The versatile physicochemical properties of amphiphilic hydrogels depend on their internal morphology and water content. Their microphase separation into percolating hydrophilic and hydrophobic domains can greatly impact the transport of small and large molecules through the network, which is especially crucial for hydrogels used for wearable devices.

In this study, we simulate the interplay between concurrent demixing and crosslinking processes via a coarse-grained dissipative particle dynamics (DPD) simulation in LAMMPS, using the bond/react package. We investigate how the relative concentration and size mismatch between the hydrophobic and hydrophilic precursors affect phase separation and to what extent the demixing can be prevented by introducing amphiphilic copolymer molecules and crosslinking. Our results show, for example, how crosslinking impedes long-range lamellar structure formation, leading to more isotropic transport properties.