[논문]Folding of Sequence-Controlled Graft Copolymers to Subdomain-Defined Single-Chain Nanoparticles

Nam, Jiyun; Kwon, Sangwoo; Yu, Yong-Guen; Seo, Ho-Bin; Lee, Jae-Suk; Lee, Won Bo; Kim, YongJoo; Seo, Myungeun

doi:10.1021/acs.macromol.1c01674

[해외논문] Folding of Sequence-Controlled Graft Copolymers to Subdomain-Defined Single-Chain Nanoparticles

Macromolecules, v.54 no.18, 2021년, pp.8829 - 8838

Nam, Jiyun (Department of Chemistry , Korea Advanced Institute of Science and Technology (KAIST) , Daejeon 34141 , Republic of Korea) , Kwon, Sangwoo (School of Chemical and Biological Engineering, Institute of Chemical Processes , Seoul National University , Seoul 08826 , Republic of Korea) , Yu, Yong-Guen (School of Materials Science and Engineering , Gwangju Institute of Science and Technology , 123 Cheomdangwagi-ro, Buk-gu , Gwangju 61005 , Republic of Korea) , Seo, Ho-Bin (School of Materials Science and Engineering , Gwangju Institute of Science and Technology , 123 Cheomdangwagi-ro, Buk-gu , Gwangju 61005 , Republic of Korea) , Lee, Jae-Suk (School of Chemical and Biological Engineering, Institute of Chemical Processes , Seoul National University , Seoul 08826 , Republic of Korea) , Lee, Won Bo , Kim, YongJoo , Seo, Myungeun

Abstract ▼ AI-Helper

We developed a methodology, inspired by the folding of proteins, for the precision synthesis of hairy polymer nanoparticles. High-molar mass and narrowly dispersed graft copolymers were synthesized by graft-through ring opening metathesis polymerization, to incorporate a designated number of side chains and dimerizable cinnamic acid groups. Intrachain photodimerization collapsed the backbone and arrested it into a compact globular conformation, resulting in hairy nanoparticles topologically equivalent to a core cross-linked star polymer. The single-chain collapse process translates the molecular information written on the 1D graft copolymer into the 3D globular polymer nanoparticle, like protein folding. Unprecedented control over structural parameters was achieved, including the length, number, and composition of the side chains as well as cross-linking density. Different side chains formed distinct subdomains in the sterically congested nanoparticle state and further self-assembled into micellar aggregates in a selective solvent. Both experimental observations and computational simulations indicated that preorganization of the side chains in the block sequence produces subdomains which primarily follow the backbone length scale, while random sequences showed side chain-dependent scaling. Polymer nanoparticles with discrete multiple subdomains were produced by folding of the ternary block graft copolymers. Drastic differences in the self-assembly behavior of ABC- and ACB-sequenced nanoparticles indicate that the spatial organization of subdomains can be achieved by sequence control.[FIG OMISSION]

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