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浙江大学学报（理学版）
浙江大学学报（理学版）  2017, Vol. 44 Issue (1): 70-75    DOI: 10.3785/j.issn.1008-9497.2017.01.011
化学     
戊二醛改性交联壳聚糖纳米纤维膜负载钯催化剂的制备及其催化性能研究
王子宁1,2, 应婷婷2, 邵林军2, 水淼1, 齐陈泽2
1. 宁波大学 材料科学与化学工程学院, 浙江 宁波 315211;
2. 绍兴文理学院 浙江省精细化学品传统工艺替代技术研究重点实验室, 浙江 绍兴 312000
Immobilization of palladium on glutaraldehyde chemical modified chitosan fiber mat and its catalytic performance
WANG Zining1,2, YING Tingting2, SHAO Linjun2, SHUI Miao1, QI Chenze2
1. College of Material Science and Chemical Engineering, Ningbo University, Ningbo 315211, Zhejiang Province, China;
2. Zhejiang Key Laboratory of Alternative Technologies for Fine Chemicals Process, Shaoxing University, Shaoxing 312000, Zhejiang Province, China
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摘要： 以壳聚糖（CS）为基体聚合物、聚甲基丙烯酸（PMAA）为共纺聚合物，通过静电纺丝和热交联技术制备了具有良好形貌和稳定性的交联壳聚糖/聚甲基丙烯酸（CS/PMAA）纳米纤维膜，然后采用戊二醛对纤维进行化学改性后用于负载钯催化剂.采用扫描电镜（SEM）表征纤维膜的微观结构；通过扫描电子显微镜-能谱仪（EM-EDS）和X-射线衍射仪（XRD）分析钯催化中心在纤维膜上的分布；采用红外光谱（FT-IR）表征戊二醛改性后纤维膜的化学结构变化；利用密度泛函理论（DFT）研究戊二醛改性对壳聚糖纤维膜与钯催化中心之间络合强度的影响.Sonogashira偶联反应催化结果显示，戊二醛改性有助于提高纤维膜负载钯催化剂的催化活性，且该催化剂在重复使用9次后，催化反应转化率和产率基本保持不变.
关键词： 壳聚糖;  静电纺丝;  钯;  Sonogashira偶合反应;  DFT    
Abstract: Using poly(methacrylic acid) (PMAA) as the coelectrospinning agent, well-defined chitosan/poly(methacrylic acid) (CS/PMAA) fiber mat was fabricated by electrospinning and crosslinked at 180℃ for 2 h, then chemically modified with glutaraldehyde to immobilize palladium species. The fiber morphologies were observed by scanning electron microscopy (SEM) and the dispersion of palladium species were analyzed by SEM-energy dispersive spectrometer (EDS) and X-ray diffraction (XRD). The chemical modification of CS/PMAA fiber was characterized by fourier transform infrared spectroscopy (FT-IR) spectra. Density functional theory (DFT) calculation results demonstrate that the chemical modification can decrease the chelating strength between the CS/PMAA fiber and palladium species. The catalytic performances of these novel chitosan fiber supported Pd catalysts were evaluated by Sonogashira coupling reaction. It is found that the glutaraldehyde modification can improve the catalytic activity of CS/PMAA fiber supported palladium catalyst. Moreover, this novel catalyst can be reused at least nine times without obvious loss of initial activity.
Key words: chitosan    electrospinning    palladium    Sonogashira coupling reaction    DFT
收稿日期: 2016-03-06 出版日期: 2017-01-22
CLC:  O643.37  
基金资助: 国家自然科学基金资助项目（11575117）；浙江省自然科学基金资助项目（LQ14E030003）
通讯作者: 齐陈泽,ORCID:http://orcid:org/0000-0002-5930-6587,E-mail:312087578@qq.com     E-mail: 312087578@qq.com
作者简介: 王子宁(1990-),ORCID:http://orcid.org/0000-0003-4120-693X,男,硕士研究生,主要从事静电纺丝材料的制备和应用研究,E-mail:471125643@qq.com.
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引用本文:

王子宁, 应婷婷, 邵林军, 水淼, 齐陈泽. 戊二醛改性交联壳聚糖纳米纤维膜负载钯催化剂的制备及其催化性能研究[J]. 浙江大学学报（理学版）, 2017, 44(1): 70-75.

WANG Zining, YING Tingting, SHAO Linjun, SHUI Miao, QI Chenze. Immobilization of palladium on glutaraldehyde chemical modified chitosan fiber mat and its catalytic performance. Journal of ZheJIang University(Science Edition), 2017, 44(1): 70-75.

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https://www.zjujournals.com/sci/CN/10.3785/j.issn.1008-9497.2017.01.011    或    https://www.zjujournals.com/sci/CN/Y2017/V44/I1/70

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