Data from: Enhanced polymer mechanical degradation through mechanochemically unveiled lactonization

• The mechanical degradation of polymers is typically limited to a single chain scission per triggering chain stretching event, and the loss of stress transfer that results from the scission limits the extent of degradation that can be achieved. Here, we report a mechanically triggered, delayed scission strategy that allows many eventual scission events to be initiated within a single polymer chain. The strategy is demonstrated via a mechanophore with a [4.2.0]bicyclooctene (BCOE) core that leverages a mechanochemical, orbital symmetry-forbidden 4-electron disrotatory ring-opening reaction to set up a subsequent, force-free and thermodynamically favorable lactonization. Ultrasonication of a 120 kDa BCOE copolymer triggers the desired mechanical remodeling of the polymer backbone, and the resulting lactonization leads to a gradual decrease in molecular weight over the course of 9 days to a final value of 4.4 kDa, more than an order of magnitude smaller than control polymers in which the ring-opened BCOE is protected from lactonizing. The force-coupled activity of the ring-opening reaction is probed by single molecule force spectroscopy and through the use of internal standards in sonication, and the forces required for activation are far smaller than is typically required for the mechanical chain scission of conventional covalent polymers. ... [Read More]

Total Size

51 files (98.2 MB)

Data Citation

• Lin, Y., Kouznetsova, T., Chang, C., & Craig, S. (2020). Data from: Enhanced polymer mechanical degradation through mechanochemically unveiled lactonization. Duke Research Data Repository. V2 https://doi.org/10.7924/r4fq9x365

Creator

• Lin, Yangju
• Craig, Stephen
• Kouznetsova, Tatiana
• Chang, Chia-Chih

DOI

• 10.7924/r4fq9x365

Subject

• Polymer degradation
• Polymer mechanochemistry

Publication Date

• August 3, 2020

ARK

• ark:/87924/r4fq9x365

Replaces

• 10.7924/r49s1r065

Affiliation

• Chemistry

Publisher

• Duke Research Data Repository

Language

• English

Type

• Dataset

Format

• PDF
• CSV
• XLSX
• CDX
• TIF
• JPG
• TIFF
• PZFX
• TXT
• XML

Related Materials

• Lin, Y., Kouznetsova, T., Chang, C., & Craig, S. (2020). Enhanced polymer mechanical degradation through mechanochemically unveiled lactonization. Nat Commun 11, 4987.  https://doi.org/10.1038/s41467-020-18809-7

Provenance

• Version 2 adds one more data package to the SMFS subfolder, NMR data for compound 5, P4 and P5 polymers, P2 post sonication plus pTSA treatment, and COSY NMR of compound 3, and the additional "Extrusion" subfolder.

Funding Agency

• National Science Foundation

Grant Number

• CHE-1808518

Contact

• Yangju Lin: yangju.lin@duke.edu, ORCID: 0000-0001-6378-7179Stephen L. Craig; ORCID: 0000-0002-8810-0369; Email: stephen.craig@duke.edu

License

• Creative Commons CC0 1.0 Universal

Title

• Data from: Enhanced polymer mechanical degradation through mechanochemically unveiled lactonization

License

• http://creativecommons.org/publicdomain/zero/1.0/

Repository

• Duke Research Data Repository

Thumbnail	Title	Date Uploaded	Visibility	Actions
	README.txt	2020-08-03	Public	Download
	Synthesis scheme.cdx	2020-08-03	Public	Download
	SI-Enhanced polymer mechanical degradation through mechanochemically unveiled lactonization.docx	2020-08-03	Public	Download
	Gel permeation chromatography	2020-08-03	Public
	Mass spectroscopy	2020-08-03	Public
	Nuclear magnetic resonance	2020-08-03	Public
	Single molecule force spectroscopy	2020-08-03	Public
	Extrusion	2020-08-03	Public

Versions

Version	DOI	Comment	Publication Date
2	10.7924/r4fq9x365	Version 2 adds one more data package to the SMFS subfolder, NMR data for compound 5, P4 and P5 polymers, P2 post sonication plus pTSA treatment, and COSY NMR of compound 3, and the additional "Extrusion" subfolder.	2020-08-03
1	10.7924/r49s1r065		2020-04-22