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Title: Polymer ligand–induced autonomous sorting and reversible phase separation in binary particle blends

The tethering of ligands to nanoparticles has emerged as an important strategy to control interactions and organization in particle assembly structures. Here, we demonstrate that ligand interactions in mixtures of polymer-tethered nanoparticles (which are modified with distinct types of polymer chains) can impart upper or lower critical solution temperature (UCST/LCST)–type phase behavior on binary particle mixtures in analogy to the phase behavior of the corresponding linear polymer blends. Therefore, cooling (or heating) of polymer-tethered particle blends with appropriate architecture to temperatures below (or above) the UCST (or LCST) results in the organization of the individual particle constituents into monotype microdomain structures. The shape (bicontinuous or island-type) and lengthscale of particle microdomains can be tuned by variation of the composition and thermal process conditions. Thermal cycling of LCST particle brush blends through the critical temperature enables the reversible growth and dissolution of monoparticle domain structures. The ability to autonomously and reversibly organize multicomponent particle mixtures into monotype microdomain structures could enable transformative advances in the high-throughput fabrication of solid films with tailored and mutable structures and properties that play an important role in a range of nanoparticle-based material technologies.
ORCiD logo [1] ;  [2] ;  [1] ; ORCiD logo [1] ;  [3] ; ORCiD logo [4] ; ORCiD logo [4] ; ORCiD logo [1] ;  [5] ;  [1]
  1. Carnegie Mellon Univ., Pittsburgh, PA (United States). Dept. of Materials Science and Engineering
  2. Carnegie Mellon Univ., Pittsburgh, PA (United States). Dept. of Materials Science and Engineering and Dept. of Chemistry; Anhui Univ., Hefei (China). School of Chemistry and Chemical Engineering
  3. Carnegie Mellon Univ., Pittsburgh, PA (United States). Dept. of Materials Science and Engineering; Rensselaer Polytechnic Inst., Troy, NY (United States). Dept. of Materials Science and Engineering
  4. Univ. of Akron, OH (United States). Dept. of Polymer Engineering, Polymer Engineering Academic Center
  5. Carnegie Mellon Univ., Pittsburgh, PA (United States). Dept. of Chemistry
Publication Date:
Grant/Contract Number:
EE0006702; DMR-1410845; DMR-1501324; DMR-1411046; MCF-677785
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 2; Journal Issue: 12; Journal ID: ISSN 2375-2548
Research Org:
Carnegie Mellon Univ., Pittsburgh, PA (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF); China Scholarship Council
Country of Publication:
United States
36 MATERIALS SCIENCE; nanoparticle; colloid; Polymer; brush; phase separation; controlled radical polymerization; ATRP; Self-assembly; surface; Nanocomposite
OSTI Identifier: