Three-Dimensional Printable Enzymatically Active Plastics

TY - JOUR

T1 - Three-Dimensional Printable Enzymatically Active Plastics

AU - Zhang, William H.

AU - Day, Graham J.

AU - Zampetakis, Ioannis

AU - Carrabba, Michele

AU - Zhang, Zhongyang

AU - Carter, Ben M.

AU - Govan, Norman

AU - Jackson, Colin

AU - Chen, Menglin

AU - Perriman, Adam W.

N1 - Funding Information: This research was funded by the EPSRC (EP/N026586/1) that was awarded in collaboration with the Defence Science and Technology Laboratory (DSTL). We also thank UKRI (Future Leaders Fellowship MR/S016430/1) for support of Professor Adam W. Perriman. We are grateful for the time allocation from Diamond Light Source, which allowed SR–WAXS experiments to be performed on the I22 beamline (proposal SM17972), and for SR–CD on the B23 beamline (proposal SM18006). We would like to thank J. Ede and I. Shortman from the Defence Science and Technology Laboratory (DSTL) for intellectual input and discussion, and we would finally like to thank R. O. Moreno for his assistance with the DSC experiments. Publisher Copyright: © 2021 The Authors. Published by American Chemical Society.

PY - 2021/12

Y1 - 2021/12

N2 - 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.

AB - 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.

KW - 3D printing

KW - enzyme

KW - functional bionanomaterials

KW - melt electrowriting

KW - nanocomposite

KW - nanoconjugate

KW - nanomorphology

UR - http://www.scopus.com/inward/record.url?scp=85119960363&partnerID=8YFLogxK

U2 - 10.1021/acsapm.1c00845

DO - 10.1021/acsapm.1c00845

M3 - Journal article

C2 - 35983011

AN - SCOPUS:85119960363

SN - 2637-6105

VL - 3

SP - 6070

EP - 6077

JO - ACS Applied Polymer Materials

JF - ACS Applied Polymer Materials

IS - 12

ER -