氨基功能化介孔硅吸附剂的制备及其对铬(Ⅲ)的吸附行为

doi:10.16085/j.issn.1000-6613.2019-0747

摘要/Abstract

摘要：

采用3-氨丙基三甲氧基硅烷（APTMS）对SBA-15介孔硅进行改性，获得氨基功能化介孔硅吸附剂（NH₂-SBA-15），从而赋予其螯合重金属离子的能力。利用XRD、SEM、TEM、EDX、TGA、BET和XPS等手段对吸附剂的表面形貌、孔道结构、元素分布和表面化学性质进行了表征。研究了NH₂-SBA-15吸附剂对水溶液中铬(Ⅲ)的吸附性能，分析了吸附动力学、吸附热力学和再生性能。结果表明，SBA-15吸附剂经过氨基功能化后，其原有的结晶结构没有明显变化，且对铬(Ⅲ)的吸附性能显著提高。NH₂-SBA-15对铬(Ⅲ)的吸附行为符合Langmuir等温吸附模型和拟二级吸附动力学方程。NH₂-SBA-15对铬(Ⅲ)的吸附过程主要依靠其表面—NH₂与铬(Ⅲ)的配位螯合作用，且为吸热过程。经过5次循环利用后，NH₂-SBA-15对铬(Ⅲ)的吸附率仍然保持在92%以上。该氨基功能化介孔硅吸附剂在吸附铬(Ⅲ)方面具有潜在的应用前景。

关键词: 介孔硅, 功能化, 吸附剂, 铬(Ⅲ)

Abstract:

SBA-15 mesoporous material was modified with 3-aminopropyltrimethoxysilane (APTMS) to obtain an amino-functionalized mesoporous silica adsorbent (NH₂-SBA-15), which had an ability to chelate heavy metal ions. The surface morphology, pore structure, element distribution and surface chemical properties of the adsorbent were characterized by XRD, SEM, TEM, EDX, TGA, BET and XPS. Moreover, the adsorption performance of NH₂-SBA-15 on chromium (Ⅲ) ions in aqueous solution was investigated. Besides, the adsorption kinetics, adsorption thermodynamics and regeneration performance of NH₂-SBA-15 toward chromium (Ⅲ) ions were analyzed. The results showed that the crystal structure of SBA-15 had no obvious change after functionalization, and the adsorption performance was significantly improved. The adsorption behavior of chromium (Ⅲ) by NH₂-SBA-15 was well described with the Langmuir isotherm adsorption model and the adsorption rate was found to follow the pseudo-second order kinetics. The adsorption process of chromium (Ⅲ) by NH₂-SBA-15 was an endothermic process and mainly relied on the coordination chelation of —NH₂ with chromium (Ⅲ). After five recycles, the adsorption rate of chromium (Ⅲ) by NH₂-SBA-15 remained above 92%. This adsorbent had potential application prospects in the adsorption of chromium (Ⅲ).

Key words: mesoporous silica, functionalization, adsorption, chromium (Ⅲ)

中图分类号:

TQ110.9

肖昱,郭宇,吴红梅,姜晓庆. 氨基功能化介孔硅吸附剂的制备及其对铬(Ⅲ)的吸附行为[J]. 化工进展, 2020, 39(1): 257-266.

Yu XIAO,Yu GUO,Hongmei WU,Xiaoqing JIANG. Adsorption of chromium (Ⅲ) ions with amino functionalized mesoporous silica adsorbent[J]. Chemical Industry and Engineering Progress, 2020, 39(1): 257-266.

图/表 17

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样品	比表面积/m²·g^-1	孔径/nm
SBA-15	757	9.69
NH₂-SBA-15	565	6.54

样品	比表面积/m²·g^-1	孔径/nm
SBA-15	757	9.69
NH₂-SBA-15	565	6.54

温度/℃	Langmuir			Freundlich
温度/℃	q _m/mg·g^-1	K _L	R ²	K _F	1/n	R ²
30	21.982	0.417	0.996	7.785	0.317	0.816
40	23.911	0.434	0.996	8.459	0.324	0.814
50	25.550	0.672	0.993	11.207	0.266	0.555

温度/℃	Langmuir			Freundlich
温度/℃	q _m/mg·g^-1	K _L	R ²	K _F	1/n	R ²
30	21.982	0.417	0.996	7.785	0.317	0.816
40	23.911	0.434	0.996	8.459	0.324	0.814
50	25.550	0.672	0.993	11.207	0.266	0.555

样品	温度 /K	K _c	ΔG /kJ?mol^-1	ΔS/kJ?mol?K^-1	ΔH/kJ?mol^-1
SBA-15	293	0.329	2.686	0.038	13.82
	303	0.432	2.306
	313	0.484	1.926
	323	0.643	1.546
	333	0.621	1.166
NH₂-SBA-15	293	3.124	-3.242	0.084	21.37
	303	5.734	-4.082
	313	8.217	-4.922
	323	9.204	-5.762
	333	9.000	-6.602