Network-based redox communication between abiotic interactive materials
Jinyang Li,
Zhiling Zhao,
Eunkyoung Kim,
John R. Rzasa,
Guanghui Zong,
Lai-Xi Wang,
William E. Bentley,
Gregory F. Payne
Affiliations
Jinyang Li
Fischell Department of Bioengineering, University of Maryland, College Park, MD 20742, USA; Robert E. Fischell Institute for Biomedical Devices, University of Maryland, College Park, MD 20742, USA
Zhiling Zhao
Institute for Bioscience and Biotechnology Research, University of Maryland, College Park, MD 20742, USA; Robert E. Fischell Institute for Biomedical Devices, University of Maryland, College Park, MD 20742, USA
Eunkyoung Kim
Institute for Bioscience and Biotechnology Research, University of Maryland, College Park, MD 20742, USA; Robert E. Fischell Institute for Biomedical Devices, University of Maryland, College Park, MD 20742, USA
John R. Rzasa
Fischell Department of Bioengineering, University of Maryland, College Park, MD 20742, USA; Robert E. Fischell Institute for Biomedical Devices, University of Maryland, College Park, MD 20742, USA
Guanghui Zong
Department of Chemistry and Biochemistry, University of Maryland, College Park, MD 20742, USA
Lai-Xi Wang
Department of Chemistry and Biochemistry, University of Maryland, College Park, MD 20742, USA
William E. Bentley
Fischell Department of Bioengineering, University of Maryland, College Park, MD 20742, USA; Institute for Bioscience and Biotechnology Research, University of Maryland, College Park, MD 20742, USA; Robert E. Fischell Institute for Biomedical Devices, University of Maryland, College Park, MD 20742, USA
Gregory F. Payne
Institute for Bioscience and Biotechnology Research, University of Maryland, College Park, MD 20742, USA; Robert E. Fischell Institute for Biomedical Devices, University of Maryland, College Park, MD 20742, USA; Corresponding author
Summary: Recent observations that abiotic materials can engage in redox-based interactive communication motivates the search for new redox-active materials. Here we fabricated a hydrogel from a four-armed thiolated polyethylene glycol (PEG-SH) and the bacterial metabolite, pyocyanin (PYO). We show that: (i) the PYO-PEG hydrogel is reversibly redox-active; (ii) the molecular-switching and directed electron flow within this PYO-PEG hydrogel requires both a thermodynamic driving force (i.e., potential difference) and diffusible electron carriers that serve as nodes in a redox network; (iii) this redox-switching and electron flow is controlled by the redox network’s topology; and (iv) the ability of the PYO-PEG hydrogel to “transmit” electrons to a second insoluble redox-active material (i.e., a catechol-PEG hydrogel) is context-dependent (i.e., dependent on thermodynamic driving forces and appropriate redox shuttles). These studies provide an experimental demonstration of important features of redox-communication and also suggest technological opportunities for the fabrication of interactive materials.
