TOCNF与磁性羧甲基壳聚糖纳米粒子复合物的制备及吸附Pb2+的特性

doi:10.16085/j.issn.1000-6613.2021-0637

摘要/Abstract

摘要：

水体中铅污染对环境及人的健康安全造成了极大的危害。本文将四甲基呱啶（TEMPO）氧化的纤维素纳米纤维（TEMPO-oxidized cellulose nanofibers，TOCNF）与磁性羧甲基壳聚糖纳米粒子（magnetic carboxymethyl chitosan nanoparticles，MCCN）交联复合制备一种经济高效且对环境无毒害的Pb²⁺吸附剂，对复合前后的材料进行结构表征。通过单因素实验研究pH、Pb²⁺初始浓度、吸附时间及温度对Pb²⁺吸附效率的影响，确定最优吸附条件后比较TOCNF/MCCN及TOCNF对Pb²⁺的吸附效果，研究复合材料对Pb²⁺的吸附特性。研究结果表明，Fe₃O₄成功被羧甲基壳聚糖纳米粒子包裹并与TOCNF交联复合，在最优吸附条件（pH=5，Pb²⁺初始浓度为100mg/L，吸附时间为240min，常温下进行实验）下，TOCNF/MCCN吸附Pb²⁺的饱和容量为193.5mg/g，比TOCNF高了近一倍。复合吸附剂吸附Pb²⁺的过程更符合准二级动力学方程，说明决定吸附速率的主要是化学吸附。等温吸附方程的相关系数R²表明，Langmuir方程能更好地拟合吸附过程，说明复合吸附剂对Pb²⁺的吸附主要是表面基团的单分子层吸附。通过线性方程的斜率计算得到的理论饱和吸附量为201.1mg/g，与实际值差3.8%，经过5次解吸再吸附的过程，吸附剂的吸附效率仅下降了13%，表明该吸附剂有良好的可再生性，具有很好的应用前景。

关键词: TEMPO氧化, 纤维素纳米纤维, 磁性羧甲基壳聚糖, 吸附, 动力学方程, 吸附等温方程

Abstract:

Lead pollution in water causes great harm to environment and human health. In this paper, TEMPO-oxidized cellulose nanofibers (TOCNF) were cross-linked with magnetic carboxymethyl chitosan nanoparticles (MCCN) to prepare an economically efficient and environmentally friendly material to adsorb Pb²⁺. The structure of TOCNF/MCCN and TOCNF were characterized. The effects of pH, initial concentration of Pb²⁺, contact time and temperature on the adsorption efficiency of Pb²⁺ were studied by single factor experiments. The adsorption effects of TOCNF/MCCN and TOCNF on Pb²⁺ were compared under the optimum reaction conditions. The results showed that Fe₃O₄ was successfully coated by carboxymethyl chitosan nanoparticles and cross-linked with TOCNF. The optimum reaction condition for Pb²⁺ adsorption was obtained at room temperature when the pH was 5, initial concentration of Pb²⁺ was 100mg/L, and contact time was 240min. The absorption saturation capacity of TOCNF/MCCN was 193.5mg/g, which was nearly double that of TOCNF. Moreover, the adsorption process followed the pseudo-second-order model, which indicated that the adsorption rate was mainly determined by chemical adsorption. The correlation coefficient showed that the adsorption equilibrium data fitted well with Langmuir isotherm model, indicating that the adsorption of Pb²⁺ by TOCNF/MCCN was mainly the monolayer adsorption of surface groups. The theoretical saturated adsorption amount calculated by the slope of the linear equation was 201.1mg/g, which was 3.8% different from the actual value. After 5 times of desorption and re-adsorption, the adsorption efficiency of the adsorbent only decreased by 13%, which indicated that the adsorbent had good reproducibility and had a good application prospect.

Key words: TEMPO oxidation, cellulose nanofibers, magnetic carboxymethyl chitosan, adsorption, kinetic equation, adsorption isotherm equation

中图分类号:

X703.1

周丽莎, 李若男, 卞雨洁, 陈舜胜. TOCNF与磁性羧甲基壳聚糖纳米粒子复合物的制备及吸附Pb²⁺的特性[J]. 化工进展, 2022, 41(2): 901-910.

ZHOU Lisha, LI Ruonan, BIAN Yujie, CHEN Shunsheng. Preparation of TOCNF and magnetic carboxymethyl chitosan nanoparticles composite and adsorption properties of Pb²⁺[J]. Chemical Industry and Engineering Progress, 2022, 41(2): 901-910.

图/表 13

参考文献 44

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吸附剂吸附Pb²⁺	q_e/mg·g^-1	k/min^-1	R²
准一级动力学方程	177.6	0.0909	0.8179
准二级动力学方程	199.3	0.0005628	0.9996

吸附剂吸附Pb²⁺	q_e/mg·g^-1	k/min^-1	R²
准一级动力学方程	177.6	0.0909	0.8179
准二级动力学方程	199.3	0.0005628	0.9996

Langmuir等温线模型				Freundlich等温线模型
q_m/mg·g^-1	b/mg·L^-1	R²		n	K/mg·L^-1	R²
201.1	0.04235	0.9980		2.663	3.265	0.8246

Langmuir等温线模型				Freundlich等温线模型
q_m/mg·g^-1	b/mg·L^-1	R²		n	K/mg·L^-1	R²
201.1	0.04235	0.9980		2.663	3.265	0.8246

吸附剂	饱和吸附容量/mg·g^-1	pH	吸附模型	循环次数	参考文献
TOCNF/MCCN复合材料	201.1	5	Langmuir和Freundlich	5	本研究
硫醇改性CNF复合膜	137.7	5	Langmuir	3	［37］
氧化石墨烯/羧甲基纤维素纳米纤维复合材料	99	5	Langmuir和Freundlich	—	［41］
丙烯酸接枝TOCNF	100	5.3	Langmuir和Freundlich	—	［28］
纤维素/壳聚糖复合气凝胶	137.8	3~6	Langmuir	5	［42］
羟基磷灰石静电纺乙酸纤维素纳米纤维	49.75	6	Langmuir	—	［43］
细菌纤维素/羟基磷灰石复合材料	192	3~5	Langmuir和Freundlich	—	［44］

TOCNF与磁性羧甲基壳聚糖纳米粒子复合物的制备及吸附Pb²⁺的特性

Preparation of TOCNF and magnetic carboxymethyl chitosan nanoparticles composite and adsorption properties of Pb²⁺

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