去除氧化铁对Al在土壤中吸附-解吸的影响

用连二亚硫酸钠-柠檬酸钠-碳酸氢钠(DCB)法研究了去除土壤中的氧化铁后Al的吸附-解吸特征的变化情况.结果表明,在pH值<4.5条件下,去除氧化铁可使土壤对Al的吸附量有所增加,这种变化在赤红壤中尤为明显;而此后随pH值的升高,原土和去铁土对Al的吸附量基本相等.造成该现象的原因可归纳为去除氧化铁能降低土壤的电荷零点(ZPC)和增加土壤表面负电荷的数量,从而增强了土壤表面与离子之间的静电引力.另一方面,去除氧化铁后Al的解吸量也增加.其原因是与原土相比,去铁土吸附Al的机理中包含有部分静电吸附,这从离子强度对去铁土吸附Al的影响实验能得到较好的验证,因为在pH值<4.5时,提高离子强度将降低Al的吸附量,用高岭石做参考材料时也发现了类似的现象.     

背景溶液对纳米氧化铁吸附病毒的影响

以噬菌体X174为病毒替代,通过等温静态批量吸附实验,研究了4种纳米氧化铁(α-Fe2O3、γ-Fe2O3-B、γ-Fe2O3-N、Fe3O4)对病毒在不同背景溶液中的吸附行为及其影响因素.结果表明,在模拟地下水中,4种纳米氧化铁对病毒均具有较高的吸附比例,其中α-Fe2O3对病毒吸附比例最高,在病毒初始浓度比较低(约1E+03PFU.mL-1)时可达100%.经Langmuir和Freundlich吸附等温线方程对上述吸附结果进行拟合表示,纳米氧化铁对病毒的吸附均为有利吸附(favorable adsorption),并可能存在多层吸附,吸附比例均随着病毒初始浓度的增加而减少.纳米氧化铁对病毒的吸附比例随着背景溶液离子强度的增加而降低,表示其吸附行为以电性吸附为主.背景溶液中阴离子存在显著降低了病毒的吸附量,这可能与阴离子竞争病毒吸附位点有关,其中HPO24-比HCO3-表现得更为明显.结果同时显示背景溶液中多价阳离子的存在(比如Ca2+和Mg2+)比单价阳离子(比如Na+和K+)更有利于纳米氧化铁对病毒的吸附.综上可知,纳米氧化铁是一种潜在的病毒净化理想材料,应用时需考虑其环境因素的影响.     

沸石负载羟基氧化铁对铬（VI）吸附的固体浓度效应研究

本文利用沸石负载羟基氧化铁作吸附剂对六价铬进行吸附和解吸附实验。探讨了沸石负载羟基氧化铁对六价铬的吸附机制和固体浓度效应。实验结果表明：当吸附剂的用量从0.05g增加到0.2g时,在实验条件下,六价铬的吸附量从27999.493μg/g降低到8930.610μg/g,吸附剂对Cr6＋的吸附存在明显的固体浓度（Cs）效应。吸附滞后角随着Cs的增加而减小,吸附反应的可逆性增大。将实验数据分别用Languir和Freundlich吸附模型进行拟合,发现Freundlich吸附模型对实验数据拟合效果较好,表明该吸附反应以单分子层吸附为主。     

萘和苯并［b］荧蒽在配位聚合物上的选择性吸附行为和机理研究

异烟酸铜配位聚合物是由[Cu(4-C5H4N-COO)2(H2O)4]n通过分子间氢键构筑而成的三维超分子化合物,选用分子形状、大小和疏水性差别较大的多环芳烃萘和苯并[b]荧蒽为研究对象,研究异烟酸铜配位聚合物对它们的选择性吸附作用.结果表明,在pH为5～6,吸附剂用量为1.0 g/L时,异烟酸铜配位聚合物对苯并[b]荧蒽的去除率可达90%以上,而对萘的去除率低于10%.萘和苯并[b]荧蒽在异烟酸铜配位聚合物上的吸附等温线既较好地符合Langmuir模式,又较好地符合Freundlich模式.热力学数据表明,异烟酸铜配位聚合物吸附苯并[b]荧蒽的过程是自发进行的,而对萘的吸附则是非自发过程.动力学试验表明,2种物质的吸附过程均为一级可逆动力学反应.     

石英砂负载氧化铁的表征及其除锑吸附性能研究

通过SEM/EDAX以及Nova-1000表面分析仪对石英砂负载的氧化铁颗粒进行了表征,发现负载氧化铁的粒径为200 nm左右,其表面孔径及孔隙率分别为2×10-9～9×10-9m及0.11%,负载氧化铁的石英砂的比表面积为原砂的5倍.考察了石英砂负载氧化铁(IOCS)在不同的实验条件下(吸附时间,pH值,温度等)对水溶液中锑的去除效果,在pH为3～9范围内,其去除率均超过了98%.吸附动力学及吸附等温线实验数据分别符合二级反应动力学模型及Langmuir等温吸附模型.热动力学实验结果进一步表明:IOCS吸附锑的过程是自发的、吸热的化学吸附反应.     

天然有机物在氧化铝表面的吸附机理研究

考察了天然有机物(NOM)的2种分离组份(憎水部分HyO,亲水部分HyI)和一种商用腐殖酸(CHA)在氧化铝表面的吸附-解吸行为规律,从芳香性、分子量、极性的角度探讨了NOM自身特性对吸附性能的影响,并通过改变溶液性质(pH值、离子强度、二价阳离子Ca2 ),进一步论证了NOM在金属氧化物表面的吸附机理.结果表明,芳香性高、弱极性的有机物吸附性能较强;降低溶液的pH值,有助于增加吸附剂的吸附容量;离子强度和Ca2 对吸附行为的影响,与NOM自身和内部组分的性质有关.NOM吸附于金属氧化物表面的机理,可以归结为配位体交换、静电作用、憎水作用、阳离子架桥等多个因素共同作用的结果.采用原子力显微成像技术,进一步从微观角度证实了憎水作用和阳离子架桥作用的存在.     

改性氧化铝对氟的吸附性能研究

以氧化铝为基本吸附材料,经过1mol/L的硝酸溶液和20%的硝酸锰浸渍,在800℃下烘焙2h等改性手段制备成Mn-Al2O3,该吸附材料对溶液中的氟离子具有较强吸附能力。在25℃室温条件下,Mn-Al2O3吸附氟离子的适宜p H=3~7,Mn-Al2O3吸附材料对氟离子的最大吸附量为26.32mg/g,对氟离子的吸附等温线符合Langmuir方程和Freundlich方程,Mn-Al2O3对氟离子的吸附动力学可以用拟二级速率方程来描述,Mn-Al2O3吸附材料对氟离子的吸收率可以达到61%。     

无定形氧化铁-胡敏酸复合胶体对Cu2+的吸附特征

采用Cu2 选择电极研究了不同pH值条件下胡敏酸(HA)、无定形Fe2O3、HA-Fe2O3复合胶体对Cu2 的等温吸附规律.结果表明,随着pH值的升高,3种胶体饱和吸附量和吸附平衡常数均增大,有利于吸附的进行.HA和无定形Fe2O3等温吸附Cu2 的4种拟合方程中,Langmuir方程整体拟合效果最佳,其次为对数方程和Freundlich方程,Linear方程较差.HA-Fe2O3复合胶体等温吸附Cu2 的4种拟合方程均达到显著相关.在相同pH值条件下,无定形Fe2O3对Cu2 吸附量最小,复合胶体次之,HA胶体最大;而且,无定形Fe2O3和复合胶体的饱和吸附量之和小于HA胶体.     

茶叶基水合氧化铁吸附水体中Pb(Ⅱ)的性能

采用原位沉积技术将水合氧化铁(HFO)负载于废弃茶叶渣表面制备了复合材料茶叶基水合氧化铁(HFO-TW),研究了HFO-TW对水溶液中Pb(Ⅱ)的吸附特性,探讨了溶液pH值、时间、共存碱土离子、温度、Pb(Ⅱ)初始浓度等因素对Pb(Ⅱ)的吸附效果的影响.结果表明酸性范围内,Pb(Ⅱ)的吸附量随溶液pH升高而增大;Pb(Ⅱ)的吸附速度较快,100 min内便可达吸附平衡,且动力学曲线较好地符合伪一级和伪二级动力学模型,拟合系数可达98.8%;在竞争离子Ca(Ⅱ)/Mg(Ⅱ)的浓度高于Pb(Ⅱ)50倍时,HFO-TW对Pb(Ⅱ)仍具有较强的吸附能力,Pb(Ⅱ)的吸附量仅分别下降12.1 mg·g-1和8.1 mg·g-1;Pb(Ⅱ)的吸附过程较好地符合Langmuir等温模型,理论最大吸附容量为89.43 mg·g-1,远高于未经改性的茶叶渣和其他生物吸附剂.所有结果均证实HFO-TW在净化实际铅污染水体中有着较为广阔的应用潜力.     

氧化铁改性沸石对Se(Ⅳ)的吸附性能及试验废物再利用研究

为解决天然沸石去除废水中Se（Ⅳ）能力低的问题,采用氯化铁对天然沸石进行改性,制备表面负载氧化铁的改性沸石,即氧化铁改性沸石,并将其应用于去除水体中Se（Ⅳ）.首先对比天然沸石和氧化铁改性沸石的结构特征,研究二者对Se（Ⅳ）溶液的吸附特性,并通过X射线荧光光谱（XRF）、X射线衍射图谱（XRD）、扫描电镜（SEM）和氮气吸附孔径分布测试（BET）对二者进行表征;其次进行吸附试验,考虑接触时间、pH、吸附剂投加量、初始溶液反应浓度的影响,并通过天然沸石和氧化铁改性沸石的吸附动力学及吸附等温线对吸附的机理进行阐述.结果表明:①氧化铁改性沸石表面形成细碎的球状颗粒,分布在沸石的表面.②氧化铁改性沸石能够高效地吸附水体中的Se（Ⅳ）,且在pH为3时吸附效率最高,其对Se（Ⅳ）溶液的去除率最高达97.7%,其理论最大吸附量为46.901 mg/g.③氧化铁改性沸石对Se（Ⅳ）的吸附过程符合准二级动力学模型和Langmuir等温吸附模型.④添加负载Se（Ⅳ）后的氧化铁改性沸石土壤均达到富硒土壤标准（>0.4 mg/kg）.研究显示,氧化铁改性沸石吸附Se（Ⅳ）的效果较好,显著优于天然沸石的吸附效果,且吸附Se（Ⅳ）废水后的废弃氧化铁改性沸石还可应用于土壤改良方向.      

Novel synthesis of aluminum hydroxide gel-coated nano zero-valent iron and studies of its activity in flocculation-enhanced removal of tetracycline

A newly designed aluminum hydroxide gel-coated nanoscale zero-valent iron(AHG@NZVI)with enhanced activity and dispersibility of NZVI was successfully synthesized.The AHG@NZVI composite was synthesized via control of the surface AHG content.AHG@NZVI-1,AHG@NZVI-2 and AHG@NZVI-3 were prepared under centrifugal mixing speeds of 1000,2000 and 4000 r/min,respectively.The activity of AHG@NZVI was evaluated by its tetracycline(TC) removal efficiency.The effects of AHG content,pH value,reaction temperatu...     

Adsorption behavior of condensed phosphate on aluminum hydroxide

Sodium pyrophosphate （pyro-P, Na4P2OT）, sodium tripolyphosphate （tripoly-P, Na3P3O10）, and sodium hexametaphosphate （meta-P, （NaPO3）6） were selected as the model compounds of condensed phosphate to investigate the adsorption behavior of condensed phosphate on aluminum hydroxide. The adsorption was found to be endothermic and divisible into two stages： （1） fast adsorption within 1 h; and （2） slow adsorption between 1 and 24 h. The modified Freundlich model simulated the fast adsorption stage well; the slow adsorption stage was described well by the first-order kinetics. The activation energies of pyro-P, tripoly-P, and meta-P adsorption on aluminum hydroxide were determined to be 20.2, 22.8 and 10.9 kJ/mol P adsorbed, respectively, in the fast adsorption stage and to be 66.3, 53.5 and 72.5 kJ/mol P adsorbed, respectively, in the slow adsorption stage. The adsorption increased the negative charge of the aluminum hydroxide surface. Transmission electron microscopy and energy dispersive X-ray analysis analyses provided evidence that the adsorption was not uniform on the surface and that the small crystals contributed more to the fast adsorption than the normal sites did. The results from X-ray fluorescence spectrometry and X-ray photoelectron spectroscopy tests also revealed the uneven adsorption of condensed phosphate as a function of the penetration depth. More condensed phosphates were adsorbed on the outer surface of aluminum hydroxide than in its inner parts.     

沉积物中氧化物结合态镉对芦苇的生物有效性研究：氧化物种类、结合形式、老化的影响

沉积物中重金属的生物有效性在很大程度上取决于其赋存形态.选用沉积物中2种典型氢氧化物矿物:氢氧化铁和氢氧化铝,以水培法和矿物结合态Cd为培养介质,以芦苇为受试植物,研究环境中吸附和共沉淀态Cd生物有效性差别,并探究老化过程对生物有效性的影响.经过13 d的培养,发现2种结合形式的Cd均可被芦苇富集,不同处理体系中富集强度不同,根中富集量为9.1~37.8 mg.kg-1;地上部分富集量为0~10.0 mg.kg-1.其中,结合在Fe0.5Al0.5(OH)3矿物上的Cd的生物有效性最大,其次是Fe(OH)3和老化的Fe0.5Al0.5(OH)3,富集量最少的是老化的Fe(OH)3的处理.采用2种低分子量有机酸对Cd进行解吸实验,Cd的解吸规律与芦苇对Cd的富集规律一致.因此,共沉淀处理降低了Cd的富集,矿物的理化性质决定了含铝矿物对Cd的结合较差,老化作用抑制了吸附态Cd的富集,有机酸解吸实验也验证了不同形态Cd生物有效性的差异.     

Effect of competing solutes on arsenic(V) adsorption using iron and aluminum oxides

The study focused on the effect of several typical competing solutes on removal of arsenic with Fe2O3 and Al2O3. The test results indicate that chloride, nitrate and sulfate did not have detectable effects, and that selenium(IV) (Se(IV)) and vanadium(V) (V(V)) show slight effects on the adsorption of As(V) with Fe2O3. The results also showed that adsorption of As(V) on Al2O3 was not affected by chloride and nitrate anions, but slightly by Se(IV) and V(V) ions. Unlike the adsorption of As(V) with Fe2O3, that with Fe2O3 was affected by the presence of sulfate in water solutions. Both phosphate and silica have significant adverse effects on the adsorption of As(V) adsorption with Fe2O3 and Al2O3. Compared to the other tested anions, phosphate anion was found to be the most prominent solute affecting the As(V) adsorption with Fe2O3 and Al2O3. In general, Fe2O3 has a better performance than Al2O3 in removal of As(V) within a water environment where multi competing solutes are present.     

Al与F的络合作用对土壤吸附Al和F的影响

研究了Al-F络合作用对土壤吸附Al和F的影响以及吸附前的溶液中铝化学形态的差异。提高Al或F的加入量将人别使分配在土壤溶液中的F或Al的数量增加，即Al-F络合作用地使Al和F在土壤固-液间的分配平衡向液相移动，土壤对Al-F络合物吸附程度很小，吸附前，3种不同F/Al比溶液中Al^3 ，AlF^2 的浓度随着F/Al比的增加逐渐降低，AlF2^ ,AlF3^0的浓度则逐渐升高，与土壤作用后，溶液中Al主要与AlF^2 ,AlF2^ 的形式存在，以AlF^2 的数量居多。     

Mechanism and kinetics of aluminum dissolution during copper sorption by acidity paddy soil in South China

Soil aggregates were prepared from a bulk soil collected from paddy soil in the Taihu Lake region and aluminum (Al) dissolution, solution pH changes during copper (Cu^2 +) sorption were investigated with static sorption and magnetic stirring. Kinetics of Cu^2 + sorption and Al dissolution were also studied by magnetic stirring method. No Al dissolution was observed until Cu^2 + sorption was greater than a certain value, which was 632, 450, 601 and 674 mg/kg for sand, clay, silt, and coarse silt fractions, respectively. Aluminum dissolution increased with increasing Cu^2 + sorption and decreasing solution pH. An amount of dissolved Al showed a significant positive correlation with non-specific sorption of Cu^2 + (R² > 0.97), and it was still good under different pH values (R² > 0.95). Copper sorption significantly decreased solution pH. The magnitude of solution pH decline increased as Cu^2 + sorption and Al dissolution increased. The sand and clay fraction had a less Al dissolution and pH drop due to the higher ferric oxide, Al oxide and organic matter contents. After sorption reaction for half an hour, the Cu^2 + sorption progress reached more than 90% while the Al dissolution progress was only 40%, and lagged behind the Cu^2 + sorption. It indicated that aluminum dissolution is associated with non-specific sorption.     

ATR-FTIR and XPS study on the structure of complexes formed upon the adsorption of simple organic acids on aluminum hydroxide

Information on the binding of organic ligands to metal （hydr）oxide surfaces is useful for understanding the adsorption behaviour of natural organic matter on metal （hydr）oxide. In this study, benzoate and salicylate were employed as the model organic ligands and aluminum hydroxide as the metal hydroxide. The attenuated total reflectance Fourier transform infrared （ATR-FTIR） spectra revealed that the ligands benzoate and salicylate do coordinate directly with the surface of hydrous aluminum hydroxide, thereby forming innersphere surface complexes. It is concluded that when the initial pH is acidic or neutral, monodentate and bridging complexes are to be formed between benzoate and aluminum hydroxide while bridging complexes predominate when the initial pH is alkalic. Monodentate and bridging complexes can be formed at pH 5 while precipitate and bridging complexes are formed at pH 7 when salicylate anions are adsorbed on aluminum hydroxide. The X-ray photoelectron （XP） spectra demonstrated the variation of C 1 s binding energy in the salicyate and phenolic groups before and after adsorption. It implied that the benzoate ligands are adsorbed through the complexation between carboxylate moieties and the aluminum hydroxide surface, while both carboxylate group and phenolic group are involved in the complexation reaction when salicylate is adsorbed onto aluminum hydroxide. The information offered by the XPS confirmed the findings obtained with ATR-FTIR.     

经饮水亚慢性铝染毒对大鼠血铁及相关蛋白水平的影响

为了探讨慢性铝暴露对大鼠铁代谢的影响,将100只4周龄清洁级雄性Wistar大鼠随机均分成摄铝组(430mg·L-1,以Al3+计)与对照组(蒸馏水),饮水染铝,每隔30d处死染铝大鼠和对照大鼠各10只,实验周期为150d.同时,在不同时间点(30d、60d、90d、120d、150d)测量大鼠体重,并进行协方差分析.最后,用火焰原子吸收分光光度法、固相竞争ELISA和比色法检测血浆Al、Fe、转铁蛋白(TF)、可溶性转铁蛋白受体(sTfR)含量及总铁结合力(TIBC).结果表明,在摄铝前期(90d前),染铝对大鼠体重无显著影响,而后期(120d后)染铝对大鼠体重抑制作用较大.在实验周期内,各时间点间对照组血浆中各指标均无显著差异,摄铝组随着时间的延长各指标变化较大.各时间点摄铝组血浆中Al含量及Al/Fe均显著高于对照组(p0.01);30d时摄铝组血浆中Fe含量与对照组相比无显著差异(p0.05),60、90、120d时均显著低于对照组(p0.01),150d时显著高于对照组(p0.01);30、60d时摄铝组血浆TF含量与对照组相比无显著差异(p0.05),90d后显著高于对照组(p0.05;p0.01);30、60d时摄铝组TIBC与对照组相比无显著差异(p0.05),其后各时间点均显著高于对照组(p0.01);30d时摄铝组sTfR含量与对照组相比无显著差异(p0.05),其后各时间点均显著低于对照组(p0.01).由此可见,铝可干扰大鼠体内铁的代谢,影响铁的生物学作用.     

Effect of competing solutes on arsenic（Ⅴ） adsorption using iron and aluminum oxides

The study focused on the effect of several typical competing solutes on removal of arsenic with Fe_2O_3 and AL_2O_3.The test results indicate that chloride,nitrate and sulfate did not have detectable effects,and that selenium(Ⅳ)(Se(Ⅳ))and vanadium(Ⅴ)(V(Ⅴ)) showed slight effects on the adsorption of As(Ⅴ)with Fe_2O_3.The results also showed that adsorption of As(Ⅴ)on AL_2O_3 was not affected by chloride and nitrate anions,but slightly by Se(Ⅳ)and V(Ⅴ)ions.Unlike the adsorption of As(Ⅴ)with Fe_2O_3,that with Fe_2O_3 was affected by the presence of sulfate in water solutions.Both phosphate and silica have significant adverse effects on the adsorption of As(Ⅴ)adsorption with Fe_2O_3 and Al_2O_3.Compared to the other tested anions,phosphate anion was found to be the most prominent solute affecting the As(Ⅴ)adsorption with Fe_2O_3 and Al_2O_3.In general,Fe_2O_3 has a better performance than Al_2O_3 in removal of As(Ⅴ)within a water environment where multi competing solutes are present.     

Formation of CoAl layered double hydroxide on the boehmite surface and its role in tungstate sorption

Sorption of tungstate on boehmite(γ-Al OOH)is increased by co-sorption with Co~(2+)over the near-neutral p H range.Batch uptake experiments show up to a 3-fold increase in tungstate uptake over the range WO_4~(2-)=50–1000μmol/L compared to boehmite not treated with Co~(2+).Desorption experiments reveal a corresponding decrease in sorption reversibility for tungstate co-sorbed with Co~(2+).Reaction of boehmite with Co~(2+)results in the formation of Co Al layered double hydroxide(LDH),as confirmed by X-ray diffraction and X-ray absorption spectroscopy.Tungsten L_3-edge X-ray absorption near edge structure(XANES)reveals that W(VI)is octahedrally coordinated in all sorption samples,with polymeric tungstate species forming at higher tungstate concentrations.X-ray diffraction and X-ray absorption spectroscopy indicate that the mechanism for enhancement of tungstate uptake is the formation of surface complexes on boehmite at low tungstate concentrations,while exchange into the Co Al LDH becomes important at higher tungstate concentrations.The results provide a basis for developing strategies to enhance tungstate sorption and to limit its environmental mobility at near-neutral pH conditions.