海藻酸钠-氢氧化镧改性Y型分子筛颗粒除氟研究

doi:10.11962/1006-4990.2020-0059

摘要/Abstract

摘要：

为解决除氟吸附剂分离困难、有效成分流失等问题,以海藻酸钠（SA）与氢氧化镧改性Y型分子筛（LHMS）为原料,采用滴球法制备了SA@LHMS颗粒吸附剂,并采用模拟废水对其进行了除氟研究。通过正交实验确定了吸附剂最佳制备条件,并通过间歇吸附实验测试了吸附剂投加量、pH、共存离子等因素对吸附的影响,探究了吸附速率、吸附等温线等吸附性能。结果表明,SA@LHMS吸附速率曲线符合拟二级反应速率方程;吸附等温线符合Ⅱ型等温线,为多分子层吸附;初始pH（3~12）对吸附效果没有显著影响;高浓度共存阴离子（50 mg/L）对吸附过程有一定抑制;1 mol/L和2 mol/L氢氧化钠溶液对SA@LHMS再生效果较好,经3次再生仍然保留较高的吸附能力。SA@LHMS颗粒表面和截面形态以及吸附前后颗粒的表面形态差异明显;吸附前后颗粒表面能谱（EDS）分析以及红外光谱（FT-IR）分析结果显示,吸附过程中溶液中的氟离子（F^-）与颗粒表面及内部的羟基（—OH）发生配体交换。

关键词: 海藻酸钠, 颗粒吸附剂, 除氟, 氢氧化镧, Y型分子筛

Abstract:

In order to solve the problem of the separation of defluorinated adsorbents and the loss of effective components,SA@LHMS adsorbents were prepared with sodium alginate（SA） and lanthanum hydroxide modified Y zeolite （LHMS） as raw materials.The optimum preparation conditions of adsorbent were determined by orthogonal experiment.The effect of factors,such as dosage of adsorbent,pH and co-existing ions etc.,was tested by batch adsorption experiment,and the adsorption performance of adsorption rate and adsorption isotherm was researched.The results showed that the adsorption rate curve of the SA@LHMS conformed to the second-order reaction rate equation.Adsorption isotherm conformed to the type Ⅱ isotherm,multilayer physical adsorption.The initial pH （3~12） had no significant effect on the adsorption effect.High concentration of co-existing anions （50 mg/L） inhibited the adsorption process.The regeneration effect of 1 mol/L and 2 mol/L NaOH solution on SA@LHMS was better,and SA@LHMS still retained a high adsorption capacity after three regeneration.The surface and cross section morphology of SA @LHMS as well as the surface morphology before and after adsorption were significantly different.EDS component analysis and FT-IR spectrum analysis before and after adsorption showed that ligand exchange occur-curred between F^- and —OH on the surface and inside of particles during adsorption.

Key words: sodium alginate, particle adsorbent, defluorination, lanthanum hydroxide, Y zeolite

中图分类号:

TQ133.3

卞晓彤,邱兆富,杨骥,严瑞琪,吕树光. 海藻酸钠-氢氧化镧改性Y型分子筛颗粒除氟研究[J]. 无机盐工业, 2020, 52(12): 86-91.

Bian Xiaotong,Qiu Zhaofu,Yang Ji,Yan Ruiqi,Lü Shuguang. Study on fluoride removal by modified Y zeolite particles with sodium alginate-lanthanum hydroxide[J]. Inorganic Chemicals Industry, 2020, 52(12): 86-91.

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水平	因素
水平	SA质量分数/%	CaCl₂ 质量分数/%	交联时间/ h	LHMS包埋量/（g·L^-1）
1	1	2	12	60
2	2	3	24	80
3	3	4	36	100

实验编号	因素水平				F^-去除率/%
实验编号	A	B	C	D	F^-去除率/%
1	1	1	1	1	85.5
2	1	2	2	2	79.7
3	1	3	3	3	84.5
4	2	1	2	2	87.9
5	2	2	3	3	80.2
6	2	3	1	1	75.4
7	3	1	3	3	57.2
8	3	2	1	1	59.6
9	3	3	2	2	59.1
k₁	83.2	76.9	73.5	73.5
k₂	81.2	73.2	75.6	75.6
k₃	58.6	73.0	74.0	74.0
R	24.6	3.9	2.1	2.1

拟一级动力学模型	q_e	k₁	R²	备注
log（q_e-q_t）=log q_e-（k₁/2.303）t	0.457	0.002	0.627 6	—
拟二级动力学模型	q_e	k₂	R²	备注
t/q_t=1/k₂q_e²+（1/q_e）t	0.454	0.040	0.999 4	—
Weber-Morris动力学模型	k_ip	C	R²	备注
q_t=k_ipt^1/2+C	0.043	-0.065	0.994 7	阶段1
	0.007	0.237	0.967 3	阶段2
	0.000	0.439	0.320 4	阶段3

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