尿素分解共沉淀法中反应时间对ZnAl类水滑石结构和磷吸附性能的影响

Influence of Reaction Time of Urea Hydrolysis-Based Co-precipitation on the Structure of ZnAl Layered Double Hydroxides and the Phosphate Adsorption

采用尿素分解均匀共沉淀法合成了一系列反应时间不同的ZnAl类水滑石,考察了其结构特征及其对水中磷酸根的吸附性能.结果表明,随着反应时间由12 h增加至96 h,制得的ZnAl均具有典型的类水滑石层状结构,但其中的n(Zn)/n(Al)由2.06降至0.70,比表面积升至ZnAl-12的7.6倍.样品中Al比例升高引起的层板正电性增加以及样品比表面积的升高引起了ZnAl对水中磷酸根的吸附性能总体上随着其制备反应时间的增加逐渐增强,同时表明表面的物理化学吸附在磷酸根的去除过程中具有重要作用.当反应时间为24 h时,制备得到的ZnAl类水滑石由于其很高的可交换阴离子含量而具有最高的磷酸根吸附性能,其在25℃的饱和吸附量(以P计)约为34.1 mg.g-1.这说明离子交换也是一种十分重要的磷去除途径.此外,不同反应时间制得的类水滑石对磷酸根的吸附等温线表现为Langmuir型;测得的磷吸附动力学结果均符合准二级动力学方程.

A series of ZnAl layered double hydroxides（LDHs） were prepared by urea hydrolysis-based homogeneous co-precipitation for studying their structure and phosphate adsorption capacities.The results show that all the samples exhibited a typical layered structure as the reaction time extended from 12 h to 96 h,whereas Zn/Al molar ratio in the ZnAls decreased from 2.06 to 0.70 and the specific surface area markedly increased to be 7.6-fold higher than that of ZnAl-12.Phosphate adsorption capacity of the ZnAl was in general increased gradually with the reaction time extension,which can be attributed to the surface area rising as well as the increased positive charge of LDHs layer caused by a higher proportion of Al.This reveals that physicochemical adsorption on LDHs surface would have played an important role during the phosphate adsorption.With a reaction time of 24 h,a high amount of exchangeable interlayer anions was observed,giving rise to a highest phosphate uptake of 34.1 mg·g-1 by the ZnAl-24.It indicates the ion exchange was another major pathway for the phosphate removal.For all the ZnAls with different reaction times,the phosphate adsorption isotherms fit well with Langmuir-type equations;the adsorption kinetics followed pseudo-second-order models.