Dendronized Polymers with Ureidopyrimidinone Groups: An Efficient Strategy To Tailor Intermolecular Interactions, Rheology, and Fracture

Leon F. Scherz, Salvatore Costanzo, Qian Huang, A. Dieter Schlutter, Dimitris Vlassopoulos

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Abstract

A library of poly(methyl methacrylate)-based dendronized polymers with generation numbers g = 1-3 was prepared, which contain different degrees of dendritic substitution (0-50%) with strongly hydrogen bonding 2-ureido-4[1H]-pyrimidinone (UPy) moieties at their respective g = 1 levels. Our rheological and thermal studies demonstrate that the strong intermolecular UPy interactions are suppressed for g = 2 and essentially eliminated for g = 3. Focusing on samples with short backbone degrees of polymerization (P-n approximate to 40), the linear viscoelastic response alters from liquid-like in the absence of UPy to gel-like with ever increasing moduli as the UPy content increases. Nonlinear rheological measurements indicate a transition from ductile to brittle behavior and, in parallel, a transition from shear strain thinning to shear strain hardening. This unique behavior makes UPy-DPs promising candidates for the design of new functional materials.
Original languageEnglish
JournalMacromolecules
Volume50
Issue number13
Pages (from-to)5176-5187
Number of pages12
ISSN0024-9297
DOIs
Publication statusPublished - 2017

Cite this

Scherz, Leon F. ; Costanzo, Salvatore ; Huang, Qian ; Schlutter, A. Dieter ; Vlassopoulos, Dimitris. / Dendronized Polymers with Ureidopyrimidinone Groups : An Efficient Strategy To Tailor Intermolecular Interactions, Rheology, and Fracture. In: Macromolecules. 2017 ; Vol. 50, No. 13. pp. 5176-5187.
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abstract = "A library of poly(methyl methacrylate)-based dendronized polymers with generation numbers g = 1-3 was prepared, which contain different degrees of dendritic substitution (0-50{\%}) with strongly hydrogen bonding 2-ureido-4[1H]-pyrimidinone (UPy) moieties at their respective g = 1 levels. Our rheological and thermal studies demonstrate that the strong intermolecular UPy interactions are suppressed for g = 2 and essentially eliminated for g = 3. Focusing on samples with short backbone degrees of polymerization (P-n approximate to 40), the linear viscoelastic response alters from liquid-like in the absence of UPy to gel-like with ever increasing moduli as the UPy content increases. Nonlinear rheological measurements indicate a transition from ductile to brittle behavior and, in parallel, a transition from shear strain thinning to shear strain hardening. This unique behavior makes UPy-DPs promising candidates for the design of new functional materials.",
author = "Scherz, {Leon F.} and Salvatore Costanzo and Qian Huang and Schlutter, {A. Dieter} and Dimitris Vlassopoulos",
year = "2017",
doi = "10.1021/acs.macromol.7b00747",
language = "English",
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publisher = "American Chemical Society",
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Dendronized Polymers with Ureidopyrimidinone Groups : An Efficient Strategy To Tailor Intermolecular Interactions, Rheology, and Fracture. / Scherz, Leon F.; Costanzo, Salvatore; Huang, Qian; Schlutter, A. Dieter; Vlassopoulos, Dimitris.

In: Macromolecules, Vol. 50, No. 13, 2017, p. 5176-5187.

Research output: Contribution to journalJournal articleResearchpeer-review

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T1 - Dendronized Polymers with Ureidopyrimidinone Groups

T2 - An Efficient Strategy To Tailor Intermolecular Interactions, Rheology, and Fracture

AU - Scherz, Leon F.

AU - Costanzo, Salvatore

AU - Huang, Qian

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AU - Vlassopoulos, Dimitris

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N2 - A library of poly(methyl methacrylate)-based dendronized polymers with generation numbers g = 1-3 was prepared, which contain different degrees of dendritic substitution (0-50%) with strongly hydrogen bonding 2-ureido-4[1H]-pyrimidinone (UPy) moieties at their respective g = 1 levels. Our rheological and thermal studies demonstrate that the strong intermolecular UPy interactions are suppressed for g = 2 and essentially eliminated for g = 3. Focusing on samples with short backbone degrees of polymerization (P-n approximate to 40), the linear viscoelastic response alters from liquid-like in the absence of UPy to gel-like with ever increasing moduli as the UPy content increases. Nonlinear rheological measurements indicate a transition from ductile to brittle behavior and, in parallel, a transition from shear strain thinning to shear strain hardening. This unique behavior makes UPy-DPs promising candidates for the design of new functional materials.

AB - A library of poly(methyl methacrylate)-based dendronized polymers with generation numbers g = 1-3 was prepared, which contain different degrees of dendritic substitution (0-50%) with strongly hydrogen bonding 2-ureido-4[1H]-pyrimidinone (UPy) moieties at their respective g = 1 levels. Our rheological and thermal studies demonstrate that the strong intermolecular UPy interactions are suppressed for g = 2 and essentially eliminated for g = 3. Focusing on samples with short backbone degrees of polymerization (P-n approximate to 40), the linear viscoelastic response alters from liquid-like in the absence of UPy to gel-like with ever increasing moduli as the UPy content increases. Nonlinear rheological measurements indicate a transition from ductile to brittle behavior and, in parallel, a transition from shear strain thinning to shear strain hardening. This unique behavior makes UPy-DPs promising candidates for the design of new functional materials.

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