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A backbone lever-arm effect enhances polymer mechanochemistry.

Publication ,  Journal Article
Klukovich, HM; Kouznetsova, TB; Kean, ZS; Lenhardt, JM; Craig, SL
Published in: Nature chemistry
February 2013

Mechanical forces along a polymer backbone can be used to bring about remarkable reactivity in embedded mechanically active functional groups, but little attention has been paid to how a given polymer backbone delivers that force to the reactant. Here, single-molecule force spectroscopy was used to directly quantify and compare the forces associated with the ring opening of gem-dibromo and gem-dichlorocyclopropanes affixed along the backbone of cis-polynorbornene and cis-polybutadiene. The critical force for isomerization drops by about one-third in the polynorbornene scaffold relative to polybutadiene. The root of the effect lies in more efficient chemomechanical coupling through the polynorbornene backbone, which acts as a phenomenological lever with greater mechanical advantage than polybutadiene. The experimental results are supported computationally and provide the foundation for a new strategy by which to engineer mechanochemical reactivity.

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Published In

Nature chemistry

DOI

EISSN

1755-4349

ISSN

1755-4330

Publication Date

February 2013

Volume

5

Issue

2

Start / End Page

110 / 114

Related Subject Headings

  • Spectrum Analysis
  • Plastics
  • Organic Chemistry
  • Molecular Structure
  • Mechanics
  • Elastomers
  • Computer Simulation
  • Butadienes
  • 34 Chemical sciences
  • 03 Chemical Sciences
 

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Klukovich, H. M., Kouznetsova, T. B., Kean, Z. S., Lenhardt, J. M., & Craig, S. L. (2013). A backbone lever-arm effect enhances polymer mechanochemistry. Nature Chemistry, 5(2), 110–114. https://doi.org/10.1038/nchem.1540
Klukovich, Hope M., Tatiana B. Kouznetsova, Zachary S. Kean, Jeremy M. Lenhardt, and Stephen L. Craig. “A backbone lever-arm effect enhances polymer mechanochemistry.Nature Chemistry 5, no. 2 (February 2013): 110–14. https://doi.org/10.1038/nchem.1540.
Klukovich HM, Kouznetsova TB, Kean ZS, Lenhardt JM, Craig SL. A backbone lever-arm effect enhances polymer mechanochemistry. Nature chemistry. 2013 Feb;5(2):110–4.
Klukovich, Hope M., et al. “A backbone lever-arm effect enhances polymer mechanochemistry.Nature Chemistry, vol. 5, no. 2, Feb. 2013, pp. 110–14. Epmc, doi:10.1038/nchem.1540.
Klukovich HM, Kouznetsova TB, Kean ZS, Lenhardt JM, Craig SL. A backbone lever-arm effect enhances polymer mechanochemistry. Nature chemistry. 2013 Feb;5(2):110–114.

Published In

Nature chemistry

DOI

EISSN

1755-4349

ISSN

1755-4330

Publication Date

February 2013

Volume

5

Issue

2

Start / End Page

110 / 114

Related Subject Headings

  • Spectrum Analysis
  • Plastics
  • Organic Chemistry
  • Molecular Structure
  • Mechanics
  • Elastomers
  • Computer Simulation
  • Butadienes
  • 34 Chemical sciences
  • 03 Chemical Sciences