改性棕榈丝吸附水中重金属的研究
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摘要
本文以廉价的天然生物质材料棕榈丝(PT)为原料,制备了NaOH改性棕榈丝(NaOH-PT)、十二烷基苯磺酸钠改性棕榈丝(SDBS-PT)和低温焚烧棕榈丝(Ash-PT)三种棕榈丝衍生物吸附剂,并将其应用于对水中阳离子Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)和阴离子Cr(Ⅵ)的吸附上,对吸附过程的影响因素及吸附机理进行了详细的探讨。
本文通过考察在相同吸附条件下,不同改性条件所得的吸附剂对水中重金属的去除率得到：NaOH改性的最佳条件——NaOH浓度3%(w/w),改性温度25℃,改性时间5h; SDBS改性的最佳条件——SDBS浓度5g·L-1,改性温度35℃,改性时间5h。
通过扫描电镜、比表面积测定、傅里叶红外光谱分析、X-ray衍射分析以及Bohem滴定等手段,对实验所用的吸附剂进行表面特性和活性基团的鉴定。分析结果表明：NaOH和SDBS改性使得棕榈丝原来闭合的孔道膨胀；低温焚烧处理的仍保留棕榈丝的基本骨架,呈蜂窝状。相对PT而言,NaOH-PT、SDBS-PT和Ash-PT的比表面积分别提高了232%、116%和408%。NaOH改性能够有效的提高吸附剂中纤维素的相对含量；SDBS被有效的接枝到棕榈丝的表面；低温焚烧使得活性SiO2更充分的暴露在外。同时三种吸附剂的的总酸性基团均有所下降,总碱性基团有所上升。
在PT和NaOH-PT对Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)、Cr(Ⅵ)的吸附研究方面,分别考察了时间、温度、初始浓度、溶液pH值、阳离子电解质、有机配位体以及其它重金属离子的竞争对吸附效果的影响。实验结果表明：在25℃下,PT和NaOH-PT对Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)、Cr(Ⅵ)的吸附基本在300min之内完成；随着温度和初始浓度的升高,PT和NaOH-PT对Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)、Cr(Ⅵ)的吸附量均逐渐增加；溶液pH值对吸附过程影响较大。该吸附过程能够很高的符合准二级动力学模型,吸附等温线其中Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)同时符合Langmuir吸附等温模型和Freundlich吸附等温模型,Cr(Ⅵ)只满足Freundlich吸附等温模型。NaOH改性后对Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)吸附量增大,分别提升了190%,96%,104%；对Cr(Ⅵ)略有降低,降低了1%。NaOH-PT吸附过程AG<0,△H在36-188kJ-mol-1范围内,△S值在90-217J·(mol·K)-1范围内,这些参数说明吸附过程为自发进行的吸热反应。
在SDBS-PT吸附Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)、Cr(Ⅵ)的方面,实验结果表明：在25℃下,SDBS-PT对四种重金属污染物的吸附基本在300min达到吸附平衡；且相对于PT的吸附量分别提高55%,45%,78%和17%。在实验考察的pH(0-7)范围内,SDBS-PT对Ni(Ⅱ)、Cd(Ⅱ)的吸附量逐渐增大,对Cr(Ⅲ)的吸附量先增加后下降,对Cr(Ⅵ)的却逐渐减小。准二级动力学模型能够很好的拟合25℃下SDBS-PT对Ni(Ⅱ)、Cd(Ⅱ)、 Cr(Ⅲ)、Cr(Ⅵ)的吸附过程,相关系数R2均大于0.99。Langmuir吸附等温模型能够更好的描述吸附过程。。
对Ash-PT吸附Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)的诸多影响因素和吸附特性进行了研究。实验结果：相对于PT, Ash-PT对Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)的吸附量分别提高了2800%,1500%,1900%。溶液中阳离子电解质(Na+、Ca2+和Fe3+)的存在影响了Ash-PT对Ni(Ⅱ)、 Cd(Ⅱ)、Cr(Ⅲ)的吸附,且影响程度Fe3+>Ca2+>Na+;有机配位体的加入会降低吸附量,并且不同种类的重金属离子间存在着竞争吸附。该吸附过程的动力学在一定程度上都符合Elovich动力学模型,准一级动力学模型,准二级动力学模型。Langmuir吸附等温模型能够极好的描述Ash-PT对Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)的吸附过程,其R2值均>0.99。热力学研究表明,Ash-PT吸附过程为自发进行的吸热反应,升高温度有利于吸附过程的进行。
Three novel biosorbents, palm thread modified with NaOH(NaOH-PT), palm thread modified with SDBS(SDBS-PT), palm thread ash burned at low temperature, were prepared from the cheap natural biomass materials palm thread(PT). And were successfully applied to the adsorption of cationic Ni (Ⅱ), Cd (Ⅱ), Cr (Ⅲ) and anionic Cr (Ⅵ) from water. The influential factors and adsorption mechanism of adsorption process were detailedly discussed.
The removal of heavy metals, sorbed by different adsorbents prepared under different conditions, was investigated.The results showed that the optimal modified conditions for NaOH were the concentration of NaOH3%(w/w), modified temperature25℃C, the modified time5h; and the optimal modified conditions for SDBS were the concentration of SDBS5g-L-', the modified temperature35℃, the modification time5h.
The quality of biomaterial is the key factor that affects the sorption potential. The surface characteristics and active groups of adsorbents were identified by using scanning electron microscopy, specific surface area measurements, Fourier transform infrared spectroscopy, X-ray diffraction analysis, Bohem titration and so on. The analysis showed that: the palm thread modified with NaOH and SDBS became more rough and their microtoubule structure expanded; Ash-PT retained the basic framework of the palm thread.Compared to PT, specific surface areas of NaOH-PT, SDBS-PT and Ash-PT were increased by232%,116%and408%. NaOH modification could effectively improve the relative content of cellulose in adsorbent.Relative PT of NaOH-PT, SDBS-PT and Ash-PT specific surface area were increased by232%,116%and408%. NaOH modification can effectively improve the relative content of cellulose adsorbent; SDBS was effectively grafted onto the surface of the palm thread; the active SiO2of Ash-PT was fully exposed. The total acidic groups of the three adsorbents were reduced, while the total basic groups increased.
PT and NaOH-PT were successfully appied to sorb Ni (Ⅱ), Cd (Ⅱ), Cr (Ⅲ) and Cr (Ⅵ). Many parameters that affected the sorption were investigated, such as contact time, temperature, initial concentration, solution pH, cation electrolytes, organic ligands and other heavy metal ions.The results showed:at25℃,300min was enough for PT and NaOH-PT to sorb Ni (Ⅱ), Cd (Ⅱ), Cr (Ⅲ) and Cr (Ⅵ) from solution; with the rise of temperature and initial concentration, the adsorption capacities of Ni (Ⅱ), Cd (Ⅱ), Cr (Ⅲ) and Cr (Ⅵ) onto the PT and NaOH-PT gradually increased. The solution pH had a severe influence on the adsorption process. The adsorption kinetics were well fitted the Lagergren pseudo-second order kinetic model; the data of Ni (Ⅱ), Cd (Ⅱ), Cr (Ⅲ) were well fitted both Langmuir isotherm model and Freundlich isotherm model, but the data of Cr (VI) just was well fitted Freundlich isotherm model. Compared to the PT, the adsorption capacities of Ni (Ⅱ), Cd (Ⅱ) and Cr (Ⅲ) onto NaOH-PT increased by190%,96%and104%; but for Cr (Ⅵ) was slightly reduced by1%. About adsorption process,△G<0,△H>0, AS>0,△H values was in the36-188kJ-mol-1range, AS values was in the90-217-(mol·K)-1range, the adsorption process is spontaneous and endothermic reaction.
The SDBS-PT were used to sorb Ni (Ⅱ), Cd (Ⅱ), Cr (Ⅲ) and Cr (Ⅵ) from water. The effect of contact time, temperature, initial concentration and solution pH were investigated The results showed:at25℃, the adsorption could reach equilibrium about300min; compared to PT, the adsorption capacities of Ni (Ⅱ), Cd (Ⅱ), Cr (Ⅲ) and Cr (Ⅵ) increased by55%,45%,78%and17%。 The solution pH had different influences on the adsorption process of Ni (Ⅱ), Cd (Ⅱ), Cr (Ⅲ) and Cr (Ⅵ). The adsorption kinetics were well fitted the Lagergren pseudo-second order kinetic model and Langmuir isotherm model, the adsorption process belongs to chemical adsorption.
The Ash-PT were applied to adsorb cation, such as Ni (Ⅱ), Cd (Ⅱ) and Cr (Ⅲ), and many parameters and adsorption characteristics were studied. Compared to PT, the capacities of Ni (Ⅱ), Cd (Ⅱ) and Cr (Ⅲ) onto Ash-PT increased by2800%,1500%and1900%. The cationic electrolytes (Na+, Ca2+and Fe3+)of the solution would effect the adsorptions of Ni (Ⅱ), Cd (Ⅱ) and Cr (Ⅲ), and the affected order was Fe3+>Ca2+>Na+; the organic ligand of solution would reduce the adsorption capacity, and the competitive adsorption was existed between the different heavy metal ions. The kinetics of the adsorption process were well fitted the Elovich kinetic model, pseudo-first-order kinetic model and pseudo-second order kinetic model. Langmuir isotherm model could simulate the experimental results very well(R2>0.99). The thermodynamic study showed that, Ash-PT adsorption processes were spontaneous endothermic reaction, and elevated temperatures were conducive to the adsorption process.
本文通过考察在相同吸附条件下,不同改性条件所得的吸附剂对水中重金属的去除率得到：NaOH改性的最佳条件——NaOH浓度3%(w/w),改性温度25℃,改性时间5h; SDBS改性的最佳条件——SDBS浓度5g·L-1,改性温度35℃,改性时间5h。
通过扫描电镜、比表面积测定、傅里叶红外光谱分析、X-ray衍射分析以及Bohem滴定等手段,对实验所用的吸附剂进行表面特性和活性基团的鉴定。分析结果表明：NaOH和SDBS改性使得棕榈丝原来闭合的孔道膨胀；低温焚烧处理的仍保留棕榈丝的基本骨架,呈蜂窝状。相对PT而言,NaOH-PT、SDBS-PT和Ash-PT的比表面积分别提高了232%、116%和408%。NaOH改性能够有效的提高吸附剂中纤维素的相对含量；SDBS被有效的接枝到棕榈丝的表面；低温焚烧使得活性SiO2更充分的暴露在外。同时三种吸附剂的的总酸性基团均有所下降,总碱性基团有所上升。
在PT和NaOH-PT对Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)、Cr(Ⅵ)的吸附研究方面,分别考察了时间、温度、初始浓度、溶液pH值、阳离子电解质、有机配位体以及其它重金属离子的竞争对吸附效果的影响。实验结果表明：在25℃下,PT和NaOH-PT对Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)、Cr(Ⅵ)的吸附基本在300min之内完成；随着温度和初始浓度的升高,PT和NaOH-PT对Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)、Cr(Ⅵ)的吸附量均逐渐增加；溶液pH值对吸附过程影响较大。该吸附过程能够很高的符合准二级动力学模型,吸附等温线其中Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)同时符合Langmuir吸附等温模型和Freundlich吸附等温模型,Cr(Ⅵ)只满足Freundlich吸附等温模型。NaOH改性后对Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)吸附量增大,分别提升了190%,96%,104%；对Cr(Ⅵ)略有降低,降低了1%。NaOH-PT吸附过程AG<0,△H在36-188kJ-mol-1范围内,△S值在90-217J·(mol·K)-1范围内,这些参数说明吸附过程为自发进行的吸热反应。
在SDBS-PT吸附Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)、Cr(Ⅵ)的方面,实验结果表明：在25℃下,SDBS-PT对四种重金属污染物的吸附基本在300min达到吸附平衡；且相对于PT的吸附量分别提高55%,45%,78%和17%。在实验考察的pH(0-7)范围内,SDBS-PT对Ni(Ⅱ)、Cd(Ⅱ)的吸附量逐渐增大,对Cr(Ⅲ)的吸附量先增加后下降,对Cr(Ⅵ)的却逐渐减小。准二级动力学模型能够很好的拟合25℃下SDBS-PT对Ni(Ⅱ)、Cd(Ⅱ)、 Cr(Ⅲ)、Cr(Ⅵ)的吸附过程,相关系数R2均大于0.99。Langmuir吸附等温模型能够更好的描述吸附过程。。
对Ash-PT吸附Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)的诸多影响因素和吸附特性进行了研究。实验结果：相对于PT, Ash-PT对Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)的吸附量分别提高了2800%,1500%,1900%。溶液中阳离子电解质(Na+、Ca2+和Fe3+)的存在影响了Ash-PT对Ni(Ⅱ)、 Cd(Ⅱ)、Cr(Ⅲ)的吸附,且影响程度Fe3+>Ca2+>Na+;有机配位体的加入会降低吸附量,并且不同种类的重金属离子间存在着竞争吸附。该吸附过程的动力学在一定程度上都符合Elovich动力学模型,准一级动力学模型,准二级动力学模型。Langmuir吸附等温模型能够极好的描述Ash-PT对Ni(Ⅱ)、Cd(Ⅱ)、Cr(Ⅲ)的吸附过程,其R2值均>0.99。热力学研究表明,Ash-PT吸附过程为自发进行的吸热反应,升高温度有利于吸附过程的进行。
Three novel biosorbents, palm thread modified with NaOH(NaOH-PT), palm thread modified with SDBS(SDBS-PT), palm thread ash burned at low temperature, were prepared from the cheap natural biomass materials palm thread(PT). And were successfully applied to the adsorption of cationic Ni (Ⅱ), Cd (Ⅱ), Cr (Ⅲ) and anionic Cr (Ⅵ) from water. The influential factors and adsorption mechanism of adsorption process were detailedly discussed.
The removal of heavy metals, sorbed by different adsorbents prepared under different conditions, was investigated.The results showed that the optimal modified conditions for NaOH were the concentration of NaOH3%(w/w), modified temperature25℃C, the modified time5h; and the optimal modified conditions for SDBS were the concentration of SDBS5g-L-', the modified temperature35℃, the modification time5h.
The quality of biomaterial is the key factor that affects the sorption potential. The surface characteristics and active groups of adsorbents were identified by using scanning electron microscopy, specific surface area measurements, Fourier transform infrared spectroscopy, X-ray diffraction analysis, Bohem titration and so on. The analysis showed that: the palm thread modified with NaOH and SDBS became more rough and their microtoubule structure expanded; Ash-PT retained the basic framework of the palm thread.Compared to PT, specific surface areas of NaOH-PT, SDBS-PT and Ash-PT were increased by232%,116%and408%. NaOH modification could effectively improve the relative content of cellulose in adsorbent.Relative PT of NaOH-PT, SDBS-PT and Ash-PT specific surface area were increased by232%,116%and408%. NaOH modification can effectively improve the relative content of cellulose adsorbent; SDBS was effectively grafted onto the surface of the palm thread; the active SiO2of Ash-PT was fully exposed. The total acidic groups of the three adsorbents were reduced, while the total basic groups increased.
PT and NaOH-PT were successfully appied to sorb Ni (Ⅱ), Cd (Ⅱ), Cr (Ⅲ) and Cr (Ⅵ). Many parameters that affected the sorption were investigated, such as contact time, temperature, initial concentration, solution pH, cation electrolytes, organic ligands and other heavy metal ions.The results showed:at25℃,300min was enough for PT and NaOH-PT to sorb Ni (Ⅱ), Cd (Ⅱ), Cr (Ⅲ) and Cr (Ⅵ) from solution; with the rise of temperature and initial concentration, the adsorption capacities of Ni (Ⅱ), Cd (Ⅱ), Cr (Ⅲ) and Cr (Ⅵ) onto the PT and NaOH-PT gradually increased. The solution pH had a severe influence on the adsorption process. The adsorption kinetics were well fitted the Lagergren pseudo-second order kinetic model; the data of Ni (Ⅱ), Cd (Ⅱ), Cr (Ⅲ) were well fitted both Langmuir isotherm model and Freundlich isotherm model, but the data of Cr (VI) just was well fitted Freundlich isotherm model. Compared to the PT, the adsorption capacities of Ni (Ⅱ), Cd (Ⅱ) and Cr (Ⅲ) onto NaOH-PT increased by190%,96%and104%; but for Cr (Ⅵ) was slightly reduced by1%. About adsorption process,△G<0,△H>0, AS>0,△H values was in the36-188kJ-mol-1range, AS values was in the90-217-(mol·K)-1range, the adsorption process is spontaneous and endothermic reaction.
The SDBS-PT were used to sorb Ni (Ⅱ), Cd (Ⅱ), Cr (Ⅲ) and Cr (Ⅵ) from water. The effect of contact time, temperature, initial concentration and solution pH were investigated The results showed:at25℃, the adsorption could reach equilibrium about300min; compared to PT, the adsorption capacities of Ni (Ⅱ), Cd (Ⅱ), Cr (Ⅲ) and Cr (Ⅵ) increased by55%,45%,78%and17%。 The solution pH had different influences on the adsorption process of Ni (Ⅱ), Cd (Ⅱ), Cr (Ⅲ) and Cr (Ⅵ). The adsorption kinetics were well fitted the Lagergren pseudo-second order kinetic model and Langmuir isotherm model, the adsorption process belongs to chemical adsorption.
The Ash-PT were applied to adsorb cation, such as Ni (Ⅱ), Cd (Ⅱ) and Cr (Ⅲ), and many parameters and adsorption characteristics were studied. Compared to PT, the capacities of Ni (Ⅱ), Cd (Ⅱ) and Cr (Ⅲ) onto Ash-PT increased by2800%,1500%and1900%. The cationic electrolytes (Na+, Ca2+and Fe3+)of the solution would effect the adsorptions of Ni (Ⅱ), Cd (Ⅱ) and Cr (Ⅲ), and the affected order was Fe3+>Ca2+>Na+; the organic ligand of solution would reduce the adsorption capacity, and the competitive adsorption was existed between the different heavy metal ions. The kinetics of the adsorption process were well fitted the Elovich kinetic model, pseudo-first-order kinetic model and pseudo-second order kinetic model. Langmuir isotherm model could simulate the experimental results very well(R2>0.99). The thermodynamic study showed that, Ash-PT adsorption processes were spontaneous endothermic reaction, and elevated temperatures were conducive to the adsorption process.
引文
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