醚化PBS与CMC液体复合材料的相互作用

doi:10.7503/cjcu20140792

高等学校化学学报 ›› 2015, Vol. 36 ›› Issue (4): 808.doi: 10.7503/cjcu20140792

• 高分子化学 • 上一篇

醚化PBS与CMC液体复合材料的相互作用

张敏¹(), 许小玲¹, 宋吉青², 何文清²

1. 陕西科技大学化学与化工学院, 教育部轻化工助剂化学与技术重点实验室, 西安 710021
2. 中国农业科学院农业环境与可持续发展研究所, 农业部农业环境与气候变化重点开放实验室,农业部旱作节水农业重点开放实验室, 北京 100081

收稿日期:2014-09-01 出版日期:2015-04-10 发布日期:2015-03-19
作者简介:联系人简介: 张敏, 女, 博士, 教授, 主要从事可生物降解材料的合成、降解和机理研究. E-mail: zhangmin@sust.edu.cn; yanjiushi206@163.com
基金资助:
国家“八六三”计划项目(批准号: 2011AA100503)和陕西科技大学科研创新团队项目(批准号: TD10-01)资助

Interfacial Interaction Mechanism of Etherified PBS and CMC Liquid Composites^†

ZHANG Min^1,^*(), XU Xiaoling¹, SONG Jiqing², HE Wenqing²

1. Key Laboratory of Auxiliary Chemistry and Technology for Chemical Industry, Ministry of Education,College of Chemistry and Chemical Engineering, Shaanxi University of Science and Technology, Xi’an 710021, China
2. Institute of Environment and Sustainable Development in Agriculture, CAAS,Key Laboratory of Agro-Environment and Climate Change, Ministry of Agriculture, Key Laboratory of Dryland Farming and Water-Saving Agriculture, Ministry of Agriculture, Beijing 100081, China

Received:2014-09-01 Online:2015-04-10 Published:2015-03-19
Contact: ZHANG Min E-mail:zhangmin@sust.edu.cn
Supported by:
† Supported by the National High Technology Research and Development Program of China(No.2011AA100503) and the Innovation Fund for Scientific Research Team of Shaanxi University of Science and Technology, China(No.TD10-01).

摘要/Abstract

摘要：

采用聚乙二醇(PEG)对聚丁二酸丁二醇酯(PBS)进行醚化改性, 得到醚化PBS(PEG/PBS), PEG/PBS与羧甲基纤维素(CMC)共混制备了在水相均匀分散的新型(PEG/PBS)-CMC液体复合材料. 结合分子模拟技术对PEG/PBS与CMC复合材料的相互作用机理进行了研究. 结果表明, PEG/PBS具有预期的化学结构和优异的水润湿性; 含醚链段PEG的引入有效提高了PBS分子链的极性和柔顺性, PEG/PBS与CMC之间存在氢键作用、范德华力作用、疏水作用和吸附作用. 红外光谱(FTIR)中官能团(如—OH, —OCO—, —COOH, —C—O—C—等)的吸收峰频率发生偏移; 光电子能谱(XPS)中C和O元素的结合能分布转移, 表明PBS及PEG/PBS与CMC的官能团之间发生了相互作用; 偏光显微镜(POM)和 X射线衍射(XRD)结果表明, 复合材料之间的相互作用为非共价键的结合; 扫描电子显微镜(SEM)结果表明醚化改性后(PEG/PBS)-CMC复合材料间的相互作用增强, 表面结合更紧密, 相容性得到提高.

关键词: 醚化聚丁二酯丁二醇酯, 羧甲基纤维素, 液体复合材料, 动力学模拟, 相互作用

Abstract:

Poly(butylene succinate)(PBS) was etherified by polyethylene glycol(PEG), and blended with carboxymethylcellulose(CMC). A novel liquid composite(PEG/PBS)-CMC was successfully prepared in water solution. The interaction mechanism of (PEG/PBS)-CMC composite was investigated by molecular simulation. The results showed that the desired structure of PEG/PBS with good hydrophilicity was achieved. Molecular simulation displayed that the polarity and flexibility of PEG/PBS was enhanced by introducing PEG to PBS. The interactions of (PEG/PBS)-CMC were hydrogen bonding, van der Waals, hydrophobic bond and adsorption. This results were explained by the deviation of absorption peak frequency on functional groups such as —OH, —OCO—, —COOH and —C—O—C— in Fourier transform infrared(FTIR) and the binding energy transfer of C and O element in X-ray photoelectron spectroseopy(XPS). Non-covalent interaction existed between composites displayed in polarizing optical microscope(POM) and X-ray diffraction(XRD). The closely integrated interface of (PEG/PBS)-CMC in scanning electron microscope(SEM) showed that the binding forces and the compatibility were enhanced after etherification modification.

Key words: Etherified polycbutylene suceinate, Carboxymethyl cellulose, Liquid composite, Dynamics simulation, Interaction

中图分类号:

O631
TQ31

TrendMD:

张敏, 许小玲, 宋吉青, 何文清. 醚化PBS与CMC液体复合材料的相互作用. 高等学校化学学报, 2015, 36(4): 808.

ZHANG Min, XU Xiaoling, SONG Jiqing, HE Wenqing. Interfacial Interaction Mechanism of Etherified PBS and CMC Liquid Composites^†. Chem. J. Chinese Universities, 2015, 36(4): 808.

图/表 12

Scheme 1 Synthesis routes of PBS and PEG/PBS copolymer

Table 1 1H NMR date information of PBS and PEG/PBS copolymer

Polymer	δ	Ownership	Structural unit
TMS	0	—CH₃	(CH₃)₄Si
PBS	1.72	—CH₂—	BDO
	2.62	—CH₂—C ＝O	SA
	4.13	—CH₂—O—	BDO
PEG/PBS(50/50)	3.68	—CH₂—O—	PEG
	4.28	—CH₂—OOC—	PEG
Solvent	7.26	—C—D—	CDCl₃

Fig.1 Contact angle of PBS and PEG/PBS

Fig.2 Structures of CMC(A, stick mode), PBS(B, ball mode) and PEG/PBS(C, ball mode) Carbon: gray; hydrogen: white; oxygen: red.

Fig.3 Dynamics simulation models of CMC-CMC(A), PBS-CMC(B) and (PEG/PBS)-CMC(C) in aqueous solution Carbon: gray; hydrogen: white; oxygen: red.

Table 2 Energy of CMC-CMC, PBS-CMC and (PEG/PBS)-CMC by dynamics simulation

Composity	10^-4 E_Mixing / (kJ·mol^-1)	10^-3E_Dihedral / (kJ·mol^-1)	10^-3 E_Angle / (kJ·mol^-1)	10^-3 E_Bond / ( kJ·mol^-1)	10^-3 E_Vdw / (kJ·mol^-1)
CMC-CMC	-11.26	6.23	5.78	13.22	21.25
PBS-CMC	-2.47	3.21	1.54	3.21	4.59
(PEG/PBS)-CMC	-8.18	3.25	4.76	10.52	15.28

Fig.4 Energy distribution of CMC-CMC(a), PBS-CMC(b) and (PEG/PBS)-CMC(c) (A) EMixing; (B) EDihedral; (C) EAngle; (D) EBond; (E) EVdw.

Fig.5 FTIR spectra of CMC-CMC(a), PBS-CMC(b) and (PEG/PBS)-CMC(c)

Fig.6 XPS spectra of composites(A) and the energy distribution of C1s(B), O1s(C),Na1s(D) of CMC-CMC(a), PBS-CMC(b) and (PEG/PBS)-CMC(c)

Table 3 Atomic composition of composites from XPS

Sample	E_B(C₁_s)/eV				E_B(O₁_s)/eV			E_binding(Na₁_s)/eV
Sample	—C—C—, C—H	—C—O—	C=O	—O—C=O	—C—O—	—C=O	—O—C=O	—COONa
CMC	282.61	284.15	285.70	290.61	529.08	530.48	533.68	1068.82
PBS-CMC	282.01	283.32	284.87		528.15	529.69	532.57	1068.22
PEG/PBS-CMC	282.23	283.55	286.01	289.85		530.05	532.75	1068.47

Fig.7 POM images(A—C) and XRD spectra(D) of CMC-CMC(A,a), PBS-CMC(B,b) and (PEG/PBS)-CMC(C,c)

Fig.8 SEM images of CMC-CMC(A), PBS-CMC(B) and (PEG/PBS)-CMC(C)

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醚化PBS与CMC液体复合材料的相互作用

Interfacial Interaction Mechanism of Etherified PBS and CMC Liquid Composites^†

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醚化PBS与CMC液体复合材料的相互作用

Interfacial Interaction Mechanism of Etherified PBS and CMC Liquid Composites†

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Interfacial Interaction Mechanism of Etherified PBS and CMC Liquid Composites^†