Accelerated Local Dynamics in Matrix-Free Polymer Grafted Nanoparticles

Jhalaria, Mayank; Buenning, Eileen; Huang, Yucheng; Tyagi, Madhusudan; Zorn, Reiner; Zamponi, Michaela; García-Sakai, Victoria; Jestin, Jacques; Benicewicz, Brian C.; Kumar, Sanat K.

doi:10.1103/physrevlett.123.158003

Cited by 31 publications

(42 citation statements)

References 38 publications

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“…Therefore, QENS provides valuable insights into understanding relaxation processes in various PNCs systems. [6,[18][19][20][21] In P2VP/SiO 2 , our previous measurements showed that the spatial dependence of the segmental relaxation time was comparable between bulk and PNCs, implying spatially similar relaxations, despite the slower average relaxation rate. [11] Beyond the primary α-process, polymer segments can exhibit secondary relaxation such as the β-process attributed to nondiffusive relaxations or reorientations of segments or pendant groups in monomers.…”

Section: Introductionmentioning

confidence: 87%

“…[1][2][3] For example, the addition of NPs to a polymer matrix can improve the mechanical properties of glassy and melt polymers [4,5] and enhance small molecule transport. [6,7] However, the microscopic origin of many of these altered macroscopic properties remains mechanistically unknown. In the specific case of mechanical and transport properties, segmental dynamics often underlie and dictate these properties in the melt.…”

Section: Introductionmentioning

confidence: 99%

“…Therefore, QENS provides valuable insights into understanding relaxation processes in various PNCs systems. [ 6,18–21 ] In P2VP/SiO 2 , our previous measurements showed that the spatial dependence of the segmental relaxation time was comparable between bulk and PNCs, implying spatially similar relaxations, despite the slower average relaxation rate. [ 11 ]…”

Section: Introductionmentioning

confidence: 99%

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Correlation between backbone and pyridine dynamics in poly(2‐vinyl pyridine)/silica polymer nanocomposites

Bailey

Tyagi

Winey

2020

Journal of Polymer Science

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Polymer segmental dynamics in polymer nanocomposites (PNCs) can be significantly perturbed from bulk and underlie macroscopic mechanical and transport properties, but fundamental studies are necessary to build correlations between dynamics and properties. To elucidate a mechanistic description of this perturbation and isolate different molecular motions, we present quasielastic neutron scattering (QENS) measurements on PNCs with attractive interactions comprised of colloidal silica nanoparticles (NPs) uniformly dispersed in poly(2-vinyl pyridine) (P2VP) with and without backbone deuteration. Measurements of fully-protonated P2VP probe the dynamics of both the polymer backbone and pyridine pendant group; whereas measurements of backbone-deuterated P2VP isolate the dynamics of only the pyridine ring. On the small length scales ($1 nm) and fast time scales ($1 ns) captured by QENS, we show that the backbone and pyridine ring dynamics are highly coupled at high temperatures and both are slowed by about 35% relative to neat polymer in 25 vol% PNCs. This observation implies that the backbone and pendant interfacial dynamics are perturbed similarly in PNCs, which further develops our fundamental understanding of microscopic properties in PNCs.

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Section: Introductionmentioning

confidence: 87%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Correlation between backbone and pyridine dynamics in poly(2‐vinyl pyridine)/silica polymer nanocomposites

Bailey

Tyagi

Winey

2020

Journal of Polymer Science

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“…尽管关于纳米颗粒对聚合物纳米复合物体系的玻璃化相变温度、黏性、弹性和力学增强的影响的实验研究越来越多 [29][30][31][32][33] , 然而, 由于在聚合物纳米复合物的微观行为和宏观性能之间缺乏确定的关系, 功能特定的聚合物纳米复合材料的生产和商业化的发展存在很大的障碍. 另一个困难是需要涉及的参数空间规模巨大, 使得单纯通过实验进行筛选变得十分昂贵, 但未来可以通过模拟帮助缩小在实验室中可能探索的参数范围 [34][35][36][37][38][39][40][41][42] . 仅进行实验研究很难阐明在与纳米颗粒和聚合物线团的大小相比拟的小尺度上纳米颗粒和聚合物基质之间的相互作用机理, 从而由此得出纳米尺度填料对相应的聚合物纳米复合材料微观行为和宏观性能的影响 [43][44][45][46][47][48] [46] .…”

Section: 聚合物纳米复合材料与聚合物网络unclassified

“…然而, 该类仿生凝胶材料的应用目前仍受到其自愈合进展缓慢的限制 [26,34] . 最近, 实验研究表明纳米颗粒对聚合物链的吸附能够被用来实现不同高分子链之间的强、快 030008-4 https://engine.scichina.com/doi/10.1360/SSPMA-2020-0427 速黏附, 以增强增多高分子链之间的非共价物理交联 [27,37]…”

Section: 聚合物纳米复合材料与聚合物网络unclassified

From polymer configuration and dynamics to protein folding

Cao¹,

Chen²,

Wu³

2021

Sci. Sin.-Phys. Mech. Astron.

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Polymer Nanocomposites

Alkhodairi

Bilchak

Chan

et al. 2022

Macromolecular Engineering

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There has been significant interest in polymer nanocomposites (PNCs) because of their promising property enhancements – however, achieving these improvements are contingent on controlling the nanoparticle (NP) dispersion state in the polymer matrix. The inherent incompatibility between a hydrophilic filler and a hydrophobic polymer is the ultimate barrier for obtaining controlled NP spatial dispersion. We can mediate this unfavorable interaction by incorporating moieties on the chains that interact favorably with the NP surface, but preparation strategies typically used to prepare nanocomposites, e.g., casting from a common solvent or melt blending, frequently result in (far) out‐of‐equilibrium NP dispersion states with the degree of non‐equilibrium character sensitively dependent on the particular preparation technique employed. This is due to the energy landscape of even a simple PNC material being very highly complex with many local equilibria and large barriers. Most theoretical studies and our current understanding are based on the assumption that an equilibrium description of the nanocomposite applies, i.e., the system attains its global minimum state. However, different preparation conditions can place the system in different local basins and the extremely slow relaxation times of these systems to go from the “as cast” state to the equilibrium state imply that nanocomposites can end up in out‐of‐equilibrium conditions, including states where properties might be favorable. These points, which are elaborated in this review, speak to the importance of preparation and annealing conditions in the NP dispersion state and hence the properties of this novel class of materials. This topic is the focus of this chapter.

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Accelerated Local Dynamics in Matrix-Free Polymer Grafted Nanoparticles

Abstract: This is a copy of the published version, or version of record, available on the publisher's website. This version does not track changes, errata, or withdrawals on the publisher's site.

Cited by 31 publications

References 38 publications

Correlation between backbone and pyridine dynamics in poly(2‐vinyl pyridine)/silica polymer nanocomposites

Correlation between backbone and pyridine dynamics in poly(2‐vinyl pyridine)/silica polymer nanocomposites

From polymer configuration and dynamics to protein folding

Polymer Nanocomposites

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