Force ahead: Emerging Applications and Opportunities of Polymer Mechanochemistry

Klok, Harm‐Anton; Herrmann, Andreas; Göstl, Robert

doi:10.1021/acspolymersau.2c00029

Cited by 32 publications

(31 citation statements)

References 65 publications

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“…28,29 In the past decade, efforts have been devoted to redirecting mechanical energy (e.g., by compression, shear, or friction) to productive chemical transformations. 28−31 The science and technology utilizing the influence of mechanical actions on chemical reactions are denoted "mechanochemistry" 28,29,31 and have sparked unprecedented developments in the fields of synthesis, 29,32 drug delivery, 30,33 and self-healing materials. 34,35 Mechanochemical synthesis is often solvent-free and can allow access to products unavailable by traditional reaction pathways, since potential energy surfaces can be distorted by external forces.…”

Section: Methodsmentioning

confidence: 99%

“…Since the mechanical degradation of polymers was observed in the 1930s, mechanically induced covalent bond scission has been regarded as a degradation pathway that limits the lifetimes of soft materials at both molecular and macroscopic scales. , In the past decade, efforts have been devoted to redirecting mechanical energy (e.g., by compression, shear, or friction) to productive chemical transformations. − The science and technology utilizing the influence of mechanical actions on chemical reactions are denoted “mechanochemistry” ,, and have sparked unprecedented developments in the fields of synthesis, , drug delivery, , and self-healing materials. , Mechanochemical synthesis is often solvent-free and can allow access to products unavailable by traditional reaction pathways, since potential energy surfaces can be distorted by external forces. − Mechanophores (force-sensitive functional molecular motifs) , can be also used to transduce external force through attached polymer chains into the mechanically selective scission of weak bonds and then trigger the release of drug molecules. , Much practical interest in the force-induced degradation of polymers also arises in the field of self-healing materials and their mechanically induced fracture and/or degradation. , …”

Section: Quantum Mechanical Challenges In Soft Materialsmentioning

confidence: 99%

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Bringing Quantum Mechanics to Coarse-Grained Soft Materials Modeling

Wang

Jackson

2023

Chem. Mater.

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Fundamental knowledge gaps are endemic in our understanding of how emergent properties of soft materials are linked to the quantum mechanical (QM) world. The limitations of current QM modeling paradigms inhibit the understanding and design of classes of soft materials for which QM phenomenology is critical. At its root, these limitations derive from the seemingly innocuous premise of requiring all atomic positions to solve the molecular Schrödinger equation, which necessitates supercomputing resources to incorporate even simple QM phenomenology into small (∼nm) systems of soft materials. Here, we review emerging efforts to overcome these challenges through the development of electronic prediction models that operate at the coarse-grained resolution. We motivate the origins of this new computational paradigm, denoted electronic coarse-graining (ECG), discuss its relationship to existing molecular modeling frameworks, and describe recent successes of ECG and related models for soft materials. Importantly, we highlight the classes of soft materials where ECG models can be potentially transformative.

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Section: Methodsmentioning

confidence: 99%

Section: Quantum Mechanical Challenges In Soft Materialsmentioning

confidence: 99%

Bringing Quantum Mechanics to Coarse-Grained Soft Materials Modeling

Wang

Jackson

2023

Chem. Mater.

View full text Add to dashboard Cite

show abstract

“…by compression, shear, or friction) to productive chemical transformations. [28][29][30][31] The science and technology utilizing the influence of mechanical actions on chemical reactions is denoted "mechanochemistry", 28,29,31 and has sparked unprecedented developments in the fields of synthesis, 29,32 drug delivery, 30,33 and self-healing materials. 34,35 Mechanochemical synthesis is often solvent-free and can allow access to products unavailable by traditional reaction pathways since potential energy surfaces can be distorted by external forces.…”

Section: Managing Polymer Mechanochemistrymentioning

confidence: 99%

“…[36][37][38] On the other hand, mechanophores (force sensitive functional molecular motifs) 28,29 can be used to transduce external force through attached polymer chains into the mechanically selective scission of weak bonds, and then trigger the release of drug molecules. 30,33 Much practical interest in the force-induced degradation of polymers also arises in the field of self-healing materials and their mechanically-induced fracture and/or degradation. 34,35 To address these challenges it is vital to understand the electronic structure of mechanophores and soft materials under the influence of an external mechanical force.…”

Section: Managing Polymer Mechanochemistrymentioning

confidence: 99%

Bringing Quantum Mechanics to Coarse-Grained Soft Materials Modeling

Wang

Jackson

2022

Preprint

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Fundamental knowledge gaps are endemic in our understanding of how emergent soft materials properties are linked to the quantum mechanical (QM) world. The limitations of current QM modeling paradigms inhibit the understanding and design of soft materials classes for which QM phenomenology is critical. At its root, these limitations derive from the seemingly innocuous premise of requiring all atomic positions to solve the molecular Schrodinger equation, which necessitates supercomputing resources to incorporate even simple QM phenomenology into small (~nm) soft materials systems. Here, we review emerging efforts to overcome these challenges through the development of electronic prediction models that operate at the coarse-grained resolution. We motivate the origins of this new computational paradigm, denoted Electronic Coarse-Graining (ECG), discuss its relationship to existing molecular modeling frameworks, and describe recent successes of ECG and related models for soft materials. Importantly, we highlight the classes of soft materials where ECG models can be potentially transformative.

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“…[8][9][10][11] Mechanophores with other chemical responses to force similarly have uses in self-healing materials, synthetic chemistry, and drug delivery, to name only a few applications. [12][13][14][15][16] A significant challenge in the development of efficient mechanochemical materials, however, is that only a limited fraction of the mechanophores are typically activated when the material is deformed. 17,18 Thus, it is critical to understand, from a fundamental perspective, what features of polymer networks determine the mechanochemical responses of the materials, and how network structure can be tuned to optimize this response.…”

Section: Introductionmentioning

confidence: 99%

Effect of Polymer Composition and Morphology on Mechanochemical Activation in Nanostructured Triblock Copolymers

Huo

Arora

Kong

et al. 2022

Preprint

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The effect of composition and morphology on mechanochemical activation in nanostructured block copolymers was investigated in a series of poly(methyl methacrylate)block-poly(n-butyl acrylate)-block-poly(methyl methacrylate) (PMMA-b-PnBA-b-PMMA) triblock copolymers containing a force-responsive spiropyran unit in the center of the rubbery PnBA midblock. Triblock copolymers with identical PnBA midblocks and varying lengths of PMMA end blocks were synthesized from a spiropyran-containing macroinitiatior via atom transfer radical polymerization, yielding polymers with volume fractions of PMMA ranging from 0.21 to 0.50. Characterization by transmission electron microscopy revealed that the polymers self-assembled into spherical and cylindrical nanostructures. Simultaneous tensile tests and optical measurements revealed that mechanochemical activation is strongly correlated to the chemical composition and morphologies of the triblock copolymers. As the glassy (PMMA) block content is increased, the overall activation increases, and the onset of activation occurs at lower strain but higher stress, which agrees with predictions from our previous computational work. These results suggest that the self-assembly of nanostructured morphologies can play an important role in controlling mechanochemical activation in polymeric materials, and provide insights into how polymer composition and morphology impact molecular-scale force distributions.

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Force ahead: Emerging Applications and Opportunities of Polymer Mechanochemistry

Cited by 32 publications

References 65 publications

Bringing Quantum Mechanics to Coarse-Grained Soft Materials Modeling

Bringing Quantum Mechanics to Coarse-Grained Soft Materials Modeling

Bringing Quantum Mechanics to Coarse-Grained Soft Materials Modeling

Effect of Polymer Composition and Morphology on Mechanochemical Activation in Nanostructured Triblock Copolymers

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