蒙脱石复合材料对Zn2+和对硝基苯酚的同步捕集

doi:10.7503/cjcu20170490

摘要/Abstract

摘要：

采用十八烷基三甲基氯化铵(STAC)和有机螯合剂乙二胺(En)复合修饰钠基膨润土制备了功能化蒙脱石复合材料(FMC), 并将其应用于复合污染废水处理. 利用X射线衍射仪(XRD)、超高分辨场发射扫描电子显微镜(FE-SEM)、傅里叶变换红外光谱仪(FTIR)、全自动物理吸附仪、元素分析仪及Zeta电位分析仪对所得复合材料进行了表征, 发现复合修饰制备的FMC层间距增大、疏水性增强; FMC能同步捕集水中重金属Zn²⁺和有机物对硝基苯酚(PNP). 研究发现, 当En/STAC摩尔比为0.75、 pH=4、吸附温度为40 ℃、吸附时间为60 min时, FMC对Zn²⁺ 和PNP的同步捕集吸附量达224.2 mmol/kg. FMC对Zn²⁺的吸附主要表现为离子交换和配位络合; 其对PNP的吸附取决于层间有机C和N含量及层间距大小.

关键词: 蒙脱石, 复合修饰, 同步捕集, 吸附机理

Abstract:

Na-bentonite was modified by cationic modification agent octadecyl trimethyl ammonium chloride(STAC) and organic chelating agent ethylenediamine(En) to prepare the functionalized montmorillonite composites(FMC) for the treatment of composite pollution wastewater. Based on the analysis and characterization of X-ray diffraction(XRD), field emission-scanning electron microscopy(FE-SEM), Fourier transform infrared spectroscopy(FTIR), automatic physical adsorption analysis, elemental analysis and zeta potential analysis, it was found that there was an increase in the basal spacing and the hydrophobic ability of FMC prepared by composite modification. FMC could realize the synchronization capture of heavy metal Zn²⁺ and the organic matter p-nitrophenyl pheno(PNP). The results showed that the synchronization capture amount of Zn²⁺ and PNP on FMC was up to 224.2 mmol/kg under the conditions that En/STAC molar ratio was 0.75, pH value was 4, the adsortption temperature was 40 ℃ and the adsorption time was 60 min. The adsorption behaviors of FMC on Zn²⁺ were mainly characterized by ion exchange and coordination complexation, while that of FMC on PNP were determined by both the content of organic C and organic N and the size of layer spacing.

Key words: Montmorillonite, Composite modification, Synchronization capture, Adsorption mechanism

中图分类号:

O647
O611.4

TrendMD:

栾敬德, 刘亚伟, 张成玉, 可欣. 蒙脱石复合材料对Zn²⁺和对硝基苯酚的同步捕集. 高等学校化学学报, 2018, 39(2): 270.

LUAN Jingde, LIU Yawei, ZHANG Chengyu, KE Xin. Synchronization Capture of Zn²⁺ and p-Nitrophenyl Phenol on Montmorillonite Composites^†. Chem. J. Chinese Universities, 2018, 39(2): 270.

图/表 15

Fig.1 Effect of REn/STAC on the synchronization sorption of Zn2+ and PNP by FMC

Fig.2 Effect of adsorption time on the adsorption performance of FMC at 30 ℃

Fig.3 Effect of adsorption temperature on the adsorption performance of FMC at 60 min

Fig.4 Synchronization and single sorption of FMC at 60 min and 40 ℃

Fig.5 Langmuir sorption isotherms of Zn2+ (A) and PNP(B) of STAC-Mt(a), FMC(b) and Mt(c)

Fig.6 XRD patterns of FMC(a), STAC-Mt(b) and Mt(c)

Table 1 Saturated sorption capacities of Zn2+ and PNP on Mt, STAC-Mt and FMC

Adsorbate	Sorption capacity/(mmol·kg^-1)
Adsorbate	Mt	STAC-Mt	FMC
Zn²⁺	223.78	114.66	164.33
PNP	37.24	56.79	61.25

Table 2 Surface property and pore structure of Mt, STAC-Mt and FMC

Adsorbent	Specific surface area/(m²·g^-1)	Pore volume/(cm³·g^-1)	Pore diameter/nm	Zeta potential/mV
Mt	48.59	0.325	17.003	-40.9
STAC-Mt	17.68	0.174	14.745	9.5
FMC	15.56	0.208	15.493	25.0

Fig.7 SEM images of samples prepared by different decoration methods (A) Mt; (B) STAC-Mt; (C) FMC; (D) FMC(Zn,PNP)

Table 3 Elemental analysis of Mt, STAC-Mt and FMC

Adsorbent	N(%)	C(%)	C/N
Mt	0	2.01
STAC-Mt	2.27	26.27	11.57
FMC	2.49	27.49	11.04

Fig.8 FTIR spectra of Mt(a), STAC-Mt(b) and FMC(c), FMC(Zn,PNP)(d)

Fig.9 Pseudo-first-order adsorption kinetics of Zn2+(A) and PNP(B) on Mt(a), STAC-Mt(b) and FMC(c)

Fig.10 Pseudo-second-order adsorption kinetics of Zn2+(A) and PNP(B) on Mt(a), STAC-Mt(b) and FMC(c)

Table 4 Change of reaction rate constants of pseudo-first-order and pseudo-second-order on Mt, STAC-Mt and FMC

Adsorbent	Adsorbate	k₁/min^-1	r₁₂	k₂/(g·mg^-1·min^-1)	$r 22$
Mt	Zn²⁺	0.0650	0.9437	0.0046	0.9993
STAC-Mt	Zn²⁺	0.0386	0.8011	0.0172	0.9947
FMC	Zn²⁺	0.0632	0.9507	0.0085	0.9985
Mt	PNP	0.0576	0.9650	0.0370	0.9999
STAC-Mt	PNP	0.0267	0.5681	0.0162	0.9999
FMC	PNP	0.0449	0.8938	0.0137	0.9999

Table 4 Change of reaction rate constants of pseudo-first-order and pseudo-second-order on Mt, STAC-Mt and FMC

Adsorbent	Adsorbate	k₁/min^-1	r₁₂	k₂/(g·mg^-1·min^-1)	$r 22$
Mt	Zn²⁺	0.0650	0.9437	0.0046	0.9993
STAC-Mt	Zn²⁺	0.0386	0.8011	0.0172	0.9947
FMC	Zn²⁺	0.0632	0.9507	0.0085	0.9985
Mt	PNP	0.0576	0.9650	0.0370	0.9999
STAC-Mt	PNP	0.0267	0.5681	0.0162	0.9999
FMC	PNP	0.0449	0.8938	0.0137	0.9999

Fig.11 Effect of cycle times on the adsorption performance of FMC

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蒙脱石复合材料对Zn²⁺和对硝基苯酚的同步捕集

Synchronization Capture of Zn²⁺ and p-Nitrophenyl Phenol on Montmorillonite Composites^†

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