Structure of swollen hollow polyelectrolyte nanogels with inhomogeneous cross-link distributionстатья
Статья опубликована в высокорейтинговом журнале
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Дата последнего поиска статьи во внешних источниках: 1 мая 2024 г.
Аннотация:Hypothesis: Recently, it has become possible to synthesize hollow polyelectrolyte nano- and microgels. The shell permeability can be controlled by external stimuli, while the cavity can serve as a storage place for guest molecules. However, there is a lack of a detailed understanding at the molecular level regarding the role of the network topology, inhomogeneities of the distribution of cross-links, and the impact of the electrostatics on the structural response of hollow microgel to external stimuli. To bridge these gaps,molecular dynamics (MD) of computer simulations are used.Experiments: Here, we propose a fresh methodology to create realistic hollow microgel particles in silico. The technique involves a gradual change in the average local length of subchains depending on the distance to the center of mass of the microgel particles resulting in the microgels with a non-uniform distribution of cross-linking species. In particular, a series of microgels with (i) a highly cross-linked inner part of the shell and gradually decreased cross-linker concentration towards the periphery, (ii) microgels with loosely cross-linked inner and outer parts, as well as (iii) microgels with a more-or-less homogeneous structure, have been created and validated. Counterions and salt ions are taken into account explicitly, and electrostatic interactions are described by the Coulomb potential.Findings: Our studies reveal a strong dependence of the microgel swelling response on the network topology. Simple redistribution of cross-links plays a significant role in the structure of the microgels, including cavity size, microgel size, fuzziness, and extension of the inner and outer parts of the microgels.