Self-Assembled Homopolymeric Spherulites from Small Molecules in Solution
Polymeric spherulites are typically formed by melt crystallization: spherulitic growth in solution is rare and requires complex polymers and dilute solutions. Here, we report the mild and unique formation of luminescent spherulites at room temperature via the simple molecule benzene-1,4-dithiol (BDT). Specifically, BDT polymerized into oligomers (PBDT) via disulfide bonds and assembled into uniform supramolecular nanoparticles in aqueous buffer; these nanoparticles were then dissolved back into PBDT in a good solvent (i.e., dimethylformamide) and underwent chain elongation to form spherulites (rPBDT) in 10 min. The spherulite geometry was modulated by changing the PBDT concentration and reaction time. Due to the step-growth polymerization and reorganization of PBDT, these spherulites not only exhibited robust structure but also showed broad clusterization-triggered emission. The biocompatibility and efficient cellular uptake of the spherulites further underscore their value as traceable drug carriers. This system provides a new pathway for designing versatile superstructures with value for hierarchical assembly of small molecules into a complicated biological system.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2023 |
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| Erschienen: |
2023 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:145 |
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| Enthalten in: |
Journal of the American Chemical Society - 145(2023), 47 vom: 29. Nov., Seite 25664-25672 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Song, Qiantao [VerfasserIn] |
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| Links: |
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| Themen: |
Journal Article |
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| Anmerkungen: |
Date Completed 30.11.2023 Date Revised 14.02.2024 published: Print-Electronic Citation Status MEDLINE |
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| doi: |
10.1021/jacs.3c08356 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| 500 | |a Citation Status MEDLINE | ||
| 520 | |a Polymeric spherulites are typically formed by melt crystallization: spherulitic growth in solution is rare and requires complex polymers and dilute solutions. Here, we report the mild and unique formation of luminescent spherulites at room temperature via the simple molecule benzene-1,4-dithiol (BDT). Specifically, BDT polymerized into oligomers (PBDT) via disulfide bonds and assembled into uniform supramolecular nanoparticles in aqueous buffer; these nanoparticles were then dissolved back into PBDT in a good solvent (i.e., dimethylformamide) and underwent chain elongation to form spherulites (rPBDT) in 10 min. The spherulite geometry was modulated by changing the PBDT concentration and reaction time. Due to the step-growth polymerization and reorganization of PBDT, these spherulites not only exhibited robust structure but also showed broad clusterization-triggered emission. The biocompatibility and efficient cellular uptake of the spherulites further underscore their value as traceable drug carriers. This system provides a new pathway for designing versatile superstructures with value for hierarchical assembly of small molecules into a complicated biological system | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a Research Support, U.S. Gov't, Non-P.H.S. | |
| 650 | 4 | |a Research Support, N.I.H., Extramural | |
| 650 | 7 | |a Polymers |2 NLM | |
| 700 | 1 | |a Li, Yi |e verfasserin |4 aut | |
| 700 | 1 | |a Jin, Zhicheng |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Hai |e verfasserin |4 aut | |
| 700 | 1 | |a Creyer, Matthew N |e verfasserin |4 aut | |
| 700 | 1 | |a Yim, Wonjun |e verfasserin |4 aut | |
| 700 | 1 | |a Huang, Yanping |e verfasserin |4 aut | |
| 700 | 1 | |a Hu, Xiaobing |e verfasserin |4 aut | |
| 700 | 1 | |a He, Tengyu |e verfasserin |4 aut | |
| 700 | 1 | |a Li, Yajuan |e verfasserin |4 aut | |
| 700 | 1 | |a Kelley, Shana O |e verfasserin |4 aut | |
| 700 | 1 | |a Shi, Lingyan |e verfasserin |4 aut | |
| 700 | 1 | |a Zhou, Jiajing |e verfasserin |4 aut | |
| 700 | 1 | |a Jokerst, Jesse V |e verfasserin |4 aut | |
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