重捕剂SDTC的合成及其处理含铊废水的研究

以小分子胺类、二硫化碳和十二烷基苯磺酸钠(SDBS)为原料合成一种复配型重捕剂SDTC,用于处理烧结脱硫含铊废水。采用响应面法通过Box-Behnken(BBD)实验设计影响铊去除率的反应条件,对废水pH、SDTC投加量、反应时间和无机离子进行了优化分析,同时通过红外光谱和紫外光谱对SDTC及其与铊生成的螯合物(SDTC-Tl)结构进行表征。结果表明,二次多项式模型的回归系数R~2为0.982 8,模型对实验数据的拟合度高。采用响应面法优化得出处理1.20mg/L含铊废水的最佳条件并对其进行修正为:废水pH 9.00,SDTC投加量2.80g/L,反应时间25.0min,无机离子21.1g/L,该条件下铊去除率为99.89%,实验结果与模型预测值吻合。红外和紫外光谱分析结果表明,SDTC与铊会发生配位反应,生成的SDTC-Tl可较长时间放置,不易产生二次污染。     

一种新型铋基光催化剂的合成及其可见光催化性能

采用水热法合成铋基光催化剂Bi4VO8Br,通过X-射线粉末衍射、扫描电镜等手段对其进行表征.选择甲基橙为目标降解物来评价不同条件下合成的Bi4VO8Br在可见光下的光催化活性,发现pH 3、反应时间15 h、反应温度160℃为材料水热合成的最佳条件.考察了Bi4VO8Br在可见光及紫外光下对几种农药和增塑剂的光催化降解性能,显示了Bi4VO8Br对不易光解的含苯环有机物的可见光高活性.五氯酚的光催化过程影响因素优化结果表明,可见光和紫外光分别照射120 min和20 min,其降解率分别达到97％和99％,Bi4VO8Br表面上活性基团的捕获即空穴的氧化作用是主要反应原理.     

蒽醌修饰石墨毡电极预处理头孢合成废水

以钛涂钌电极为阳极、自制蒽醌修饰石墨毡电极为阴极,对头孢合成废水(COD=25 000~30 000 mg/L、ρ(NH3-N)=850~1 300 mg/L、色度为2 300~2 680度)进行了电化学氧化预处理,优化了电解条件,并对电化学体系的动力学和稳定性进行了分析。实验结果表明:蒽醌的存在可改善电化学氧化降解效果;在电解时间50 min、电流密度0.14 A/cm2、Na2SO4浓度0.1 mol/L、极板间距2 cm、初始废水p H 7.0的条件下,废水的COD、色度、NH3-N的去除率分别可达45.3%,66.9%,33.6%;BOD5/COD由处理前的0.27增至0.40,可生化性得到改善;COD、色度、NH3-N的电化学氧化降解过程均近似符合一级动力学方程;且该电化学体系的应用稳定性良好。     

Zr掺杂TiO_2介孔材料光催化降解头孢氨苄

采用固相合成法制备了Zr掺杂TiO_2(Zr-TiO_2),运用XRD技术对其进行了表征,并将其用于水中头孢氨苄的光催化降解,通过单因素实验及正交实验优化了光催化反应条件。结果表明:制备的Zr-TiO_2为锐钛矿型介孔材料,孔径约为8.12 nm;各因素对头孢氨苄去除率的影响由大到小依次为光照时间、Zr-TiO_2投加量、初始头孢氨苄质量浓度;在Zr-TiO_2投加量为1.5 g/L、初始头孢氨苄质量浓度为10 mg/L、溶液pH为7.0、光照(300 W UV)时间为1.5 h的优化条件下,头孢氨苄去除率高达99.46%;Zr-TiO_2光催化剂的重复使用性能良好。     

Iron and lead ion adsorption by microbial flocculants in synthetic wastewater and their related carbonate formation

Although microbial treatments of heavy metal ions in wastewater have been studied, the removal of these metals through incorporation into carbonate minerals has rarely been reported. To investigate the removal of Fe^3＋ and Pb^2＋, two representative metals in wastewater, through the precipitation of carbonate minerals by a microbial flocculant （MBF） produced by Bacillus mucilaginosus. MBF was added to synthetic wastewater containing different Fe^3＋ and Pb^2＋ concentrations, and the extent of flocculation was analyzed. CO2 was bubbled into the mixture of MBF and Fe^3＋/Pb^2＋ to initiate the reaction. The solid substrates were analyzed via X-ray diffraction, transmission electron microscopy and energy dispersive spectroscopy. The results showed that the removal efficiency decreased and the MBF adsorption capacity for metals increased with increasing heavy metal concentration. In the system containing MBF, metals （Fe^3＋ and Pb^2＋）, and CO2, the concentrated metals adsorbed onto the MBF combined with the dissolved CO2, resulting in oversaturation of metal carbonate minerals to form iron carbonate and lead carbonates. These results may be used in designing a method in which microbes can be utilized to combine CO2 with wastewater heavy metals to form carbonates, with the aim of mitigating environmental problems.     

Efficient dechlorination of chlorinated solvent pollutants under UV irradiation by using the synthesized TiO2 nano-sheets in aqueous phase

Titanium dioxide(TiO2), which is the widely used photo-catalyst, has been synthesized by simple hydrothermal solution containing tetrabutyl titanate and hydrofluoric acid. The synthesized product has been applied to photo-degradation in aqueous phase of chlorinated solvents, namely tetrachloroethene(PCE), trichloroethene(TCE) and 1,1,1-trichloroethane(TCA). The photo-degradation results revealed that the degradation of these harmful chemicals was better in UV/synthesized TiO2 system compared to UV/commercial P25 system and UV only system. The photo-catalytic efficiency of the synthesized TiO2 was 1.4, 1.8 and 3.0 folds higher compared to the commercial P25 for TCA, TCE and PCE degradation, respectively. Moreover, using nitrobenzene(NB) as a probe of hydroxyl radical(.OH), the degradation rate was better over UV/synthesized TiO2, suggesting the high concentration of.OH generated in UV/synthesized TiO2system. In addition,.OH concentration was confirmed by the strong peak displayed in EPR analysis over UV/synthesized TiO2system. The characterization result using XRD and TEM showed that the synthesized TiO2 was in anatase form and consisted of well-defined sheet-shaped structures having a rectangular outline with a thickness of 4 nm, side length of 50 nm and width of 33 nm and a surface 90.3 m2/g. XPS analysis revealed that ≡Ti-F bond was formed on the surface of the synthesized TiO2. The above results on both photocatalytic activity and the surface analysis demonstrated the good applicability of the synthesized TiO2 nano-sheets for the remediation of chlorinated solvent contaminated groundwater.     

Dyes adsorption using a synthetic carboxymethyl cellulose-acrylic acid adsorbent

Removal of noxious dyes is gaining public and technological attention. Herein grafting polymerization was employed to produce a novel adsorbent using acrylic acid and carboxymethyl cellulose for dye removal. Scanning electron microscopy and Fourier-transform infrared spectroscopy verified the adsorbent formed under optimized reaction conditions. The removal ratio of adsorbent to Methyl Orange, Disperse Blue 2BLN and malachite green chloride reached to 84.2%, 79.6% and 99.9%, respectively. The greater agreement between the calculated and experimental results suggested that pseudo second-order kinetic model better represents the kinetic adsorption data. Equilibrium adsorptions of dyes were better explained by the Temkin isotherm. The results implied that this new cellulose-based absorbent had the universaiity for removal of dyes through the chemical adsorption mechanism.     

温度对合成钛酸盐纳米材料的影响及其对水中Cd (Ⅱ)的去除效果

为有效去除水中Cd（Ⅱ）,以TiO₂纳米粉和NaOH为原料,调节水热反应温度分别为100、120、150和190℃,制备出了不同形貌的TNs（钛酸盐纳米材料）,分别记为TNs-100、TNs-120、TNs-150和TNs-190,并对其形貌、结构、比表面积、化学组成等物理化学性能进行了表征;通过对水中Cd（Ⅱ）的静态吸附试验,考察了TNs对Cd（Ⅱ）的吸附性能.结果表明:随着合成温度的升高,TNs的形貌逐渐从纳米片演变成纳米管,管长逐渐变长,最后变成纳米棒.TNs-100的晶型结构主要是锐钛矿型;随着温度升高,结晶度逐渐增强;TNs-190出现了部分金红石相.TNs-150对Cd（Ⅱ）的吸附能力最强,最大平衡吸附量为254.66 mg/g,最佳吸附pH为5.0.再生的TNs-150对Cd（Ⅱ）循环吸附6次的去除率和解吸率均可达93%以上.TNs-150对Cd（Ⅱ）的吸附过程符合准二阶动力学方程和Langmuir吸附等温模型,吸附机制主要是TNs层间Na+和H+与溶液中Cd（Ⅱ）的离子交换.研究显示,TNs的饱和吸附量均高于同类吸附剂,能有效去除水中Cd（Ⅱ）.      

废旧锌锰电池生物淋滤-水热法制备纳米锰锌铁氧体

以氧化硫硫杆菌(A.thiooxidans)和氧化亚铁钩端螺旋菌(L.ferrooxidans)为混合淋滤菌株对废旧锌锰电池进行了生物浸提,并以获取的淋滤液为前驱体,采用水热法制备出系列锰锌铁氧体软磁材料(Mn_(1-x)Zn_xFe_2O_4,x=0.2~0.8);结合X射线衍射(XRD)、扫描电镜-能谱(SEMEDX)、振动样品磁强计(VSM)、透射电镜(TEM)、红外光谱(FT-IR)、热重-差热分析(TG-DTA)等表征手段对制备材料的结构、形貌、磁学性能和稳定性进行分析.结果表明,在5%固液比(质量体积比,5 g/100 mL,以下均表述为"5%固液比")下,经过5 d的外源酸调控生物浸提,分别获得了84.5%、63.2%的Zn、Mn浸出效率;当Zn∶Mn∶Fe=0.4∶0.6∶2.0(物质的量比,即x=0.4)时,制备的纳米级Mn_(0.6)Zn_(0.4)Fe_2O_4性能最优,属纯相的立方尖晶石结构,颗粒分布均匀,饱和磁化强度(M_s)、剩余磁化强度(M_r)和矫顽力(H_c)分别为68.9 emu·g~(-1)、4.7 emu·g~(-1)和53.6 Oe,具有热稳定性和耐酸碱性,有望成为一种新型的水处理磁性材料.     

反应气氛对绿色合成纳米铁的组分及其活性的影响

成本低廉和无二次污染的"绿色"合成纳米材料是发展原位纳米环境修复技术的前沿研究课题之一.本文以绿茶提取液为还原剂和稳定剂进行"绿色"合成纳米铁,探讨在不同的气氛下"绿色"合成的纳米铁颗粒的主要成分,以期为调控合成纳米铁系材料提供基础研究.首先,利用扫描电子显微镜(SEM)、X射线能谱(EDS)、X射线光电子能谱分析(XPS)和傅里叶变换红外光谱(FTIR)等表征手段对不同反应气氛下合成的纳米铁颗粒的表面微观形貌、尺寸和价态结构进行分析.结果发现,在通入N2情况下,合成的纳米铁颗粒粒径为(84.7±11.5)nm,其主要成分以纳米零价铁为主;在通入空气情况下,合成的纳米铁粒径为(117.8±26.2)nm,其主要成分是纳米零价铁、氧化铁和四氧化三铁的混合物;通入O2时,合成的纳米铁粒径为(141.2±26.3)nm,其主要成分以四氧化三铁为主.其次,评价在不同气氛条件下合成纳米铁颗粒对去除亚甲基蓝(MB)的反应活性.结果表明,在反应温度313 K下降解初始浓度为50 mg·L-1的MB溶液,反应5 min时已达到平衡,通入N2合成的纳米铁降解MB,去除率高达98.7%,而通入O2合成的纳米铁反应效率低,对MB的去除率仅为65.3%.最后,从以上发现提出不同气氛下可以调控"绿色"合成的铁系纳米材料成分,从而导致不同的纳米修复环境中污染物的能力.