Salt Responsive Morphologies of ssDNA-Based Triblock Polyelectrolytes in Semi-Dilute Regime: Effect of Volume Fractions and Polyelectrolyte Length

被引：13
作者：
Li, Nan K. [1 ]
Kuang, Huihui [2 ]
Fuss, William H. [1 ]
Zauscher, Stefan [3 ]
Kokkoli, Efrosini [2 ]
Yingling, Yaroslava G. [1 ]
机构：
[1] North Carolina State Univ, Dept Mat Sci & Engn, 911 Partners Way, Raleigh, NC 27695 USA
[2] Univ Minnesota, Dept Chem Engn & Mat Sci, Minneapolis, MN 55455 USA
[3] Duke Univ, Dept Mech Engn & Mat Sci, 144 Hudson Hall, Durham, NC 27708 USA
来源：
MACROMOLECULAR RAPID COMMUNICATIONS | 2017年 / 38卷 / 20期
基金：
美国国家科学基金会;
关键词：
block copolymers; dissipative particle dynamics simulations; polyelectrolytes; responsive morphology; self-assembly; ssDNA; SOL-GEL TRANSITION; RHEOLOGICAL PROPERTIES; TELECHELIC POLYELECTROLYTE; DIBLOCK COPOLYMER; SELF-ORGANIZATION; AQUEOUS-SOLUTIONS; BLOCK; MICELLES; DYNAMICS; HYDROGELS;
D O I：
10.1002/marc.201700422
中图分类号：
O63 [高分子化学（高聚物）];
学科分类号：
070305 ; 080501 ; 081704 ;
摘要：
A comprehensive study is reported on the effect of salt concentration, polyelectrolyte block length, and polymer concentration on the morphology and structural properties of nanoaggregates self-assembled from BAB single-strand DNA (ssDNA) triblock polynucleotides in which A represents polyelectrolyte blocks and B represents hydrophobic neutral blocks. A morphological phase diagram above the gelation point is developed as a function of solvent ionic strength and polyelectrolyte block length utilizing an implicit solvent ionic strength method for dissipative particle dynamics simulations. As the solvent ionic strength increases, the self-assembled DNA network structures shrinks considerably, leading to a morphological transition from a micellar network to worm-like or hamburger-shape aggregates. This study provides insight into the network morphology and its changes by calculating the aggregation number, number of hydrophobic cores, and percentage of bridge chains in the network. The simulation results are corroborated through cryogenic transmission electron microscopy on the example of the self-assembly of ssDNA triblocks.
引用
收藏
页数：8
相关论文
共 57 条
[1]   DNA multiblock copolymers [J].
Alemdaroglu, Fikri E. ;
Safak, Meryem ;
Wang, Jie ;
Berger, Ruediger ;
Herrmann, Andreas .
CHEMICAL COMMUNICATIONS, 2007, (13) :1358-1359
[2]   Network formation and its consequences for the physical behaviour of associating polymers in solution [J].
Annable, T ;
Buscall, R ;
Ettelaie, R .
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS, 1996, 112 (2-3) :97-116
[3]   Structural analysis of telechelic polymer solution using dissipative particle dynamics simulations [J].
Arai, Noriyoshi .
MOLECULAR SIMULATION, 2015, 41 (10-12) :996-1001
[4]   Morphology of micelles formed by diblock copolymer with a polvelectrolyte block [J].
Borisov, OV ;
Zhulina, EB .
MACROMOLECULES, 2003, 36 (26) :10029-10036
[5]   pH-triggered reversible sol-gel transition in aqueous solutions of amphiphilic gradient copolymers [J].
Borisova, O. ;
Billon, L. ;
Zaremski, M. ;
Grassl, B. ;
Bakaeva, Z. ;
Lapp, A. ;
Stepanek, P. ;
Borisov, O. .
SOFT MATTER, 2011, 7 (22) :10824-10833
[6]   Entangled triblock copolymer gel: Morphological and mechanical properties [J].
Chantawansri, Tanya L. ;
Sirk, Timothy W. ;
Sliozberg, Yelena R. .
JOURNAL OF CHEMICAL PHYSICS, 2013, 138 (02)
[7]   Rheology of associative polymer solutions [J].
Chassenieux, Christophe ;
Nicolai, Taco ;
Benyahia, Lazhar .
CURRENT OPINION IN COLLOID & INTERFACE SCIENCE, 2011, 16 (01) :18-26
[8]   Theory of polyelectrolytes in solutions and at surfaces [J].
Dobrynin, AV ;
Rubinstein, M .
PROGRESS IN POLYMER SCIENCE, 2005, 30 (11) :1049-1118
[9]   Modeling the effects of pH and ionic strength on swelling of polyelectrolyte gels [J].
Drozdov, A. D. ;
Christiansen, J. deClaville .
JOURNAL OF CHEMICAL PHYSICS, 2015, 142 (11)
[10]   Salt effects over the swelling of ionized mesoscopic gels [J].
Fernández-Nieves, A ;
Fernández-Barbero, A ;
de las Nieves, FJ .
JOURNAL OF CHEMICAL PHYSICS, 2001, 115 (16) :7644-7649
123456