邻苯二甲酸酯降解细菌的多样性、降解机理及环境应用

邻苯二甲酸酯(phthalic acid esters,PAEs)是一类对人体内分泌系统有干扰作用的持续性有机污染物(persistent organic pol utants,POPs)。PAEs在环境介质如水体、底泥和土壤中长期赋存会对生物体产生毒害效应,其分布广、浓度高和难降解等特点是限制有效环境治理的主要因素。作为环境的重要组成部分,微生物对污染物有很强的适应能力和高效的降解能力,这为PAEs的生物修复提供了可能。与物理化学修复法相比,微生物修复技术具有可控性强、修复面广和灵活性高等优势。本文综述了已报道的大部分PAEs降解细菌的种类及其代谢机制,并分析了其在PAEs污染水体和土壤修复中的应用现状与前景,以期为PAEs环境行为与生物修复研究提供参考。     

重金属污染下龟壳攀鲈组织中ACP和AKP的活力比较

龟壳攀鲈是一种在极端污染水域中具备生存优势的鱼类,收集重污染区和轻污染区的龟壳攀鲈,并通过比较其体内各组织中的酸性磷酸酶(ACP)及碱性磷酸酶(AKP)活性来揭示其耐污能力。贵屿作为重污染区有4个采样点:大陇村、市上村、联堤村和北林村;潮州作为轻污染区有2个采样点:卧石村和洗马桥。水质结果表明,贵屿采样地水中的Pb、Cd、Cr、As、Hg含量分别是潮州采样点的27.6倍、3.9倍、5.8倍、3.9倍和3.5倍,说明贵屿采样地的污染远高于潮州的。酶活结果表明,在龟壳攀鲈所有组织中,内脏组织(胃肠、性腺、肝脏、脾脏、肾脏)中的ACP和AKP活力均高于外周组织(肌肉、鳞片、鳃);重金属污染均能提高攀鲈体内所有组织的ACP和AKP活力;AKP活性更容易受到重金属的影响,各组织的AKP活力增幅普遍超过ACP活力增幅;其中,受重金属影响最大的组织是脾脏,ACP和AKP活力可增长到2.37倍和6.21倍。这些结果说明了龟壳攀鲈可以通过显著升高内脏组织(如肠胃、肝脏、肾脏等)中ACP和AKP活性,以便更好地应对高污染环境;其中AKP更容易受到重金属的影响,适合用于作为评估污染的指标。     

腐殖酸与典型碳纳米材料协同光致产生活性氧物种的研究

采用电子自旋共振光谱(EPR)技术,分析腐殖酸在光照下对4种典型碳纳米材料诱导产生单线态氧(~1O_2)和羟基自由基(·OH)的影响。基于密度泛函理论计算4种典型碳纳米材料的前线轨道能,比较了它们分别经能量转移诱导产生~1O_2的能力以及经电子传递诱导产生·OH的能力。结果显示,4种不同形状的碳纳米材料(富勒烯、单壁碳纳米管、多壁碳纳米管以及石墨烯)悬浮液在紫外光照下均无~1O_2和·OH产生。与腐殖酸共同存在下,4种碳纳米材料均显著诱导~1O_2的产生,且富勒烯和石墨烯还能光致生成·OH。协同产生~1_O2的能力大小为:单壁碳纳米管富勒烯多壁碳纳米管石墨烯,协同产生·OH的能力大小为:石墨烯富勒烯。~1O_2的产生能力与碳纳米材料的能隙大小和颗粒聚集程度有关,而诱导产生·OH的能力主要取决于化学硬度。总之,我们的研究表明腐殖酸与碳纳米颗粒可协同产生活性氧物种。     

Wastewater-nitrogen removal using polylactic acid/starch as carbon source: Optimization of operating parameters using response surface methodology

The use of PLA/starch blends for nitrogen removal was achieved. The influence of different operating parameters on responses was verified using RSM. The conditions for desired responses were successfully optimized simultaneously. Blends material may have a promising application prospect in the future. Nitrogen removal from ammonium-containing wastewater was conducted using polylactic acid (PLA)/starch blends as carbon source and carrier for functional bacteria. The exclusive and interactive influences of operating parameters (i.e., temperature, pH, stirring rate, and PLA-to-starch ratio (PLA proportion)) on nitrification (Y₁), denitrification (Y₂), and COD release rates (Y₃) were investigated through response surface methodology. Experimental results indicated that nitrogen removal could be successfully achieved in the PLA/starch blends through simultaneous nitrification and denitrification. The carbon release rate of the blends was controllable. The sensitivity of Y₁, Y₂, and Y₃ to different operating parameters also differed. The sequence for each response was as follows: for Y₁, pH>stirring rate>PLA proportion>temperature; for Y₂, pH>PLA proportion>temperature>stirring rate; and for Y₃, stirring rate>pH>PLA proportion>temperature. In this study, the following optimum conditions were observed: temperature, 32.0°C; pH 7.7; stirring rate, 200.0 r·min^-1; and PLA proportion, 0.4. Under these conditions, Y₁, Y₂, and Y₃ were 134.0 μg-N·g-blend^-1·h^-1, 160.9 μg-N·g-blend^-1·h^-1, and 7.6 × 10³ μg-O·g-blend^-1·h^-1, respectively. These results suggested that the PLA/starch blends may be an ideal packing material for nitrogen removal.     

Effects of water quality on the coagulation performances of humic acids irradiated with UV light

The presence of humic acid in drinking water treatment has received significant attention in recent years because of its adverse effects on the removal of many pollutants in coagulation. In this paper, the effects of water quality including pH, turbidity, alkalinity, and hardness on the removal of humic acid were investigated in a UV light hybridized coagulation process. Our results suggested that UV light radiation could effectively improve the removal rate of humic acid in coagulation under both neutral and basic conditions, and the variations of the selected water quality parameters had little adverse effect on the function of UV light. After UV light radiation, the removal rate of the nitro-humic acid (NHA) increased from 20% to 60% in coagulation, and increased further to 75% and 85% for the raw waters with 10.0 NTU kaolin and 100 mg·L^-1 hardness, respectively. In addition to NHA, the removal rates of the humic acid extracted from peat coal (PHA) and the humic acid provided by Japan metals and chemicals company (JHA) in coagulation were also improved, both in the range of 80%–90% after undergoing UV light radiation. By changing the radiation location from prior to coagulation to the flocculation process, similar experimental results were obtained. The formation of positive charged sites after UV light radiation was considered to be the primary factor that led to an enhanced removal of the humic acid in coagulation.     

Effect of effluent organic matter on ozonation of bezafibrate

The influence of three effluent organic matter (EfOM) model compounds, humic acid (HA), bovine serum albumin (BSA), and sodium alginate (AGS), on the ozonation of bezafibrate (BF), a typical pharmaceutical and personal care product (PPCP), was investigated. The results show that ozonation efficiently removed BF from aqueous solution with removal efficiencies>95% within 8 min for all conditions. The reaction rate of BF decreased with increasing model compounds concentrations and the influence was more pronounced for HA and BSA, while less pronounced for AGS. Although BF concentration was significantly reduced, the degree of mineralization achieved was only approximately 11%. The addition of HA and BSA improved the mineralization of the solution, while the influence of AGS was minor. The acute toxicity of BF solution during ozonation was determined using the Luminescent bacteria test, and the toxicity exhibited an initial increase and a successive reduction. An overall decreased acute toxicity was observed with an increase of HA. The presence of BSA increased the formation rate of toxicity intermediates and resulted in inhibition peak forward.     

硅藻土强化混凝去除铜绿微囊藻的影响因素研究

以原水中常见的铜绿微囊藻为研究对象,研究了联合硅藻土与聚合氯化铝(PAC)强化混凝去除铜绿微囊藻的效果.考察了PAC和硅藻土的投加量、溶液pH值、天然有机物腐植酸(HA)对藻和浊度去除的影响,并用zeta电位分析方法对混凝剂的静电中和能力进行表征.结果表明:硅藻土具有良好的助凝作用,投加其有助于改善絮体的沉降性能,提高铜绿微囊藻的混凝去除效果,PAC为6mg/L,pH值为7~8,硅藻土投加量为30mg/L时,叶绿素a(Chl-a)去除率可达96%,剩余浊度低于0.9NTU. HA存在会明显抑制铜绿微囊藻的混凝去除,当HA浓度大于1.0mg/L时, Chl-a去除率大幅度下降同时剩余浊度明显上升,硅藻土的投加可以在一定程度上缓解负面作用.     

亲水荷电超滤膜的制备及对腐殖酸的分离性能

为改善聚醚砜(PES)超滤膜的抗污染性能和提高对腐殖酸(HA)的截留率,以介孔二氧化硅(MS)为添加剂,采用相转化法制备了亲水性PES/MS复合超滤膜,并对膜表面进行荷电改性.研究了MS对膜的断面结构、表面化学性质和过滤性能的影响,考察了荷电改性PES/MS超滤膜对水中HA的分离性能以及溶液pH值、离子强度和钙离子浓度等因素对荷电膜超滤过程的影响.SEM表征结果显示,MS颗粒在PES/MS复合膜的表面分散均匀,膜孔的连通性改善.亲水荷电改性后,膜表面接触角由68°降至57°,zeta电位由-6.31mV降至-11.45mV,膜对HA的去除率由72%提高到95%,通量衰减率由29.8%减小到4.9%.结果表明,对PES超滤膜进行亲水荷电改性可有效提高对HA的截留率,同时减轻膜污染;另外,溶液的pH值、离子强度和钙离子浓度对荷电超滤膜的过滤性能有较大影响,调节合适的溶液环境可在提高截留率的同时,减轻膜污染.     

稀酸预处理铜藻制备生物乙醇工艺

选取暖温带海洋生态环境生物修复的首选物种——铜藻(Sargassum horneri)为原料进行生物乙醇的制备,以稀硫酸水解后的还原糖收率为响应值,考察水解温度、液固比、水解时间和w(H₂SO₄)等参数对水解效率的影响. 为优化稀酸水解铜藻预处理的工艺条件,在单因素试验的基础上,利用Box-Benhnken中心组合设计法和响应面分析法,建立稀酸预处理工艺参数的回归模型,并与酶水解及发酵相结合验证了铜藻稀酸预处理效果. 结果表明:①稀酸水解铜藻的最优工艺参数. 水解温度为120 ℃,液固比为20∶1,水解时间为2.00 h,w(H₂SO₄)为4.50%. ②稀酸水解铜藻过程中各影响因素之间存在交互作用,水解时间和w(H₂SO₄)的非线性作用显著. ③对经最佳稀酸预处理工艺处理后的铜藻粉进行酶水解,其还原糖收率为44.05%,是未预处理下的8.14倍,并且后续进行发酵后,乙醇产率达7.80%,是未预处理下的2.00倍. 表明铜藻是一种潜在的生物乙醇原料,稀酸预处理方法对铜藻生物乙醇的制备行之有效.      

致癌性卤代醌介导的脂质氢过氧化物分解的分子机制

卤代醌是许多卤芳香持久有机污染物的致癌代谢产物和饮用水消毒副产物.13-过氧羟基-9,11-十八碳二烯酸(13-HPODE)是最为广泛研究的内源性脂质过氧化物.众所周知,过渡金属离子可以催化分解13-HPODE,但尚不清楚卤代醌是否可以通过不依赖金属离子的途径促进其分解;若是如此,又有什么特异性和相似性?我们发现卤化醌如2,5-二氯-1,4-苯醌(DCBQ)可显著促进13-HPODE的分解.综合采用电子自旋共振-自旋捕获、HPLC-MS和GC-MS等分析方法,可检测到反应形成的脂质烷基自由基如戊烷基自由基、7-羧甲基自由基以及具有基因毒性的4-羟基-2-壬烯醛(HNE)等.在DCBQ和13-HPODE的反应中也能检测到两种氯醌-脂质烷氧基耦合物.我们认为卤代醌促进内源性脂质过氧化物13-HPODE分解生成活性脂质烷基自由基和基因毒性的HNE是通过一类新型的金属非依赖亲核取代与裂解机理来实现的,这也在一定程度上解释了其潜在的基因毒性和致癌性.