钯/铁双金属对土壤中2,2′,3,4,4′,5,5′-七氯联苯的催化脱氯研究

采用Fe⁰还原、钯催化法对土壤中2,2′,3,4,4′,5,5′-七氯联苯的的还原特性进行了实验研究.结果表明,Pd/Fe双金属能有效地进行2,2′,3,4,4′,5,5′-七氯联苯的催化脱氯.在钯化率为0.05%、钯/铁加入量1g、初始pH为5.6、反应时间5 d的条件下,钯/铁双金属对土壤中2,2′,3,4,4′,5,5′-七氯联苯去除率达54%.实验还考察了钯化率、初始pH、反应时间、钯/铁投加量、2,2′,3,4,4′,5,5′-七氯联苯初始浓度等参数对2,2′,3,4,4′,5,5′-七氯联苯脱氯效果的影响.研究表明,较高的钯化率、钯/铁加入量,较低的2,2′,3,4,4′,5,5′-七氯联苯初始浓度及弱酸性等条件更有利于Pd/Fe对2,2′,3,4,4′,5,5′-七氯联苯的还原脱氯.在Pd/Fe双金属表面,2,2′,3,4,4′,5,5′-七氯联苯的脱氯符合一级动力学反应,反应速率常数为0.014 2/h,其半衰期为49h.利用实验数据,对钯/铁双金属作用下的2,2′,3,4,4′,5,5′-七氯联苯还原脱氯的反应机制也进行了分析.     

碳纳米管改性PVDF中空纤维超滤膜处理二级出水抗污染性能研究

采用碳纳米管改性PVDF中空纤维超滤膜以缓解膜污染.考察了CNTs的乙醇分散液浓度、CNTs尺寸和负载量对改性中空纤维膜的抗污染性能和改性膜内表面CNTs层稳定性的影响,分析了该改性膜对二级出水DOC、UV254的去除效果,并对改性膜出水的荧光特性进行了表征.结果表明,选用体积分数为50%的乙醇分散液、外径为30~50 nm碳纳米管、负载量为3 g·m-2时,制备的改性中空纤维膜CNTs层稳定,抗污染能力显著提高.与未改性膜相比,改性膜对二级出水DOC和UV254的去除率分别提高了37%和56%;且对二级出水中的腐殖类和蛋白质类物质去除能力明显增强.     

钯/泡沫镍对水体中4-氯酚的氢解脱氯研究

采用置换沉积法制备泡沫镍负载钯(Pd/Ni)催化剂,研究了其在H2作为供氢体时对水相中4-氯酚(4-CP)的催化氢解脱氯作用.考察了Pd负载量、H2流量和反应液pH值对4-CP转化率的影响.结果表明,在相对较低的Pd负载量和H2流量下即可实现4-CP的快速高效去除,且反应液pH值在3.04~10.97的范围对反应影响不显著.当Pd负载量为0.1%、H2流量为10mL/min、pH值为6.80时,反应1h,4-CP转化率达92.6%.Pd/Ni具有较高的稳定性,重复实验表明,该催化剂使用3次后,催化活性仅下降了2.0%.     

城市污水二级出水超滤膜污染与膜特性的研究

以城市污水二级出水为过滤介质,考察了PVA、PVP、PMMA等与PVDF的二元及三元共混超滤膜的过滤污染行为.结果表明,共混优化了PVDF超滤膜的结构参数,添加剂PVP、PVA可有效改善膜的亲水化程度,提高膜渗透通量.超滤膜的亲水性和结构特性对膜抗污染性能影响较大;堵孔阻力是二级出水过滤膜污染不可逆的主要原因.亲水性较强的超滤膜,二级出水过滤初期易因浓差极化而导致滤饼层污染,造成一定的通量衰减,但易清洗恢复,不可逆污染指数(rir)为0,抗污染性能好.致密的超滤膜表面有利于防止二级出水中的中低分子量污染物进入膜内部,而断面通透大孔和疏松海绵层结构的超滤膜,能减少二级出水中的污染物在膜中沉积形成堵孔阻力.膜表面多孔,内部大孔发育不充分,易形成堵孔污染,通量衰减大且不易清洗恢复,膜污染不可逆.     

三维Pd/OMC粒子电极体系电催化泛影酸盐还原脱碘研究

以泛影酸盐(DTZ)的高效还原脱碘为目标,通过硼氢化钠还原法制备钯负载有序介孔碳(Pd/OMC)作为粒子电极,以碳纤维(CFP)电极作为主阴极,建立了三维电极电催化还原体系.该体系在低阴极电位下(-0.6～-0.8 V)可实现电化学/感应电化学的耦合还原,其脱碘速率是单独阴极体系的2.38～3.65倍;在阴极电位高于析氢电位(-1.5 V)时,可实现电化学/感应电化学/化学催化加氢多还原过程协同去除碘代有机物,其反应速率为单独阴极体系的1.27～4.69倍.进一步研究了DTZ初始浓度、Pd/OMC投加量及Pd的负载量对DTZ还原去除的影响.电化学测试结果表明三维电化学体系具有良好的电子传递能力与电还原性能.利用自由基淬灭实验与ESR自由基捕获对活性还原物种分析,表明原子H~*在三维电化学还原脱碘过程中起重要作用.     

Pd/CeO2催化水中溴酸盐的加氢还原研究

采用溶胶-凝胶法制备了CeO2载体,以浸渍法和沉积沉淀法制备了负载型催化剂Pd/CeO2.使用透射电镜(TEM)和Zeta电位仪对催化剂进行了表征.结果表明两种材料的等电点都在5.0左右; Pd颗粒在载体表面具有良好的分散性,且Pd负载量越高,Pd颗粒的粒径越大.采用Pd/CeO2催化剂催化溴酸盐加氢还原,发现在溴酸盐初始浓度为0.39mmol/L时,采用沉积沉淀法和浸渍法合成的Pd/CeO2催化剂反应50min后对溴酸盐的去除率分别为100%和71%,表明使用沉积沉淀法合成的催化剂具有较高的催化活性.改变催化剂用量,溴酸盐的催化还原速率不受传质阻力的影响,反应过程符合Langmuir–Hinshelwood模型,即催化还原反应由溴酸盐在催化剂表面的吸附控制.增加Pd的负载量,溴酸盐的还原速率增大.溶液pH值较低时,有利于对溴酸盐的催化还原.     

Enhanced catalytic degradation process of o-nitrochlorobenzene by palladium-catalyzed Fe0 particles

Over Pd/Fe bimetallic catalyst, o-nitrochlorobenzene（o-NCB）, at a concentration of 20 mg/L in aqueous solutions, is rapidly converted to o-chloroaniline（o-CAN） first, and then quickly dechlorinated to aniline（AN） and Cl^- , without other intermediate reaction products. The aminated and dechlorinated reactions are believed to take place on the surface site of the Pd/Fe. The o-NCB removal efficiency and the next dechlorination rate increase with an increase of bulk loading of palladium and catalysts addition due to the increase of both the surface loading of palladium and the total surface area. These results indicate that reduction, amination and dechlorination of o- NCB by palladium-catalyzed Fe^0 particles, can be designed for remediation of contaminated groundwater.     

基于微气泡曝气的生物膜反应器处理废水研究

微气泡曝气有助于强化氧传质过程,在废水好氧生物处理中具有潜在的应用优势;生物膜反应器是应用微气泡曝气的可行工艺形式.本研究在生物膜反应器中采用SPG膜微气泡曝气处理模拟生活废水,探讨反应器连续运行过程中,SPG膜空气通透性、溶解氧变化、污染物去除效果及氧利用情况.结果表明,基于SPG膜微气泡曝气的生物膜反应器能够实现长期连续稳定运行,是微气泡曝气与废水好氧生物处理结合的可行方式.SPG膜表面性质及膜孔径影响其空气通透性,疏水性膜的空气通透性优于亲水性膜;膜孔径越大,空气通透性越好.一定的SPG膜空气通量下,反应器内的溶解氧浓度主要受有机负荷影响.SPG膜微气泡曝气生物膜反应器较优的COD处理负荷(以SPG膜面积计算)为6.88 kg·(m2.d)-1.氨氮的去除主要受溶解氧浓度及生物膜内氧扩散传质的影响,在高有机负荷下生物膜内出现同步硝化反硝化.微气泡曝气的氧利用率显著高于传统曝气方式,在优化的运行条件下,氧利用率可以接近100%.     

无机微滤膜分离草浆黑液中木素的机理

选用50nm,0.2μm和0.8μm的无机微滤膜,研究了它们对黑液中木素的截留效果.结果表明,微滤膜能够有效地分离黑液中的木素,0.2μm α-Al₂O₃和ZrO₂膜的通量高于50nm和0.8μm膜的通量,当黑液SS较低时,随着SS浓度的增加各个微滤膜的通量急剧下降,当SS较高时,微滤膜的通量和SS浓度成线性关系.2g/L聚乙二醇4000(PEG4000)溶液不会显著影响0.2μm和50nm膜的通量,但却能使0.8μm膜的通量下降60%.2g/L聚乙二醇20000(PEG20000)溶液能使各个微滤膜的通量急剧下降.按照微滤膜污染模型的计算结果和实测被稀释黑液的粒径分布,膜面形成滤饼层和木素分子形成的絮体是引起膜通量下降并改变了膜的截留性能的原因.     

Pd/Al2O3粒子电极电催化还原BrO3-的研究

针对常规方法难以去除水中Br_3~-的问题,采用浸渍煅烧法制备了负载型纳米Pd/Al_2O_3粒子电极,研究了该电极电催化还原Br O-3的效果.催化剂的结构表征表明该反应实现了Pd纳米晶的均匀负载,纳米Pd/Al_2O_3具有较高的电催化活性和较低的能耗,其最佳反应条件为3%Pd负载量,0.9 m A·cm-2电流密度和1 g·L催化剂投量,酸性条件可促进Br O-3的直接或间接还原.ESR检测证实了Pd的负载增强了反应体系活性物种[H]的生成,进而促进了Br O-3的间接电催化还原.     

Catalytic dechlorination of chlorobenzene in water by Pd/Fe bimetallic system

IntroductionChlorinatedorganiccompoundshavebeenusedonalargescaleinthechemical,petrochemical,andelectronicindustries.Inrecentyears ,worldwideattentionhasbeengiventotheenvironmentalandhealthimpactofthemasaclassofcontaminants .Severalareknowntocauseozonedepletion ,whileothersproduceadverseeffectsonthehumancentralnervoussystemandhavebeenlinkedtodiseasessuchascancer.Almostallofthechlorinatedaromaticcompoundsaretoxicandthermallystable .Oncereleasedintoenvironment,theywillaccumulateinthesurroundings…     

Preparation and characterization of Pd/Fe bimetallic nanoparticles immobilized on Al2O3/PVDF membrane: Parameter optimization and dechlorination of dichloroacetic acid

Using a liquid–solid phase inversion method, a hybrid matrix poly(vinylidene fluoride)(PVDF) membrane was prepared with alumina(Al2O3) nanoparticle addition. Pd/Fe nanoparticles(NPs) were successfully immobilized on the Al2O3/PVDF membrane, which was characterized by Scanning Electron Microscopy(SEM) and Transmission Electron Microscopy(TEM). The micrographs showed that the Pd/Fe NPs were dispersed homogeneously. Several important experimental parameters were optimized, including the mechanical properties, contact angle and surface area of Al2O3/PVDF composite membranes with different Al2O3 contents. At the same time, the ferrous ion concentration and the effect of hydrophilization were studied. The results showed that the modified Al2O3/PVDF membrane functioned well as a support. The Al2O3/PVDF membrane with immobilized Pd/Fe NPs exhibited high efficiency in terms of dichloroacetic acid(DCAA) dechlorination. Additionally, a reaction pathway for DCAA dechlorination by Pd/Fe NPs immobilized on the Al2O3/PVDF membrane system was proposed.     

TiO_2光催化降解活性艳兰KN-R的研究

以纳米TiO2为光催化剂,以活性艳兰KN-R为模拟染料废水,研究了溶液pH值、TiO2投加量、H2O2用量及染料初始浓度对染料脱色率的影响。结果表明,活性艳兰KN-R的脱色率随溶液pH值的升高及染料初始浓度的降低而增大;TiO2和H2O2的投加量均存在一个最佳值,在本实验条件下,它们分别为0.5g/L和2.0×10-2mol/L,低于或超过该值都会导致染料脱色率的下降。在适宜的操作条件下,活性艳兰KN-R的脱色率可达98%以上,化学需氧量(COD)的去除率在70%以上。     

Effects of ion concentration and natural organic matter on arsenic(V) removal by nanofiltration under different transmembrane pressures

The removal of As(V) from synthetic water was studied using four different nanofiltration (NF) membranes (ESNA-1-K1, NF270, ESNA-1-LF, and HODRA-CORE). The influences of ion concentration, transmembrane pressure (TMP), and the presence of natural organic matter (humic acid, HA) on the arsenic removal efficiency and permeate flux were investigated. The arsenic rejection of ESNA- 1-LF was higher than those of the other membranes in all experiments (> 94%), and the HODRA-CORE membrane gave the lowest removal of arsenic (< 47%). An increase in the ion concentration in the feed solution and addition of HA decreased the arsenic rejection of the HODRA-CORE membrane. However, both increasing of the ion concentration and addition of HA made the rejection increased for the other membranes (ESNA-1-K1, NF270, and ESNA-1-LF). With increasing TMP, for all four NF membranes, increases in both arsenic rejection and permeate flux were observed. The permeate fluxes of the four NF membranes decreased to some extent after addition of HA to the solutions for operating time of 6 hr.     

铁阳极电凝聚处理活性黑KN-B染料废水动力学分析

采用铁为阳极的原位电凝聚方法处理活性黑KN-B染料废水。以活性黑KN-B在特征吸收波长600nm和255nm的吸光度变化为分析指标,考察了电流密度、染料溶液初始pH值、电介质浓度及种类、温度、染料浓度等影响因素对染料废水脱色过程及脱色速率常数的影响。同时根据化学反应动力学理论对其脱色的动力学过程及脱色机理进行了初步探讨与分析。实验结果表明:染料溶液的脱色反应符合一级反应动力学过程;电流密度、染料浓度、染料溶液初始pH值及电解质的种类及浓度对一级反应速率常数影响显著,而染料溶液温度对一级反应速率常数的影响较小;染料废水的脱色过程是电凝聚和染料还原共同作用的过程。     

Preparation, characterization and performance of poly(m-phenylene isophthalamide)/organically modified montmorillonite nanocomposite membranes in removal of perfluorooctane sulfonate

Nanocomposite membranes containing poly(m-phenylene isophthalamide) (PMIA) and organically modified montmorillonite (OMMT) were prepared by a combination of solution dispersion and wet-phase inversion methods, and the effects of OMMT addition on the properties and performance of fabricated nanofiltration membranes were investigated. The membranes were characterized by contact angle measurements, scanning electron microscopy (SEM), atomic force microscopy (AFM), thermogravimetric analysis, and zeta potential. The performance of the membranes was elucidated by the removal of perfluorooctane sulfonate (PFOS) at neutral pH. Increasing OMMT concentration improved the thermal stability and hydrophilicity of the membranes. The permeation and rejection of PFOS were significantly improved. The performance of fabricated nanofiltration membranes in removal of PFOS varied depending on the solute and membrane properties as well as solution conditions. Finally, a comparison between fabricated membranes and a commercial NF membrane (ESNA1-K1, Hydecanme) proved that the OMMT addition is a convenient procedure for producing nanocomposite membranes with superior properties and performance.     

海藻酸钠固定化纳米铁还原脱色活性红X3B

采用海藻酸钠固定纳米铁制备海藻酸钠纳米铁小球,研究了海藻酸钠浓度、纳米铁含量、活性红X3B浓度、反应温度、pH值等对海藻酸钠固定化纳米铁小球还原活性红X3B的影响.采用高效液相色谱（HPLC）、紫外可见分光光度计（UV-Vis）、扫描电镜（SEM）、透射电镜（TEM）等方法分析污染物的还原脱色过程.结果表明,X3B的还原脱色获得了较好的效果,当温度25.0℃,海藻酸钠浓度2.0%,纳米铁含量2.0g/L,转速200r/min,pH值10.9时,反应720min后,25.0mg/L活性红X3B的脱色率达98.9%.海藻酸钠凝胶对活性红X3B没有吸附作用,海藻酸钠固定化纳米铁小球降解活性红X3B的主要机制为纳米零价铁的还原作用.     

不同因素对平板膜污泥浓缩工艺膜污染演变的影响研究

以临界通量表征膜污染趋势,利用响应面模型考察污泥浓度、膜间距和曝气量对上下层膜组件的膜污染影响,发现响应面模型具有较好的显著性和拟合性,且污泥浓度、膜间距和曝气量均对上下层膜组件膜污染有显著影响。同时发现,随着污泥浓度的增加上下层膜组件临界通量大幅下降;而在不同污泥浓度下,曝气量和膜间距的变化对上下层膜组件膜污染的变化有不同的影响。利用模型模拟获得了不同污泥浓度下的最优化参数,在四段式平板膜污泥浓缩中试运行中获得了较好的效果。     

二级SBR系统处理染料废水长期运行的稳定性

考察了处理染料废水的二级SBR系统在连续运行120个周期过程中的稳定性.系统的运行先后经历了低染料浓度和高染料浓度2种情况.试验发现在长期运行过程中,二级SBR系统对进水水质及操作条件具有良好的适应性;能够有效去除废水中的污染物,对染料的平均去除率为81%～92.5%,对COD的平均去除率为89.4%～93.1%;出水水质比较稳定.在二级SBR系统中,厌氧污泥活性高,降解污染物能力强;好氧活性污泥形成团簇状结构,有利于稳定出水水质.     

Pd/CeZr/TiO2/Al2O3蜂窝状金属丝网催化剂选择催化还原NOX

采用溶胶-凝胶法和浸渍法制备了Pd/CeZr/TiO2Al2O3蜂窝状金属丝网催化剂,并将其应用于在富氧条件下以丙烯选择催化还原NOx的研究.利用扫描电镜(SEM)分析了钛酸四丁酯的含量以及涂敷次数对TiO2涂层的影响,系统地考察了Pd含量、氧气浓度和空速对蜂窝状金属丝网催化剂催化性能的影响.实验结果表明,采用钛酸四丁酯的含量为20.0%的溶胶,涂敷2次,可以在金属丝网载体上氧化铝涂层表面获得均匀、无皲裂的TiO2涂层;Pd含量在0.23%～1.06%的范围内, NOx的转化率随Pd含量的增加而减小, Pd含量为0.23%时, NOx表现最高的NOx转化率;反应气体中氧气浓度从1.5%增加到6.0%, NOx的转化率随氧气浓度的增加而增大,当氧气浓度高于6.0%, NOx的转化率则随氧气浓度的增加而迅速减小; NOx的转化率随着空速的增加而降低,在高温条件下空速对转化率的影响要大于在低温条件下.