制备方法对GO/P(NIPAM-MA)水凝胶La3+吸附性能的影响

doi:10.11949/j.issn.0438-1157.20190371

化工学报 ›› 2019, Vol. 70 ›› Issue (10): 4072-4079.DOI: 10.11949/j.issn.0438-1157.20190371

• 材料化学工程与纳米技术 • 上一篇下一篇

制备方法对GO/P(NIPAM-MA)水凝胶La³⁺吸附性能的影响

杨新蔚^1,²(),单国荣^1,²(),曹志海³,吕挺⁴,潘鹏举^1,²

1. 化学工程联合国家重点实验室，浙江大学化学工程与生物工程学院，浙江杭州 310027
2. 浙江大学衢州研究院，浙江衢州 324000
3. 浙江理工大学先进纺织材料与制备技术教育部重点实验室，浙江杭州 310018
4. 杭州电子科技大学材料与环境工程学院，浙江杭州 310018

收稿日期:2019-04-10 修回日期:2019-05-09 出版日期:2019-10-05 发布日期:2019-10-05
通讯作者: 单国荣
作者简介:杨新蔚（1995—），女，硕士研究生，475105259@qq.com

Effect of preparation methods on La³⁺ adsorption properties ofGO/P(NIPAM-MA) hydrogels

Xinwei YANG^1,²(),Guorong SHAN^1,²(),Zhihai CAO³,Ting LYU⁴,Pengju PAN^1,²

1. State Key Laboratory of Chemical Engineering, College of Chemical and Biological Engineering, Zhejiang University, Hangzhou 310027, Zhejiang, China
2. Institute of Zhejiang University-Quzhou, Quzhou 324000, Zhejiang, China
3. Key Laboratory of Advanced Textile Materials and Manufacturing Technology, Ministry of Education, Zhejiang Sci-Tech University, Hangzhou 310018, Zhejiang, China
4. College of Materials and Environmental Engineering, Hangzhou Dianzi University, Hangzhou 310018, Zhejiang, China

Received:2019-04-10 Revised:2019-05-09 Online:2019-10-05 Published:2019-10-05
Contact: Guorong SHAN

摘要/Abstract

摘要：

用冷冻聚合法和非冷冻聚合法制备了氧化石墨烯/聚(N-异丙基丙烯酰胺-顺丁烯二酸)(GO/P(NIPAM-MA))水凝胶，比较制备方法对GO/P(NIPAM-MA)水凝胶La³⁺吸附能力的影响，发现通过冷冻聚合法合成的水凝胶，具有更加优异的溶胀-退溶胀性能和吸附性能。NIPAM与MA摩尔比为10∶1的冷冻聚合法水凝胶，在370 mg/L的LaCl₃溶液中平衡吸附量为(29.87±0.073)mg/g，而相同条件下的非冷冻聚合法水凝胶平衡吸附量仅为(20.29±0.395)mg/g。冷冻聚合法水凝胶的Freundlich等温线拟合参数n值随着MA含量的增加呈线性增加，而非冷冻聚合法水凝胶增加幅度小于冷冻聚合法。经过5次吸附-解吸循环，冷冻聚合法水凝胶的形状和体积没有明显变化且吸附能力没有明显下降，而非冷冻聚合法水凝胶经过3次吸附-解吸循环就出现破碎，无法再使用。冷冻聚合法合成的GO/P(NIPAM-MA)水凝胶具有La³⁺平衡吸附量大、可重复使用等优点。

关键词: 吸附, 脱附, 水凝胶, 冷冻聚合, La³⁺

Abstract:

Graphene oxide/poly(N-isopropylacrylamide-maleic acid) (GO/P(NIPAM-MA)) hydrogel was prepared by freeze polymerization and non-freeze polymerization, and the preparation method was compared to GO/P(NIPAM-MA) hydrogel La³⁺ adsorption capacity. It was found that the hydrogel synthesized by freeze polymerization method has an excellent swelling-shrinking and adsorption properties. With an equivalent molar ratio of 10∶1 for NIPAM∶MA and 370 mg/L of LaCl₃ solution, the equilibrium adsorption capacity of hydrogel synthesized by freeze polymerization method was (29.87±0.073) mg/g, while that of by non-freeze polymerization method was only (20.29±0.395) mg/g. Fitting parameter, n, of the Freundlich isotherm increased linearly with the increase of MA content for hydrogel synthesized by freeze polymerization method, and the increasing degree was larger than that of by non-freeze polymerization method. After five repeated adsorption-desorption cycles, it was found that there was no significant deformation and the adsorption capacity was not obviously decreased for hydrogel synthesized by freeze polymerization method, while it was broken after three repeated adsorption-desorption cycles for hydrogel synthesized by non-freeze polymerization method. The GO/P(NIPAM-MA) hydrogel synthesized by the freeze polymerization method has the advantages of large La³⁺ equilibrium adsorption capacity and reusability.

Key words: adsorption, desorption, hydrogel, freeze polymerization, La³⁺

中图分类号:

TQ 314.2

杨新蔚, 单国荣, 曹志海, 吕挺, 潘鹏举. 制备方法对GO/P(NIPAM-MA)水凝胶La³⁺吸附性能的影响[J]. 化工学报, 2019, 70(10): 4072-4079.

Xinwei YANG, Guorong SHAN, Zhihai CAO, Ting LYU, Pengju PAN. Effect of preparation methods on La³⁺ adsorption properties ofGO/P(NIPAM-MA) hydrogels[J]. CIESC Journal, 2019, 70(10): 4072-4079.

图/表 8

图1 不同制备方法合成水凝胶的SEM图

Fig.1 SEM of hydrogels prepared by different methods (n NIPAM∶n MA=20∶1)

图2 两种制备方法合成水凝胶孔径分布

Fig.2 Pore size distribution of hydrogels prepared by different methods (n NIPAM∶n MA=20∶1)

图3 两种制备方法得到水凝胶溶胀/退溶胀动力学

Fig.3 Swelling/shrinking kinetics of hydrogels prepared by different methods (n NIPAM∶n MA=20∶1)

表1 制备方法对水凝胶平衡吸附量的影响

Table 1 Effect of preparation method on equilibrium adsorption capacity of hydrogels

n _NIPAM∶n _MA	Equilibrium adsorption capacity, q _e/(mg/g)
n _NIPAM∶n _MA	By freeze polymerization	By non-freeze polymerization
10∶1	29.87±0.073	20.29±0.395
15∶1	25.61±0.084	17.43±0.257
20∶1	19.53±0.403	11.78±0.237
25∶1	15.56±0.166	9.94±0.046
30∶1	9.16±0.174	5.57±0.091
40∶1	3.95±0.171	3.84±0.131
PNIPAM	3.13±0.033	3.16±0.015

表2 两种制备方法合成的不同单体摩尔比水凝胶吸附实验数据Freundlich拟合结果

Table 2 Freundlich fitting parameters of adsorption experimental data of different monomer ratio hydrogels prepared by freeze and non-freeze polymerization

n _NIPAM∶n _MA	By freeze polymerization		By non-freeze polymerization
n _NIPAM∶n _MA	1/n	K	1/n	K
10∶1	0.2011	9.0448	0.2791	4.6970
15∶1	0.2495	5.5447	0.3487	2.8022
20∶1	0.2989	3.3927	0.4332	1.2057
25∶1	0.3563	2.1598	0.5396	0.7828
30∶1	0.4197	1.4711	0.6097	0.3656
40∶1	0.5345	0.7539	0.6307	0.2673

图4 两种制备方法合成水凝胶的Freundlich拟合参数n随MA摩尔分数变化关系

Fig.4 Relationship between n of Freundlich fitting parameter and MA molar fraction of hydrogels prepared by freeze and non-polymerization (n NIPAM∶n MA=10∶1)

图5 两种方法制备的水凝胶由温度改变触发的溶胀/退溶胀循环比较(25℃中溶胀，60℃中退溶胀)

Fig.5 Swelling/shrinking cycles of hydrogels prepared by freeze and non-freeze polymerization trigged by changing temperature (hydrogels were alternatively transferred into deionized water at 25 and 60 ℃) (n NIPAM∶n MA=10∶1)

图6 两种制备方法合成水凝胶的La3+吸附-脱附循环比较

Fig.6 Adsorption and desorption cycles of La3+ for hydrogels prepared by freeze and non-freeze polymerization (n NIPAM∶n MA=10∶1)

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制备方法对GO/P(NIPAM-MA)水凝胶La³⁺吸附性能的影响

Effect of preparation methods on La³⁺ adsorption properties ofGO/P(NIPAM-MA) hydrogels

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