2-吡啶甲醛功能化SBA-15介孔材料的制备及其对Cr(Ⅲ)离子的吸附

doi:10.16085/j.issn.1000-6613.2021-1827

摘要/Abstract

摘要：

通过席夫碱反应将2-吡啶甲醛成功嫁接到氨基化的SBA-15介孔分子筛上，本文获得了一种新型功能化SBA-15吸附剂（N-SBA-15）。采用傅里叶变换红外光谱、X射线衍射、元素分析、扫描电子显微镜、透射电子显微镜、X射线光电子能谱、热重分析和氮气吸附-脱附等手段对N-SBA-15的表面官能团、形貌、孔道结构和表面化学性质进行了详细的表征分析。利用N-SBA-15对水溶液中的Cr(Ⅲ)进行了吸附实验，其最大吸附容量为84.3mg/g。动力学分析和等温吸附研究结果表明，N-SBA-15对Cr(Ⅲ)的吸附过程符合准二级动力学模型和Langmuir模型。吸附热力学分析表明，该吸附过程是自发的吸热过程（?G<0、?S>0、?H>0）。吸附机理分析表明该吸附过程主要是由N-SBA-15表面有机官能团与Cr(Ⅲ)的配位作用实现的。而且，N-SBA-15吸附剂经过5次吸附-脱附测试，仍然对Cr(Ⅲ)具有较高的吸附容量。

关键词: SBA-15, 2-吡啶甲醛, 席夫碱, 吸附, Cr (Ⅲ)

Abstract:

A novel functionalized SBA-15 material (N-SBA-15) was synthesized via Schiff's base reaction of 2-pyridinecarboxaldehyde with amino modified SBA-15 mesoporous material for adsorption of Cr(Ⅲ) ions from aqueous solution. The organic functional groups, morphology, pore structure and chemical property of N-SBA-15 were determined by FTIR, XRD, EDX, SEM, TEM, XPS, TGA and N₂ adsorption-desorption. Moreover, the adsorption performance of N-SBA-15 adsorbent on Cr(Ⅲ) ions in aqueous solution was investigated. The adsorption capacity of 84.3mg/g toward Cr(Ⅲ) ions was obtained. The kinetics analysis and adsorption isotherms revealed that the adsorption process of Cr(Ⅲ) ions by N-SBA-15 was consistent with pseudo-second-order kinetic model and Langmuir isotherm model. The thermodynamic parameters showed that Cr(Ⅲ) adsorption onto N-SBA-15 was spontaneous, endothermic and entropy-increasing process (?G<0, ?S>0, ?H>0). The adsorption mechanism analysis indicated that Cr(Ⅲ) adsorption onto N-SBA-15 was mainly based on the chemical combination of N atoms on the organic functional groups of N-SBA-15 through coordination bond. Furthermore, N-SBA-15 still kept high adsorption capacity after five adsorption–desorption cycles.

Key words: SBA-15, 2-pyridinecarboxaldehyde, Schiff's base, adsorption, Cr(Ⅲ)

中图分类号:

O647

姜晓庆, 郭宇, 吴红梅. 2-吡啶甲醛功能化SBA-15介孔材料的制备及其对Cr(Ⅲ)离子的吸附[J]. 化工进展, 2022, 41(7): 3915-3924.

JIANG Xiaoqing, GUO Yu, WU Hongmei. Synthesis of 2-pyridinecarboxaldehyde functionalized SBA-15 mesoporous material for the adsorption of Cr(Ⅲ) ions from aqueous solution[J]. Chemical Industry and Engineering Progress, 2022, 41(7): 3915-3924.

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样品	比表面积/cm³·g^-1	孔径/nm	孔容/cm³·g^-1
SBA-15	757.40	9.60	1.04
NH₂-SBA-15	462.92	8.12	0.91
N-SBA-15	335.04	7.67	0.54

温度/℃	Langmuir模型			Freundlich模型
温度/℃	q_m/g·mg^-1	K_L/L·mg^-1	R²	K_F/mg·g^-1	n	R²
30	88.34	0.105	0.968	20.60	2.96	0.935
40	91.66	0.269	0.996	31.84	3.51	0.950
50	91.74	0.859	0.999	45.24	4.65	0.775

温度 /℃	q_e（实验） /mg·g^-1	准一级动力学模型			准二级动力学模型
温度 /℃	q_e（实验） /mg·g^-1	K₁/g·mg^-1·min^-1	q_e（计算）/mg·g^-1	R²	K₂/g·mg^-1·min^-1	q_e（计算）/mg·g^-1	R²
30	84.3	0.0162	56.07	0.983	4.36×10^-4	74.96	0.972
40		0.0156	60.42	0.944	4.32×10^-4	79.74	0.966
50		0.0145	64.89	0.969	4.02×10^-4	87.03	0.973

温度/K	K_c	ΔG/kJ·mol^-1	ΔS/kJ·mol^-1·K^-1	ΔH/kJ·mol^-1
293	1.165	-0.485	0.135	39.07
303	2.300	-1.835
313	3.202	-3.185
323	5.369	-4.535

吸附剂	最大吸附容量/mg·g^-1	参考文献
coir pith	11.56	［37］
NZVI-SDBC	28.89	［38］
XPB	56.50	［39］
Fe₃O₄@SiO₂	39.27	［40］
NH₂-SBA-15	24.88	［21］
N-SBA-15	84.3	本文