Linker-mediated self-assembly of mobile DNA-coated colloids

Xia, Xiuyang; Hu, Hao; Ciamarra, Massimo Pica; Ni, Ran

doi:10.1126/sciadv.aaz6921

Cited by 21 publications

(14 citation statements)

References 41 publications

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“…Similarly, at the fixed polymer length n and φp, increasing m decreases ∆S conf , which drives the formation of more crosslinking P2C bonds. Similar entropic effects in linker-mediated self-assembly were recently observed in linker-mediated DNAcoated colloids (28). In Fig.…”

Section: Significancesupporting

confidence: 84%

Entropy-controlled cross-linking in linker-mediated vitrimers

Lei

Xia

Ciamarra

et al. 2020

Proc. Natl. Acad. Sci. U.S.A.

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Recently developed linker-mediated vitrimers based on metathesis of dioxaborolanes with various commercially available polymers have shown both good processability and outstanding performance, such as mechanical, thermal, and chemical resistance, suggesting new ways of processing cross-linked polymers in industry, of which the design principle remains unknown [M. Röttger et al., Science 356, 62–65 (2017)]. Here we formulate a theoretical framework to elucidate the phase behavior of the linker-mediated vitrimers, in which entropy plays a governing role. We find that, with increasing the linker concentration, vitrimers undergo a reentrant gel–sol transition, which explains a recent experiment [S. Wu, H. Yang, S. Huang, Q. Chen, Macromolecules 53, 1180–1190 (2020)]. More intriguingly, at the low temperature limit, the linker concentration still determines the cross-linking degree of the vitrimers, which originates from the competition between the conformational entropy of polymers and the translational entropy of linkers. Our theoretical predictions agree quantitatively with computer simulations, and offer guidelines in understanding and controlling the properties of this newly developed vitrimer system.

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Section: Significancesupporting

confidence: 84%

Entropy-controlled cross-linking in linker-mediated vitrimers

Lei

Xia

Ciamarra

et al. 2020

Proc. Natl. Acad. Sci. U.S.A.

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“…S1c). This non-monotonic dependence originates from an entropic effect recently found in linker-mediated vitrimers [34,37,38]. Moreover, the position and height of f P2C can be also tuned by changing the concentration of B and D molecules, i.e., βµ B and βµ D (Fig.…”

Section: Entropy Driven Crosslinkingmentioning

confidence: 81%

Entropy driven thermo-gelling vitrimer

Xia,

Rao,

Yang

et al. 2022

Preprint

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Thermo-gelling polymers have been envisioned as promising smart biomaterials but limited to their weak mechanical and thermodynamic stabilities. Here we propose a new thermo-gelling vitrimer, which remains at a liquid state because of the addition of protector molecules preventing the crosslinking, and with increasing temperature, an entropy driven crosslinking occurs to induce the sol-gel transition. Moreover, we find that the activation barrier in the metathesis reaction of vitrimers plays an important role, and experimentally one can use catalysts to tune the activation barrier to drive the vitrimer to form an equilibrium gel at high temperature, which is not subject to any thermodynamic instability. We formulate a mean field theory to describe the entropy driven crosslinking of the vitrimer, which agrees quantitatively with computer simulations, and paves the way for design and fabrication of novel vitrimers for biomedical applications.

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“…It was interesting to find that the phase behavior becomes less dependent on the linker concentration when the asymmetry of linker grows [64]. Xia and Ni et al [67] formulated a mean-field theory to simulate the self-assembly of colloids with mobile DNA coating and free DNA linkers. They showed that the interaction between colloids mediated by DNA linker changes nonmonotonically as the concentration of linker increases, as the result of the competition between the entropies of various species in the system.…”

Section: Crystallization Of Dna-coated Colloidsmentioning

confidence: 99%

Programming Self-Assembled Materials With DNA-Coated Colloids

Zhang

Lyu

et al. 2021

Front. Phys.

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Introducing the concept of programmability paves the way for designing complex and intelligent materials, where the materials’ structural information is pre-encoded in the components that build the system. With highly tunable interactions, DNA-coated particles are promising building elements to program materials at the colloidal scale, but several grand challenges have prevented them from assembling into the desired structures and phases. In recent years, the field has seen significant progress in tackling these challenges, which has led to the realization of numerous colloidal structures and dynamics previously inaccessible, including the desirable colloidal diamond structure, that are useful for photonic and various other applications. We review this exciting progress, focusing in detail on how DNA-coated colloids can be designed to have a sophisticatedly tailored surface, shape, patches, as well as controlled kinetics, which are key factors that allow one to program in principle a limitless number of structures. We also share our view on how the field may be directed in future.

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Linker-mediated self-assembly of mobile DNA-coated colloids

Cited by 21 publications

References 41 publications

Entropy-controlled cross-linking in linker-mediated vitrimers

Entropy-controlled cross-linking in linker-mediated vitrimers

Entropy driven thermo-gelling vitrimer

Programming Self-Assembled Materials With DNA-Coated Colloids

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