Flow chemistry controls self-assembly and cargo in Belousov-Zhabotinsky driven polymerization-induced self-assembly

被引:21
作者
Hou, Liman [1 ,2 ]
Duenas-Diez, Marta [1 ,2 ,3 ]
Srivastava, Rohit [1 ,2 ]
Perez-Mercader, Juan [1 ,2 ,4 ]
机构
[1] Harvard Univ, Dept Earth & Planetary Sci, 20 Oxford St, Cambridge, MA 02138 USA
[2] Harvard Univ, Origins Life Initiat, 20 Oxford St, Cambridge, MA 02138 USA
[3] Repsol Technol Lab, C Agustin Betancourt S-N, Madrid 28935, Spain
[4] Santa Fe Inst, Santa Fe, NM 87501 USA
关键词
STIMULI-RESPONSIVE POLYMERSOMES; COPOLYMER NANO-OBJECTS; OSCILLATIONS; VESICLES; PHOTOPOLYMERIZATION; BATCH; PISA;
D O I
10.1038/s42004-019-0241-1
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Amphiphilic block-copolymer vesicles are increasingly used for medical and chemical applications, and a novel method for their transient self-assembly orchestrated by periodically generated radicals during the oscillatory Belousov-Zhabotinsky (BZ) reaction was recently developed. Here we report how combining this one pot polymerization-induced self-assembly (PISA) method with a continuously stirred tank reactor (CSTR) strategy allows for continuous and reproducible control of both the PISA process and the chemical features (e.g. the radical generation and oscillation) of the entrapped cargo. By appropriately tuning the residence time (tau), target degree of polymerization (DP) and the BZ reactants, intermediate self-assembly structures are also obtained (micelles, worms and nano-sized vesicles). Simultaneously, the chemical properties of the cargo at encapsulation are known and tunable, a key advantage over batch operation. Finally, we also show that BZ-driven polymerization in CSTR additionally supports more non-periodic dynamics such as bursting.
引用
收藏
页数:8
相关论文
共 52 条
[1]   Emergent Properties of Giant Vesicles Formed by a Polymerization-Induced Self-Assembly (PISA) Reaction [J].
Albertsen, Anders N. ;
Szymanski, Jan K. ;
Perez-Mercader, Juan .
SCIENTIFIC REPORTS, 2017, 7
[2]  
[Anonymous], 1993, CHEM CHAOS
[3]   Vesicles and liposomes:: A self-assembly principle beyond lipids [J].
Antonietti, M ;
Förster, S .
ADVANCED MATERIALS, 2003, 15 (16) :1323-1333
[4]  
Ball P, 1999, THE SELF MADE TAPEST
[5]   Flow-distributed oscillation patterns in the Oregonator model [J].
Bamforth, JR ;
Merkin, JH ;
Scott, SK ;
Tóth, R ;
Gáspár, V .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2001, 3 (08) :1435-1438
[6]   Autonomous Ex Novo Chemical Assembly with Blebbing and Division of Functional Polymer Vesicles from a "Homogeneous Mixture" [J].
Bastakoti, Bishnu Prasad ;
Perez-Mercader, Juan .
ADVANCED MATERIALS, 2017, 29 (43)
[7]   Facile One-Pot Synthesis of Functional Giant Polymeric Vesicles Controlled by Oscillatory Chemistry [J].
Bastakoti B.P. ;
Perez-Mercader J. .
Angewandte Chemie - International Edition, 2017, 56 (40) :12086-12091
[8]  
Belousov B.P., 1958, Sb. Ref. Radiat. Med, P145
[9]   Artificial Cells: Synthetic Compartments with Life-like Functionality and Adaptivity [J].
Buddingh, Bastiaan C. ;
van Hest, Jan C. M. .
ACCOUNTS OF CHEMICAL RESEARCH, 2017, 50 (04) :769-777
[10]   Preparation and Cross-Linking of All-Acrylamide Diblock Copolymer Nano-Objects via Polymerization-Induced Self-Assembly in Aqueous Solution [J].
Byard, Sarah J. ;
Williams, Mark ;
McKenzie, Beulah E. ;
Blanazs, Adam ;
Armes, Steven P. .
MACROMOLECULES, 2017, 50 (04) :1482-1493