟基化反应生成5-[1-(3-溴-4,5-二羟基-苯基)-1-甲基-乙基]-苯-1,2,3-三醇,随后发生脱溴、羟基化和甲基化反应,生成5-[1-(3-羟基-4,5-二甲氧基-苯基)-1-甲基-乙基]-2-甲氧基-苯-1,3-二醇;最后,利用发光细菌对该降解过程进行毒性评价,结果表明,活性污泥降解TBBPA的过程中其毒性未被完全去除,仍存在一定的环境风险.     

2015~2019年日照市PM2.5长期变化特征及其潜在源区分析

利用2015~2019年山东省日照市PM_2.5质量浓度和气象要素的小时数据,对日照市PM_2.5季节污染特征和日照市海陆风特征进行了分析,并基于HYSPLIT模式计算了5年逐日02：00、08：00、14：00和20：00（BTC）的48h后向轨迹,不仅通过轨迹聚类分析和潜在源区分析探讨了日照市不同季节PM_2.5主要传输路径和其轨迹污染特征及其潜在源区分布和贡献,也分析了海陆风对日照市污染物的影响.结果表明：日照市PM_2.5呈现冬季最高、夏季最低的分布特征,监测站点颗粒物浓度在偏西北风影响下较高.日照市不同季节主要输送路径存在差异：春季主要受到偏东和偏北方向气流影响;夏季在副热带高压影响下主要受到来自海上的较为清洁的偏东气流影响;秋季主要受到西北和偏东气流影响;冬季主要受西北和偏北气流影响.整体而言,不同季节受偏西至偏南气流影响时,日照市对应的PM_2.5浓度较高.日照市海陆风春秋季多,夏冬季少;在海陆风影响下,日照市PM_2.5污染和臭氧污染呈现不同的分布特征,且在不同PM_2.5污染等级下,PM_2.5浓度日变化特征也与其在非海陆风日的日变化有所差异.污染潜在源区分析结果表明,日照市最主要的潜在源区位于山东省临沂市、潍坊市、青岛市和江苏省连云港市.     

Biodegradation of typical azole fungicides in activated sludge under aerobic conditions

Widespread use of azole fungicides and low removal efficiency in wastewater treatment plants (WWTPs) have led to the elevated concentration of azole fungicides in receiving environment. However, there was limited research about the removal mechanism of azole fungicides in the biological treatment of WWTPs. Imidazole fungicide climbazole and triazole fungicide fluconazole were selected to investigate the biodegradation mechanism of azole fungicides in activated sludge under aerobic conditions. Climbazole was found to be adsorbed to solid sludge and resulted in quick biodegradation. The degradation of climbazole in the aerobic activated sludge system was fitted well by the first-order kinetic model with a half-life of 5.3 days, while fluconazole tended to stay in liquid and had only about 30% of loss within 77 days incubation. Ten biotransformation products of climbazole were identified by high resolution mass spectrometry using suspect and non-target screening method. But no biodegradation products of fluconazole were identified due to its limited removal. The possible biodegradation pathways for climbazole were proposed based on the products identification and pathway prediction system, and involves oxidative dehalogenation, side chain oxidation and azole ring loss. The findings from this study suggest that it should be a concern for the persistence of fluconazole in the environment.     

降解菌djl-6多菌灵水解酶的提取及性质

以往对多菌灵降解菌Rhodococcus qingshengii sp.nov.djl-6的降解途径研究显示,该菌株首先通过多菌灵水解酶将多菌灵水解成二氨基苯并咪唑,从而对多菌灵进行脱毒.为开发酶制剂并有效应用于环境中残留污染物多菌灵的降解,比较了不同提取方法(高压细胞破碎、超声波破碎和添加溶菌酶破碎)对多菌灵水解酶提取效率的影响,并对其酶学特性进行了初步研究.结果表明,djl-6菌株在LB培养基中培养72~84 h,生长量和产酶量均达到最大值.采用超声波破碎提取酶的效率较高(蛋白浓度为7.92 mg/mL),但酶活损失较大(比酶活只有1.2 U/μg protein).多菌灵水解酶属于一种胞内组成型酶.该酶水解多菌灵的最适pH值为7.0,最适温度为30℃,Zn2+和K+对酶活有一定的抑制作用.     

土壤及地下水污染点不同暴露途径的健康风险比较

选择目前国际上应用最为广泛的RBCA模式和Csoil模式,进行土壤污染和地下水污染暴露途径考虑异同的比较,并在此基础上设置典型的污染情景,对不同暴露途径的健康风险进行了计算.Csoil模式比RBCA模式多考虑了3种可能的暴露途径.将2种模式结合进行案例计算的结果表明,表层土壤污染的风险最大;对于浅层土壤污染,考虑淋溶作用时的风险较高.挥发暴露和饮水暴露是土壤及地下水污染点最主要的暴露途径,在RBCA模式中没有考虑的洗澡过程中的暴露也非常重要.对于表层土壤污染,覆土是减小健康风险的有效办法.     

Degradation of Azo dye direct black BN based on adsorption and microwave-induced catalytic reaction

The novel microwave catalyst MgFe₂O₄-SiC was synthesized via sol-gel method, to remove azo dye Direct Black BN (DB BN) through adsorption and microwave-induced catalytic reaction. Microwave-induced catalytic degradation of DB BN, including adsorption behavior and its influencing factors of DB BN on MgFe₂O₄-SiC were investigated. According to the obtained results, it indicated that the pseudo-second-order kinetics model was suitable for the adsorption of DB BN onto MgFe₂O₄-SiC. Besides, the consequence of adsorption isotherm depicted that the adsorption of DB BN was in accordance with the Langmuir isotherm, which verified that the singer layer adsorption of MgFe₂O₄-SiC was dominant than the multi-layer one. The excellent adsorption capacities of MgFe₂O₄-SiC were kept in the range of initial pH from 3 to 7. In addition, it could be concluded that the degradation rate of DB BN decreased over ten percent after the adsorption equilibrium had been attained, and the results from the result of comparative experiments manifested that the adsorption process was not conducive to the process of microwave-induced catalytic degradation. The degradation intermediates and products of DB BN were identified and determined by GC-MS and LC-MS. Furthermore, combined with the catalytic mechanism of MgFe₂O₄-SiC, the proposed degradation pathways of DB BN were the involution of microwave-induced $OH and holes in this catalytic system the breakage of azo bond, hydroxyl substitution, hydroxyl addition, nitration reaction, deamination reaction, desorbate reaction, dehydroxy group and ring-opening reaction.

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Insights into simultaneous anammox and denitrification system with short-term pyridine exposure: Process capability,inhibition kinetics and metabolic pathways

• Short-term effect of the pyridine exposure on the SAD process was investigated. • The SAA at 150 mg/L pyridine reduced by 56.7% of the maximum value. • Inhibition kinetics models and inhibitory parameters were indicated. • Collaboration of AnAOB, HDB and PDB promoted the SAD. • Possible metabolic pathways of nitrogen and pyridine were proposed. In-depth knowledge on the role of pyridine as a bottleneck restricting the successful application of anammox-based process treating refractory coking wastewater remains unknown. In this study, the effect of short-term pyridine addition on a simultaneous anammox and denitrification (SAD) system fed with 25–150 mg/L pyridine was explored. The short-term operation showed that the highest total nitrogen (TN) removal efficiency was achieved at 25–50 mg/L of pyridine. As the pyridine addition increased, the contribution of the anammox pathway in nitrogen removal decreased from 99.3% to 79.1%, while the denitrification capability gradually improved. The specific anammox activity (SAA) at 150 mg/L pyridine decreased by 56.7% of the maximum SAA. The modified non-competitive inhibition model indicated that the 50% inhibitory concentration (IC₅₀) of pyridine on anammox was 84.18 mg/L and the substrate inhibition constant (K_i) of pyridine for self-degradation was 135.19 mg/L according to the Haldane model. Moreover, high-throughput sequencing confirmed the abundance of Candidatus Kuenenia as the amount of anammox species decreased, while the amounts of denitrifiers and pyridine degraders significantly increased as the pyridine stress increased. Finally, the possible pathways of nitrogen bioconversion and pyridine biodegradation in the SAD system were elucidated through metagenomic analysis and gas chromatography/mass spectrometry results. The findings of this study enlarge the understanding of the removal mechanisms of complex nitrogenous pyridine-containing wastewater treated by the SAD process.