基于G-四联体的聚多肽-DNA水凝胶响应性研究
收稿日期: 2015-04-19
网络出版日期: 2015-06-02
基金资助
项目受国家重点基础研究发展计划(973 program, No. 2013CB932803)和国家自然科学基金(Nos. 91027046, 21121004)资助.
Responsive Polypeptide-DNA Hydrogel Crosslinked by G-quadruplex
Received date: 2015-04-19
Online published: 2015-06-02
Supported by
Project supported by the National Basic Research Program of China (973 program, No. 2013CB932803) and the National Natural Science Foundation of China (Nos. 91027046 & 21121004).
邵昱 , 李闯 , 周旭 , 陈平 , 杨忠强 , 李志波 , 刘冬生 . 基于G-四联体的聚多肽-DNA水凝胶响应性研究[J]. 化学学报, 2015 , 73(8) : 815 -818 . DOI: 10.6023/A15040267
In the past thirty years, DNA molecule has received considerable attention as a promising building material due to its precise base-paring recognition, the programmable sequences, the predictable secondary structures, etc. Based on DNA self-assembly technique, DNA supramolecular hydrogels can be fabricated which are crosslinked networks swollen in an aqueous phase by the supramolecular interaction and also have widely applications in the biomedical field. In this paper, a new type of DNA-based supramolecular hydrogel was prepared by simply mixing two components: Polypeptide-DNA and G-quadruplex. We have successfully synthesized single-stranded DNA (ssDNA) grafted polypeptide via the copper-catalyzed click reaction. By introducing the intermolecular G-quadruplex structure, which is rich in guanine and is capable of forming a four-stranded structure in the presence of potassium, the hydrogel can be formed by DNA hybridization in a fast and in-situ manner and also obtain thermal and ionic responsive gel-sol transition, respectively. In this experiment, we firstly used polyacrylamide gel electrophoresis (PAGE), circular dichroism spectra (CD), UV-Vis spectroscopy to demonstrate the G-quadruplex structure formation, and the assembling process was efficient which are formed the parallel structure and the melting temperature (Tm) was about 43 ℃. Then by the rheological tests, the shear-storage modulus (G') was obviously higher (up to 2.4 kPa) than the shear-loss modulus (G") over the entire time range, and a minimum concentration of 0.5 wt% polypeptide-DNA was required to form a gel-like state, and the mechanical strength of the DNA hydrogels increased with increasing concentration of the DNA building blocks. What’s more, the hydrogels can switch between the gel and the sol state when changing the temperature from 25 to 50 ℃ many times, indicating that the DNA hydrogels respond to thermal in a reversible way. At last, by using the properties of crown ether complexing potassium ion, the DNA hydrogel can obtain the ion responsiveness properties. Due to its designable responsiveness and good biocompatibility, this supramolecular hydrogel would have great potential applications in tissue engineering and 3D bioprinting field.
Key words： DNA; polypeptide; self-assembly; G-quadruplex; hydrogel; responsiveness
[1] Seeman, N. C. Nature 2003, 421, 427.
[2] Moyzis, R. K.; Buckingham, J. M.; Cram, L. S.; Dani, M.; Deaven, L. L.; Jones, M. D.; Meyne, J.; Ratliff, R. L.; Wu, J. R. Proc. Natl. Acad. Sci. U. S. A. 1988, 85, 6622.
[3] Hazel, P.; Huppert, J.; Balasubramanian, S.; Neidle, S. J. Am. Chem. Soc. 2004, 126, 16405.
[4] Huppert, J. L. Chem. Soc. Rev. 2008, 37, 1375.
[5] Balagurumoorthy, P.; Brahmachari, S. K.; Mohanty, D.; Bansal, M.; Sasisekharan, V. Nucleic Acids Res. 1992, 20, 4061.
[6] Wang, W. X.; Liu, H. J.; Wang, Y. D.; Yang, Y.; Liu, D. S. Acta Polymerica Sinica 2008, (1), 55. (王文星, 柳华杰, 王一丁, 杨洋, 刘冬生, 高分子学报, 2008, (1), 55.)
[7] Davis, J. T. Angew. Chem., Int. Ed. 2004, 43, 668.
[8] Ambrus, A.; Chen, D.; Dai, J. X.; Bialis, T.; Jones, R. A.; Yang, D. Z. Nucleic Acids Res. 2006, 34, 2723.
[9] Balagurumoorthy, P.; Brahmachari, S. K. J. Biol. Chem. 1994, 269, 21858.
[10] Li, J. J.; Tan, W. H. Nano Lett. 2002, 2, 315.
[11] Alberti, P.; Mergny, J. L. Proc. Natl. Acad. Sci. U. S. A. 2003, 100, 1569.
[12] Ho, H. A.; Boissinot, M.; Bergeron, M. G.; Corbeil, G.; Dore, K.; Boudreau, D.; Leclerc, M. Angew. Chem., Int. Ed. 2002, 41, 1548.
[13] Ho, H. A.; Leclerc, M. J. Am. Chem. Soc. 2004, 126, 1384.
[14] Wang, L. H.; Liu, X. F.; Hu, X. F.; Song, S. P.; Fan, C. H. Chem. Commun. 2006, 36, 3780.
[15] Hou, X.; Guo, W.; Xia, F.; Nie, F. Q.; Dong, H.; Tian, Y.; Wen, L. P.; Wang, L.; Cao, L. X.; Yang, Y.; Xue, J. M.; Song, Y. L.; Wang, Y. G.; Liu, D. S.; Jiang, L. J. Am. Chem. Soc. 2009, 131, 7800.
[16] Li, T.; Wang, E. K.; Dong, S. J. J. Am. Chem. Soc. 2009, 131, 15082.
[17] Lin, C.; Zhai, W.; Fan, L. Z.; Li, X. H. Acta Chim. Sinica 2014, 72, 709. (蔺超, 翟伟, 范楼珍, 李晓宏, 化学学报, 2014, 72, 709.)
[18] Golub, E.; Freeman, R.; Willner, I. Angew. Chem., Int. Ed. 2011, 50, 11710.
[19] Lu, C. H.; Qi, X. J.; Orbach, R.; Yang, H. H.; Mironi-Harpaz, I.; Seliktar, D.; Willner, I. Nano Lett. 2013, 13, 1298.
[20] Wei, B.; Cheng, I.; Luo, K. Q.; Mi, Y. L. Angew. Chem., Int. Ed. 2008, 47, 331.
[21] Liu, D. S.; Cheng, E. J.; Yang, Z. Q. NPG Asia Mater. 2011, 3, 109.
[22] Liu, J. W. Soft Matter. 2011, 7, 6757.
[23] Um, S. H.; Lee, J. B.; Park, N.; Kwon, S. Y.; Umbach, C. C.; Luo, D. Nat. Mater. 2006, 5, 797.
[24] Park, N.; Um, S. H.; Funabashi, H.; Xu, J. F.; Luo, D. Nat. Mater. 2009, 8, 432.
[25] Cheng, E. J.; Xing, Y. Z.; Chen, P.; Yang, Y.; Sun, Y. W.; Zhou, D. J.; Xu, L. J.; Fan, Q. H.; Liu, D. S. Angew. Chem., Int. Ed. 2009, 48, 7660.
[26] Cheng, E. J.; Li, Y. L.; Yang, Z. Q.; Deng, Z. X.; Liu, D. S. Chem. Commun. 2011, 47, 5545.
[27] Xing, Y. Z.; Cheng, E. J.; Yang, Y.; Chen, P.; Zhang, T.; Sun, Y. W.; Yang, Z. Q.; Liu, D. S. Adv. Mater. 2011, 23, 1117.
[28] Jin, J.; Xi, Y. L.; Liu, X. L.; Zhou, T.; Ma, X. X.; Yang, Z. Q.; Wang, S. T.; Liu, D. S. Adv. Mater. 2013, 25, 4714.
[29] Wu, Y. Z.; Li, C.; Boldt, F.; Wang, Y. R.; Kuan, S. L.; Tran, T. T.; Mikhalevich, V.; Förtsch, C.; Barth, H.; Yang, Z. Q.; Liu, D. S.; Weil, T. Chem. Commun. 2014, 50, 14620.
[30] Li, C.; Chen, P.; Shao, Y.; Zhou, X.; Yang, Z. Q.; Li, Z. B.; Liu, D. S. Small 2015, 11, 1138.
[31] Li, C.; Jones, A. F.; Dun, A. R.; Jin, J.; Chen, P.; Xing, Y. Z.; Yang, Z. Q.; Li, Z. B.; Shu W. M.; Liu, D. S.; Duncan, R. R. Angew. Chem., Int. Ed. 2015, 54, 3957.
[32] Chen, P.; Li, C.; Liu, D. S.; Li, Z. B. Macromolecules 2012, 45, 9579.
[33] Dong, Y. C.; Liu, D. S.; Yang, Z. Q. Methods 2014, 67, 116.
[34] Mironov, V.; Prestwich, G.; Forgacs, G. J. Mater. Chem. 2007, 17, 2054.
[35] Kharkar, P. M.; Kiick, K. L.; Kloxin, A. M. Chem. Soc. Rev. 2013, 42, 7335.
[36] Annabi, N.; Tamayol, A.; Uquillas, J. A.; Akbari, M.; Bertassoni, L. E.; Cha, C.; Camci-Unal, G.; Dokmeci, M. R.; Peppas, N. A.; Khademhosseini, A. Adv. Mater. 2014, 26, 85.
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