Simple and Inexpensive Fabrication of High Surface-Area Paper-Based Gold Electrodes for Electrochemical and Surface-Enhanced Raman Scattering Sensing

Abstract

Paper has emerged as an excellent alternative to create environmentally benign disposable electrochemical sensing devices. The critical step to fabricating electrochemical sensors is making paper conductive. In this work, paper-based electrodes with a high electroactive surface area (ESA) were fabricated using a simple electroless deposition technique. The polymerization time of a polydopamine adhesion layer and the gold salt concentration during the electroless deposition step were optimized to obtain uniformly conductive paper-based electrodes. The optimization of these fabrication parameters was key to obtaining the highest ESA possible. Roughening factors (R_f) of 7.2 and 2.3 were obtained when cyclic voltammetry was done in sulfuric acid and potassium ferricyanide, respectively, demonstrating a surface prone to fast electron transfer. As a proof of concept, mercury detection was done through anodic stripping, achieving a limit of quantification (LOQ) of 0.9 ppb. By changing the metal deposition conditions, the roughness of the metalized papers could also be tuned for their use as surface-enhanced Raman scattering (SERS) sensors. Metallized papers with the highest SERS signal for thiophenol detection yielded a LOQ of 10 ppb. We anticipate that this method of fabricating nanostructured paper-based electrodes can accelerate the development of simple, cost-effective, and highly sensitive electrochemical and SERS sensing platforms.

Keywords: amperometric nanoroughening; mercury sensing; micro/nanostructured electrodes; paper-based microanalytical devices; solution-based fabrication; thermal shrinking; thiophenol detection.