Abstract
Here, we describe a facile route to the synthesis of enzymatically active highly fabricable plastics, where the enzyme is an intrinsic component of the material. This is facilitated by the formation of an electrostatically stabilized enzyme–polymer surfactant nanoconstruct, which, after lyophilization and melting, affords stable macromolecular dispersions in a wide range of organic solvents. A selection of plastics can then be co-dissolved in the dispersions, which provides a route to bespoke 3D enzyme plastic nanocomposite structures using a wide range of fabrication techniques, including melt electrowriting, casting, and piston-driven 3D printing. The resulting constructs comprising active phosphotriesterase (arPTE) readily detoxify organophosphates with persistent activity over repeated cycles and for long time periods. Moreover, we show that the protein guest molecules, such as arPTE or sfGFP, increase the compressive Young’s modulus of the plastics and that the identity of the biomolecule influences the nanomorphology and mechanical properties of the resulting materials. Overall, we demonstrate that these biologically active nanocomposite plastics are compatible with state-of-the-art 3D fabrication techniques and that the methodology could be readily applied to produce robust and on-demand smart nanomaterial structures.
Highlights
Functional bionanomaterials comprising enzymes and synthetic polymers provide an attractive opportunity to increase the diversity of chemical milieu encountered by protein-based components
Temperature-dependent synchrotron radiation wide-angle X-ray scattering (WAXS) experiments performed on the [arPTE][S+][S−] showed that the endothermic transition observed in the Differential scanning calorimetry (DSC) was commensurate with a loss of the crystalline features at qvalues of 1.34 and 1.63 Å and a midpoint melting transition temperature of approximately 33.6 °C (Figure S2)
We have demonstrated that these composite enzyme plastics have high levels of temporal activity retention and can be readily fabricated using 3D printing technologies to create micro- and macroscale structures, both with and without thermal extrusion
Summary
Functional bionanomaterials comprising enzymes and synthetic polymers provide an attractive opportunity to increase the diversity of chemical milieu encountered by protein-based components. The bioconjugates can be dehydrated to produce solvent-free liquid proteins with oxygen-binding properties,[2] hierarchically selfassembled to produce porous membranes with recyclable catalytic activity,[3−5] or partitioned into hydrophobic cell membrane domains to yield artificial membrane-binding proteins.[6−8] Significantly, the proteins in these hybrid materials are folded, biologically active, hyper-thermostable (Tm = 155 °C),[9] and have protein dynamics that closely resembled those of fully hydrated proteins.[10−12] using this approach, we developed a new self-contained enzymatic biofluid, where lipases were re-engineered to produce room temperature liquids that required no dispersion medium, could solubilize substrates, and catalyze the hydrolysis of fatty acid esters up to temperatures of 150 °C.13 Modifying enzymes such that they could be utilized in heterogeneous catalysis is an attractive prospect.
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