单根DNA短链构筑pH响应超分子水凝胶

史杰中; 贾昊旸; 刘冬生

doi:10.11777/j.issn1000-3304.2017.16278

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单根DNA短链构筑pH响应超分子水凝胶

研究论文 | 更新时间：2021-03-12

- 单根DNA短链构筑pH响应超分子水凝胶
- pH-Responsive Supramolecular Hydrogel Based on One Short Strand DNA
- 高分子学报 2017年第1期页码：135-142
- 作者机构：
  
  有机光电子与分子工程教育部重点实验室清华大学化学系北京 100084
- 作者简介：
  
  E-mail: liudongsheng@tsinghua.edu.cn Dong-sheng Liu, E-mail: liudongsheng@tsinghua.edu.cn
- 基金信息：
  
  国家重点基础研究发展计划(973计划，项目号2013CB932803);国家自然科学基金资助项目(基金号91427302，21534007)
- DOI：10.11777/j.issn1000-3304.2017.16278
  中图分类号：
- 纸质出版日期：2017-1，
  
  收稿日期：2016-9-11，
  
  修回日期：2016-10-10，
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史杰中, 贾昊旸, 刘冬生. 单根DNA短链构筑pH响应超分子水凝胶[J]. 高分子学报, 2017,(1):135-142.

Shi Jie-zhong, Jia Hao-yang, Liu Dong-sheng. pH-Responsive Supramolecular Hydrogel Based on One Short Strand DNA[J]. Acta Polymerica Sinica, 2017,(1):135-142.
史杰中, 贾昊旸, 刘冬生. 单根DNA短链构筑pH响应超分子水凝胶[J]. 高分子学报, 2017,(1):135-142. DOI： 10.11777/j.issn1000-3304.2017.16278.

Shi Jie-zhong, Jia Hao-yang, Liu Dong-sheng. pH-Responsive Supramolecular Hydrogel Based on One Short Strand DNA[J]. Acta Polymerica Sinica, 2017,(1):135-142. DOI： 10.11777/j.issn1000-3304.2017.16278.

摘要

设计合成了一条包含两段自互补序列和一段富含胞嘧啶（C）序列的DNA单链.在碱性条件下，两段自互补序列可通过分子间自组装形成一维DNA纳米线，调节pH至酸性条件后，胞嘧啶序列通过形成双分子i-motif结构将纳米线交联，从而形成DNA水凝胶.当加入酸或碱调节体系的pH时，水凝胶的力学强度会发生变化.在pH为5.3时，水凝胶力学强度达到最大，增大或减小pH都会使水凝胶强度降低.同时，改变DNA单链浓度也能够调节水凝胶的力学强度.此凝胶制备过程原料合成简便，无需涉及不同DNA链定量配比的问题，大大简化了实验操作；另外i-motif结构在形成与解离两态之间的转换非常迅速，在几秒钟之内便可完成，也赋予该凝胶快速pH响应的特性.

Abstract

We design a single strand DNA containing two self-complementary sequences and a half i-motif structure. The two self-complementary sequences can self-assemble to form DNA nanowires. Then

the hydrogel can be formed by crosslinking the half i-motif structures under acid condition. The single strand DNA is diluted to 3 mmol/L in 1×TAE buffer (pH=7.5) containing 12.5 mmol/L MgCl

. The system is heated to 95℃ for 5 min and slowly annealed to room temperature. The pH is adjusted to 5.3 to form the DNA hydrogel. The DNA oligomers and assemblies are characterised by PAGE. Then circular dichroism is used to characterize the structure of the duplex and the i-motif. Rheological characterization is used to evaluate the mechanical properties and thermal stability of the hydrogels at different concentration and pH. By changing concentration of the single strand DNA

one can adjust the mechanical strength and thermal stability of the hydrogels. Besides

the mechanical strength can be tuned by changing pH values. When pH value is 5.3

the storage modulus (

') of the hydrogel is 243.9 Pa. When the pH value is increased to 6.0

the

' is lowered to 225.7 Pa because the stability of the i-motif structure decreases as the pH value increases. However

when pH value is changed to 5

the

' is greatly reduced to 57.4 Pa

which is caused by the instability of the duplex structure under acidic condition. In this procedure

the single strand DNA is very easy to be synthesized and the ratio of DNA strands has not to be controlled. Thus

the experimental steps are greatly simplified. Also

the transition of the i-motif between hydrogel formation and its dissociation is reversible and fast (within several seconds)

which makes the DNA hydrogel fast pH responsive. Due to these characteristics

this DNA hydrogel holds great potential in bio-sensing

drug delivery and 3D printing.

关键词

DNA水凝胶自互补i-motif结构pH响应

Keywords

DNA hydrogelSelf-complementationI-motif structurepH responsiveness

references

N C Seeman . . Nature , 2003 . 421 427 - 431 . DOI:10.1038/nature01406http://doi.org/10.1038/nature01406.

N C Seeman . . J Theor Biol , 1982 . 99 237 - 247 . DOI:10.1016/0022-5193(82)90002-9http://doi.org/10.1016/0022-5193(82)90002-9.

P W K Rthemund . . Nature , 2006 . 440 297 - 302 . DOI:10.1038/nature04586http://doi.org/10.1038/nature04586.

H Yan , S H Park , G Finkelstein , J H Reif , T H Labean . . Science , 2003 . 301 1882 - 1884 . DOI:10.1126/science.1089389http://doi.org/10.1126/science.1089389.

Y He , T Ye , M Su , C Zhang , A E Ribbe , W Jiang , C D Mao . . Nature , 2008 . 452 198 - 201 . DOI:10.1038/nature06597http://doi.org/10.1038/nature06597.

Z Y Zhao , C Chen , Y C Dong , Z Q Yang , Q H Fan , D S Liu . . Angew Chem Int Ed , 2014 . 53 13468 - 13470 . DOI:10.1002/anie.201408231http://doi.org/10.1002/anie.201408231.

Y C Dong , Y W Sun , L Y Wang , D M Wang , T Zhou , Z Q Yang , Z Chen , W B Wang , Q H Fan , D S Liu . . Angew Chem Int Ed , 2014 . 53 2607 - 2610 . DOI:10.1002/anie.201310715http://doi.org/10.1002/anie.201310715.

D S Liu , E J Cheng , Z Q Yang . . NPG Asia Mater , 2011 . 3 109 - 114 . DOI:10.1038/asiamat.2011.147http://doi.org/10.1038/asiamat.2011.147.

Y C Dong , Z Q Yang , D S Liu . . Acc Chem Res , 2014 . 47 1853 - 1860 . DOI:10.1021/ar500073ahttp://doi.org/10.1021/ar500073a.

Yu Shao , Chuang Li , Xu Zhou , Fen Wu , Haoyang Jia , Yijie Wang , Dongsheng Liu . . Polymer Bulletin , 2015 . ( 10 ): 100 .

邵昱 , 李闯 , 周旭 , 吴芬 , 贾昊旸 , 王一杰 , 刘冬生 . . 高分子通报 , 2015 . ( 10 ): 100 .

Y H Roh , R C H Ruiz , S M Peng , J B Lee , D Luo . . Chem Soc Rev , 2011 . 40 5730 - 5744 . DOI:10.1039/c1cs15162bhttp://doi.org/10.1039/c1cs15162b.

J D Watson , F H C Crick . . Nature , 1953 . 171 737 - 738 . DOI:10.1038/171737a0http://doi.org/10.1038/171737a0.

K Gehring , J L Leroy , M Gueron . . Nature , 1993 . 363 561 - 565 . DOI:10.1038/363561a0http://doi.org/10.1038/363561a0.

J L Leroy , K Gehring , A Kettani , M Gueron . . Biochemistry , 1993 . 32 6019 - 6031 . DOI:10.1021/bi00074a013http://doi.org/10.1021/bi00074a013.

C Chen , M Li , Y Z Xing , Y M Li , C C Joedecke , J Jin , Z Q Yang , D S Liu . . Langmuir , 2012 . 28 17743 - 17748 . DOI:10.1021/la303851ahttp://doi.org/10.1021/la303851a.

D S Liu , S Balasubramanian . . Angew Chem Int Ed , 2003 . 42 5734 - 5736 . DOI:10.1002/(ISSN)1521-3773http://doi.org/10.1002/(ISSN)1521-3773.

W M Shu , D S Liu , M Watari , C K Riener , T Strunz , M E Welland , S Balasubramanian , R A Mckendry . . J Am Chem Soc , 2005 . 127 17054 - 17060 . DOI:10.1021/ja0554514http://doi.org/10.1021/ja0554514.

D S Liu , A Bruckbauer , C Abell , S Balasubramanian , D J Kang , Klenerman , D , D J Zhou . . J Am Chem Soc , 2006 . 128 2067 - 2071 . DOI:10.1021/ja0568300http://doi.org/10.1021/ja0568300.

S T Wang , H J Liu , D S Liu , X Y Ma , X H Fang , L Jiang . . Angew Chem Int Ed , 2007 . 46 3915 - 3917 . DOI:10.1002/(ISSN)1521-3773http://doi.org/10.1002/(ISSN)1521-3773.

X Hou , W Guo , F Xia , F Q Nie , H Dong , Y Tian , L P Wen , L Wang , L X Cao , Y Yang , J M Xue , Y L Song , Y G Wang , D S Liu , L Jiang . . J Am Chem Soc , 2009 . 131 7800 - 7805 . DOI:10.1021/ja901574chttp://doi.org/10.1021/ja901574c.

E J Cheng , Y Z Xing , P Chen , Y Yang , Y W Sun , D J Zhou , L J Xu , Q H Fan , D S Liu . . Angew Chem Int Ed , 2009 . 48 7660 - 7663 . DOI:10.1002/anie.v48:41http://doi.org/10.1002/anie.v48:41.

Y Z Xing , E J Cheng , Y Yang , P Chen , T Zhang , Y W Sun , Z Q Yang , D S Liu . . Adv Mater , 2011 . 23 1117 - 1121 . DOI:10.1002/adma.201003343http://doi.org/10.1002/adma.201003343.

C Li , A F Jones , A R Dun , J Jin , P Chen , Y Z Xing , Z Q Yang , Z B Li , W M Shu , D S Liu , R R Duncan . . Angew Chem Int Ed , 2015 . 54 3957 - 3961 . DOI:10.1002/anie.201411383http://doi.org/10.1002/anie.201411383.

H L Jiang , V Pan , S Vivek , E R Weeks , Y G Ke . . ChemBioChem , 2016 . 17 1156 - 1162 . DOI:10.1002/cbic.201500686http://doi.org/10.1002/cbic.201500686.

S J Horvath , J R Firca , T Hunkapiller , M W Hunkapiller , L Hood . . Method Enzymol , 154 ( 1987 ): 314 - 326.

N Berova , K Nakanishi , R W Woody . Circular Dichroism:Principles and Application , : 2nd ed.. New York Wiley , 2000 . 707 - 727.

H H Winter , F Chambon . . J Rheol , 1986 . 30 367 - 382 . DOI:10.1122/1.549853http://doi.org/10.1122/1.549853.

S Fernández , R Eritja , A Aviñó , J Jaumot , R Gargallo . . Int J Biol Macromol , 2011 . 49 729 - 736 . DOI:10.1016/j.ijbiomac.2011.07.004http://doi.org/10.1016/j.ijbiomac.2011.07.004.

D S Liu , S Balasubramanian . . Angew Chem Int Ed , 2003 . 42 5734 - 5736 . DOI:10.1002/(ISSN)1521-3773http://doi.org/10.1002/(ISSN)1521-3773.

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