Mechanoradicals Created in “Polymeric Sponges” Drive Reactions in Aqueous Media

Baytekin, H. Tarık; Baytekin, Bilge; Grzybowski, Bartosz A.

doi:10.1002/anie.201108110

Cited by 87 publications

(102 citation statements)

References 37 publications

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“…(Figure 1a), but as stated in the Introduction, Baytekin and Grzybowski showed that hydrogen peroxide formed when polymer materials were compressed. 33 Hydrogen peroxide can be converted to hydroxyl radical using iron(II) salts via the Fenton reaction. Having determined that 100 μM FeCl 2 could activate APF in the presence of hydrogen peroxide without sacrificing significant fluorescein emission ( Figure S2), 10 wt % disulfide gels loaded with either APF or fluorescein were compressed to 30% strain and then incubated with 100 μM FeCl 2 .…”

Section: Chemistry Of Materialsmentioning

confidence: 99%

Mechanochemical Reaction Cascade for Sensitive Detection of Covalent Bond Breakage in Hydrogels

Fitch

Goodwin

2014

Chem. Mater.

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A novel strategy is reported for sensing chemical bond breakage in hydrogels at low levels of mechanical stress using a mechanochemical reaction cascade to generate fluorescence. Hydrogels are promising substrates and frameworks for cell growth and tissue engineering, particularly for cardiovascular repair and cartilage replacement. For these applications, it is important to maintain careful control over gel mechanical properties so that these hydrogels not only match the properties of the desired tissue for replacement but also retain their integrity for extended periods. Since the failure of hydrogels begins with the breakage of cross-links within the structure, methods are needed to sense these initial events for monitoring the performance of implants. In this work, it was hypothesized that nonspecific covalent bond breakage would produce radicals that would react with water to produce reactive oxygen species, which in turn could activate fluorophores sensitive to these. A series of multiarm poly(ethylene glycol) hydrogels were synthesized with a variety of cross-links of different bond dissociation energies. It was found that gels loaded with the masked fluorophore 3′-(p-aminophenyl) fluorescein became fluorescent during compression, even with as little as 5 kPa of pressure. The effect of compression on fluorescence activation was found to depend primarily on the strength of the cross-linking functional group. Future studies include utilizing this system to image mechanical variability in heterogeneous gel structures.

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Section: Chemistry Of Materialsmentioning

confidence: 99%

Mechanochemical Reaction Cascade for Sensitive Detection of Covalent Bond Breakage in Hydrogels

Fitch

Goodwin

2014

Chem. Mater.

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“…We propose such a connection between LP formation and the above mentioned “tracking” can be made by coupling a mechanical input to the reaction–diffusion process. It has been already shown that mechanical input is used to initiate and affect chemical reactions (referred to as mechanochemistry), chemically functionalize surfaces, and sometimes even alter conventional (thermal or photo) reaction pathways . In material science, there are also applications of macroscopic mechanical inputs, such as prestraining (printing on a stretched substrate), that have been used for transformation of 2D structures into 3D objects.…”

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confidence: 99%

Mechanical Control of Periodic Precipitation in Stretchable Gels to Retrieve Information on Elastic Deformation and for the Complex Patterning of Matter

et al. 2020

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Material design using nonequilibrium systems provides straightforward access to complexity levels that are possible through dynamic processes. Pattern formation through nonequilibrium processes and reaction–diffusion can be used to achieve this goal. Liesegang patterns (LPs) are a kind of periodic precipitation patterns formed through reaction–diffusion. So far, it has been shown that the periodic band structure of LPs and the geometry of the pattern can be controlled by experimental conditions and external fields (e.g., electrical or magnetic). However, there are no examples of these systems being used to retrieve information about the changes in the environment as they form, and there are no studies making use of these patterns for complex material preparation. This work shows the formation of LPs by a diffusion–precipitation reaction in a stretchable hydrogel and the control of the obtained patterns by the unprecedented and uncommon method of mechanical input. Additionally, how to use this protocol and how deviations from “LP behavior” of the patterns can be used to “write and store” information about the time, duration, extent, and direction of gel deformation are presented. Finally, an example of using complex patterning to deposit polypyrrole by using precipitation patterns is shown as a template.

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“…In 2012, Baytekin and co-workers [87] found some polymers, such as poly(dimethylsiloxane) (PDMS), tygon and PVC could create radicals by mechanical force, with concomitant H 2 O 2 as product. Polymer/water interface was proved essential for the mechanical energy conversion, where H 2 O 2 was generated when the water-filled hollow polymer tubes were squeezed manually.…”

Section: Cascade Mechanoluminescen Cementioning

confidence: 99%

Recent advances in mechanoluminescent polymers

Yuan

Chen

2016

Sci. China Mater.

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In recent years, mechanoluminescence from polymers is emerging as a new cutting-edge area of polymer mechanochemistry research. It refers to the release of energy from polymers in the form of light when they are under various mechanical stimuli. To spur more researchers to join in such interesting and new burgeoning area, and promote its development to practical applications, in this review, we try to briefly summarize the recent advances in mechanoluminescent polymers with the aspects of non-covalent, covalent, and cascade reactions systems. We pay much attention on the applications of such polymer systems in molecular level failure and stress sensors, and give a perspective of their potential applications in novel energy conversion materials and devices, as well as self-healing materials.

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Mechanoradicals Created in “Polymeric Sponges” Drive Reactions in Aqueous Media

Cited by 87 publications

References 37 publications

Mechanochemical Reaction Cascade for Sensitive Detection of Covalent Bond Breakage in Hydrogels

Mechanochemical Reaction Cascade for Sensitive Detection of Covalent Bond Breakage in Hydrogels

Mechanical Control of Periodic Precipitation in Stretchable Gels to Retrieve Information on Elastic Deformation and for the Complex Patterning of Matter

Recent advances in mechanoluminescent polymers

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