pH Sensing Properties of Flexible, Bias‐Free Graphene Microelectrodes in Complex Fluids: From Phosphate Buffer Solution to Human Serum

Abstract

Advances in techniques for monitoring pH in complex fluids can have a significant impact on analytical and biomedical applications. This study develops flexible graphene microelectrodes (GEs) for rapid (<5 s), very‐low‐power (femtowatt) detection of the pH of complex biofluids by measuring real‐time Faradaic charge transfer between the GE and a solution at zero electrical bias. For an idealized sample of phosphate buffer solution (PBS), the Faradaic current is varied monotonically and systematically with the pH, with a resolution of ≈0.2 pH unit. The current–pH dependence is well described by a hybrid analytical–computational model, where the electric double layer derives from an intrinsic, pH‐independent (positive) charge associated with the graphene–water interface and ionizable (negative) charged groups. For ferritin solution, the relative Faradaic current, defined as the difference between the measured current response and a baseline response due to PBS, shows a strong signal associated with ferritin disassembly and the release of ferric ions at pH ≈2.0. For samples of human serum, the Faradaic current shows a reproducible rapid (<20 s) response to pH. By combining the Faradaic current and real‐time current variation, the methodology is potentially suitable for use to detect tumor‐induced changes in extracellular pH.

Document Details

Document Type
Pub Defense Publication
Publication Date
Jun 14, 2017
Source ID
10.1002/smll.201700564

Entities

People

  • Alan T. Charlie Johnson
  • Amey Vrudhula
  • Carl H. Naylor
  • Jacquelyn E. Blum
  • Jeffery G Saven
  • Jinglei Ping
  • Ramya Vishnubhotla
  • Zhaoli Gao

Organizations

  • Army Research Office
  • Defense Advanced Research Projects Agency
  • National Institute of Environmental Health Sciences
  • National Science Foundation
  • University of Pennsylvania

Tags

Readers

  • Electrochemical Surface Science
  • Molecular and Cellular Biochemistry
  • Nanoscale Plasmonic Nanotechnology

Technology Areas

  • Biotechnology
  • Microelectronics