TiO2胶体光催化降解罗丹明B染料

TiO2胶体从钛氧有机物水解制备,表征的方法有:X射线衍射光谱(XRD)、激光散射粒径分布、傅立叶变换红外光谱(FT-IR)、X射线光电子谱(XPS)和透射电子显微镜(TEM)。利用罗丹明B染料分子作为探针分子研究TiO2胶体的光催化活性,分析了pH、催化剂用量、外加氧化剂(H2O2)用量及罗丹明B初始浓度对TiO2胶体光催化活性的影响。结果表明:制备的TiO2胶体粒子平均粒径为13.8 nm(激光散法测定),光催化降解罗丹明B染料的反应属于一级动力学反应,可以用Langmuir-Hinshewood模型加以描述,反应速率常数k1为0.08413 mg/(L.min),平衡吸附常数k2为1.5305 L/mg;在pH为6,TiO2胶体用量为0.04%,H2O2(含量30%)用量为0.2%(V/V),光照度为69.6μW/cm2时,5 h后罗丹明B染料的降解率可达到99%以上;相似的条件,0.2%的P25 TiO2粉体光催化处理染料水时,罗丹明B的降解率为90%。纳米TiO2胶体不仅可以提高罗丹明B的光催化降解率,还具有用量少,可有效降低水处理成本的特点。     

沉积物和土壤中胶体对氯霉素吸附行为的影响

天然胶体（NCs）在沉积物和土壤中广泛存在,并可影响抗生素等污染物的环境归趋.以氯霉素（CAP）为抗生素代表,选取不同来源的沉积物和土壤样品,结合切向超滤技术、动态光散射、紫外-可见吸收光谱和三维荧光光谱等多种纳米分析技术和方法,揭示了沉积物/土壤中不同相对分子质量NCs对CAP的吸附能力及其影响因素.结果表明,相对分子质量小的NCs自生源贡献率大且腐殖化程度高,而相对分子质量大的NCs以陆源来源为主,且芳环上含有更加丰富的羧基、羟基和羰基等官能团.平行因子分析共识别出4个荧光组分,其中类腐殖质组分是主要成分.基于传统批处理实验探究了沉积物/土壤不同组分对CAP的吸附行为,结果表明,线性模型和Freundlich模型能较好地拟合土样不同组分对CAP的吸附.原始样品、去除有/无机碳样品中的NCs对CAP的吸附率均值分别为4.46%、3.93%和6.61%,说明NCs中的有机碳对CAP的吸附行为具有重要影响.CAP更易被相对分子质量小的NCs吸附,这可能是因为相对分子质量小的NCs腐殖化程度高,芳环上取代基以脂肪链为主,且NCs中的色氨酸类蛋白物质会抑制其对CAP的吸附.冗余分析结果表明,沉积物和土壤NCs对CAP的吸附主要与其NCs来源、芳香性、芳环上的有氧官能团、腐殖化程度和类腐殖物质有关.     

Unraveling the size distributions of surface properties for purple soil and yellow soil

Soils contain diverse colloidal particles whose properties are pertinent to ecological and human health, whereas few investigations systematically analyze the surface properties of these particles. The objective of this study was to elucidate the surface properties of particles within targeted size ranges (i.e. > 10, 1–10, 0.5–1, 0.2–0.5 and < 0.2 μm) for a purple soil (Entisol) and a yellow soil (Ultisol) using the combined determination method. The mineralogy of corresponding particle-size fractions was determined by X-ray diffraction. We found that up to 80% of the specific surface area and 85% of the surface charge of the entire soil came from colloidal-sized particles (< 1 μm), and almost half of the specific surface area and surface charge came from the smallest particles (< 0.2 μm). Vermiculite, illite, montmorillonite and mica dominated in the colloidal-sized particles, of which the smallest particles had the highest proportion of vermiculite and montmorillonite. For a given size fraction, the purple soil had a larger specific surface area, stronger electrostatic field, and higher surface charge than the yellow soil due to differences in mineralogy. Likewise, the differences in surface properties among the various particle-size fractions can also be ascribed to mineralogy. Our results indicated that soil surface properties were essentially determined by the colloidal-sized particles, and the < 0.2 μm nanoparticles made the largest contribution to soil properties. The composition of clay minerals within the diverse particle-size fractions could fully explain the size distributions of surface properties.     

Behavior of fenhexamid in soil and water

A study was conducted to investigate fenhexamid (FEX) behavior in soil and in water. FEX proved to be rather stable at acid pH but showed slight degradation at neutral and alkaline pH. After 101 days of FEX spiking of a soil sample, 94% at pH 4, 12% at pH 7 and 23% at pH 9 of the active ingredient was still present. In natural water the rate of FEX disappearance appeared to be slow which may be due to abiotic rather than biotic processes. The soil degradation tests showed low persistence of the active ingredient if a good microflora activity is guaranteed (DT₅₀ about 1 day). Moreover, in absence of microorganisms, FEX proved to be stable. Humidities of 25 and 50% of Water Holding Capacity (WHC) influenced in equal measure the rate of degradation. From the same soil, a bacterium was isolated and identified as Bacillus megaterium, which was able to metabolize FEX with the hydroxylation of the cyclohexane ring. Moreover, FEX showed an elevated affinity for humic acid (73%), smectite (31%), and ferrihydrite(20%) and low affinity for vermiculite (11%) and kaolinite (7%).     

高岭土和蒙脱土存在下nC60纳米颗粒稳定性研究

通过沉降实验研究了不同浓度高岭土和蒙脱土分别对富勒烯纳米颗粒（nC₆₀）稳定性的影响,利用沉降模型并结合zeta电位、粒径、SEM、TEM进行原因分析.单体系中nC₆₀的稳定性好,高岭土胶体稳定性差且随浓度增加而降低,蒙脱土胶体稳定性好且与浓度无明显关系.整体上,高岭土和蒙脱土可以降低nC₆₀的稳定性.随着高岭土浓度增加,nC₆₀稳定性显著降低;而蒙脱土对nC₆₀稳定性降低较小且与浓度无明显关系.结果表明,nC₆₀的稳定性由黏土控制,两种黏土在结构和比表面积上的差异,使它们对nC₆₀稳定性影响不同.模型分析表明,一阶沉降模型和修正的一阶沉降模型分别适用于高岭土和蒙脱土参与的胶体沉降过程.该研究可为评估nC₆₀对地下水环境的影响提供重要参考.     

离子强度和胡敏酸影响下不同土壤胶体稳定性研究

土壤胶体的稳定性对其携带污染物的能力产生重要影响,但离子强度和胡敏酸（HA）对不同土壤胶体稳定性的影响程度尚不明确.本实验通过土壤胶体沉降实验以及DLVO理论研究离子强度、HA对黑钙土、潮土和黄壤3种土壤胶体稳定性的影响.结果表明：即使在高离子强度背景下,黑钙土胶体和黄壤胶体因有机质和黏土矿物（黑钙土胶体：伊/蒙混合层;黄壤胶体：伊利石）较高,表面负电荷多、静电斥力大,故稳定性好;而潮土胶体的稳定性受离子强度影响明显,在低离子强度下,静电斥力占主导,稳定性达到最高.HA通过增加土壤胶体表面的负电荷,提高土壤胶体间静电斥力而增强其稳定性,且HA浓度越高土壤胶体的稳定性越强.不同粒径HA对土壤胶体稳定性的影响受pH值控制,相对于大粒径HA,酸性条件下,小粒径HA （F-HA）自身稳定性更强,同时也会自凝聚形成较大的团聚体来提高土壤胶体的稳定性;中、碱性条件下,F-HA产生的链状凸起结构较小,导致空间弹性斥力和渗透性斥力减弱,进而降低土壤胶体的稳定性.结果为明晰离子强度和HA对不同土壤胶体稳定性产生差异性影响提供数据支撑.     

五氯酚在土壤胶体界面的还原转化

提取玄武岩发育的红壤胶体,用恒温厌氧平衡动力学方法,研究土壤胶体界面五氯酚的降解效果,以及外加Fe2+和草酸对五氯酚还原转化的影响. 结果表明,厌氧条件下玄武岩发育赤红壤和砖红壤胶体对五氯酚均具有一定的降解能力,其表观降解速率常数分别为(0.032±0.002)和(0.057±0.003) d-1. 草酸或Fe2+对土壤表面五氯酚的降解均有显著的促进作用. 在探讨土壤胶体对五氯酚的降解能力与其理化性质关系的基础上,说明利用铁氧化物可进行复杂土壤体系中有机氯类污染物的修复.      

Laboratory migration experiments with radionuclides and natural colloids in a granite fracture

Natural colloids in groundwater could facilitate radionuclide transport, provided the colloids are mobile, are present in sufficient concentrations and can adsorb radionuclides. This paper describes the results of a laboratory migration study carried out with combinations of radionuclides and natural colloids within a fracture in a large granite block to experimentally determine the impact of colloids on radionuclide transport. The 85Sr used in this study is an example of a moderately sorbing radionuclide, while the 241Am is typical of a strongly sorbed radionuclide with very low solubility. The natural colloids used in this study were isolated from granite groundwater from Atomic Energy of Canada (AECL) Underground Research Laboratory (URL), and consisted of mostly 1-10 nm organic colloids, along with lesser amounts of 10-450 nm colloids (organics and aluminosilicates). The measured coefficients for radionuclide sorption onto these colloids were between 3 x 10(2) and 1 x 10(3) ml/g for 85Sr, and between 7 x 10(4) and 7 x 10(5) mg/l for 241Am. The 85Sr sorption on the natural colloids appeared to be reversible. Migration experiments in the granite block were carried out by establishing a flow field between two boreholes (out of a total of nine) intersecting a main horizontal fracture. These experiments showed that dissolved 85Sr behaved as a moderately sorbing tracer, while dissolved 241Am was completely adsorbed by the fracture surfaces and showed no evidence of transport. However, when natural colloids were injected together with dissolved 241Am, a small amount of 241Am transport was observed, demonstrating the ability of natural colloids to facilitate the transport of radionuclides with low solubility. Natural colloids had only a minor effect on the transport of 85Sr. In a separate experiment to test the effect of higher colloid concentrations on 85Sr migration, synthetic colloids were produced from Avonlea bentonite. The introduction of a relatively high concentration of bentonite colloids actually reduced 85Sr transport because, compared to natural colloids, the bentonite colloids were less mobile and they sorbed 85Sr more strongly.     

饱和多孔介质中水流停滞对胶体吸附与解吸的影响

地下水水流停滞区域是胶体污染物吸附的重要场所.为研究水流停滞时间对胶体在饱和多孔介质中再迁移的影响,在石英砂柱与胶体达到稳定吸附后中断水流,分别设置水流停滞时间0、15、32、64、87、120 h,比较胶体的再迁移能力.结果表明:①水流停滞时间在32 h以内时,通入去离子水可使5.2%~5.3%的胶体被解吸出来再次随水流迁移,解吸量介于0.54~0.56 mg之间,对胶体再迁移能力的影响不明显;水流停滞时间为32~120 h时,水流停滞时间增加会导致胶体再迁移能力降低;水流停滞时间达到120 h,胶体主要楔在石英砂颗粒间,难以被解吸出来,此时仅有1.8%的胶体再次随水流迁移.②水流停滞时,以自上而下的流通方式吸附在土柱中的胶体受重力作用可能跨过能垒吸附在初级势阱中,使再迁移能力降低;然而在自下而上的流通方式下吸附在土柱中的胶体受重力影响难以跨过能垒吸附在初级势阱中,胶体再迁移能力较强.③当以≤ 30.2 m/d的流速通入背景液时,流速对胶体解吸的影响不如通入去离子水时显著.研究显示,水流停滞时间对吸附在饱和含水介质上胶体的再迁移能力有明显影响,重力作用在不同的流通方式下不同.      

TiO_2胶体光催化降解罗丹明B染料

TiO2胶体从钛氧有机物水解制备,表征的方法有：X射线衍射光谱（XRD）、激光散射粒径分布、傅立叶变换红外光谱（FT-IR）、X射线光电子谱（XPS）和透射电子显微镜（TEM）。利用罗丹明B染料分子作为探针分子研究TiO2胶体的光催化活性,分析了pH、催化剂用量、外加氧化剂（H2O2）用量及罗丹明B初始浓度对TiO2胶体光催化活性的影响。结果表明：制备的TiO2胶体粒子平均粒径为13.8 nm（激光散法测定）,光催化降解罗丹明B染料的反应属于一级动力学反应,可以用Langmuir-Hinshewood模型加以描述,反应速率常数k1为0.08413 mg/（L.min）,平衡吸附常数k2为1.5305 L/mg;在pH为6,TiO2胶体用量为0.04%,H2O2（含量30%）用量为0.2%（V/V）,光照度为69.6μW/cm2时,5 h后罗丹明B染料的降解率可达到99%以上;相似的条件,0.2%的P25 TiO2粉体光催化处理染料水时,罗丹明B的降解率为90%。纳米TiO2胶体不仅可以提高罗丹明B的光催化降解率,还具有用量少,可有效降低水处理成本的特点。