Development and understanding of antifreezing materials are fundamentally and practically important for materials design and delivery. However, almost all of antifreezing materials are either organic/icephobic materials containing no water or hydrophilic hydrogels containing antifreezing additives. Here, a general crosslinking strategy to fabricate a family of EGINA‐crosslinked double‐network hydrogels with intrinsic, built‐in antifreezing and mechanical properties, but without any antifreezing additives is proposed and demonstrated. The resultant hydrogels, despite large structural and compositional variations of hydrophilies, electrolytes, zwitterions, and macromolecules of polymer chains, achieved strong antifreezing and mechanical properties in different environments including solution state, gel state, and hydrogel/solid interfaces. Such general antifreezing property of EGINA‐crosslinked hydrogels, regardless network compositions, is likely stemmed from their highly hydrophilic and tightly crosslinked DN structures for inducing strong water–network bindings to prevent ice crystal formation from free waters in hydrogel networks. EGINA‐crosslinked hydrogels can also serve as a key component to be fabricated into smart windows with high optical transmittance and supercapacitors with excellent electrochemical stability at subzero temperatures. This work provides a simple, blueprint antifreezing design concept and a family of antifreezing hydrogels for the better understanding of the composite–structure–property relationship of antifreezing materials and the fundamentals of confined water in wet soft materials.
In this paper, we perform concurrent atomistic-continuum (CAC) simulations to: (i) characterize the internal stress induced by the microscale dislocation pileup at an atomically structured interface; (ii) decompose this stress into two parts, one of which is from the dislocations behind the pileup tip according to the Eshelby model and the other is from the dislocations at the pileup tip according to a super-dislocation model; and (iii) assess how such internal stresses contribute to the atomicscale phase transformations (PTs), reverse PTs, and twinning. The main novelty of this work is to unify the atomistic description of the interface and the coarse-grained (CG) description of the lagging dislocations away from the interface within one single framework. Our major findings are: (a) the interface dynamically responds to a pileup by forming steps/ledges, the height of which is proportional to the number of dislocations arriving at the interface; (b) the stress intensity factors are linearly proportional to the number of the dislocations in a nanoscale pileup, but upper bends to a high level when tens of dislocations are involved in a microscale pileup; (c) when the presheared sample is compressed, a direct square-to-hexagonal PT occurs ahead of the pileup tip and eventually grows into a wedge shape. The two variants of the hexagonal phases form a twin with respect to each other; (d) upon a further increase of the loading, part of the newly formed hexagonal phase transforms back to the square phase. The square product phase resulting from this reverse PT forms a twin with respect to the initial square phase. All phase boundaries (PBs) and twin boundaries (TBs) are stationary and correspond to zero thermodynamic Eshelby driving forces; and (e) the stress intensity induced by a pileup consisting of 16 dislocations reduces the stress required for initiating a PT by a factor of 5.5, comparing with that in the sample containing no dislocations. This work is a first characterization of the behavior of PTs/twinning resulting from the reaction between a microscale dislocation slip and an atomically structured interface. The gained knowledge will advance our understanding on how the multi-phase material behaves in many complex physical processes, such as the synthesis of multi-phase high-entropy alloys or superhard ceramics under high pressure torsion, deep mantle earthquakes in geophysics, and so on, which all involve dislocation slip, PTs, twinning, and their interactions across from the atomistic to the microscale and beyond.
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