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Title: Sequence-Mandated, Distinct Assembly of Giant Molecules

Abstract

Although controlling the primary structure of synthetic polymers is itself a great challenge, the potential of sequence control for tailoring hierarchical structures remains to be exploited, especially in the creation of new and unconventional phases. A series of model amphiphilic chain-like giant molecules was designed and synthesized by interconnecting both hydrophobic and hydrophilic molecular nanoparticles in precisely defined sequence and composition to investigate their sequence-dependent phase structures. Not only compositional variation changed the self-assembled supramolecular phases, but also specific sequences induce unconventional phase formation, including Frank-Kasper phases. The formation mechanism was attributed to the conformational change driven by the collective hydrogen bonding and the sequence-mandated topology of the molecules. Lastly, these results show that sequence control in synthetic polymers can have a dramatic impact on polymer properties and self-assembly.

Authors:
 [1];  [1];  [2];  [1];  [1];  [1];  [1];  [1];  [3];  [4];  [5];  [6];  [1]
  1. Univ. of Akron, OH (United States). Dept. of Polymer Science, College of Polymer Science and Polymer Engineering
  2. Univ. of Akron, OH (United States). Dept. of Chemistry
  3. Univ. of Akron, OH (United States). Dept. of Polymer Science, College of Polymer Science and Polymer Engineering, and Dept. of Chemistry
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS), X-ray Science Division; Northern Illinois Univ., DeKalb, IL (United States). Dept. of Chemistry and Biochemistry
  5. Peking Univ., Beijing (China). Key Lab. of Polymer Chemistry and Physics of the Ministry of Education, College of Chemistry and Molecular Engineering, Center for Soft Matter Science and Engineering
  6. Sichuan Univ., Chengdu (China). College of Polymer Science and Engineering, State Key Lab. of Polymer Materials Engineering
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Science Foundation (NSF); National Natural Science Foundation of China (NNSFC)
OSTI Identifier:
1432999
Alternate Identifier(s):
OSTI ID: 1408927
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 56; Journal Issue: 47; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Frank-Kasper phase; POSS; polymer; sequence; supramolecular structure; polyhedral oligomeric silsesquioxane

Citation Formats

Zhang, Wei, Lu, Xinlin, Mao, Jialin, Hsu, Chih-Hao, Mu, Gaoyan, Huang, Mingjun, Guo, Qingyun, Liu, Hao, Wesdemiotis, Chrys, Li, Tao, Zhang, Wen-Bin, Li, Yiwen, and Cheng, Stephen Z.D. Sequence-Mandated, Distinct Assembly of Giant Molecules. United States: N. p., 2017. Web. doi:10.1002/anie.201709354.
Zhang, Wei, Lu, Xinlin, Mao, Jialin, Hsu, Chih-Hao, Mu, Gaoyan, Huang, Mingjun, Guo, Qingyun, Liu, Hao, Wesdemiotis, Chrys, Li, Tao, Zhang, Wen-Bin, Li, Yiwen, & Cheng, Stephen Z.D. Sequence-Mandated, Distinct Assembly of Giant Molecules. United States. doi:10.1002/anie.201709354.
Zhang, Wei, Lu, Xinlin, Mao, Jialin, Hsu, Chih-Hao, Mu, Gaoyan, Huang, Mingjun, Guo, Qingyun, Liu, Hao, Wesdemiotis, Chrys, Li, Tao, Zhang, Wen-Bin, Li, Yiwen, and Cheng, Stephen Z.D. Tue . "Sequence-Mandated, Distinct Assembly of Giant Molecules". United States. doi:10.1002/anie.201709354. https://www.osti.gov/servlets/purl/1432999.
@article{osti_1432999,
title = {Sequence-Mandated, Distinct Assembly of Giant Molecules},
author = {Zhang, Wei and Lu, Xinlin and Mao, Jialin and Hsu, Chih-Hao and Mu, Gaoyan and Huang, Mingjun and Guo, Qingyun and Liu, Hao and Wesdemiotis, Chrys and Li, Tao and Zhang, Wen-Bin and Li, Yiwen and Cheng, Stephen Z.D.},
abstractNote = {Although controlling the primary structure of synthetic polymers is itself a great challenge, the potential of sequence control for tailoring hierarchical structures remains to be exploited, especially in the creation of new and unconventional phases. A series of model amphiphilic chain-like giant molecules was designed and synthesized by interconnecting both hydrophobic and hydrophilic molecular nanoparticles in precisely defined sequence and composition to investigate their sequence-dependent phase structures. Not only compositional variation changed the self-assembled supramolecular phases, but also specific sequences induce unconventional phase formation, including Frank-Kasper phases. The formation mechanism was attributed to the conformational change driven by the collective hydrogen bonding and the sequence-mandated topology of the molecules. Lastly, these results show that sequence control in synthetic polymers can have a dramatic impact on polymer properties and self-assembly.},
doi = {10.1002/anie.201709354},
journal = {Angewandte Chemie (International Edition)},
number = 47,
volume = 56,
place = {United States},
year = {2017},
month = {10}
}

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