不同直径改性PAN纳米纤维膜与Fe<sup>3+</sup>的配位反应及其配合物对有机染料降解的催化性能

引用本文: 赵雪婷, 董永春, 程博闻, 康卫民. 不同直径改性PAN纳米纤维膜与Fe³⁺的配位反应及其配合物对有机染料降解的催化性能[J]. 物理化学学报, 2013, 29(12): 2513-2522. doi: 10.3866/PKU.WHXB201310233 shu

Citation: ZHAO Xue-Ting, DONG Yong-Chun, CHENG Bo-Wen, KANG Wei-Min. Coordination Kinetics of Fe³⁺ with Membranes Based on Modified PAN Nanofibers with Different Diameters, and Catalytic Effect of Their Complexes on Decomposition of Organic Dye[J]. Acta Physico-Chimica Sinica, 2013, 29(12): 2513-2522. doi: 10.3866/PKU.WHXB201310233 shu

不同直径改性PAN纳米纤维膜与Fe³⁺的配位反应及其配合物对有机染料降解的催化性能

基金项目:
天津市应用基础与前沿技术重点研究计划(11JCZDJC24600, 11ZCKFGX03200) (11JCZDJC24600, 11ZCKFGX03200)

国家自然科学基金(2020773093, 51102178)资助项目 (2020773093, 51102178)

摘要:

使用静电纺丝技术和偕胺肟反应制备了三种不同直径的改性聚丙烯腈(PAN)纳米纤维膜, 然后将它们作为配体分别与Fe³⁺进行配位反应制备改性PAN纳米纤维膜铁配合物, 重点研究了三种改性PAN纳米纤维膜与Fe³⁺配位反应的动力学特性及其温度和Fe³⁺初始浓度的影响. 最后将其作为非均相Fenton 反应催化剂应用于染料降解反应中, 考察了改性PAN纳米纤维膜直径对其催化活性的影响. 结果表明, 在所涉及的温度和浓度范围内, 改性PAN纳米纤维膜与Fe³⁺之间配位反应不仅符合Langmuir 和Freundlich 吸附等温式, 而且可理想地使用Lagergren 准二级动力学方程进行描述, 反应速率常数随着Fe³⁺初始浓度的增加而逐渐降低. 在相同反应条件下, 较小直径的纤维膜更容易与Fe³⁺发生配位反应, 且反应速率常数和Fe³⁺配合量均随着纤维直径的降低而增大. 不同直径改性PAN纳米纤维膜铁配合物在暗态条件下对染料的氧化降解反应表现出很好的催化活性, 且在辐射光下其催化活性得到加强. 改性PAN纳米纤维膜铁配合物的催化作用受到纤维直径的显著影响,由中等直径纳米纤维构成的配合物表现出最高的催化活性.

关键词:

English

Coordination Kinetics of Fe³⁺ with Membranes Based on Modified PAN Nanofibers with Different Diameters, and Catalytic Effect of Their Complexes on Decomposition of Organic Dye

1.
1 Division of Textile Chemistry & Ecology, School of Textiles, Tianjin Polytechnic University, Tianjin 300387, P. R. China;
2 Key Laboratory of Advanced Textile Composites, Ministry of Education, Tianjin Polytechnic University, Tianjin 300387, P. R. China
Received Date: 12 August 2013
Available Online: 28 November 2013
Fund Project:
天津市应用基础与前沿技术重点研究计划(11JCZDJC24600, 11ZCKFGX03200)

国家自然科学基金(2020773093, 51102178)资助项目

Abstract:

Membranes produced from modified polyacrylonitrile (PAN) nanofibers with different diameters were prepared by electrospinning and amidoximation. They were then used as ligands to coordinate with Fe³⁺ for preparing modified PAN nano-fibrous membrane Fe complexes. The coordination kinetics of three modified PAN nano-fibrous membranes with Fe³⁺ were studied, and the effects of temperature and the Fe³⁺ initial concentration on the coordination kinetics were also examined. Finally, the catalytic activities of the three modified PAN nano- fibrous membrane Fe complexes were evaluated as heterogeneous Fenton catalysts in the degradation of an organic dye. The effect of fiber diameter on the catalytic activity of the complexes was investigated. The results indicated that within the observed temperature and concentration ranges, the equilibrium data for the coordination of Fe³⁺ with the modified PAN nano-fibrous membranes correlated with the Langmuir and Freundlich isotherm equations, but the coordination kinetics showed better agreement with the Lagergren second-order equation. Modified PAN nanofibrous membranes with small diameters showed higher Fe- coordinating capacities and reaction rate constants under the same conditions, indicating that they reacted with Fe³⁺ more easily than the others did. Better catalytic activities for dye degradation were found for the three modified PAN nanofibrous membrane Fe complexes in the dark, and these were further improved by light irradiation. The catalytic activities of the complexes were significantly affected by the nanofiber diameter. The complex prepared using a modified PAN nanofibrous membrane with fibers of an appropriate diameter exhibited the best catalytic activity.

Key words:

1. [1]
  
  (1) Janiak, C. Chem. Soc. Dalton Trans. 2003, 14 (6), 2781.
  (1) Janiak, C. Chem. Soc. Dalton Trans. 2003, 14 (6), 2781.
2. [2]
  (2) Vassilev, K.; Turmanova, S. Polym. Bull. 2008, 60 (2), 243.(2) Vassilev, K.; Turmanova, S. Polym. Bull. 2008, 60 (2), 243.
3. [3]
  (3) Wu, S. H.; Xie, Q. X.; Zhu, C. Y.; Huang,W. P.; Yang, X. L.;Wu,W. Y. Polym. Mater. Sci. Eng. 2000, 16 (3), 1. [吴世华,解勤兴, 朱常英, 黄唯平, 杨秀檩, 吴文艳. 高分子材料科学与工程, 2000, 16 (3), 1.](3) Wu, S. H.; Xie, Q. X.; Zhu, C. Y.; Huang,W. P.; Yang, X. L.;Wu,W. Y. Polym. Mater. Sci. Eng. 2000, 16 (3), 1. [吴世华,解勤兴, 朱常英, 黄唯平, 杨秀檩, 吴文艳. 高分子材料科学与工程, 2000, 16 (3), 1.]
4. [4]
  (4) Espenson, J. H. Chemical Kinetics and Reaction Mechanisms,2nd ed.; McGraw-Hill Inc: New York, 1995; pp 1-3.(4) Espenson, J. H. Chemical Kinetics and Reaction Mechanisms,2nd ed.; McGraw-Hill Inc: New York, 1995; pp 1-3.
5. [5]
  (5) Xu, Y. Chemical Reaction Kinetics; Chemical Industry Press:Beijing, 2005; pp 151-153. [许越. 化学反应动力学. 北京:化学工业出版社, 2005: 151-153.](5) Xu, Y. Chemical Reaction Kinetics; Chemical Industry Press:Beijing, 2005; pp 151-153. [许越. 化学反应动力学. 北京:化学工业出版社, 2005: 151-153.]
6. [6]
  (6) Zhang, D. Y.;Wu, Z. C.; Zhou, K.; Chen, P. G. Polym. Mater. Sci. Eng. 2008, 24 (6), 38. [张宇东, 吴之传, 周凯, 陈培根.高分子材料科学与工程, 2008, 24 (6), 38.](6) Zhang, D. Y.;Wu, Z. C.; Zhou, K.; Chen, P. G. Polym. Mater. Sci. Eng. 2008, 24 (6), 38. [张宇东, 吴之传, 周凯, 陈培根.高分子材料科学与工程, 2008, 24 (6), 38.]
7. [7]
  (7) Dong, Y. C.;Wu, J. N.; Sun, S. T.; Zheng, X.; Han, Z. B.; Liu,C. Y. Journal of Sichuan University (Engineering Science Edition) 2011, 43 (1), 173. [董永春, 武金娜, 孙苏婷, 郑戌,韩振邦, 刘春燕. 四川大学学报(工程科学版), 2011, 43 (1),173.](7) Dong, Y. C.;Wu, J. N.; Sun, S. T.; Zheng, X.; Han, Z. B.; Liu,C. Y. Journal of Sichuan University (Engineering Science Edition) 2011, 43 (1), 173. [董永春, 武金娜, 孙苏婷, 郑戌,韩振邦, 刘春燕. 四川大学学报(工程科学版), 2011, 43 (1),173.]
8. [8]
  (8) Han, Z. B.; Dong, Y. C.; Liu, C. Y. Chem. J. Chin. Univ. 2010,31 (5), 986. [韩振邦, 董永春, 刘春燕. 高等学校化学学报,2010, 31 (5), 986.](8) Han, Z. B.; Dong, Y. C.; Liu, C. Y. Chem. J. Chin. Univ. 2010,31 (5), 986. [韩振邦, 董永春, 刘春燕. 高等学校化学学报,2010, 31 (5), 986.]
9. [9]
  (9) Bagheri, B.; Abdouss, M.; Aslzadeh, M. M.; Shoushtari, A. M.Iran. Polym. J. 2010, 19 (12), 911.(9) Bagheri, B.; Abdouss, M.; Aslzadeh, M. M.; Shoushtari, A. M.Iran. Polym. J. 2010, 19 (12), 911.
10. [10]
  (10) Feng, Q.;Wang, Q. Q.; Tang, B.;Wei, A. F.;Wang, X. Q.;Wei,Q. F.; Huang, F. L.; Cai, Y. B.; Hou, D. Y.; Bi, S. M. Polym. Int.2013, 62 (2), 251. doi: 10.1002/pi.2013.62.issue-2(10) Feng, Q.;Wang, Q. Q.; Tang, B.;Wei, A. F.;Wang, X. Q.;Wei,Q. F.; Huang, F. L.; Cai, Y. B.; Hou, D. Y.; Bi, S. M. Polym. Int.2013, 62 (2), 251. doi: 10.1002/pi.2013.62.issue-2
11. [11]
  (11) Kampalanonwat, P.; Supaphol, P. ACS Appl. Mater. Inter. 2010,2 (2), 3619.(11) Kampalanonwat, P.; Supaphol, P. ACS Appl. Mater. Inter. 2010,2 (2), 3619.
12. [12]
  (12) Ishtchenko, V. V.; Huddersman, K. D.; Vitkovskaya, R. F. Appl. Catal. A. 2003, 242 (1), 123. doi: 10.1016/S0926-860X(02)00511-2(12) Ishtchenko, V. V.; Huddersman, K. D.; Vitkovskaya, R. F. Appl. Catal. A. 2003, 242 (1), 123. doi: 10.1016/S0926-860X(02)00511-2
13. [13]
  (13) Ishtchenko, V. V.; Huddersman, K. D.; Vitkovskaya, R. F. Appl. Catal. A 2003, 242 (2), 221. doi: 10.1016/S0926-860X(02)00512-4(13) Ishtchenko, V. V.; Huddersman, K. D.; Vitkovskaya, R. F. Appl. Catal. A 2003, 242 (2), 221. doi: 10.1016/S0926-860X(02)00512-4
14. [14]
  (14) Vitkovskaya, R. F.; Rumynskaya, I. G.; Romanova, E. P.;Tereshchenko, L. Y. Fiber Chem. 2003, 35 (3), 202. doi: 10.1023/A:1026109923284(14) Vitkovskaya, R. F.; Rumynskaya, I. G.; Romanova, E. P.;Tereshchenko, L. Y. Fiber Chem. 2003, 35 (3), 202. doi: 10.1023/A:1026109923284
15. [15]
  (15) Dong, Y. C.; Du, F.; Han, Z. B. Acta Phys. -Chim. Sin. 2008, 24 (11), 2114. [董永春, 杜芳, 韩振邦. 物理化学学报, 2008,24 (11), 2114.] doi: 10.3866/PKU.WHXB20081130(15) Dong, Y. C.; Du, F.; Han, Z. B. Acta Phys. -Chim. Sin. 2008, 24 (11), 2114. [董永春, 杜芳, 韩振邦. 物理化学学报, 2008,24 (11), 2114.] doi: 10.3866/PKU.WHXB20081130
16. [16]
  (16) Dong, Y. C.; Han, Z. B.; Liu, C. Y.; Du, F. Sci. Total. Environ.2010, 408 (10), 2245. doi: 10.1016/j.scitotenv.2010.01.020(16) Dong, Y. C.; Han, Z. B.; Liu, C. Y.; Du, F. Sci. Total. Environ.2010, 408 (10), 2245. doi: 10.1016/j.scitotenv.2010.01.020
17. [17]
  (17) Han, Z. B.; Dong, Y. C.; Dong, S. M. J. Hazard. Mater. 2011,189 (1-2), 241. doi: 10.1016/j.jhazmat.2011.02.026(17) Han, Z. B.; Dong, Y. C.; Dong, S. M. J. Hazard. Mater. 2011,189 (1-2), 241. doi: 10.1016/j.jhazmat.2011.02.026
18. [18]
  (18) Dong, Y. C.; Dong,W. J.; Han, Z. B. Catal. Today 2011, 175 (1),299. doi: 10.1016/j.cattod.2011.04.026(18) Dong, Y. C.; Dong,W. J.; Han, Z. B. Catal. Today 2011, 175 (1),299. doi: 10.1016/j.cattod.2011.04.026
19. [19]
  (19) Yang, X.W.; Luo, Y. Y. Textbook of Chemical Products: Dyestuffs; Chemical Industry Press: Beijing, 2005; pp 156-541.[杨新玮, 罗钰言. 化工产品手册: 染料. 北京: 化学工业出版社, 2005: 156-541.](19) Yang, X.W.; Luo, Y. Y. Textbook of Chemical Products: Dyestuffs; Chemical Industry Press: Beijing, 2005; pp 156-541.[杨新玮, 罗钰言. 化工产品手册: 染料. 北京: 化学工业出版社, 2005: 156-541.]
20. [20]
  (20) Li, S. F.; Chen, J. P.;Wu,W. T. J. Mol. Catal. B 2007, 47 (3-4),117. doi: 10.1016/j.molcatb.2007.04.010(20) Li, S. F.; Chen, J. P.;Wu,W. T. J. Mol. Catal. B 2007, 47 (3-4),117. doi: 10.1016/j.molcatb.2007.04.010
21. [21]
  (21) Feng, Q.;Wang, X. Q.;Wei, Q. F.; Hou, D. Y.;Wei, L.; Liu, X.H.;Wang, Z. Q. Fiber. Polym. 2011, 12 (8), 1025. doi: 10.1007/s12221-011-1025-0(21) Feng, Q.;Wang, X. Q.;Wei, Q. F.; Hou, D. Y.;Wei, L.; Liu, X.H.;Wang, Z. Q. Fiber. Polym. 2011, 12 (8), 1025. doi: 10.1007/s12221-011-1025-0
22. [22]
  (22) Neghlani, P. K.; Rafizadeh, M.; Taromi, F. A. J. Hazard. Mater.2011, 186 (1), 182. doi: 10.1016/j.jhazmat.2010.10.121(22) Neghlani, P. K.; Rafizadeh, M.; Taromi, F. A. J. Hazard. Mater.2011, 186 (1), 182. doi: 10.1016/j.jhazmat.2010.10.121
23. [23]
  (23) Lee, K. H.; Kim, H. Y.; Khil, M. S.; Ra, Y. M.; Lee, D. R.Polym. 2003, 44 (4), 1287. doi: 10.1016/S0032-3861(02)00820-0(23) Lee, K. H.; Kim, H. Y.; Khil, M. S.; Ra, Y. M.; Lee, D. R.Polym. 2003, 44 (4), 1287. doi: 10.1016/S0032-3861(02)00820-0
24. [24]
  (24) Vassilev, K.; Turmanova, S. Polym. Bull. 2005, 1 (5), 575.(24) Vassilev, K.; Turmanova, S. Polym. Bull. 2005, 1 (5), 575.
25. [25]
  (25) Qin, X. H.;Wang, X.W.; Hu, Z. M.; Liu, Z. F.;Wang, S. Y.Journal of Donghua University (Natural Science) 2005, 31 (6),16. [覃小红, 王新威, 胡祖明, 刘兆峰, 王善元. 东华大学学报(自然科学版), 2005, 31 (6), 16.](25) Qin, X. H.;Wang, X.W.; Hu, Z. M.; Liu, Z. F.;Wang, S. Y.Journal of Donghua University (Natural Science) 2005, 31 (6),16. [覃小红, 王新威, 胡祖明, 刘兆峰, 王善元. 东华大学学报(自然科学版), 2005, 31 (6), 16.]
26. [26]
  (26) Yordem, O. S.; Papila, M.; Menceloglu, Y. Z. Mater. Des. 2008,29 (1), 34. doi: 10.1016/j.matdes.2006.12.013(26) Yordem, O. S.; Papila, M.; Menceloglu, Y. Z. Mater. Des. 2008,29 (1), 34. doi: 10.1016/j.matdes.2006.12.013
27. [27]
  (27) Wang, N.; Burugapalli, K.; Song,W.; Hall, J.; Moussy, F.;Zheng, Y. D.; Ma, Y. X.;Wu, Z. T.; Li, K. J. Membr. Sci. 2013,427 (10), 207.(27) Wang, N.; Burugapalli, K.; Song,W.; Hall, J.; Moussy, F.;Zheng, Y. D.; Ma, Y. X.;Wu, Z. T.; Li, K. J. Membr. Sci. 2013,427 (10), 207.
28. [28]
  (28) Chen, X.; Chen, N. L. Journal of DongHua University (Natural Science) 2009, 35 (1), 30. [陈霄, 陈南梁. 东华大学学报(自然科学版), 2009, 35 (1), 30.]
  (28) Chen, X.; Chen, N. L. Journal of DongHua University (Natural Science) 2009, 35 (1), 30. [陈霄, 陈南梁. 东华大学学报(自然科学版), 2009, 35 (1), 30.]

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

不同直径改性PAN纳米纤维膜与Fe³⁺的配位反应及其配合物对有机染料降解的催化性能

English

Coordination Kinetics of Fe³⁺ with Membranes Based on Modified PAN Nanofibers with Different Diameters, and Catalytic Effect of Their Complexes on Decomposition of Organic Dye

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

不同直径改性PAN纳米纤维膜与Fe3+的配位反应及其配合物对有机染料降解的催化性能

English

Coordination Kinetics of Fe3+ with Membranes Based on Modified PAN Nanofibers with Different Diameters, and Catalytic Effect of Their Complexes on Decomposition of Organic Dye

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

不同直径改性PAN纳米纤维膜与Fe³⁺的配位反应及其配合物对有机染料降解的催化性能

Coordination Kinetics of Fe³⁺ with Membranes Based on Modified PAN Nanofibers with Different Diameters, and Catalytic Effect of Their Complexes on Decomposition of Organic Dye

CCS Chemistry：颜徐州、鲍哲南：你的皮肤可能是一片SPMs