Antimony(V) removal from water by iron-zirconium bimetal oxide: Performance and mechanism

A Fe-Zr binary oxide adsorbent has been successfully synthesized using a co-precipitation method. It showed a better performance for antimonate (Sb(V)) removal than zirconium oxide or amorphous ferric oxide. The experimental results showed that the Fe-Zr adsorbent has a capacity of 51 mg/g at an initial Sb(V) concentration of 10 mg/L at pH 7.0. Sb(V) adsorption on the Fe-Zr bimetal oxide is normally an endothermic reaction. Most of the Sb(V) adsorption took place within 3 hr and followed a pseudo second-order rate law. Co-existing anions such as SO₄^2-, NO₃^- and Cl^- had no considerable effects on the Sb(V) removal; PO₃^4- had an inhibitory effect to some extent at high concentration; while CO_₃^2- and SiO₄^4- showed significant inhibitory effects when they existed in high concentrations. The mechanism of Sb(V) adsorption on the adsorbent was investigated using a combination of zeta potential measurements, XPS, Raman, FT-IR observations and SO₄^2- release determination. The ionic strength dependence and zeta potential measurements indicated that inner-sphere surface complexes were formed after Sb(V) adsorption. Raman and XPS observations demonstrated that both Fe-OH and Zr-OH sites at the surface of the Fe-Zr adsorbent play important roles in the Sb(V) adsorption. FT-IR characterization and SO₄^2- release determination further demonstrated that the exchange of SO₄^2- with Sb(V) also could promote the adsorption process. In conclusion, this adsorbent showed high potential for future application in Sb(V) removal from contaminated water.     

支化聚乙烯亚胺功能化磁性纳米吸附剂的制备及对Cu2+的吸附研究

为解决水体中重金属Cu²⁺污染,本研究首先采用水热法制备得到超顺磁四氧化三铁纳米粒子,然后使用对Cu²⁺具有强络合作用的含有丰富氨基官能团的支化聚乙烯亚胺接枝到纳米粒子表面,得到Fe₃O₄@BPEI磁性纳米吸附剂。采用红外光谱(FTIR)、X射线粉末衍射(XRD)、透射电子显微镜(TEM)等对其结构、尺寸及形貌进行表征。研究了不同吸附因素对吸附剂吸附Cu²⁺的影响,确定了最佳吸附条件,并通过吸附动力学模型和吸附等温线模型进一步探讨吸附机理。结果表明：支化聚乙烯亚胺成功接枝到四氧化三铁纳米粒子表面。最佳吸附条件为pH=6.0、吸附平衡时间为40 min、吸附剂用量为10 mg。通过实验数据拟合,Fe₃O₄@PEI吸附Cu²⁺的过程符合Langmuir等温吸附方程和拟二级动力学模型,表明吸附过程为化学吸附控制的单分子层覆盖,在303 K时,模型理论饱和吸附量为141.24 mg/g。表明支化聚乙烯亚胺修饰的磁性纳米吸...     

淀粉稳定Fe3O4纳米粒子对水中As(V)的吸附特性研究

以可溶性淀粉作为稳定剂制备纳米Fe_3O_4粒子,探讨了反应时间、p H值、初始砷浓度和腐殖酸对Fe_3O_4纳米粒子吸附水体中As(V)的吸附效果影响.实验结果表明,淀粉稳定的Fe_3O_4纳米粒子对水体中As(V)的吸附动力学过程符合准二级动力学,吸附等温线符合Langmuir吸附模型;吸附容量随着溶液p H的增加逐渐降低,在p H为8.0的弱碱性水体中对As(V)的最大吸附容量可达202.56 mg·g~(-1);此外,腐殖酸(HA)能降低纳米粒子对As(V)的吸附能力.     

羟基磷灰石-四氧化三铁-沸石复合材料制备及去除水中刚果红研究

采用可溶性磷酸盐、钙离子、二价铁离子、三价铁离子和天然沸石等材料制备了羟基磷灰石-四氧化三铁-沸石(HAPFe3O4-沸石)复合材料,对该复合材料进行了表征,并考察了该复合材料对水中刚果红的吸附作用.结果表明,HAP-Fe3O4-沸石复合材料对水中的刚果红具备良好的吸附能力.当pH由3增加到4或由7增加到11时,HAP-Fe3O4-沸石复合材料对水中刚果红的去除能力下降;当pH由4增加到7时,对刚果红的吸附能力基本保持不变.HAP-Fe3O4-沸石复合材料对水中刚果红的去除率随吸附剂投加量的增加而增加,而对水中刚果红的单位吸附量则随吸附剂投加量的增加而降低.HAP-Fe3O4-沸石复合材料对水中刚果红的吸附动力学过程可以较好地采用准二级动力学模型加以描述,对刚果红的吸附平衡数据可以采用Langmuir和Freundlich等温吸附模型加以描述.根据Langmuir模型确定的最大吸附容量为117 mg·g-1.(pH 7和303 K).HAP-Fe3O4-沸石复合材料对水中刚果红的吸附是自发吸热并伴随熵增加的过程.当pH为7时,HAP-Fe3O4-沸石复合材料吸附水中刚果红的主要机制包括表面配位作用、氢键作用以及路易斯酸碱反应.采用热再生的方法可以使吸附刚果红后的HAP-Fe3O4-沸石复合材料得到再生,热再生后的复合材料可以循环使用并且对水中刚果红的吸附性能良好.X射线衍射分析结果表明HAP-Fe3O4-沸石复合材料含Fe3O4,磁滞回线结果表明HAP-Fe3O4-沸石复合材料具备较高的磁饱和强度,复合材料吸附刚果红后可以很容易地通过外加磁场的作用快速地与水溶液分离.结果表明,HAP-Fe3O4-沸石复合材料适合作为一种吸附剂去除废水中的刚果红.     

Fe3O4@SiO2-Chitosan的制备及其对水中Cu2+的吸附效能研究

以SiO_2包覆Fe_3O_4,戊二醛为交联剂,交联壳聚糖(Chitosan, CTS),制得Fe_3O_4@SiO_2-Chitosan复合磁性纳米粒子.以Fe_3O_4和Fe_3O_4@SiO_2为对照,采用X射线衍射、透射电镜和傅立叶红外光谱对其进行表征分析,并测定了投加量、pH值、吸附时间和温度等因素对Cu~(2+)吸附效果的影响,从动力学、热力学以及再生回用性能评价等方面对其吸附性能进行了探究.结果表明Fe_3O_4@SiO_2-Chitosan对Cu~(2+)的吸附过程符合准二级吸附动力学模型和Langmuir模型,为自发、放热、优惠型的单分子层化学吸附.在pH为6.0, 298 K下达到最大吸附量154.8 mg·g~(-1),吸附解吸4次后吸附容量变化不大,说明Fe_3O_4@SiO_2-Chitosan具有较高的吸附容量,可作为处理含铜废水和回收铜的高效吸附剂.     

Immobilization of antimony in soil and groundwater using ferro-magnesium bimetallic organic frameworks

Sb(Ⅲ) is often detected in contaminated soil and groundwater. Hence, high-efficiency technology is needed. In this study, bimetallic organic frameworks were used for the first time to immobilize Sb(Ⅲ) from contaminated soil and groundwater. The materials were synthesized by the hydrothermal method. Both ends of the prepared material were hexagonal tip rods,and the length became shorter as the ratio of Fe/Mg decreased. The bimetallic organic framework with a Fe/Mg feeding ratio of 0.5 was the opt...     

响应曲面法优化Fe(Ⅲ)改性卡氏变形杆菌吸附去除Sb(Ⅴ)及其机理

水环境中过量Sb（Ⅴ）所引起的环境危害受到越来越多的关注.为了考察工艺参数对铁盐改性生物吸附剂吸附Sb（Ⅴ）效果影响、交互作用及其机理,以Fe（Ⅲ）改性卡氏变形杆菌吸附剂（简称“FMPAs”）为研究对象,采用Box-Behnken响应曲面法对FMPAs吸附处理合成含Sb（Ⅴ）废水的吸附时间、FMPAs投加量、pH、温度及Sb（Ⅴ）初始浓度等因素进行优化,确定了最优吸附条件,并对吸附过程的等温模型、动力学模型及吸附机理进行了研究.结果表明:①FMPAs吸附Sb（Ⅴ）的最优条件为吸附时间3.0 h、FMPAs投加量1 910.04 mg/L、pH 2.31、温度45.0℃、Sb（Ⅴ）初始浓度24.80 mg/L,且最优条件下Sb（Ⅴ）的去除率高达97.03%.②FMPAs对Sb（Ⅴ）的吸附符合Langmuir等温吸附模型,其最大吸附容量（q_max）为60.506 mg/g,其吸附动力学过程可采用准一级动力学模型拟合,属于单层吸附和化学吸附.③FMPAs吸附Sb的机理主要为Fe（Ⅲ）改性卡氏变形杆菌生成了Fe—O—OH、Polyose—Fe、Polyose—O—Fe（OH）₂等化合物,这些物质中羟基被Sb（Ⅴ）取代生成新的配合物Fe—O—Sb,使Sb（Ⅴ）得到吸附去除.研究显示,FMPAs对Sb（Ⅴ）具有较高的吸附容量,是一种极具潜在应用价值的绿色生物质吸附剂,可用于处理含Sb（Ⅴ）废水.      

Removal of Cs from water and soil by ammonium-pillared montmorillonite/Fe3O4 composite

To remove cesium ions from water and soil, a novel adsorbent was synthesized by following a one-step co-precipitation method and using non-toxic raw materials. By combining ammonium-pillared montmorillonite (MMT) and magnetic nanoparticles (Fe₃O₄), an MMT/Fe₃O₄ composite was prepared and characterized. The adsorbent exhibited high selectivity of Cs⁺ and could be rapidly separated from the mixed solution under an external magnetic field. Above all, the adsorbent had high removal efficiency in cesium-contaminated samples (water and soil) and also showed good recycling performance, indicating that the MMT/Fe₃O₄ composite could be widely applied to the remediation of cesium-contaminated environments. It was observed that the pH, solid/liquid ratio and initial concentration affected adsorption capacity. In the presence of coexisting ions, the adsorption capacity decreased in the order of Ca^2 + > Mg^2 + > K⁺ > Na⁺, which is consistent with our theoretical prediction. The adsorption behavior of this new adsorbent could be expressed by the pseudo-second-order model and Freundlich isotherm. In addition, the adsorption mechanism of Cs⁺ was NH₄⁺ ion exchange and surface hydroxyl group coordination, with the former being more predominant.     

Antimony(V) removal from water by hydrated ferric oxides supported by calcite sand and polymeric anion exchanger

We fabricated and characterized two hybrid adsorbents originated from hydrated ferric oxides(HFOs) using a polymeric anion exchanger D201 and calcite as host. The resultant adsorbents(denoted as HFO-201 and IOCCS) were employed for Sb(V) removal from water. Increasing solution pH from 3 to 9 apparently weakened Sb(V) removal by both composites, while increasing temperature from 293 to 313 K only improved Sb(V) uptake by IOCCS. HFO-201 exhibited much higher capacity for Sb(V) than for IOCCS in the absence of other anions in solution. Increasing ionic strength from 0.01 to 0.1 mol/L NaNO3would result in a significant drop of the capacity of HFO-201 in the studied pH ranges; however, negligible effect was observed for IOCCS under similar conditions. Similarly, the competing chloride and sulfate pose more negative effect on Sb(V) adsorption by HFO-201 than by IOCCS, and the presence of silicate greatly decreased their adsorption simultaneously, while calcium ions were found to promote the adsorption of both adsorbents. XPS analysis further demonstrated that preferable Sb(V) adsorption by both hybrids was attributed to the inner sphere complexation of Sb(V) and HFO, and Ca(II) induced adsorption enhancement possibly resulted from the formation of HFO-Ca-Sb complexes. Column adsorption runs proved that Sb(V) in the synthetic water could be effectively removed from 30 μg/L to below 5 μg/L(the drinking water standard regulated by China), and the effective treatable volume of IOCCS was around 6 times as that of HFO-201, implying that HFO coatings onto calcite might be a more effective approach than immobilization inside D201.     

High phosphate removal using La(OH)3 loaded chitosan based composites and mechanistic study

Our present study was to prepare a biomass-supported adsorbents with high adsorptive capacity and high selectivity to prevent the accelerated eutrophication in water body. To this end, different metal hydroxide (La, Zr and Fe) first was successfully loaded on chitosan microspheres. Then the quaternary ammonium group with different content was introduced into the adsorbent by polymerization. By comparison of adsorption properties, chitosan-La(OH)₃-quaternary ammonium-20% (CS-La-N-20%) has strong adsorption to phosphate (160 mg/g) by immobilizing nano-sized La(OH)₃ within a quaternary-aminated chitosan and it maintain high adsorption in the presence of salt ions. The pH results indicated that the CS-La-N-20% would effectively sequestrate phosphate over a wide pH range between 3 and 7 without significant La³⁺ leaching. What's more, adsorption capacity on the introduce of positively charged quanternary-aminated groups was significantly higher than that of the unmodified adsorbents at alkaline conditions. The column adsorption capacity reached 1300 bed volumes (BV) when phosphate concentration decreased until 0.5 mg/L at 6 BV/hr. The column adsorption/desorption reveals that no significant capacity loss is observed, indicating excellent stability and repeated use property. Characterizations revealed that phosphate adsorption on CS-La-N-20% through ligand exchange (impregnated nano-La(OH)₃) and electrostatic attraction (positively charged quanternary-aminated groups). All the results suggested that CS-La-N-20% can serve as a promising adsorbent for preferable phosphate removal in realistic application.