氨基功能化KIT-6两步后嫁接制备及其吸附Pb~(2+)性能
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摘要
以正硅酸乙酯作为硅源,三嵌段共聚物P123作为模板剂制备介孔材料KIT-6。再采用后嫁接法,先将3-氯丙基三甲氧基硅烷嫁接到KIT-6上,再用聚乙烯亚胺(PEI)进一步嫁接,合成出PEI功能化的PEI/KIT-6。用傅立叶变换红外光谱分析(FTIR)、X射线衍射(XRD)、热重分析(TGA)、元素分析、N_2吸附-脱附、扫描电镜等手段进行结构的表征。用电感耦合等离子体光谱(ICP)测定材料的Pb~(2+)吸附性能。结果表明氨基的表面平均负载量为0.374 mmol·g~(-1),并且改性后KIT-6仍具有高度有序性,并未出现孔道堵塞的现象。PEI/KIT-6在投加量为1 g·L~(-1),室温条件下,吸附100 mg·L~(-1) Pb~(2+)的最佳p H值为6.0;吸附容量伴随温度的提高先增加后减小,最佳反应温度为35℃;材料在120 min内可以达到吸附平衡,吸附过程符合拟二级动力学方程;Langmuir和Freundlich模型均能较好地描述该吸附过程。吸附倾向于发生单分子层的化学吸附。
Mesoporous material KIT-6 was prepared using tetraethyl orthosilicate as the silicon source, triblock copolymer P123 as the template. The PEI functionalized PEI/KIT-6 was prepared with two-step post-grafting method,namely, 3-chloropropyltrimethoxysilane was firstly grafted onto KIT-6 and then polyethyleneimine(PEI) was further grafted. The samples were characterized by Fourier transform infrared spectroscopy(FTIR), X-ray diffraction(XRD),thermal gravimetric analysis(TGA), elemental analysis, N_2 adsorption-desorption and scanning electron microscopy(SEM). The Pb~(2+) adsorption performance was determined by inductively coupled plasma(ICP). The results showed that the average loading of the amino groups was 0.374 mmol·g~(-1), and the modified KIT-6 remained highly ordered and no pore blockage occurred. With the dosage of 1 g·L~(-1)PEI/KIT-6, the optimum pH value for adsorption of 100mg·L~(-1)Pb~(2+)was 6.0 at room temperature. The adsorption capacity of PEI/KIT-6 for Pb~(2+)increased firstly and then decreased with the increase of temperature, and the optimum adsorption temperature was 35 ℃. The adsorption capacity tends to reach equilibrium after 120 min. The pseudo-second-order kinetic model was found to be suited well for the entire adsorption process. Adsorption equilibrium data could be also described well by Langmuir and Freundlich isotherm models. The adsorption tends to take chemisorption of monolayer.
Mesoporous material KIT-6 was prepared using tetraethyl orthosilicate as the silicon source, triblock copolymer P123 as the template. The PEI functionalized PEI/KIT-6 was prepared with two-step post-grafting method,namely, 3-chloropropyltrimethoxysilane was firstly grafted onto KIT-6 and then polyethyleneimine(PEI) was further grafted. The samples were characterized by Fourier transform infrared spectroscopy(FTIR), X-ray diffraction(XRD),thermal gravimetric analysis(TGA), elemental analysis, N_2 adsorption-desorption and scanning electron microscopy(SEM). The Pb~(2+) adsorption performance was determined by inductively coupled plasma(ICP). The results showed that the average loading of the amino groups was 0.374 mmol·g~(-1), and the modified KIT-6 remained highly ordered and no pore blockage occurred. With the dosage of 1 g·L~(-1)PEI/KIT-6, the optimum pH value for adsorption of 100mg·L~(-1)Pb~(2+)was 6.0 at room temperature. The adsorption capacity of PEI/KIT-6 for Pb~(2+)increased firstly and then decreased with the increase of temperature, and the optimum adsorption temperature was 35 ℃. The adsorption capacity tends to reach equilibrium after 120 min. The pseudo-second-order kinetic model was found to be suited well for the entire adsorption process. Adsorption equilibrium data could be also described well by Langmuir and Freundlich isotherm models. The adsorption tends to take chemisorption of monolayer.
引文
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[5]Bois L, Bonhommme A, Ribes A, et al. Colloids Surf. A,2003,221(1/2/3):221-230
[6]Lam K F, Chen X, Fong C M, et al. Chem. Commun., 2008,112(17):2034-2036
[7]Wu Z, Webley P A, Zhao D. Langmuir, 2010,26(12):10277-10286
[8]WEI Jian-Wen(魏建文), WANG Ji-Hua(王记华), ZHAO Song-Sheng(赵松盛), et al. Journal of Inorganic Materials(无机材料学报), 2016,31(5):449-453
[9]Awual M R, Hasan M M. Microporous Mesoporous Mater.,2014,196(13):261-269
[10]LI Yan-Bin(李延斌), GAO Bao-Jiao(高保娇), AN Fu-Qiang(安富强). Environmental Chemistry(环境化学), 2008,27(4):463-467
[11]AN Fu-Qiang(安富强), GAO Bao-Jiao(高保娇), LIU Qing(刘青). Chemistry(化学通报), 2006,69(3):201-206
[12]Gao B J, An F Q, Liu K K. Appl. Surf. Sci., 2006,253(4):495-500
[13]Shariati S, Khabazipour M, Safa F. J. Porous Mater., 2017,24(1):129-139
[14]Kleitz F, Choi S H, Ryoo R. Chem. Commun., 2003,9(17):2136-2137
[15]Jiang Y J, Gao Q M, Yu H G, et al. Microporous Mesoporous Mater., 2007,103(1/2/3):316-324
[16]Mello M R, Phanon D, Silveira G Q, et al. Microporous Mesoporous Mater., 2011,143(1):174-179
[17]Wang W L, Yang X X, Fang Y T, et al. Appl. Energy, 2009,86(2):170-174
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[23]SHAO Yan-Qiu(邵艳秋), LU Yuan-Xuan(芦原萱), FU WenTing(付文婷), et al. Bulletin of the Chinese Ceramic Society(硅酸盐通报), 2016,35(11):3649-3653
[24]YIN Jia-Xing(尹甲兴), WANG Xue-Zhao(王雪兆), QI LianHuai(齐连怀), et al. Journal of Functional Materials(功能材料), 2013,44(17):2511-2515
[25]ZHAI Shang-Ru(翟尚儒), LI Mimg-Hui(李明慧), KOU ZiNong(寇自农), et al. Chinese J. Inorg. Chem.(无机化学学报), 2011,27(7):1271-1276
[26]Vasilie A N, Golovko L V, Trachevsky V V, et al. Microporous Mesoporous Mater., 2009,118(1/2/3):251-257