AOPAN@Mg(OH)2多层次电纺纤维膜的制备及除铬性能

doi:10.7503/cjcu20160217

高等学校化学学报 ›› 2016, Vol. 37 ›› Issue (11): 2117.doi: 10.7503/cjcu20160217

• 高分子化学 • 上一篇

AOPAN@Mg(OH)₂多层次电纺纤维膜的制备及除铬性能

张凡^1,², 汪滨^1,², 王娇娜^1,², 李秀艳¹, 李从举^1,²()

1. 北京服装学院材料科学与工程学院,2. 服装材料研究开发与评价北京市重点实验室, 北京 100029

收稿日期:2016-04-08 出版日期:2016-11-10 发布日期:2016-09-19
作者简介:联系人简介: 李从举, 男, 博士, 教授, 博士生导师, 主要从事纳米技术与纤维材料研究. E-mail: congjuli2014@126.com
基金资助:
国家自然科学基金(批准号: 21274006, 51503005)、北京市科技北京百名领军人才工程项目(批准号: LJ201614)、北京市百千万人才工程项目(批准号: 110403000402)、北京市属高等学校高层次人才引进与培养计划项目-北京市长城学者培育计划项目(批准号: CIT&TCD20150306)、北京市属高校创新能力提升计划项目(批准号: TJSHG201310012021)、北京服装学院创新团队与优秀人才选拔与培养计划项目(批准号: 2014AL-68)、北京服装学院重点项目(批准号: 2016A-03)和服装材料研究开发与评价北京市重点实验室开放课题(批准号: 2015ZK-02)资助

Preparation of Hierarchically Structured AOPAN@Mg(OH)₂ Composite Nanofibrous Membrane and Cr(Ⅵ)-removal Capacity^†

ZHANG Fan^1,², WANG Bin^1,², WANG Jiaona^1,², LI Xiuyan¹, LI Congju^1,^2,^*()

1. College of Material Science and Engineering, Beijing Institute of Fashion Technnology,2. Beijing Key Laboratory of Clothing Materials R&D and Assessment, Beijing 100029, China

Received:2016-04-08 Online:2016-11-10 Published:2016-09-19
Contact: LI Congju E-mail:congjuli2014@126.com
Supported by:
† Supported by the National Natural Science Foundation of China(Nos.21274006, 51503005), the Beijing Science and Technology Leading Talent Project, China(No.LJ201614), the Beijing Baiqianwan Talents Program, China(No.110403000402), the Importation and Development of High-Caliber Talents Project of Beijing Municipal Institutions-the Beijing Great Wall Scholars Incubator Program, China(No.CIT&TCD20150306), the Beijing City Board of Education Upgrade Project, China(No.TJSHG201310012021), the Project of Construction of Innovative Teams and Selection and Development of Excellent Talents for Beijing Institute of Fashion Technology, China(No.2014AL-68), the Research Project of Beijing Institute of Fashion Technology, China(No.2016A-03) and the Open Project Program of Beijing Key Laboratory, China(No.2015ZK-02)

摘要/Abstract

摘要：

以含有—NH₂和C═N的偕胺肟化聚丙烯腈(AOPAN)纳米纤维膜为载体, 通过水热法在AOPAN纳米纤维膜表面原位生长片状Mg(OH)₂纳米粒子, 得到具有多层次结构的有机-无机电纺复合纳米纤维膜[AOPAN@Mg(OH)₂], 并研究了AOPAN@Mg(OH)₂的除铬性能. 研究结果表明, 当水热温度为40 ℃, 水热时间为7 h时, AOPAN纳米纤维膜表面形成了明显的多层次结构的Mg(OH)₂纳米晶体. 当溶液pH=2时, AOPAN@Mg(OH)₂复合纳米纤维膜对Cr(Ⅵ)的吸附符合Langmuir模型, 且满足二级动力学方程, 5 h后最大吸附量达到123.5 mg/g. AOPAN@Mg(OH)₂复合纳米纤维膜中含有—NH₂基团和Mg(OH)₂纳米粒子, 在酸性条件下可以质子化为带正电的—N $H 3 +$ 和Mg(OH)₂H⁺, 通过静电吸附更易与HCr $O 4 -$ 结合. 此类复合纳米纤维膜材料在水体中易取出, 并且在稀NaOH溶液中可以解吸附, 循环使用4次去除率仍可以保持在50%以上.

关键词: 静电纺丝, 复合纳米纤维膜, 多层结构, 重金属铬离子, 聚丙烯腈

Abstract:

The hierarchial aminated polyacrylonitrile(AOPAN)@Mg(OH)₂ composite nanofibrous membrane was obtained by electrospinning technique and surface modification with hydroxylamine chloride prior to hydrothermal method. The composite nanofibrous membranes were characterized by Fourier transform infrared spectroscopy(FTIR), scanning electron microscopy(SEM), X-ray diffraction(XRD) and transmission electron microscope(TEM) to confirm the formation of Mg(OH)₂ nanoparticles on the AOPAN nanofibers. The results revealed that 40 ℃/7 h was the best hydrothermal condition and Mg(OH)₂ nanoparticles were effectively loaded on the surface of AOPAN nanofibrous membrane. The adsorption process showed pH dependence and the maximum Cr(Ⅵ) adsorption occurred at pH=2. The Langmuir adsorption model described well the experimental adsorption data and estimated a maximum loading capacity of 123.5 mg/g. This is mainly due to the protonation of —NH₂ groups and Mg(OH)₂ nanoparticles under the acid condition, which is benefit for adsorbing HCr $O 4 -$ . The kinetics studies indicated that the adsorption equilibrium was attained after 5 h and the experimental data followed the pseudo-second order model. Meanwhile, the AOPAN@Mg(OH)₂ composite nanofibrous membrane can be easily separated from liquid solutions and shows excellent cyclic utilization performance. The composite membrane maintained over 50% removal rate after rinsing with dilute NaOH solution by four cycles. Therefore, the AOPAN@Mg(OH)₂ composite nanofibrous membrane could be a good candidate for removing Cr(Ⅵ) from wastewater, and the study provides a simple and effective route for the development of new environmental remediation nanomaterials.

Key words: Electrospinning, Composite nanofibrous membrane, Hierarchical structure, Hexavalent chromium, Polyacrylonitrile

中图分类号:

O632.62

TrendMD:

张凡, 汪滨, 王娇娜, 李秀艳, 李从举. AOPAN@Mg(OH)₂多层次电纺纤维膜的制备及除铬性能. 高等学校化学学报, 2016, 37(11): 2117.

ZHANG Fan, WANG Bin, WANG Jiaona, LI Xiuyan, LI Congju. Preparation of Hierarchically Structured AOPAN@Mg(OH)₂ Composite Nanofibrous Membrane and Cr(Ⅵ)-removal Capacity^†. Chem. J. Chinese Universities, 2016, 37(11): 2117.

图/表 11

Scheme 1 Reaction of hydroxylamine hydrochloride with PAN nitrile group

Fig.1 SEM images of AOPAN nanofibrous membranes with different hydrothermal timeTime/h: (A) 0; (B) 1; (C) 3; (D) 5; (E) 7; (F) 9 h. Inset of (A): photo of the AOPAN nanofibrous membrane; inset of (E): photo of AOPAN@Mg(OH)2 composite nanofibrous membrane.

Fig.2 FTIR spectra for PAN nanofibrous membrane(a), AOPAN nanofibrous membrane(b) and AOPAN@Mg(OH)2 composite nanofibrous membrane(c)

Fig.3 TEM image of AOPAN@Mg(OH)2 composite nanofibrous nanofibers

Fig.4 XRD patterns for PAN fibers(a), AOPAN fibers(b) and AOPAN@Mg(OH)2 compo-site nanofibrous membranes with hydrothermal time of 3 h(c) and 7 h(d)

Fig.5 Adsorbing Cr(Ⅵ) capacity of AOPAN@Mg(OH)2 composite nanofibrous membranes with different hydrothermal time at pH=2

Fig.6 Change of the total Cr(Ⅵ) in AOPAN nanofiber(a) and AOPAN@Mg(OH)2 nanofiber(b) solution with time at pH=2(A), pseudo-frist-order plot(B) and pseudo-second-order plot(C) for adsorption of Cr(Ⅵ) onto the AOPAN@Mg(OH)2 composite nanofibrous membrane

Fig.7 Relationship between concentration of Cr(Ⅵ) and adsorption capacity at pH=2(A) and equilibrium adsorption isotherm of Cr(Ⅵ) fitted with Langmuir adsorption model(B)a. AOPAN; b. AOPAN@Mg(OH)2.

Fig.8 Recyclable property of AOPAN@Mg(OH)2

Fig.9 SEM images of AOPAN@Mg(OH)2 composite nanofibrous membrane(A) and the AOPAN@Mg(OH)2 composite nanofibrous membrane(B) washed by 0.1 mol/L NaOH solutions

Fig.10 Mechanism illustration for the adsorption of Cr(Ⅵ) on the surface of AOPAN@Mg(OH)2 composite nanofibrous membrane

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AOPAN@Mg(OH)₂多层次电纺纤维膜的制备及除铬性能

Preparation of Hierarchically Structured AOPAN@Mg(OH)₂ Composite Nanofibrous Membrane and Cr(Ⅵ)-removal Capacity^†

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