Onyango Maurice S, Kojima Yoshihiro, Aoyi Ochieng, Bernardo Eileen C, Matsuda Hitoki
Department of Chemical Engineering, Nagoya University, Nagoya 464-8603, Japan.
J Colloid Interface Sci. 2004 Nov 15;279(2):341-50. doi: 10.1016/j.jcis.2004.06.038.
Fluoride in drinking water above permissible levels is responsible for human dental and skeletal fluorosis. In this study, therefore, the large internal surface area of zeolite was utilized to create active sites for fluoride sorption by exchanging Na+-bound zeolite with Al3+ or La3+ ions. Fluoride removal from water using Al3+- and La3+-exchanged zeolite F-9 particles was subsequently investigated to evaluate the fluoride sorption characteristics of the sorbents. Equilibrium isotherms such as the two-site Langmuir (L), Freundlich (F), Langmuir-Freundlich (LF), Redlich-Peterson (RP), Toth (T), and Dubinin-Radushkevitch (DR) were successfully used to model the experimental data. Modeling results showed that the isotherm parameters weakly depended on the solution temperature. From the DR isotherm parameters, it was considered that the uptake of fluoride by Al3+-exchanged zeolite proceeded by an ion-exchange mechanism (E = 11.32-12.13 kJ/mol), while fluoride-La3+-exchanged zeolite interaction proceeded by physical adsorption (E = 7.41-7.72 kJ/mol). Factors from the solution chemistry that affected fluoride removal from water were the solution pH and bicarbonate content. The latter factor buffered the system pH at higher values and thus diminished the affinity of the active sites for fluoride. Natural groundwater samples from two Kenyan tube wells were tested and results are discussed in relation to solution chemistry. In overall, Al3+-exchanged zeolite was found to be superior to La3+-exchanged zeolite in fluoride uptake within the tested concentration range.
饮用水中氟化物含量超过允许水平会导致人类牙齿和骨骼氟中毒。因此,在本研究中,利用沸石较大的内表面积,通过用Al3+或La3+离子交换Na+结合的沸石来创建氟化物吸附的活性位点。随后研究了使用Al3+和La3+交换的沸石F-9颗粒从水中去除氟化物的情况,以评估吸附剂的氟化物吸附特性。成功地使用了双位点朗缪尔(L)、弗伦德利希(F)、朗缪尔-弗伦德利希(LF)、雷德利希-彼得森(RP)、托特(T)和杜比宁-拉杜舍维奇(DR)等平衡等温线对实验数据进行建模。建模结果表明,等温线参数对溶液温度的依赖性较弱。根据DR等温线参数,认为Al3+交换的沸石对氟化物的吸收是通过离子交换机制进行的(E = 11.32 - 12.13 kJ/mol),而氟化物与La3+交换的沸石之间的相互作用是通过物理吸附进行的(E = 7.41 - 7.72 kJ/mol)。影响从水中去除氟化物的溶液化学因素是溶液pH值和碳酸氢盐含量。后一个因素将系统pH值缓冲在较高水平,从而降低了活性位点对氟化物的亲和力。对来自肯尼亚两口管井的天然地下水样本进行了测试,并结合溶液化学对结果进行了讨论。总体而言,发现在测试浓度范围内,Al3+交换的沸石在氟化物吸收方面优于La3+交换的沸石。