Citation: LI Ya-Jing, SUN Xiao-Feng, YE Qing, LIU Bai-Chen, WU Yao-Guo. Preparation and Properties of a Novel Hemicellulose-Based Magnetic Hydrogel[J]. Acta Physico-Chimica Sinica, 2014, 30(1): 111-120. doi: 10.3866/PKU.WHXB201310313
新型半纤维素基磁性水凝胶的制备及性能
采用H2O2-Vc氧化还原体系引发半纤维素衍生物,以表面修饰的Fe3O4粒子作为磁性组分,利用接枝共聚方法制备了新型半纤维素基磁性水凝胶. 分别用傅里叶变换红外(FTIR)光谱、X射线光电子能谱(XPS)和扫描电子显微镜(SEM)对水凝胶的结构及形貌进行了表征,利用X射线衍射(XRD)和振动样品磁强计(VSM)对水凝胶的晶型结构及磁性能进行了分析,发现Fe3O4粒子均匀分散在凝胶网络中,半纤维素基磁性水凝胶表现出良好的顺磁性. 考察了丙烯酸/半纤维素比例、Fe3O4粒子含量及交联剂用量对水凝胶溶胀性能的影响,并探讨了该水凝胶的溶胀机理,它在pH 8 缓冲溶液中的溶胀较好符合Fickian 和Schott 动力学模型. 通过SEM和溶胀性能分析表明,随着pH值的升高水凝胶的孔径增大,水凝胶的溶胀率逐渐增大. 制备的水凝胶被用于溶菌酶吸附研究,结果表明磁性凝胶的吸附量大于非磁性水凝胶,水凝胶的吸附行为符合Freundlich 和Temkin 等温模型.
English
Preparation and Properties of a Novel Hemicellulose-Based Magnetic Hydrogel
Hydrogels are important functional materials with many potential applications. Anovel hemicellulosebased magnetic hydrogel was synthesized using a graft copolymer method, with H2O2-Vc as a redox initiator system to initiate the hemicellulosic derivative and surface-modified Fe3O4 particles as the magnetic component. The structures and morphologies of the prepared magnetic hydrogels were investigated using Fourier-transform infrared (FTIR) spectroscopy, X-ray photoelectron spectroscopy (XPS), and scanning electron microscopy (SEM). The crystal structure of the modified Fe3O4 particles and the magnetic behaviors of the hemicellulosebased magnetic hydrogels were analyzed using X-ray diffraction (XRD) and a vibration sample magnetometer (VSM), respectively. The results showed that the Fe3O4 particles were well dispersed in the hydrogel matrix and the prepared hydrogels had paramagnetic properties. The effects of the acrylic acid/hemicellulose ratio and the amounts of Fe3O4 particles and cross-linker on the swelling ratio of the hydrogels were studied, and the swelling mechanism of the hydrogels was explored. The swelling behaviors of the hydrogels were simulated using Fickian and Schott kinetic models in a pH 8 buffer solution. The pore size and swelling ratio of the prepared hydrogels increased with increasing the pH value because the ―COOH groups in the hydrogels were converted to ―COO- at higher pH values. In addition, the prepared hydrogels were used to adsorb lysozyme; the adsorption capacity of the magnetic hydrogel was much higher than that of a non-magnetic hydrogel, and the equilibrium adsorption data fitted the Freundlich and Temkin isotherm models well.
-
Key words:
-
Hemicellulose
- / Fe3O4
- / Hydrogel
- / Swelling kinetics
- / Lysozyme
- / Adsorption
-
-
[1]
(1) Suzuki, D.; Yamakawa, S. Langmuir 2012, 28 (29), 10629.
(1) Suzuki, D.; Yamakawa, S. Langmuir 2012, 28 (29), 10629.
-
[2]
(2) Shang, J.; Shao, Z.; Chen, X. Biomacromolecules 2008, 9 (4),1208.(2) Shang, J.; Shao, Z.; Chen, X. Biomacromolecules 2008, 9 (4),1208.
-
[3]
(3) Xiang, M.; He, C. C.;Wang, H. L. Acta Phys. -Chim. Sin. 2011,27 (5), 1267. [相梅, 贺昌城, 汪辉亮. 物理化学学报, 2011,27 (5), 1267.] doi: 10.3866/PKU.WHXB20110429(3) Xiang, M.; He, C. C.;Wang, H. L. Acta Phys. -Chim. Sin. 2011,27 (5), 1267. [相梅, 贺昌城, 汪辉亮. 物理化学学报, 2011,27 (5), 1267.] doi: 10.3866/PKU.WHXB20110429
-
[4]
(4) Jin, S. P.; Liu, M. Z.; Chen, S. L.; Bian, F. L.; Chen, Y.;Wang,B.; Zhan, F. L.; Liu, S. X. Acta Phys. -Chim. Sin. 2007, 23 (3),438. [金淑萍, 柳明珠, 陈世兰, 卞凤玲, 陈勇, 王斌, 詹发禄, 刘守信. 物理化学学报, 2007, 23 (3), 438.] doi: 10.3866/PKU.WHXB20070330(4) Jin, S. P.; Liu, M. Z.; Chen, S. L.; Bian, F. L.; Chen, Y.;Wang,B.; Zhan, F. L.; Liu, S. X. Acta Phys. -Chim. Sin. 2007, 23 (3),438. [金淑萍, 柳明珠, 陈世兰, 卞凤玲, 陈勇, 王斌, 詹发禄, 刘守信. 物理化学学报, 2007, 23 (3), 438.] doi: 10.3866/PKU.WHXB20070330
-
[5]
(5) Cho, E. C.; Kim, J.W.; Fernandez-Nieves, A.;Weitz, D. A.Nano Letters 2007, 8 (1), 168.(5) Cho, E. C.; Kim, J.W.; Fernandez-Nieves, A.;Weitz, D. A.Nano Letters 2007, 8 (1), 168.
-
[6]
(6) Ozay, O.; Ekici, S.; Baran, Y.; Kubilay, S.; Aktas, N.; Sahiner,N. Desalination 2010, 260 (1-3), 57.(6) Ozay, O.; Ekici, S.; Baran, Y.; Kubilay, S.; Aktas, N.; Sahiner,N. Desalination 2010, 260 (1-3), 57.
-
[7]
(7) Zhai, D.; Liu, B.; Shi, Y.; Pan, L.;Wang, Y.; Li,W.; Zhang, R.;Yu, G. ACS Nano 2013, 7 (4), 3540.(7) Zhai, D.; Liu, B.; Shi, Y.; Pan, L.;Wang, Y.; Li,W.; Zhang, R.;Yu, G. ACS Nano 2013, 7 (4), 3540.
-
[8]
(8) Ramanujan, R. V.; Lao, L. L. Smart Materials and Structures2006, 15 (4), 952. doi: 10.1088/0964-1726/15/4/008(8) Ramanujan, R. V.; Lao, L. L. Smart Materials and Structures2006, 15 (4), 952. doi: 10.1088/0964-1726/15/4/008
-
[9]
(9) Yang, J. Y.; Zhou, X. S.; Fang, J. Carbohydrate Polymers 2011,86 (3), 1113. doi: 10.1016/j.carbpol.2011.05.043(9) Yang, J. Y.; Zhou, X. S.; Fang, J. Carbohydrate Polymers 2011,86 (3), 1113. doi: 10.1016/j.carbpol.2011.05.043
-
[10]
(10) Kim, J. K.; Kim, K. I.; Basavaraja, C.; Rabai, G.; Huh, D. S.J. Phys. Chem. B 2013, 117 (20), 6294.(10) Kim, J. K.; Kim, K. I.; Basavaraja, C.; Rabai, G.; Huh, D. S.J. Phys. Chem. B 2013, 117 (20), 6294.
-
[11]
(11) Peng, C. L.; Shih, Y. H.; Liang, K. S.; Chiang, P. F.; Yeh, C. H.;Tang, I. C.; Yao, C. J.; Lee, S. Y.; Luo, T. Y.; Shieh, M. J. Mol. Pharmaceutics 2013, 10 (5), 1854. doi: 10.1021/mp3006424(11) Peng, C. L.; Shih, Y. H.; Liang, K. S.; Chiang, P. F.; Yeh, C. H.;Tang, I. C.; Yao, C. J.; Lee, S. Y.; Luo, T. Y.; Shieh, M. J. Mol. Pharmaceutics 2013, 10 (5), 1854. doi: 10.1021/mp3006424
-
[12]
(12) Sivakumaran, D.; Maitland, D.; Hoare, T. Biomacromolecules2011, 12 (11), 4112. doi: 10.1021/bm201170h(12) Sivakumaran, D.; Maitland, D.; Hoare, T. Biomacromolecules2011, 12 (11), 4112. doi: 10.1021/bm201170h
-
[13]
(13) Ding, Z.; Salim, A.; Ziaie, B. Anal. Chem. 2010, 82 (8), 3377.doi: 10.1021/ac100579v(13) Ding, Z.; Salim, A.; Ziaie, B. Anal. Chem. 2010, 82 (8), 3377.doi: 10.1021/ac100579v
-
[14]
(14) Pronyk, C.; Mazza, G. Ind. Eng. Chem. Res. 2010, 49 (14),6367. doi: 10.1021/ie1003625(14) Pronyk, C.; Mazza, G. Ind. Eng. Chem. Res. 2010, 49 (14),6367. doi: 10.1021/ie1003625
-
[15]
(15) Lindblad, M. S.; Albertsson, A. C.; Ranucci, E.; Laus, M.;Giani, E. Biomacromolecules 2005, 6 (2), 684. doi: 10.1021/bm049515z(15) Lindblad, M. S.; Albertsson, A. C.; Ranucci, E.; Laus, M.;Giani, E. Biomacromolecules 2005, 6 (2), 684. doi: 10.1021/bm049515z
-
[16]
(16) Sun, X. F.;Wang, H. H.; Jing, Z. X.; Mohanathas, R. Carbohyd. Polym. 2013, 92 (2), 1357. doi: 10.1016/j.carbpol.2012.10.032(16) Sun, X. F.;Wang, H. H.; Jing, Z. X.; Mohanathas, R. Carbohyd. Polym. 2013, 92 (2), 1357. doi: 10.1016/j.carbpol.2012.10.032
-
[17]
(17) Park, J. H.; Bae, Y. H. Biomaterials 2002, 23 (8), 1797. doi: 10.1016/S0142-9612(01)00306-4(17) Park, J. H.; Bae, Y. H. Biomaterials 2002, 23 (8), 1797. doi: 10.1016/S0142-9612(01)00306-4
-
[18]
(18) Zhang, J. H. Journal of Henan Normal University (Natural Science) 2004, 32 (3), 57. [张建合. 河南师范大学学报(自然科学版) 2004, 32 (3), 57.](18) Zhang, J. H. Journal of Henan Normal University (Natural Science) 2004, 32 (3), 57. [张建合. 河南师范大学学报(自然科学版) 2004, 32 (3), 57.]
-
[19]
(19) Liu, T. Y.; Hu, S. H.; Liu, K. H.; Liu, D. M.; Chen, C. Y. Journal of Magnetism and Magnetic Materials 2006, 304 (1), 397.(19) Liu, T. Y.; Hu, S. H.; Liu, K. H.; Liu, D. M.; Chen, C. Y. Journal of Magnetism and Magnetic Materials 2006, 304 (1), 397.
-
[20]
(20) Li, X. M.; Zhang, J. H.; Cui, Y. D.; Liao, L.W.; Jia, Z. Y.; Yin,G. Q.; Guo, P. Journal of Xinyang Normal University (Natural Science) 2007, 20 (2), 174. [黎新明, 张建合, 崔英德, 廖列文, 贾振宇, 尹国强, 郭鹏. 信阳师范学院学报(自然科学版)2007, 20 (2), 174.](20) Li, X. M.; Zhang, J. H.; Cui, Y. D.; Liao, L.W.; Jia, Z. Y.; Yin,G. Q.; Guo, P. Journal of Xinyang Normal University (Natural Science) 2007, 20 (2), 174. [黎新明, 张建合, 崔英德, 廖列文, 贾振宇, 尹国强, 郭鹏. 信阳师范学院学报(自然科学版)2007, 20 (2), 174.]
-
[21]
(21) Sun, X. F.; Sun, R.; Fowler, P.; Baird, M. S. J. Agr. Food Chem.2005, 53 (4), 860. doi: 10.1021/jf040456q(21) Sun, X. F.; Sun, R.; Fowler, P.; Baird, M. S. J. Agr. Food Chem.2005, 53 (4), 860. doi: 10.1021/jf040456q
-
[22]
(22) Sun, X. F.; Sun, R.; Tomkinson, J.; Baird, M. S. Carbohyd. Polym. 2003, 53, 485.(22) Sun, X. F.; Sun, R.; Tomkinson, J.; Baird, M. S. Carbohyd. Polym. 2003, 53, 485.
-
[23]
(23) Ren, J. L.; Sun, R. C.; Liu, C. F.; Cao, Z. N.; Luo,W. Carbohyd. Polym. 2007, 70 (4), 406. doi: 10.1016/j.carbpol.2007.04.022(23) Ren, J. L.; Sun, R. C.; Liu, C. F.; Cao, Z. N.; Luo,W. Carbohyd. Polym. 2007, 70 (4), 406. doi: 10.1016/j.carbpol.2007.04.022
-
[24]
(24) Sun, R. C.; Fang, J. M.; Tomkinson, J. Carbohyd. Polym. 2001,44 (1), 29. doi: 10.1016/S0144-8617(00)00196-X(24) Sun, R. C.; Fang, J. M.; Tomkinson, J. Carbohyd. Polym. 2001,44 (1), 29. doi: 10.1016/S0144-8617(00)00196-X
-
[25]
(25) Xuan, S. H.;Wang, Y. X.; Yu, J. C. Chemistry of Materials2009, 21 (21), 5079. doi: 10.1021/cm901618m(25) Xuan, S. H.;Wang, Y. X.; Yu, J. C. Chemistry of Materials2009, 21 (21), 5079. doi: 10.1021/cm901618m
-
[26]
(26) Takami, S.; Sato, T.; Mousavand, T.; Ohara, S. Materials Letters2007, 61 (26), 4769. doi: 10.1016/j.matlet.2007.03.024(26) Takami, S.; Sato, T.; Mousavand, T.; Ohara, S. Materials Letters2007, 61 (26), 4769. doi: 10.1016/j.matlet.2007.03.024
-
[27]
(27) Sun, X. F.; Li, Y. J. Functional Modification and Preparation ofSuperparamagnetic Fe3O4. In Buiding Materials and Structural Engineering II, Proceedings of the International Conference,Beijing, May 25-26, 2013; Xu, B., Li H. Y., Eds.; AdvancedMaterials Research: Beijing, 2013.(27) Sun, X. F.; Li, Y. J. Functional Modification and Preparation ofSuperparamagnetic Fe3O4. In Buiding Materials and Structural Engineering II, Proceedings of the International Conference,Beijing, May 25-26, 2013; Xu, B., Li H. Y., Eds.; AdvancedMaterials Research: Beijing, 2013.
-
[28]
(28) Frickel, N.; Messing, R.; Gelbrich, T.; Schmidt, A. M. Langmuir2009, 26 (4), 2839.(28) Frickel, N.; Messing, R.; Gelbrich, T.; Schmidt, A. M. Langmuir2009, 26 (4), 2839.
-
[29]
(29) Perez de Vargas-Sansalvador, I. M.; Canfarotta, F.; Piletsky, S.A. Synthesis of Monodisperse Polymeric Nano- andMicroparticles and Their Application in Bioanalysis, InBioanalytical Reviews; Springer: Heidelberg, 2013; pp 1-24.doi: 10.1007/11663_2013_4(29) Perez de Vargas-Sansalvador, I. M.; Canfarotta, F.; Piletsky, S.A. Synthesis of Monodisperse Polymeric Nano- andMicroparticles and Their Application in Bioanalysis, InBioanalytical Reviews; Springer: Heidelberg, 2013; pp 1-24.doi: 10.1007/11663_2013_4
-
[30]
(30) Li, Y.; Leng, T.; Lin, H.; Deng, C.; Xu, X.; Yao, N.; Yang, P.;Zhang, X. J. Proteome. Res. 2007, 6 (11), 4498. doi: 10.1021/pr070167s(30) Li, Y.; Leng, T.; Lin, H.; Deng, C.; Xu, X.; Yao, N.; Yang, P.;Zhang, X. J. Proteome. Res. 2007, 6 (11), 4498. doi: 10.1021/pr070167s
-
[31]
(31) Wang, Z.;Wu, L.; Zhou, J.; Shen, B.; Jiang, Z. RSC Adv. 2013, 3 (10), 3309. doi: 10.1039/c2ra23404a(31) Wang, Z.;Wu, L.; Zhou, J.; Shen, B.; Jiang, Z. RSC Adv. 2013, 3 (10), 3309. doi: 10.1039/c2ra23404a
-
[32]
(32) Wang, Y. P.; Yuan, K.; Pei, X.W. Acta Poly. Sin. 2005, No. 4,584. [王云普, 袁昆, 裴小维. 高分子学报, 2005, No. 4,584.](32) Wang, Y. P.; Yuan, K.; Pei, X.W. Acta Poly. Sin. 2005, No. 4,584. [王云普, 袁昆, 裴小维. 高分子学报, 2005, No. 4,584.]
-
[33]
(33) Ye, Q.; Sun, X. F.; Jing, Z. X.;Wang, G. Z.; Li, Y. J. Modern Chemical Industry 2012, 32 (5), 62. [叶青, 孙晓锋, 景占鑫, 王广征, 李亚婧. 现代化工, 2012, 32 (5), 62.](33) Ye, Q.; Sun, X. F.; Jing, Z. X.;Wang, G. Z.; Li, Y. J. Modern Chemical Industry 2012, 32 (5), 62. [叶青, 孙晓锋, 景占鑫, 王广征, 李亚婧. 现代化工, 2012, 32 (5), 62.]
-
[34]
(34) Chen, Y. F.; Yi, M. Radiat. Phys. Chem. 2001, 61 (1), 65. doi: 10.1016/S0969-806X(00)00374-1(34) Chen, Y. F.; Yi, M. Radiat. Phys. Chem. 2001, 61 (1), 65. doi: 10.1016/S0969-806X(00)00374-1
-
[35]
(35) Dalaran, M.; Emik, S.; Guclu, G.; Iyim, T. B.; Ozgumus, S.Desalination 2011, 279 (1-3), 170. doi: 10.1016/j.desal.2011.06.004(35) Dalaran, M.; Emik, S.; Guclu, G.; Iyim, T. B.; Ozgumus, S.Desalination 2011, 279 (1-3), 170. doi: 10.1016/j.desal.2011.06.004
-
[36]
(36) Katime, I.; Novoa, R.; Zuluaga, F. Eur. Polym. J. 2001, 37 (7),1465. doi: 10.1016/S0014-3057(01)00004-0(36) Katime, I.; Novoa, R.; Zuluaga, F. Eur. Polym. J. 2001, 37 (7),1465. doi: 10.1016/S0014-3057(01)00004-0
-
[37]
(37) Quintana, J. R.; Valderruten, N. E.; Katime, I. Langmuir 1999,15 (14), 4728. doi: 10.1021/la980982+(37) Quintana, J. R.; Valderruten, N. E.; Katime, I. Langmuir 1999,15 (14), 4728. doi: 10.1021/la980982+
-
[38]
(38) Bayram lu, G.; Y?lmaz, M.; Ar?ca, M. Y. Biochem. Eng. J.2003, 13 (1), 35. doi: 10.1016/S1369-703X(02)00098-0(38) Bayram lu, G.; Y?lmaz, M.; Ar?ca, M. Y. Biochem. Eng. J.2003, 13 (1), 35. doi: 10.1016/S1369-703X(02)00098-0
-
[39]
(39) Vijayaraghavan, K.; Padmesh, T. V. N.; Palanivelu, K.; Velan,M. J. Hazard. Mater. 2006, 133 (1-3), 304. doi: 10.1016/j.jhazmat.2005.10.016(39) Vijayaraghavan, K.; Padmesh, T. V. N.; Palanivelu, K.; Velan,M. J. Hazard. Mater. 2006, 133 (1-3), 304. doi: 10.1016/j.jhazmat.2005.10.016
-
[40]
(40) Johnson, R. D.; Arnold, F. H. Biochimica et Biophysica Acta- Protein Structure and Molecular Enzymology 1995, 1247 (2),293. doi: 10.1016/0167-4838(95)00006-G
(40) Johnson, R. D.; Arnold, F. H. Biochimica et Biophysica Acta- Protein Structure and Molecular Enzymology 1995, 1247 (2),293. doi: 10.1016/0167-4838(95)00006-G
-
[1]
-
扫一扫看文章
计量
- PDF下载量: 570
- 文章访问数: 1418
- HTML全文浏览量: 20

下载: