黑藻生物吸附剂吸附水体中重金属离子的研究
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摘要
随着全球生态环境的恶化,各国日益重视对水体中各种污染物的治理。生物吸附技术是环境领域近年来迅速发展起来的处理工业污染废水的新技术,它以各种生物(菌类或藻类)吸附废水中的重金属离子,与传统的离子交换法和沉淀法相比,生物吸附法具有投资少,效率高,消耗少,并能有效的处理低浓度重金属离子废水等优点,是治理重金属污染水质的新途径。
藻类细胞壁中的多聚糖可提供吸附重金属的位点,廉价而资源丰富的藻类对多种重金属表现出很强的吸附能力。本文选用廉价易得的黑藻作为生物吸附剂,通过分批实验,研究了黑藻对水体中重金属离子Pb2+、Cd2+、Zn2+、Cu2+和Ni2+的吸附影响因子、吸附热力学、吸附动力学及吸附机理,吸附平衡用Langmiur、 Freundlich和D-R等温吸附模型进行拟合。
通过吸附影响因子实验发现,黑藻吸附Pb2+的最佳pH值为4.0,黑藻吸附Cd2+、Zn2+、Cu2+和Ni2+的最佳pH值为5.0。黑藻用量的最佳值为0.1g·(50mL)-1(2g/L),此时黑藻对Pb2+、Cd2+、Zn2+、Cu2+和Ni2+具有较高的吸附效率和吸附量。黑藻对Pb2+、Cd2+、Zn2+、Cu2+和Ni2+的吸附都为快速吸附过程,其中黑藻对Zn2+的吸附20min即基本达到平衡；黑藻对Pb2+、 Cu2+、Ni2+的吸附,在前30min随着时间的增加,吸附量很快增加,30min后吸附量基本稳定；黑藻对Cd2+的吸附,前60min内的吸附量为吸附总量的95%；实验中黑藻对Pb2+、Zn2+、Cu2+和Ni2+的吸附时间为60min,对Cd2+的吸附时间为120min。黑藻对Pb2+、Cd2+Zn2+、Cu2+和Ni2+的吸附都随着温度的升高而稍有降低。
实验结果表明,黑藻对Pb2+、Cd2+、Zn2+、Cu2+和Ni2+的吸附都符合Langmiur、 Freundlich和D-R等温吸附模型,其吸附能力依次为：Pb2+>Cd2+>Zn2+>Cu2+>Ni2+。黑藻吸附Pb2+、Cd2+、Zn2+、Cu2+和Ni2+的吸附自由能大小依次为Pb2+>Cd2+>Zn2+、Cu2+、Ni2,且都大于8kJ/mol,表明吸附过程为化学吸附。根据吸附热力学参数可知,黑藻吸附重金属离子过程自发进行程度依次为：Pb2+>Cd2+>Zn2+>Cu2+>Ni2+,且吸附过程都为放热过程。
黑藻对Pb2+、Cd2+、Zn2+、Cu2+和Ni2+的吸附动力学过程符合Pseudo二级动力学方程,由动力学常数k：可知,黑藻吸附重金属离子的吸附速率依次为：Zn2+、Ni2+>Pb2+、Cu2+>Cd2+
通过ICP-AES比较黑藻吸附Pb2+、Cd2+、Zn2+、Cu2+和Ni2+前后的黑藻中主要元素浓度的变化,发现吸附后Pb、Cd、Zn、Cu、Ni增加,而K、Na、Mg减少,由此可知,在吸附过程中,发生了阳离子交换。通过SEM-EDX对黑藻吸附Pb2+、Cd2+、Zn2+、Cu2+和Ni2+前后进行能谱分析可知,在黑藻吸附Pb2+、Cd2+、Zn2+、Cu2+和Ni2+的生物吸附过程中,发生了阳离子交换吸附。比较黑藻吸附Pb2+、Cd2+、Zn2+、Cu2+和Ni2+前后的傅立叶红外变换光谱图,发现峰形基本不变,但羟基中C-O伸缩振动峰和硫酸基特征峰的波数向低波数明显移动,表明硫酸基和C-O参与了吸附过程。解吸实验表明,用EDTA可以对重金属离子进行回收。
实验表明黑藻是一种高效、经济适用的生物吸附材料,可用来吸附水体中的Pb2+、Cd2+、Zn2+、Cu2+和Ni2+。
As more and more attention is paid to environment, it is important to remove pollutants in aqueous solution. Biosorption is a process that utilizes inexpensive active/dead biomass to sequester heavy metals and is particularly useful for the removal of contaminants from industrial effluents. Compared with conventional methods such as ion exchange and precipitation with lime, the biosorption process offers the advantages of low operating cost, minimization of the volume of chemical and biological sludge to be disposed of, high efficiency in detoxifying very dilute effluents. These advantages have served as the primary incentives for developing full-scale biosorption processes to clean up heavy-metal pollution.
Polysaccharides of algal cell wall can provide sites to adsorb heavy metal. Cheap and rich source algaes showed strong adsorptivity to heavy metals. In this study, biosorption of Pb2+, Cd2+, Zn2+, Cu2+and Ni2+by Hydrilla verticillata were investigated as a function of environment effects, biosorption thermodynamics, biosorption kinetics and biosorption mechanism. Adsorption equilibriums were described by Langmuir, Freundlich and Dubinin-Radushkevich (D-R) isotherm model.
The environment effects results were as follows:Maximum biosorption capacities were obtained at pH4.0for Pb2+, Maximum biosorption capacities were obtained at pH5.0for Cd2+、Zn2+、Cu2+and Ni2+. The higher biosorption efficiency and biosorption capacities were obtained at biosorbent dosage2g/L for Pb2+, Cd2+Zn2+, Cu2+and Ni2+. The biosorption of Pb2+, Cd2+, Zn2+, Cu2+and Ni2+by Hydrilla verticillata were rapid biosorption processes. The biosorption of Zn2+by Hydrilla verticillata attained equilibrium after20min. The Pb2+、Cu2+and Ni2+biosorption capacities onto Hydrilla verticillata increased by increasing contact time up to30min, the biosorption capacities obtained steady value after30min. The biosorption capacity was maximum capacity's95%within60min. The biosorption capacities of Pb2+、Cd2+、Zn2+、Cu2+and Ni2+by Hydrilla verticillata decreased with the rise in temperature. The results indicated that these biosorption processes wer exothermic in nature.
The Sorption isotherms of Pb2+, Cd2+, Zn2+, Cu2+and Ni2+followed well Langmiur, Freundlich and D-R equation. The biosorption efficiency in the order of Pb2+> Cd2+> Zn2+> Cu2+> Ni2+. The mean free energy of adsorption E(kJ/mol) in the order of Pb2+> Cd2+> Zn2+, Cu2+, Ni2+. The mean free energy of adsorption E>8kJ/mol for all biosorption processes, it indicated that the biosorption of Pb2+, Cd2+, Zn2+, Cu2+and Ni2+by Hydrilla verticillata may be carried out via chemical ion-exchange mechanism. The negative ΔG0values showed that the biosorption of Pb2+, Cd2+, Zn2+, Cu2+and Ni2+by Hydrilla verticillata were feasible and spontaneous. The negative ΔH0values depicted exothermic nature of the adsorption. The negative ΔS0values revealed that the orderliness of the adsorbed system were higher than that in the solution phase before adsorption. The biosorption kinetics followed the pseudo-second order model.
In order to investigate the mechanisms of heavy metal biosorption by Hydrilla verticillata, the amounts of metal ions of biosorbent before and after biosorption were measured by using Inductively Coupled plasma (ICP) Atomic Emission Spectrometer. The results showed the amounts of biosorbed Pb2+, Cd2+, Zn2+, Cu2+and Ni2+on Hydrilla verticillata increased as well as light metal ions (K+、Mg2+and Na+) decreased on Hydrilla verticillata during biosorption experiment. It indicated that ions exchange mechanism would be involved. Fresh and the Pb2+, Cd2+, Zn2+, Cu2+and Ni2+loaded Hydrilla verticillata were analyzed by SEM equipped with EDX. The results showed that a remarkable amount of Pb2+, Cd2+, Zn2+, Cu2+and Ni2+were adsorbed by Hydrilla verticillata. To compare the change of Hydrilla verticillata's Fourier transform infrared spectrum before and after biosorption, the peaks of C-O group and Sulfate group were shifted towards low wave numbers. It showed that the sulfate group and C-O group involved in the biosorption process. Desorption experiments showed that heavy metal ions can be recovered by EDTA.
The study indicated that Hydrilla verticillata may be used as an inexpensive, effective and easily obtained biosorbent for the removal of Pb2+, Cd2+, Zn2+, Cu2+and Ni2+.
藻类细胞壁中的多聚糖可提供吸附重金属的位点,廉价而资源丰富的藻类对多种重金属表现出很强的吸附能力。本文选用廉价易得的黑藻作为生物吸附剂,通过分批实验,研究了黑藻对水体中重金属离子Pb2+、Cd2+、Zn2+、Cu2+和Ni2+的吸附影响因子、吸附热力学、吸附动力学及吸附机理,吸附平衡用Langmiur、 Freundlich和D-R等温吸附模型进行拟合。
通过吸附影响因子实验发现,黑藻吸附Pb2+的最佳pH值为4.0,黑藻吸附Cd2+、Zn2+、Cu2+和Ni2+的最佳pH值为5.0。黑藻用量的最佳值为0.1g·(50mL)-1(2g/L),此时黑藻对Pb2+、Cd2+、Zn2+、Cu2+和Ni2+具有较高的吸附效率和吸附量。黑藻对Pb2+、Cd2+、Zn2+、Cu2+和Ni2+的吸附都为快速吸附过程,其中黑藻对Zn2+的吸附20min即基本达到平衡；黑藻对Pb2+、 Cu2+、Ni2+的吸附,在前30min随着时间的增加,吸附量很快增加,30min后吸附量基本稳定；黑藻对Cd2+的吸附,前60min内的吸附量为吸附总量的95%；实验中黑藻对Pb2+、Zn2+、Cu2+和Ni2+的吸附时间为60min,对Cd2+的吸附时间为120min。黑藻对Pb2+、Cd2+Zn2+、Cu2+和Ni2+的吸附都随着温度的升高而稍有降低。
实验结果表明,黑藻对Pb2+、Cd2+、Zn2+、Cu2+和Ni2+的吸附都符合Langmiur、 Freundlich和D-R等温吸附模型,其吸附能力依次为：Pb2+>Cd2+>Zn2+>Cu2+>Ni2+。黑藻吸附Pb2+、Cd2+、Zn2+、Cu2+和Ni2+的吸附自由能大小依次为Pb2+>Cd2+>Zn2+、Cu2+、Ni2,且都大于8kJ/mol,表明吸附过程为化学吸附。根据吸附热力学参数可知,黑藻吸附重金属离子过程自发进行程度依次为：Pb2+>Cd2+>Zn2+>Cu2+>Ni2+,且吸附过程都为放热过程。
黑藻对Pb2+、Cd2+、Zn2+、Cu2+和Ni2+的吸附动力学过程符合Pseudo二级动力学方程,由动力学常数k：可知,黑藻吸附重金属离子的吸附速率依次为：Zn2+、Ni2+>Pb2+、Cu2+>Cd2+
通过ICP-AES比较黑藻吸附Pb2+、Cd2+、Zn2+、Cu2+和Ni2+前后的黑藻中主要元素浓度的变化,发现吸附后Pb、Cd、Zn、Cu、Ni增加,而K、Na、Mg减少,由此可知,在吸附过程中,发生了阳离子交换。通过SEM-EDX对黑藻吸附Pb2+、Cd2+、Zn2+、Cu2+和Ni2+前后进行能谱分析可知,在黑藻吸附Pb2+、Cd2+、Zn2+、Cu2+和Ni2+的生物吸附过程中,发生了阳离子交换吸附。比较黑藻吸附Pb2+、Cd2+、Zn2+、Cu2+和Ni2+前后的傅立叶红外变换光谱图,发现峰形基本不变,但羟基中C-O伸缩振动峰和硫酸基特征峰的波数向低波数明显移动,表明硫酸基和C-O参与了吸附过程。解吸实验表明,用EDTA可以对重金属离子进行回收。
实验表明黑藻是一种高效、经济适用的生物吸附材料,可用来吸附水体中的Pb2+、Cd2+、Zn2+、Cu2+和Ni2+。
As more and more attention is paid to environment, it is important to remove pollutants in aqueous solution. Biosorption is a process that utilizes inexpensive active/dead biomass to sequester heavy metals and is particularly useful for the removal of contaminants from industrial effluents. Compared with conventional methods such as ion exchange and precipitation with lime, the biosorption process offers the advantages of low operating cost, minimization of the volume of chemical and biological sludge to be disposed of, high efficiency in detoxifying very dilute effluents. These advantages have served as the primary incentives for developing full-scale biosorption processes to clean up heavy-metal pollution.
Polysaccharides of algal cell wall can provide sites to adsorb heavy metal. Cheap and rich source algaes showed strong adsorptivity to heavy metals. In this study, biosorption of Pb2+, Cd2+, Zn2+, Cu2+and Ni2+by Hydrilla verticillata were investigated as a function of environment effects, biosorption thermodynamics, biosorption kinetics and biosorption mechanism. Adsorption equilibriums were described by Langmuir, Freundlich and Dubinin-Radushkevich (D-R) isotherm model.
The environment effects results were as follows:Maximum biosorption capacities were obtained at pH4.0for Pb2+, Maximum biosorption capacities were obtained at pH5.0for Cd2+、Zn2+、Cu2+and Ni2+. The higher biosorption efficiency and biosorption capacities were obtained at biosorbent dosage2g/L for Pb2+, Cd2+Zn2+, Cu2+and Ni2+. The biosorption of Pb2+, Cd2+, Zn2+, Cu2+and Ni2+by Hydrilla verticillata were rapid biosorption processes. The biosorption of Zn2+by Hydrilla verticillata attained equilibrium after20min. The Pb2+、Cu2+and Ni2+biosorption capacities onto Hydrilla verticillata increased by increasing contact time up to30min, the biosorption capacities obtained steady value after30min. The biosorption capacity was maximum capacity's95%within60min. The biosorption capacities of Pb2+、Cd2+、Zn2+、Cu2+and Ni2+by Hydrilla verticillata decreased with the rise in temperature. The results indicated that these biosorption processes wer exothermic in nature.
The Sorption isotherms of Pb2+, Cd2+, Zn2+, Cu2+and Ni2+followed well Langmiur, Freundlich and D-R equation. The biosorption efficiency in the order of Pb2+> Cd2+> Zn2+> Cu2+> Ni2+. The mean free energy of adsorption E(kJ/mol) in the order of Pb2+> Cd2+> Zn2+, Cu2+, Ni2+. The mean free energy of adsorption E>8kJ/mol for all biosorption processes, it indicated that the biosorption of Pb2+, Cd2+, Zn2+, Cu2+and Ni2+by Hydrilla verticillata may be carried out via chemical ion-exchange mechanism. The negative ΔG0values showed that the biosorption of Pb2+, Cd2+, Zn2+, Cu2+and Ni2+by Hydrilla verticillata were feasible and spontaneous. The negative ΔH0values depicted exothermic nature of the adsorption. The negative ΔS0values revealed that the orderliness of the adsorbed system were higher than that in the solution phase before adsorption. The biosorption kinetics followed the pseudo-second order model.
In order to investigate the mechanisms of heavy metal biosorption by Hydrilla verticillata, the amounts of metal ions of biosorbent before and after biosorption were measured by using Inductively Coupled plasma (ICP) Atomic Emission Spectrometer. The results showed the amounts of biosorbed Pb2+, Cd2+, Zn2+, Cu2+and Ni2+on Hydrilla verticillata increased as well as light metal ions (K+、Mg2+and Na+) decreased on Hydrilla verticillata during biosorption experiment. It indicated that ions exchange mechanism would be involved. Fresh and the Pb2+, Cd2+, Zn2+, Cu2+and Ni2+loaded Hydrilla verticillata were analyzed by SEM equipped with EDX. The results showed that a remarkable amount of Pb2+, Cd2+, Zn2+, Cu2+and Ni2+were adsorbed by Hydrilla verticillata. To compare the change of Hydrilla verticillata's Fourier transform infrared spectrum before and after biosorption, the peaks of C-O group and Sulfate group were shifted towards low wave numbers. It showed that the sulfate group and C-O group involved in the biosorption process. Desorption experiments showed that heavy metal ions can be recovered by EDTA.
The study indicated that Hydrilla verticillata may be used as an inexpensive, effective and easily obtained biosorbent for the removal of Pb2+, Cd2+, Zn2+, Cu2+and Ni2+.
引文
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