Fe3+改性类水滑石对废水中氟化物的吸附性能

doi:10.12422/j.issn.1672-6952.2024.06.001

摘要/Abstract

摘要：

采用共沉淀法合成两种吸附剂镁铝焙烧态水滑石（MgAl LDO）和镁铝铁焙烧态水滑石（MgAlFe LDO），并通过X射线粉末衍射（XRD）分析、扫描电子显微镜（SEM）分析、傅里叶变换红外光谱（FT?IR）分析、BET比表面积测试分析等手段对其进行了表征，同时研究了两种吸附剂对废水中F^－的吸附性能；考察了金属的物质的量比、煅烧温度、F^－初始质量浓度、吸附剂投加量对废水中F^－去除效果的影响。结果表明，MgAlFe LDO孔结构分布均匀，拥有较大的比表面积，对废水中F^－的吸附能力高于MgAl LDO；当n(Mg²⁺)/n(Al³⁺)/n(Fe³⁺)=3.0∶0.6∶0.4、F^－初始质量浓度为20 mg/L、煅烧温度为300 ℃、MgAlFe LDO的投加量为0.4 g时，废水中F^－的去除效果最佳；反应2 h后，废水中F^－的去除率为98.35%。

关键词: 镁铝铁焙烧态水滑石, 废水氟化物, 吸附

Abstract:

Two adsorbents, magnesium aluminum calcined hydrotalcite (MgAl LDO) and magnesium aluminum iron calcined hydrotalcite (MgAlFe LDO), were synthesized by coprecipitation method, and characterized by X?ray powder diffraction (XRD) analysis, scanning electron microscopy (SEM) analysis, Fourier transform infrared spectroscopy (FT?IR) analysis and BET specific surface area test analysis, etc. The adsorption performance of the two adsorbents for fluoride in wastewater was also studied. The effects of the ratio of metal substances, calcination temperature, initial mass concentration of F^-, and adsorbent dosage on the removal efficiency of fluoride in wastewater were investigated. The results showed that MgAlFe LDO had a uniform pore structure distribution, a large specific surface area, and a higher adsorption capacity for fluoride in wastewater than that of MgAl LDO. When n (Mg²⁺)/n (Al³⁺)/n (Fe³⁺)=3.0∶0.6∶0.4, the initial mass concentration of F^- was 20 mg/L, the calcination temperature was 300 ℃, and the dosage of MgAlFe LDO was 0.4 g, the removal effect of fluoride in wastewater was optimal. After 2 hours of reaction, the removal rate of fluoride in the wastewater was 98.35%.

Key words: MgAlFe LDO, Waste water fluoride, Adsorbent

中图分类号:

TQ110.9

尹波, 李政, 顾贵洲, 于喜洋, 王辉, 徐习习. Fe³⁺改性类水滑石对废水中氟化物的吸附性能[J]. 辽宁石油化工大学学报, 2024, 44(6): 1-9.

Bo YIN, Zheng LI, Guizhou GU, Xiyang YU, Hui WANG, Xixi XU. Adsorption Performance of Fe³⁺Modified Hydrotalcite for Fluoride in Wastewater[J]. Journal of Liaoning Petrochemical University, 2024, 44(6): 1-9.

图/表 17

图1 MgAl LDO和MgAlFe LDO的XRD谱图

Fig.1 XRD patterns of MgAl LDO and MgAlFe LDO

表1 MgAl LDO和MgAlFe LDO的XRD晶体参数

Table 1 XRD crystal parameters of MgAl LDO andMgAlFe LDO

样品	d₀₀₃/nm	d₁₁₀/nm	a/nm	c/nm
MgAl LDO	0.778 0	0.176 6	0.353 2	2.334 0
MgAlFe LDO	0.785 9	0.176 4	0.352 9	2.357 9

图2 吸附剂煅烧前后的SEM图像

Fig.2 SEM images of adsorbent before and after calcination

图3 MgAl LDO和MgAlFe LDO的FT?IR谱图

Fig.3 FT?IR spectra for MgAl LDO and MgAlFe LDO

表2 MgAl LDO和MgAlFe LDO的比表面积、孔容、平均粒径的BET计算结果

Table 2 BET calculation results of specific surface area, pore volume and average particle size of MgAl LDO and MgAlFe LDO

参数	数值
参数	MgAl LDO	MgAlFe LDO
比表面积/(m²·g^-1)	170.72	196.30
孔容/(mL·g^-1)	0.299 1	0.810 1
平均粒径/nm	8.14	33.65

图4 金属的物质的量比对MgAl LDO和MgAlFe LDO吸附性能的影响

Fig.4 Effect of substance ratio on the adsorption performance of MgAl LDO and MgAlFe LDO

图5 煅烧温度对MgAl LDO和MgAlFe LDO吸附性能的影响

Fig.5 Effect of calcination temperature on the adsorption properties of MgAl LDO and MgAlFe LDO

图6 MgAl LDO和MgAlFe LDO投加量对吸附性能的影响

Fig.6 Effect of MgAl LDO and MgAlFe LDO dosage on adsorption performance

图7 F-初始质量浓度对MgAl LDO和MgAlFe LDO吸附性能的影响

Fig.7 Effect of initial mass concentration on the adsorption properties of MgAl LDO and MgAlFe LDO

图8 溶液的初始pH对MgAl LDO和MgAlFe LDO吸附性能的影响

Fig.8 Effect of initial pH of solution on the adsorption properties of MgAl LDO and MgAlFe LDO

图9 循环再生次数对MgAl LDO、MgAlFe LDO吸附性能的影响

Fig.9 Effect of cycle regeneration times on the adsorption properties of MgAl LDO and MgAlFe LDO

图10 MgAlFe LDO的拟一级动力方程和拟二级动力方程的拟合结果

Fig.10 The fitting results of the pseudo first and pseudo second order dynamic equations for MgAlFe LDO

表3 MgAlFe LDO的拟一级动力学和拟二级动力学模型参数

Table 3 Parameters of pseudo first and pseudo second order kinetic models for MgAlFe LDO

模型	k₁/min^-1	R $12$	k₂/( g·mg^-1·min^-1)	R $22$
拟一级动力学模型	0.010 0	0.966 8
拟二级动力学模型			0.108 0	0.999 0

表3 MgAlFe LDO的拟一级动力学和拟二级动力学模型参数

Table 3 Parameters of pseudo first and pseudo second order kinetic models for MgAlFe LDO

模型	k₁/min^-1	R $12$	k₂/( g·mg^-1·min^-1)	R $22$
拟一级动力学模型	0.010 0	0.966 8
拟二级动力学模型			0.108 0	0.999 0

图11 MgAlFe LDO的Langmuir和Freundlich吸附等温线

Fig.11 Langmuir and Freundlich adsorption isotherms of MgAlFe LDO

表4 MgAlFe LDO吸附等温方程的拟合参数

Table 4 Fitting parameters of MgAlFe LDO adsorption isotherm equation

方程	k_L/(L·mg^－1)	q_m/（mg·L^－1）	R $12$	k_F/(mg·g^－1)	n/(L·g^－1)	R $22$
Langmuir	0.214 5	21.93	0.997 4
Freundlich				4.936 9	2.010 0	0.957 2

表4 MgAlFe LDO吸附等温方程的拟合参数

Table 4 Fitting parameters of MgAlFe LDO adsorption isotherm equation

方程	k_L/(L·mg^－1)	q_m/（mg·L^－1）	R $12$	k_F/(mg·g^－1)	n/(L·g^－1)	R $22$
Langmuir	0.214 5	21.93	0.997 4
Freundlich				4.936 9	2.010 0	0.957 2

图12 MgAlFe LDO的范特霍夫热力学曲线

Fig.12 Van der Hoff thermodynamic curves of MgAlFe LDO

表5 MgAlFe LDO的范特霍夫热力学参数

Table 5 Van der Hoff thermodynamic parameters of MgAlFe LDO

参数	数值
∆G/(kJ·mo1^－l)	－3.15
∆S/(kJ·mo1^－l)	38.74
∆H/(kJ·mo1^－l)	8.39

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Fe³⁺改性类水滑石对废水中氟化物的吸附性能

Adsorption Performance of Fe³⁺Modified Hydrotalcite for Fluoride in Wastewater

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