Solution Structure and Scaling Laws of Cylindrical and Tapered Bottlebrush Polymers

Alaboalirat, Mohammed; Scannelli, Samantha J.; Rahmaninejad, Hadi; Carrillo, Jan-Michael; Do, Changwoo; Matson, John B.; Ashkar, Rana

doi:10.1021/acs.macromol.3c01412

Title: Solution Structure and Scaling Laws of Cylindrical and Tapered Bottlebrush Polymers

Journal Article · Thu Nov 09 00:00:00 EST 2023 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.3c01412· OSTI ID:2217703

Alaboalirat, Mohammed ^[1]; Scannelli, Samantha J. ^[1]; Rahmaninejad, Hadi ^[1];

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Virginia Tech, Blacksburg, VA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Bottlebrush polymers are a unique class of macromolecular architectures with a plethora of potential industrial and pharmaceutical applications that critically depend on the bottlebrush shape and dimensions. Here, a systematic series of 12 cylindrical and 12 cone-shaped (tapered) bottlebrush polymers with poly(tert-butyl acrylate) (PtBA) or polystyrene (PS) side chains were synthesized using the sequential addition of macromonomers ring-opening metathesis polymerization (SAM-ROMP) grafting-through method. Small-angle neutron scattering (SANS) studies on dilute solutions of the two types of bottlebrush polymers provided noninvasive characterization of their structural dimensions and chain conformations. Simulated SANS traces, generated using coarse-grained molecular dynamics simulations, reproduced the distinctive features observed in the experimental SANS signals and provided necessary validation for data modeling. The combined analysis of experimental and simulated SANS signals yielded key structural and conformational parameters, including the bottlebrush radius, length, and Kuhn length as well as the excluded volume parameter and the correlation length of the polymer side chains. Importantly, the obtained structural parameters followed well-defined scaling laws as a function of the backbone and side chain degrees of polymerization, as predicted by mean field theories. In conclusion, these findings provide clear experimental and computational evidence of the interdependence of structural and conformational properties in an important class of polymer architectures.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); US Army Research Office (ARO); U.S.-Israel Binational Science Foundation (BSF); National Science Foundation (NSF)

Grant/Contract Number:: AC05-00OR22725; W911NF-19-1-0331; DMR-2104602; DMR-0520547

OSTI ID:: 2217703

Journal Information:: Macromolecules, Vol. 56, Issue 22; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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36 MATERIALS SCIENCE
Comb polymers
atom-transfer radical polymerization
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small-angle neutron scattering
molecular dynamics simulations
structure-property relations

Title: Solution Structure and Scaling Laws of Cylindrical and Tapered Bottlebrush Polymers

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