化工学报 ›› 2023, Vol. 74 ›› Issue (6): 2689-2698.DOI: 10.11949/0438-1157.20230298

• 材料化学工程与纳米技术 • 上一篇    下一篇

聚(N-异丙基丙烯酰胺-共聚-烯丙基硫脲)智能微凝胶的制备及其Hg2+响应性能的研究

谢诗婷1(), 刘壮1,2(), 谢锐1,2, 巨晓洁1,2, 汪伟1,2, 潘大伟1,2, 褚良银1,2   

  1. 1.四川大学化学工程学院,四川 成都 610065
    2.四川大学高分子材料工程国家重点实验室,四川 成都 610065
  • 收稿日期:2023-03-27 修回日期:2023-05-10 出版日期:2023-06-05 发布日期:2023-07-27
  • 通讯作者: 刘壮
  • 作者简介:谢诗婷(1998—),女,硕士研究生,3142174373@qq.com
  • 基金资助:
    国家自然科学基金项目(22022810)

Study on preparation of poly(N-isopropylacrylamide-co-allylthiourea) smart microgels and responsive performance of Hg2+

Shiting XIE1(), Zhuang LIU1,2(), Rui XIE1,2, Xiaojie JU1,2, Wei WANG1,2, Dawei PAN1,2, Liangyin CHU1,2   

  1. 1.School of Chemical Engineering, Sichuan University, Chengdu 610065, Sichuan, China
    2.State Key Laboratory of Polymer Materials Engineering, Sichuan University, Chengdu 610065, Sichuan, China
  • Received:2023-03-27 Revised:2023-05-10 Online:2023-06-05 Published:2023-07-27
  • Contact: Zhuang LIU

摘要:

N-异丙基丙烯酰胺(NIPAM)和烯丙基硫脲(ATU)为共聚单体,N,N'-亚甲基双丙烯酰胺(MBA)为交联剂,2,2′-偶氮二(2-甲基丙基咪)二盐酸盐(V50)为引发剂,通过沉淀聚合法制备了一种可用于Hg2+检测与去除的聚(N-异丙基丙烯酰胺-共聚-烯丙基硫脲)(PNA)智能微凝胶。利用傅里叶变换红外光谱仪(FT-IR)、X射线光电子能谱仪(XPS)和扫描电镜(SEM)对微凝胶进行了化学成分和形貌表征。利用动态光散射纳米粒度分析仪(DLS)对微凝胶的粒径分布及温度响应性进行了研究。探究了干扰离子、pH和温度对微凝胶Hg2+响应性能的影响。利用原子吸收光谱仪(AAS)探究了PNA微凝胶对Hg2+的吸附去除效果。结果显示,PNA微凝胶具有良好的温敏性以及对Hg2+的特异响应性,响应Hg2+后引起的收缩比(RD)随着ATU单体比例的增加而减小,并确定了最佳检测温度为30℃。随着Hg2+浓度的增加,RD值逐渐减小,根据Hg2+浓度与RD之间的对应关系拟合出相应的Hg2+浓度计算公式。该PNA微凝胶最低检测浓度可达10-8 mol·L-1。在吸附实验中,PNA微凝胶的吸附容量随着Hg2+浓度的增加而增加,对10-4 mol·L-1以下的Hg2+溶液,吸附率可达80%以上,最低可使Hg2+浓度降至0.0005 mg·L-1。相比Zn2+、Cd2+和Pb2+,微凝胶对Hg2+的吸附率是其他金属离子的7倍左右。研究结果为有害金属Hg2+的检测和去除提供了新方法。

关键词: N-异丙基丙烯酰胺, 烯丙基硫脲, 微凝胶, Hg2+响应

Abstract:

In this paper, a kind of smart microgels, poly(N-isopropylacrylamide-co-allylthiourea) (PNA), for the detection and removal of Hg2+ was prepared by using N-isopropylacrylamide (NIPAM) and allylthiourea (ATU) as copolymer monomers, N,N'-methylenebisacrylamide (MBA) as a crosslinking agent, and 2,2'-azobis(2-methylpropionamidine) dihydrochloride (V50) as an initiator through precipitation polymerization. The chemical composition and morphology of the microgels were characterized by Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS) and scanning electron microscopy (SEM). The particle size distribution and temperature responsiveness of microgels were studied by dynamic light scattering nanoparticle analyzer (DLS). The effects of interfering ions, pH and temperature on the Hg2+-response of microgels were investigated. The adsorption and removal efficiency of PNA microgels for Hg2+ were explored by using atomic absorption spectrometer (AAS). The results show that, the PNA microgels have a temperature sensitivity and specific responsiveness to Hg2+. The shrinkage ratio (RD) caused by Hg2+-response decreases with the increase of ATU monomer ratio. The optimal detection temperature was determined to be 30℃. With the increase of Hg2+ concentration, the RD value gradually decreased. According to the corresponding relationship between the Hg2+ concentration and the RD of microgels, the calculation formula of Hg2+ concentration was fitted. The lowest detection concentration of PNA microgels can reach 10-8 mol·L-1. In the adsorption experiment, the adsorption capacity of the PNA microgel was found to increase with the Hg2+ concentration. An adsorption rate of over 80% was achieved for Hg2+ solutions below 10-4 mol·L-1, and the minimum concentration of Hg2+ could be reduced to 0.0005 mg·L-1. Compared with Zn2+, Cd2+and Pb2+, the adsorption rate of PNA microgels for Hg2+ is about 7 times more than other metal ions. The research results provide a new method for the detection and removal of harmful metal Hg2+.

Key words: N-isopropylacrylamide, allylthiourea, microgels, Hg2+ response

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