Preparation of NaA zeolite with fly ash and its adsorption properties for lead ions
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摘要: 以粉煤灰为原料，采用碱熔-水热法合成NaA型分子筛。通过单因素试验探究了水热温度、水热时间、碱浓度、碱灰比对制备分子筛的影响，采用静态饱和吸水量和钙离子交换量对所制备分子筛的性能进行评价。结果表明：水热温度100 ℃、水热时间5 h、NaOH浓度2.73 mol/L、碱灰比2.8有利于NaA型分子筛的合成，其钙离子交换量最高可达374.63 mg/g。利用合成的NaA型分子筛对液相中的铅离子进行吸附研究，在分子筛投加量1 g/L、溶液pH值6.2、吸附温度25 ℃、吸附60 min时，吸附容量(Qe)最高可达471.51 mg/g；分子筛的吸附等温线更加符合Langmuir等温线模型，饱和吸附容量(Qm)可达580.18 mg/g。Abstract: This study synthesized NaA zeolite by alkali melting-hydrothermal method based on fly ash as raw material. The effects of hydrothermal temperature, hydrothermal time, alkali concentration and alkali/FA mass ratio on the preparation of zeolites were investigated by single factor experiments, and the performance of the prepared zeolites was evaluated by water adsorption capacity and Cation Exchange Capacity (CEC) value.Results show that it is beneficial to the synthesis of NaA zeolite under hydrothermal temperature of 100 ℃, hydrothermal time of 5 h, NaOH concentration of 2.73 mol/L, and alkali/FA mass ratio of 2.8, in which the highest CEC value can reach 374.63 mg/g. The adsorption of Pb(Ⅱ) in liquid phase was studied by using the synthetic NaA zeolite. The adsorption capacity was up to 471.51 mg/g with 1 g/L dosage of zeolite, at pH 6.2 and 25 ℃ of adsorption temperature and the adsorption time was 60 min.The adsorption data of Pb(Ⅱ) by NaA zeolite was fitted better with Langmuir model, and the saturated adsorption capacity of Pb(Ⅱ) could reach to 580.18 mg/g.
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Key words:
- fly ash /
- NaA zeolite /
- alkali melting-hydrothermal /
- lead ion /
- adsorption
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图 1 样品的静态饱和吸水量与钙离子交换量随水热温度的变化
Figure 1. Water adsorption capacity and CEC value of samples at different hydrothermal temperatures
图 2 样品的静态饱和吸水量与钙离子交换量随水热时间的变化
Figure 2. Water adsorption capacity and CEC value of samples at different hydrothermal time
图 3 样品的静态饱和吸水量与钙离子交换量随NaOH浓度的变化
Figure 3. Water adsorption capacity and CEC value of samples at different NaOH concentrations
图 4 样品的静态饱和吸水量与钙离子交换量随碱灰比的变化
Figure 4. Water adsorption capacity and CEC value of samples at different NaOH/FA mass ratios
图 5 粉煤灰及不同碱灰比样品的XRD图谱
Figure 5. XRD patterns of FA and samples at different NaOH/FA mass ratios
图 7 碱灰比分别为1.2和2.8时制备样品的SEM图
Figure 7. SEM images of zeolites obtained at NaOH/FA mass ratio of 1.2 and 2.8
图 8 碱灰比为2.8时制备样品的能谱图
Figure 8. EDS images of zeolites obtained at NaOH/FA mass ratio of 2.8
图 9 粉煤灰及不同碱灰比下制备样品的红外图谱
Figure 9. FTIR spectra of FA and samples at different NaOH/FA mass ratios
图 10 样品的铅离子吸附容量随碱灰比的变化
Figure 10. Pb(Ⅱ) adsorption capacity of samples at different NaOH/FA mass ratios
图 14 初始浓度对Pb(Ⅱ)吸附性能的影响
Figure 14. Effect of initial concentration on adsorption of Pb(Ⅱ)
图 15 最优样品Pb(Ⅱ)吸附动力学拟合
Figure 15. Adsorption kinetics fitting of Pb(Ⅱ) on optimum sample
表 1 粉煤灰化学成分
Table 1. Chemical compositions of FA
% 化学组成 SiO2 Al2O3 Fe2O3 CaO SO3 TiO2 MgO K2O Na2O Cl P2O5 质量分数 51.18 36.76 3.21 2.74 1.78 1.35 1.16 0.98 0.25 0.15 0.20 
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表 2 动力学拟合参数
Table 2. Kinetic fitting parameters for Pb(Ⅱ) adsorption
模型 Qe/(mg·g-1) k R2 准一级动力学模型 453.09 0.295 6 0.989 8 准二级动力学模型 477.18 0.001 3 0.999 3
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表 3 吸附等温线拟合参数
Table 3. Langmuir and Freundlich parameters for Pb(Ⅱ) adsorption
Langmuir参数 Freundlich参数 b/(L·mg-1) Qm/(mg·g-1) R2 k n R2 0.143 1 580.18 0.991 0 375.16 13.43 0.909 7
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