Effect of Graft Molecular Weight and Density on the Mechanical Properties of Polystyrene-Grafted Cellulose Nanocrystal Films

Lettow, James H.; Yang, Han; Nealey, Paul F.; Rowan, Stuart J.

doi:10.1021/acs.macromol.1c01886

Title: Effect of Graft Molecular Weight and Density on the Mechanical Properties of Polystyrene-Grafted Cellulose Nanocrystal Films

Journal Article · Sun Nov 14 00:00:00 EST 2021 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.1c01886· OSTI ID:1968735

Lettow, James H. ^[1];

^[1];

^[2]

Univ. of Chicago, IL (United States)
Univ. of Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)

In this work, polymer-grafted nanoparticle (PGN) films were prepared from polystyrene (PS) grafted to rodlike cellulose nanocrystals (MxG-CNC-g-PS) with a controllable grafting density (0.03–0.25 chains/nm²) and molecular weight (5–60 kg/mol). These nanorod-based PGNs are solution- and melt-processible, permitting access to one-component composite films with high nanofiller loadings (with up to 55 wt %). The impact of both grafted polymer density and molecular weight on the mechanical properties of the films was investigated and related to the polymer brush conformation: concentrated polymer brush (CPB), semidilute polymer brush (SDPB), or CPB core with SDPB corona (CPB/SDPB). The rubbery regime storage modulus (above $$T_g$$) showed 2 orders of magnitude increase, maximizing at a low degree of polymerization (N) and low grafting density (σ). Fracture toughness was maximized in samples with the grafted polymer in the SDPB or CPD/SDPB (higher N and relatively low σ) regime and showed enhancement relative to PS of molecular weight similar to the graft. In line with prior computation predictions, optimizing for both rubbery modulus and fracture toughness in such nanorod-based PGN films requires the polymers in the SDPB regime and CNC loading levels (ca. 50–60 wt %) that are difficult to attain in more traditional two-component CNC composites.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: National Science Foundation (NSF); US Army Research Office (ARO); Northwestern University; The Dow Chemical Company; DuPont de Nemours, Inc.; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division

Grant/Contract Number:: AC02-06CH11357; W911NF-15-1-0190; W911NF-18-1-0287; 0960140; DMR-2011854

OSTI ID:: 1968735

Journal Information:: Macromolecules, Vol. 54, Issue 22; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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