摘要
采用共沉淀法合成了阳离子摩尔比为2∶1(2Mg/Al LDHs)和4∶1(4Mg/Al LDHs)的镁铝水滑石,利用X射线衍射仪、比表面积及孔径分布仪和zeta电位分析仪表征了两种水滑石的基本性质,并且研究了不同p H值、不同时间、不同初始浓度以及共存离子种类等因素对镁铝水滑石吸附Sb(V)的影响。结果表明,由于CO_3~(2-)在层间的排列方式不同导致镁铝水滑石晶面间距存在明显差异;并且两种水滑石具有较高的总孔容积、比表面积和等电点。镁铝水滑石对Sb(V)的吸附动力学和吸附等温式分别可以由假二级动力学模型和Langmuir吸附等温式描述。模型拟合结果显示,2Mg/Al LDHs的吸附速率和吸附量分别高达0.19 g/(mg·h)和50.52 mg/g。镁铝水滑石对Sb(V)的去除机制主要包括表面物理吸附、阴离子交换和静电吸引等。
Magnesium-aluminium layered double hydroxides with cationic molar ratio of 2:1(2 Mg/Al LDHs) and 4:1(4 Mg/Al LDHs) was synthesized by coprecipitation method. The basic properties of the two layered double hydroxides were characterized by X-ray diffraction, specific surface area and pore size distribution and zeta potential analyzer. The adsorption of Sb(V) on magnesium-aluminium layered double hydroxides at different pH, different time, different initial concentration and types of coexisting ions was studied. The results show that the spacing between crystal planes of Mg/Al layered double hydroxides is obviously different due to the different arrangement of CO_3~(2-)between layers, and the two layered double hydroxides have higher total pore volume, specific surface area and isoelectric point. The adsorption kinetics and isotherm of Mg/Al layered double hydroxides on Sb(V) can be described by pseudo-second-order kinetic model and Langmuir adsorption isotherm, respectively. The model fitting results showed that the adsorption rate and amount of 2 Mg/Al LDHs were as high as 0.19 g/(mg·h) and 50.52 mg/g, respectively. The removal mechanism of Sb(V) by Mg/Al layered double hydroxides mainly includes surface physical adsorption, anion exchange and electrostatic attraction.
引文
[1]黄艳超,武雪芳,周羽化,等.水环境中锑污染及其修复技术研究进展[J].南京师范大学学报(自然科学版),2015,38(4):122-128.
[2]赵雪芹.新型铁基铝基吸附剂去除水中锑性能及其机理研究[D].北京:北京林业大学,2014.
[3]李志萍,杨晶晶,孙程奇,等.水中锑污染处理方法的研究进展[J].工业水处理,2018,38(6):12-16.
[4]Lei C,Zhu X,Zhu B,et al.Superb adsorption capacity of hierarchical calcined Ni/Mg/Al layered double hydroxides for Congo red and Cr(VI)ions[J].Journal of Hazardous Materials,2017,321:801-811.
[5]孙媛媛.Mg/Al双金属氧化物对As(V)吸附性能的研究[J].环境科学学报,2011,31(7):1377-1385.
[6]郭亚祺,杨洋,伍新花,等.煅烧的水滑石同时去除水体中砷和氟[J].环境工程学报,2014,8(6):2485-2491.
[7]WANG S L,WANG P C.In situ XRD and ATR-FTIR study on the molecular orientation of interlayer nitrate in Mg/Al-layered double hydroxides in water[J].Colloids and Surfaces A(Physicochemical and Engineering Aspects),2007,292(2/3):131-138.
[8]DORE E,FRAU F.Antimonate uptake by calcined and uncalcined layered double hydroxides:effect of cationic composition and M2+/M3+molar ratio[J].Environmental Science&Pollution Research,2018,25(2):1-14.
[9]SING K S.Reporting physisorption data for gas/solid systems with special reference to the determination of surface area and porosity(Recommendations 1984),Pure Appl Chem,1985,57:603-619.
[10]KAMEDA T,NAKAMURA M,YOSHIOKA T.Removal of antimonate ions from an aqueous solution by anion exchange with magnesium-aluminum layered double hydroxide and the formation of a brandholzite-like structure[J].Environmental Letters,2012,47(8):6.
[11]BOURAADA M,BELHALFAOUI F,OUALI M S,et al.Sorption study of an acid dye from an aqueous solution on modified Mg-Al layered double hydroxides[J].Journal of Hazardous Materials,2009,163(1):463-467.
[12]LAZARIDIS N K,ASOUHIDOU D D.Kinetics of sorptive removal of chromium(VI)from aqueous solutions by calcined Mg-Al-CO3hydrotalcite[J].Water Research,2003,37(12):2875-2882.
[13]HO Y S,MCKAY G.Pseudo-second order model for sorption processes[J].Process Biochemistry,1999,34(5):451-465.
[14]ARAMENDA M A,BORAU V,JIMENEZ C,et al.Comparative study of Mg/M(M=AI,Ga,In)layered double hydroxides obtained by coprecipitation and the sol-gel method.Journal of Solid State Chemistry,2002,168(1):156-161.
[15]LIU L,LIN Y,LIU Y,et al.Removal of Methylene Blue from Aqueous Solutions by Sewage Sludge Based Granular Activated Carbon:Adsorption Equilibrium,Kinetics,and Thermodynamics[J].Journal of Chemical&Engineering Data,2013,58(8):2248-2253.
[16]CONSTANTINO L V,QUIRINO J N,ABRAO T,et al.Sorptiondesorption of antimony species onto calcined hydrotalcite:surface structure and control of competitive anions[J].Journal of Hazardous Materials,2018,344:649-656.
[17]张慧,吴攀,李怡.铁氧化物改性凹凸棒土吸附Sb(V)的性能研究[J].贵州大学学报(自然科学版),2015,32(3):131-136.