Journal
SCIENCE
Volume 368, Issue 6496, Pages 1247-+Publisher
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.abb3962
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Funding
- Northwestern University
- NIH [R01GM128037, 1S10OD012016-01]
- Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF) [ECCS-1542205]
- State of Illinois
- International Institute for Nanotechnology (IIN)
- SHyNE Resource (NSF) [ECCS-1542205]
- MRSEC program at the Materials Research Center, IIN [NSF DMR-1720139]
- Keck Foundation
- State of Illinois through IIN
- National Cancer Institute award [CCSG-P30-CA060553]
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Mechanically interlocked molecules are likely candidates for the design and synthesis of artificial molecular machines. Although polyrotaxanes have already found niche applications in exotic materials with specialized mechanical properties, efficient synthetic protocols to produce them with precise numbers of rings encircling their polymer dumbbells are still lacking. We report the assembly line-like emergence of poly[n]rotaxanes with increasingly higher energies by harnessing artificial molecular pumps to deliver rings in pairs by cyclical redox-driven processes. This programmable strategy leads to the precise incorporation of two, four, six, eight, and 10 rings carrying 8+, 16+, 24+, 32+, and 40+ charges, respectively, onto hexacationic polymer dumbbells. This strategy depends precisely on the number of redox cycles applied chemically or electrochemically, in both stepwise and one-pot manners.
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