Highly Cross-Linked, Physiologically Responsive, Mechanically Adaptive Polymer Networks Made by Photopolymerization

[Image: see text] Mechanically adaptive materials that soften upon exposure to physiological conditions are useful for biomedical applications, notably as substrates for implantable neural electrodes. So far, device fabrication efforts have largely relied on shaping such devices by laser cutting, but this process makes it difficult to produce complex electrode architectures and leads to ill-defined surface chemistries. Here, we report mechanically adaptive, physiologically responsive polymers that can be photopolymerized and thus patterned via soft lithography and photolithography. The adaptive polymer networks produced exhibit, in optimized compositions, a ca. 500-fold decrease of their storage modulus when exposed to simulated physiological conditions, for example, from 2.5 GPa to 5 MPa. This effect is caused by modest swelling (30% w/w), which in turn leads to plasticization so that the polymer network’s glass transition temperature is reduced from 145 to 25 °C. The polymer networks can further be rendered pH-responsive by the incorporation of methacrylic acid. The dual stimuli-responsive materials thus made show promise as coatings or substrates for drug delivery devices.