MnFe2O4@HTC活化过硫酸盐体系除藻效能与机制

采用水热法和共沉淀法将MnFe₂O₄负载在水热炭（HTC）表面制备磁性MnFe₂O₄@HTC复合催化剂.采用SEM、XRD、BET、FTIR、XPS对催化剂进行表征,通过考察MnFe₂O₄/HTC负载比、过硫酸钠（PS）投加量、初始pH和不同化学体系对除藻效果的影响,探究无供氧条件下MnFe₂O₄@HTC活化PS体系除藻的效能.基于自由基屏蔽实验和XPS分析对MnFe₂O₄@HTC活化PS体系反应机制进行研究验证.结果表明,当初始藻浓度为1.4×10⁹个·L^-1（OD₆₈₀=0.14）,催化剂投加量为0.2 g·L^-1,PS投加量为0.4 g·L^-1,pH为6时,降解30 min,该体系除藻率可达到99%.在该体系中,MnFe₂O₄@HTC材料可将藻细胞吸附在材料表面,通过Mn、Fe的价态循环和HTC的协同效应反应催化PS产生空穴、¹O₂、·O₂^-、SO₄^-·和·OH多种氧化物质,使藻细胞破裂死亡.     

基于MGWR模型的中国城市PM2.5影响因素空间异质性

基于全国297个地级市2018年PM_2.5浓度数据、自然与社会经济数据,采用多尺度地理加权回归（MGWR）模型分析了各影响因素对PM_2.5浓度的作用尺度与影响效果的空间异质性.结果表明,MGWR模型适用于中国地级市PM_2.5浓度影响因素研究.在作用尺度上,人均GDP、技术支持水平作用尺度最大,其次是相对湿度、居民地比重、人口密度与风速,降水量、第二产业比重、植被覆盖状况、温度与能源消费强度作用尺度最为局限.在影响效果上,相对湿度、人口密度与居民地比重全部为正向作用;第二产业比重和能源消费强度主要为正向作用,分别占总样本的70.71%与64.98%;风速、温度既存在正向作用也存在负向作用,空间上呈两极分化,其中正向作用分别占总样本的49.83%与57.91%;降水量、植被覆盖状况主要为负向作用,分别占总样本的91.58%与69.70%;人均GDP、技术支持水平全部为负向作用.研究结果表明各因素对于中国城市PM_2.5浓度的影响均存在着不同程度的空间异质性.     

基于HYSPLIT4模式的天水市颗粒物输送路径

首先利用后向轨迹模式（HYSPLIT）模拟了天水市2017~2019年冬季后向轨迹,分析了50,200,500和1000m 4个不同高度以及500m高度不同聚类数量对路径输送聚类统计结果的影响,并以500m高度四个季节的后向轨迹进行聚类分析,进一步运用权重潜在源贡献分析法（WPSCF）,探讨了研究期间天水市细颗粒物的潜在源区及不同源区对天水市颗粒物浓度的贡献,结果表明,（1）起始点高度为500m时,颗粒物浓度极值比和极值差均较大,聚类结果最具代表性;（2）不同聚类数量分析结果表明,按照总空间变化（Total spatial variation,TSV）显著增加的原则选取的聚类数量较少,且能反映不同方向的轨迹输送特征;（3）天水市不同季节的轨迹聚类结果表明,冬季来自陕西南部的东南路径是PM_2.5污染程度最高的路径,该路径下PM_2.5浓度为78.2μg/m³,春季西北路径的颗粒物浓度最高,PM₁₀和PM_2.5的平均浓度分别是127.9~129.9和40.6~41.0 μg/m³,夏秋季节不同路径的颗粒物浓度相差不大.     

光催化与生物膜直接耦合降解4-氟苯酚废水

为了实现4-氟苯酚（4-FP）废水的快速持续降解,本文构建了光催化与生物膜直接耦合系统.该耦合系统由N掺杂TiO₂涂覆光催化光纤束、生物膜、核孔膜和紫外-可见LED光源构成.实验研究了单独光催化、单独微藻生物膜及光催化-生物膜耦合3种体系对4-FP的降解性能.研究发现：光催化系统降解4-FP速率慢、脱氟效率低,12h内降解率为94.3%,脱氟率仅为24.7%.微藻生物膜在第一个周期内对4-FP的降解性能高于单独光催化,10h内降解率达到98.9%,脱氟率达到90.9%,但3个周期后4-FP降解率降低至75.5%,脱氟率降低至69.5%.在耦合系统中,生物膜中微生物种群发生了自适应调整,富集了大量的红球菌、假单胞菌和无色杆菌,导致了光催化、生物降解及光合作用三者亲密协作,实现了4-FP快速持续地降解,运行12个周期后,5h即可将4-FP完全降解,同时溶解有机碳及脱氟率分别达到89.4%和78.3%.     

Aging of PVDF and PES ultrafiltration membranes by sodium hypochlorite: Effect of solution pH

Sodium hypochlorite (NaClO) is a commonly applied cleaning agent for ultrafiltration membranes in water and wastewater treatment. Long-term exposure to NaClO might change the properties and performance of polymeric membranes, and ultimately shorten membrane lifespan. Active species in NaClO solution vary with solution pH, and the aging effects can change depending on the membrane material. In this study, the aging of polyvinylidene fluoride (PVDF) and polyethersulfone (PES) membranes by NaClO at pH 3–11 was investigated by examining variations in chemical composition, surface charge, surface morphology, mechanical strength, permeability, and retention ability. Polyvinyl pyrrolidone (PVP), which was blended in both membranes, was oxidized and dislodged due to NaClO aging at all investigated pH values, but the oxidation products and dislodgement ratio of PVP varied with solution pH. For the PVDF membrane, NaClO aging at pH 3–11 caused a moderate increase in permeability and decreased retention due to the oxidation and release of PVP. The tensile strength decreased only at pH 11 because of the defluorination of PVDF molecules. For the PES membrane, NaClO aging at all investigated pH resulted in chain scission of PES molecules, which was favored at pH 7 and 9, potentially due to the formation of free radicals. Therefore, a decrease in tensile strength and retention ability, as well as an increase in permeability, occurred in the PES membrane for NaClO aging at pH 3–11. Overall, the results can provide a basis for selecting chemical cleaning conditions for PVDF and PES membranes.     

Green and efficient degradation of cefoperazone sodium by Bi4O5Br2 leading to the production of non-toxic products: Performance and degradation pathway

Photocatalytic process represents a promising approach to overcome the pollution challenge associated with the antibiotics-containing wastewater. This study provides a green, efficient and novel approach to remove cephalosporins, particularly cefoperazone sodium (CFP). Bi₄O₅Br₂ was chosen for the first time to systematically study its degradation for CFP, including the analysis of material structure, degradation performance, the structure and toxicity of the transformation products, etc. The degradation rate results indicated that Bi₄O₅Br₂ had an excellent catalytic activity leading to 78% CFP removal compared with the pure BiOBr (38%) within 120 min of visible light irradiation. In addition, the Bi₄O₅Br₂ presents high stability and good organic carbon removal efficiency. The effects of the solution pH (3.12 - 8.75) on catalytic activity revealed that CFP was mainly photocatalyzed under acidic conditions and hydrolyzed under alkaline conditions. Combined with active species and degradation product identification, the photocatalytic degradation pathways of CFP by Bi₄O₅Br₂ was proposed, including hydrolysis, oxidation, reduction and decarboxylation. Most importantly, the identified products were all hydrolysis rather than oxidation byproducts transformed from the intermediate of β-lactam bond cleavage in CFP molecule, quite different from the mostly previous studies. Furthermore, the final products were demonstrated to be less toxic through the toxicity analysis. Overall, this study illustrates the detailed mechanism of CFP degradation by Bi₄O₅Br₂ and confirms Bi₄O₅Br₂ to be a promising material for the photodegradation of CFP.     

Degradation of poly(butylene adipate-co-terephthalate) by Stenotrophomonas sp. YCJ1 isolated from farmland soil

In recent years, poly (butylene adipate-co-terephthalate) (PBAT) has been widely used. However, PBAT-degrading bacteria have rarely been reported. PBAT-degrading bacteria were isolated from farmland soil and identified. The effects of growth factors on the degradation of PBAT and the lipase activity of PBAT-degrading bacteria were assessed. The degradation mechanism was analyzed using scanning electron microscopy, attenuated total reflection Fourier transform infrared spectroscopy, proton nuclear magnetic resonance, X-ray diffraction, and liquid chromatography-mass spectrometry. The results showed that Stenotrophomonas sp. YCJ1 had a significant degrading effect on PBAT. Under certain conditions, the strain could secrete 10.53 U/mL of lipase activity and degrade 10.14 wt.% of PBAT films. The strain secreted lipase to catalyze the degradation of the ester bonds in PBAT, resulting in the production of degradation products such as terephthalic acid, 1,4-butanediol, and adipic acid. Furthermore, the degradation products could participate in the metabolism of YCJ1 as carbon sources to facilitate complete degradation of PBAT, indicating that the strain has potential value for the bioremediation of PBAT in the environment.     

Influence of particle size on the aggregation behavior of nanoparticles: Role of structural hydration layer

More and more attention has been paid to the aggregation behavior of nanoparticles, but little research has been done on the effect of particle size. Therefore, this study systematically evaluated the aggregation behavior of nano-silica particles with diameter 130–480 nm at different initial particle concentration, pH, ionic strength, and ionic valence of electrolytes. The modified Smoluchowski theory failed to describe the aggregation kinetics for nano-silica particles with diameters less than 190 nm. Besides, ionic strength, cation species and pH all affected fast aggregation rate coefficients of 130 nm nanoparticles. Through incorporating structural hydration force into the modified Smoluchowski theory, it is found that the reason for all the anomalous aggregation behavior was the different structural hydration layer thickness of nanoparticles with various sizes. The thickness decreased with increasing of particle size, and remained basically unchanged for particles larger than 190 nm. Only when the distance at primary minimum was twice the thickness of structural hydration layer, the structural hydration force dominated, leading to the higher stability of nanoparticles. This study clearly clarified the unique aggregation mechanism of nanoparticles with smaller size, which provided reference for predicting transport and fate of nanoparticles and could help facilitate the evaluation of their environment risks.     

Ag3PO4/g-C3N4复合光催化剂的制备及其可见光催化性能

采用简单的原位沉淀法合成了可见光驱动型光催化剂Ag₃PO₄/g-C₃N₄.利用X-射线衍射（XRD）、傅里叶红外光谱（FT-IR）、扫描电子显微镜（SEM）、X-射线能谱（XPS）以及紫外可见漫反射光谱（UV-Vis DRS）等表征手段对合成的样品进行了表征.与单一的Ag₃PO₄和g-C₃N₄相比,Ag₃PO₄/g-C₃N₄复合材料对左氧氟沙星表现出了更高的催化效率.根据能带分析和自由基捕获试验,提出了Ag₃PO₄/g-C₃N₄复合材料Z型异质结构的作用机制.     

Properties of a Poly(3-hydroxybutyrate) Depolymerase from Penicillium funiculosum

A poly(3-hydroxybutyrate) (PHB) depolymerase was purified from a fungus, Penicillium funiculosum (IFO6345), with phenyl-Toyopearl and its properties were compared with those of other PHB depolymerases. The molecular mass of the purified enzyme was estimated at about 33 kDa by sodium dodecyl sulfate (SDS) polyacrylamide gel electrophoresis. The pH optimum and pI were 6.5 and 6.5, respectively. The purified protein showed affinity to Con A-Sepharose, indicating that it is a glycoprotein. Diisopropylfluorophosphate and dithiothreitol inhibited the depolymerase activity completely. The N-terminal amino acid sequence of the purified enzyme was TALPAFNVNPNSVSVSGLSSGGYMAAQL, which contained a lipase box sequence. This purified enzyme is one of the extracellular PHB depolymerase which belong to serine esterase. The purified enzyme showed relatively strong hydrolytic activity against 3-hydroxybutyrate oligomers compared with its PHB-degrading activity. PHB-binding experiments showed that P. funiculosum depolymerase has the weakest affinity for PHB of all the depolymerases examined.