Abstract

DNA dissolved in ionic liquid (IL) solution (1-ethyl-3-methylimidazolium chloride, [C2mim][Cl]) showed a transition to the gel phase ([DNA] >= 1% (w/v)). The gelation time was 400 s for the 1% [IL] sample which reduced to 260 s for 5% [IL] concentration. Gelation times, obtained from the viscosity and ergodicity breaking from the dynamic structure factor data, were remarkably identical to each other. Correspondingly, the gelation temperature which was similar to 60 degrees C increased to 67 degrees C with [IL] content. The small angle neutron scattering (SANS) structure factor profile revealed the presence of the following three distinct length scales: (a) mesh size, xi approximate to 3 +/- 0.5 nm for ionogels, and approximate to 0.73 +/- 0.06 nm, for sol; (b) cross-sectional radius of DNA strand, R-c approximate to 1.6 +/- 0.1 nm; and (c) the characteristic inter-cluster distance approximate to 33 +/- 5 nm. Physical conformation of the DNA-IL complexes remained close to the Gaussian coil definition. It was observed that without IL, in the sol phase, the system was completely ergodic and did not gel, while on addition of IL a sudden transition to the non-ergodic (arrested) gel phase occurred. This was due to the formation of an amorphous network of DNA-IL complexes preceding gelation. In summary, it is shown that the DNA ionogels can be prepared with a tunable gel strength (27-70 Pa) and gelation temperature (60-67 degrees C). Further, the relaxation dynamics was found to be hierarchical in IL content of the gel, revealing considerable self-organization.

Authors

Pandey, Pankaj Kumar;  Rawat, Kamla;  Aswal, V. K.;  Kohlbrechere, J.;  Bohidar, H. B.

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