Internal Microstructure Dictates Interactions of Polymer-grafted Nanoparticles in Solution

Gury, Leo; Kamble, Samruddhi; Parisi, Daniele; Zhang, Jianan; Lee, Jaejun; Abdullah, Ayesha; Matyjaszewski, Krzysztof; Bockstaller, Michael R.; Vlassopoulos, Dimitris; Fytas, George

doi:10.1021/acs.macromol.1c00907

Title: Internal Microstructure Dictates Interactions of Polymer-grafted Nanoparticles in Solution

Journal Article · 27 July 2021 · Macromolecules

DOI: https://doi.org/10.1021/acs.macromol.1c00907 · OSTI ID:1816664

Gury, Leo ^[1]; Kamble, Samruddhi ^[2]; Parisi, Daniele ^[3];

^[4]; Lee, Jaejun ^[4]; Abdullah, Ayesha ^[4];

^[5];

^[4];

^[2];

^[6]

Univ. of Crete (Greece). Inst. of Electronic Structure and Laser. FORTH; Univ. of Crete (Greece). Dept. of Materials Science and Technology; OSTI
Univ. of Crete (Greece). Inst. of Electronic Structure and Laser. FORTH
Univ. of Crete (Greece). Inst. of Electronic Structure and Laser. FORTH; Univ. of Crete (Greece). Dept. of Materials Science and Technology
Carnegie Mellon Univ., Pittsburgh, PA (United States). Dept. of Materials Science and Engineering
Carnegie Mellon Univ., Pittsburgh, PA (United States). Chemistry Dept.
Max Planck Inst. for Polymer Research, Mainz (Germany)

Understanding the effects of polymer brush architecture on particle interactions in solution is requisite to enable the development of functional materials based on self-assembled polymer-grafted nanoparticles (GNPs). Static and dynamic light scattering of polystyrene-grafted silica particle solutions in toluene reveals that the pair interaction potential, inferred from the second virial coefficient, A₂, is strongly affected by the grafting density, σ, and degree of polymerization, N, of tethered chains. In the limit of intermediate σ (~0.3 to 0.6 nm^-2) and high N, A₂ is positive and increases with N. This confirms the good solvent conditions and can be qualitatively rationalized on the basis of a pair interaction potential derived for grafted (brush) particles. In contrast, for high σ > 0.6 nm^-2 and low N, A₂ displays an unexpected reversal to negative values, thus indicating poor solvent conditions. These findings are rationalized by means of a simple analysis based on a coarse-grained brush potential, which balances the attractive core-core interactions and the excluded volume interactions imparted by the polymer grafts. The results suggest that the steric crowding of polymer ligands in dense GNP systems may fundamentally alter the interactions between brush particles in solution and highlight the crucial role of architecture (internal microstructure) on the behavior of hybrid materials. The effect of grafting density also illustrates the opportunity to tailor the physical properties of hybrid materials by altering geometry (or architecture) rather than a variation of the chemical composition.

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Sponsoring Organization:: European Research Council (ERC); US Air Force; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: SC0018784

OSTI ID:: 1816664

Journal Information:: Macromolecules, Journal Name: Macromolecules Journal Issue: 15 Vol. 54; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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