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Title: Poly[n]catenanes: Synthesis of molecular interlocked chains

Abstract

As the macromolecular version of mechanically interlocked molecules, mechanically interlocked polymers are promising candidates for the creation of sophisticated molecular machines and smart soft materials. Poly[n]catenanes, where the molecular chains consist solely of interlocked macrocycles, contain one of the highest concentrations of topological bonds. We report, herein, a synthetic approach toward this distinctive polymer architecture in high yield (similar to 75%) via efficient ring closing of rationally designed metallosupramolecular polymers. Light-scattering, mass spectrometric, and nuclear magnetic resonance characterization of fractionated samples support assignment of the high-molar mass product (number-average molar mass similar to 21.4 kilograms per mole) to a mixture of linear poly[7-26]catenanes, branched poly[13-130]catenanes, and cyclic poly[4-7]catenanes. As a result, increased hydrodynamic radius (in solution) and glass transition temperature (in bulk materials) were observed upon metallation with Zn2+.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [3];  [4]; ORCiD logo [3]; ORCiD logo [5]
+ Show Author Affiliations
  1. Univ. of Chicago, Chicago, IL (United States); Case Western Reserve Univ., Cleveland, OH (United States)
  2. Univ. of Chicago, Chicago, IL (United States)
  3. Case Western Reserve Univ., Cleveland, OH (United States)
  4. Univ. of Chicago, Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
  5. Univ. of Chicago, Chicago, IL (United States); Case Western Reserve Univ., Cleveland, OH (United States); Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
National Science Foundation (NSF); USDOE
OSTI Identifier:
1425221
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Science
Additional Journal Information:
Journal Volume: 358; Journal Issue: 6369; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Wu, Qiong, Rauscher, Phillip M., Lang, Xiaolong, Wojtecki, Rudy J., de Pablo, Juan J., Hore, Michael J. A., and Rowan, Stuart J. Poly[n]catenanes: Synthesis of molecular interlocked chains. United States: N. p., 2017. Web. doi:10.1126/science.aap7675.
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Wu, Qiong, Rauscher, Phillip M., Lang, Xiaolong, Wojtecki, Rudy J., de Pablo, Juan J., Hore, Michael J. A., & Rowan, Stuart J. Poly[n]catenanes: Synthesis of molecular interlocked chains. United States. doi:10.1126/science.aap7675.
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Wu, Qiong, Rauscher, Phillip M., Lang, Xiaolong, Wojtecki, Rudy J., de Pablo, Juan J., Hore, Michael J. A., and Rowan, Stuart J. Fri . "Poly[n]catenanes: Synthesis of molecular interlocked chains". United States. doi:10.1126/science.aap7675. https://www.osti.gov/servlets/purl/1425221.
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@article{osti_1425221,
title = {Poly[n]catenanes: Synthesis of molecular interlocked chains},
author = {Wu, Qiong and Rauscher, Phillip M. and Lang, Xiaolong and Wojtecki, Rudy J. and de Pablo, Juan J. and Hore, Michael J. A. and Rowan, Stuart J.},
abstractNote = {As the macromolecular version of mechanically interlocked molecules, mechanically interlocked polymers are promising candidates for the creation of sophisticated molecular machines and smart soft materials. Poly[n]catenanes, where the molecular chains consist solely of interlocked macrocycles, contain one of the highest concentrations of topological bonds. We report, herein, a synthetic approach toward this distinctive polymer architecture in high yield (similar to 75%) via efficient ring closing of rationally designed metallosupramolecular polymers. Light-scattering, mass spectrometric, and nuclear magnetic resonance characterization of fractionated samples support assignment of the high-molar mass product (number-average molar mass similar to 21.4 kilograms per mole) to a mixture of linear poly[7-26]catenanes, branched poly[13-130]catenanes, and cyclic poly[4-7]catenanes. As a result, increased hydrodynamic radius (in solution) and glass transition temperature (in bulk materials) were observed upon metallation with Zn2+.},
doi = {10.1126/science.aap7675},
journal = {Science},
number = 6369,
volume = 358,
place = {United States},
year = {2017},
month = {12}
}
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Journal Article:
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DOI:  10.1126/science.aap7675
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Cited by: 63 works
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Figures / Tables:

Fig. 1 Fig. 1: Conformational mobility and synthetic approach to poly[n]catenane. (A) A robust and flexible metal chain, the macroscopic equivalent of the poly[n]catenane architecture; (B) the common conformational motions observed in catenanes; (C) Comparison of poly[n]catenane and poly[2]catenane; (D) the targeted synthesis of poly[n]catenane 3 via assembling 1 and 2 intomore » a metallo-supramolecular polymer (MSP) followed by ring-closing to yield poly[n]catenate (i.e. metallated poly[n]catenane) and demetallation; and (E) the structure of 1, 2 and 4 (ring-closed product of 1). A few key protons are labeled with blue capital letters in 4 and red lower-case letters in 2. The box highlights the structure of the Bip ligand moiety.« less
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    journal, January 2020

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