pH和Ni2+对人工纳米氧化硅吸附菲的影响

为了揭示菲在人工纳米氧化硅上的吸附行为,采用批量平衡实验对比研究了灼烧前后纳米氧化硅对菲的吸附,考察了pH值和重金属离子(Ni2+)对吸附行为的影响,并应用位点能量分布模型分析了菲吸附行为的变化.结果表明,吸附数据可用Freundlich模型较好地拟合,高温灼烧后纳米氧化硅对菲的吸附增加,lgKF由1.48增加到2.43;吸附的非线性也增加,结合孔分布及表面积变化,说明纳米氧化硅对菲的吸附为孔填充与表面吸附共同作用,内部孔对菲的吸附起主要作用.pH值的变化没有显著改变原始纳米氧化硅对菲的吸附;但是显著影响灼烧后纳米氧化硅对菲的吸附,吸附随着pH值的增加而降低,pH值由4.0增加到8.0,lgKF减少了73.7%.主要因为提高pH值,可明显增加灼烧纳米氧化硅的表面电荷,降低孔的可及性.不同浓度的Ni2+对菲吸附的影响不同,在Ni2+低浓度时(<5 mmol.L-1),表现为吸附抑制;在Ni2+高浓度时,对低浓度菲(50μg.L-1)表现为促进吸附,对高浓度菲(500μg.L-1)吸附的抑制程度不再增加.这是多个机制共同作用的结果.     

雌二醇在土壤/沉积物中的吸附特征及猪粪DOM对吸附的影响

天然类固醇雌激素如17β-雌二醇(E2)在极低质量浓度下(ng.L-1)即可干扰水生生物的生殖功能.为准确预测E2向水体迁移,通过摇床实验研究了E2在中国北方3种不同土壤/沉积物表面的吸附特征,同时探讨了猪粪及其堆肥可溶态有机质(DOM)对E2吸附的影响.结果发现,E2在土壤/沉积物表面吸附符合Freundlich等温吸附方程(R2>0.76),E2在河流沉积物、潮土、黑土皆表现为非线性,其中黑土吸附的非线性最强(n=0.74);吸附系数Kf介于26.2～57.5,并与有机质含量呈显著正相关(P<0.05).猪粪及其堆肥DOM显著抑制E2在土壤/沉积物表面的吸附,其中堆肥DOM的影响尤为显著.研究认为,有机质是土壤/沉积物中吸附E2的主要组分,共存猪粪DOM在较低浓度下可提高E2迁移性,增加E2向地表和地下水的迁移风险.     

Sorption mechanism of naphthalene by diesel soot: Insight from displacement with phenanthrene/p-nitrophenol

The nonlinear sorption of hydrophobic organic contaminants (HOCs) could be changed to linear sorption by the suppression of coexisting solutes in natural system, resulting in the enhancement of mobility, bioavailability and risks of HOCs in the environment. In previous study, inspired from the competitive adsorption on activated carbon (AC), the displaceable fraction of HOCs sorption to soot by competitor was attributed to the adsorption on elemental carbon fraction of soot (EC-Soot), while the linear and nondisplaceable fraction was attributed to the partition in authigenic organic matter of soot (OM-Soot). In this study, however, we observed that the linear and nondisplaceable fraction of HOC (naphthalene) to a diesel soot (D-Soot) by competitor (phenanthrene or p-nitrophenol) should be attributed to not only the linear partition in OM-Soot, but also the residual linear adsorption on EC-Soot. We also observed that the competition on the surface of soot dominated by external surface was different from that of AC dominated by micropore surface, i.e., complete displacement of HOCs by p-nitrophenol could occur for the micropore surface of AC, but not for the external surface of soot. These observations were obtained through the separation of EC-Soot and OM-Soot from D-Soot with organic-solvent extraction and the sorption comparisons of D-Soot with an AC (ACF300) and a multiwalled carbon nanotube (MWCNT30). The obtained results would give new insights to the sorption mechanisms of HOCs by soot and help to assess their environmental risks.     

Selective sorptive removal of Methyl Red from individual and binary component solutions by mesoporous organosilicas of MCM-41 type

Organosilicas with chemically immobilized 3-aminopropyl and Methyl Red-containing surface groups were prepared by sol-gel condensation of tetraethyl orthosilicate and (3-aminopropyl)triethoxysilane in the presence of dye as part of the mixed micelles or dye-containing silane as silica source. The hexagonally arranged mesoporous structure of synthesized materials was confirmed by low-temperature nitrogen adsorption-desorption, x-ray diffraction, and TEM studies. Chemical composition of MCM-41-type organosilicas was established by FT-IR spectroscopy and chemical analysis of surface layer. Sorption of Methyl Red by organosilicas was studied from diluted phosphate buffer solutions in dependence of medium pH, duration of contact, and equilibrium concentration of dye. It was found that effective removal of Methyl Red takes place at pH values within a range of 2.5?5. Kinetic curves of Methyl Red sorption on organosilicas were analyzed by the Lagergren, Ho-McKey, and Weber-Morris kinetic models. It was found that the pseudo-second-order model fits the kinetics of Methyl Red sorption on all synthesized materials and the intraparticle diffusion is not the only one mechanism controlling the rate of Methyl Red sorptive removal. The parameters of equilibrium sorption of Methyl Red on organosilicas of MCM-41 type were calculated using Langmuir, Freundlich, Redlich-Peterson, and Brunauer-Emmett-Teller models. Sorption of acid dyes with geometry similar or substantially different from Methyl Red on mesoporous silicas was studied from single and binary component mixtures in aqueous solutions with pH 4.8 and 5.5. It was found that selective sorption process is highly dependent on the structural characteristics and protolytic state of silica surface as well as acid dye.     

磺胺二甲基嘧啶对镉在针铁矿上吸附行为的影响

环境中抗生素与重金属的共存会使各自在土壤中的迁移转化和生态效应变得更为复杂,为了准确评估磺胺二甲基嘧啶(SMT)与重金属镉复合污染下的环境风险,采用紫外光谱法,研究了中性条件下磺胺二甲基嘧啶与镉的络合特性;采用批量振荡吸附平衡法,研究了SMT存在的条件下针铁矿对镉的吸附特性.结果表明:SMT与镉有一定的络合能力,络合常数log K值为-3.31;针铁矿对SMT和镉都有一定的吸附作用;在SMT存在条件下,针铁矿对镉的吸附容量明显增强,这可能是由于SMT改变了针铁矿表面带电情况,红外结果表明在吸附过程中形成了针铁矿-SMT-镉三元络合物.因此,在评估抗生素与重金属复合污染的环境影响时,需要考虑到污染物之间的协同效应.     

水稻土对磷的吸持能力及环境风险研究

以湖南Cd污染区水稻土为供试土壤,研究了土壤活性Al(Al_(ox))、活性Fe(Fe_(ox))、磷吸持指数(PSI)、吸持饱和度(DPSS)和释放风险指数(ERI)及其相关性关系.结果表明:供试水稻土中Al_(ox)和Fe_(ox)含量变异性较大,分别为55.67~1495.90 mg·kg~(-1)和1.50~13.63 g·kg~(-1),但有效磷含量变化幅度不大.水稻土吸持磷能力较弱,全部样品中PSI均低于30,但水稻土磷的吸持饱和度较低,85%的土壤样品DPSS低于磷淋失临界值(15%),且磷释放失风险(ERI)较小.水稻土中Al_(ox)含量和Fe_(ox)含量与PSI存在显著正相关关系(p0.05),而与DPSS之间表现为显著负相关关系(p0.01),DPSS和PSI呈现为显著负相关关系(p0.01).     

四溴双酚A在煤胶体上的表面吸附和分配作用特征

以采自内蒙古霍林河煤矿的煤样为研究对象,通过模拟实验研究了四溴双酚A在煤胶体上的吸附行为,重点探讨了温度、p H值和离子强度对四溴双酚A在煤胶体上表面吸附和分配作用的影响.结果表明:煤胶体对四溴双酚A的吸附过程可由Freundlich表面吸附-分配复合模型很好地描述.随着温度的升高,四溴双酚A在煤胶体上吸附的分配作用和表面吸附同样都有所下降,但温度的升高对分配作用的影响程度较大.p H值主要影响四溴双酚A在煤胶体上的分配作用,在p H值为9时,四溴双酚A在煤胶体上的吸附以表面吸附为主,其对总吸附量的贡献率为97.5%;而在p H值为6~8时,则以分配作用为主,其对总吸附量的贡献率为64.0%~78.9%.Ca~(2+)浓度为0.001~0.1 mol·L~(-1)时,离子强度对于四溴双酚A在煤胶体上的表面吸附和分配作用均影响较小.     

新型铁铜锰复合氧化物颗粒吸附剂As(Ⅲ)吸附行为与机制研究

以壳聚糖为黏合剂,采用包覆法制备了一种新型除砷吸附剂——颗粒状铁铜锰复合氧化物(GFCM). GFCM吸附剂为不完全球状,直径0.7～1.0 mm,可以有效地将As(Ⅲ)氧化成As(V),并对形成的As(V)具有良好的吸附效果. GFCM对As(Ⅲ)的最大吸附容量(pH 7.0)为56.5 mg·g~(-1),显著优于目前已报道的多数颗粒状除砷吸附剂.溶液pH在5.0～9.0范围内, GFCM对As(Ⅲ)均有较好的吸附效果,离子强度则对砷吸附效果影响较小.共存阴离子对As(Ⅲ)吸附具有抑制作用,影响的大小顺序为:PO■ SiO■ CO■ Cl~- SO■.吸附As(Ⅲ)后的GFCM可用NaOH溶液进行有效脱附再生,可重复使用.在As(Ⅲ)的去除过程中,吸附剂中锰氧化物的主要作用是氧化As(Ⅲ),铁氧化物与铜氧化物的主要作用是吸附As(Ⅲ)与氧化形成的As(V),且铜氧化物有助于增强GFCM的砷吸附性能.     

滇池底泥制备的生物炭对菲的吸附-解吸

将滇池草海底泥在不同烧制温度下制成生物炭,并用元素分析法表征其元素组成,溴化钾压片法表征其红外光谱,CO2和N2法表征其比表面积、孔体积、孔径．以菲作为模型化合物来研究有机污染物在生物炭上的吸附一解吸行为,以此深入了解生物炭施用中对有机污染物环境行为和风险的影响．结果表明,生物炭随烧制温度升高,芳香性升高、亲水性降低、...     

抗生素在沉积物中的吸附机制及其影响因素

抗生素作为医疗业和农业使用量最大的药物之一,由于其本身的特性,很容易进入沉积物一水环境中。抗生素在沉积物中的吸附过程是影响抗生素的反应活性、可移动性、持久性及生物可利用性的关键过程。本文选择四环素类、喹诺酮类、磺胺类和大环内酯类4类常用抗生素,在总结了这4类抗生素在湖泊沉积物中污染状况的基础上,分析了抗生素在沉积物中的吸附机制,并归纳论述了pH值、盐度、重金属离子、表面活性剂以及水动力条件对其在沉积物上吸附的影响机制。