A precise polyrotaxane synthesizer

Yunyan Qiu; Bo Song; Cristian Pezzato; Dengke Shen; Wenqi Liu; Long Zhang; Yuanning Feng; Qing Hui Guo; Kang Cai; Weixingyue Li; Hongliang Chen; Minh T. Nguyen; Yi Shi; Chuyang Cheng; R. Dean Astumian; Xiaopeng Li; J. Fraser Stoddart

doi:10.1126/science.abb3962

A precise polyrotaxane synthesizer

Yunyan Qiu, Bo Song, Cristian Pezzato, Dengke Shen, Wenqi Liu, Long Zhang, Yuanning Feng, Qing Hui Guo, Kang Cai, Weixingyue Li, Hongliang Chen, Minh T. Nguyen, Yi Shi, Chuyang Cheng, R. Dean Astumian, Xiaopeng Li, J. Fraser Stoddart^*

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

164 Scopus citations

Abstract

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.

Original language	English (US)
Pages (from-to)	1247-1253
Number of pages	7
Journal	Science
Volume	368
Issue number	6496
DOIs	https://doi.org/10.1126/science.abb3962
State	Published - Jun 12 2020

Funding

We thank Y. Zhang for help with NMR measurements, A. Gaisin for help with SEC measurements, and T. Kosikova, H. Sun, X. Zhou, and W. Cao for discussions. We thank Northwestern University for its continued support of this research. B.S. and X.L. were supported by NIH grant R01GM128037. This work made use of the Integrated Molecular Structure Education and Research Center (IMSERC) at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205), the State of Illinois, and the International Institute for Nanotechnology (IIN). The Bruker 600 MHz NMR spectrometer used in this work is partially funded by NIH grant 1S10OD012016-01. This work made use of the Keck-II facility of Northwestern University's NUANCE Center, which has received support from the SHyNE Resource (NSF ECCS-1542205), the MRSEC program (NSF DMR-1720139) at the Materials Research Center, IIN, the Keck Foundation, and the State of Illinois through IIN. Use of resources of the Keck Biophysics Facility was supported in part by National Cancer Institute award CCSG-P30-CA060553 to the Robert H. Lurie Comprehensive Cancer Center at Northwestern University.

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abstract = "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.",

author = "Yunyan Qiu and Bo Song and Cristian Pezzato and Dengke Shen and Wenqi Liu and Long Zhang and Yuanning Feng and Guo, {Qing Hui} and Kang Cai and Weixingyue Li and Hongliang Chen and Nguyen, {Minh T.} and Yi Shi and Chuyang Cheng and {Dean Astumian}, R. and Xiaopeng Li and {Fraser Stoddart}, J.",

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AU - Feng, Yuanning

AU - Guo, Qing Hui

AU - Cai, Kang

AU - Li, Weixingyue

AU - Chen, Hongliang

AU - Nguyen, Minh T.

AU - Shi, Yi

AU - Cheng, Chuyang

AU - Dean Astumian, R.

AU - Li, Xiaopeng

AU - Fraser Stoddart, J.

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A precise polyrotaxane synthesizer

Abstract

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